Ethanol selectively inducing the separation of single-chirality carbon nanotubes from polymer-dispersed mixture

Ethanol selectively inducing the separation of single-chirality carbon nanotubes from polymer-dispersed mixture | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Ethanol selectively inducing the separation of single-chirality carbon nanotubes from polymer-dispersed mixture Dehua Yang, Xuan Chang, Xiaoyang Yuan, Xiaofei Yang, Linhai Li, and 3 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-4431799/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract Structural separation of single-wall carbon nanotubes (SWCNTs) is crucial for high-performance SWCNT-based devices. Compared with separation methods in aqueous systems, SWCNTs separated via polymer wrapping are more conducive to being processed into uniform and well-oriented films for high-speed nanoelectronic devices. However, high-purity separation of multiple single-chirality SWCNTs in organic systems remains a challenge due to the limited chiral resolution of polymer-based methods. Herein, we develop a straightforward technique to enlarge the polymer coating differences of different SWCNT species by employing ethanol and precisely recognize the various (n, m) species by introducing undispersed SWCNTs to induce a spontaneous chiral selective reaggregation. With this technique, we obtained eight types of single-chirality SWCNTs in organic systems, including ( 6 , 5 ), ( 7 , 5 ), ( 7 , 6 ), ( 8 , 6 ), ( 8 , 7 ), ( 9 , 7 ), ( 10 , 5 ) and ( 10 , 6 ), with purities higher than 90% in five of them. Ethanol also induces the reaggregation of metallic SWCNTs, increasing the purity of large-diameter semiconducting SWCNTs. This technique makes significant progress in the polymer-based method for achieving single-chirality separation. We believe that this work promotes the SWCNT-based electronics. Physical sciences/Materials science/Nanoscale materials/Carbon nanotubes and fullerenes Physical sciences/Materials science/Nanoscale materials/Electronic properties and materials Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 1. Introduction Single-wall carbon nanotubes (SWCNTs) stand out due to their ultrahigh carrier mobility and structure-dependent optical transitions 1–3 . Recently, SWCNT-based metal-oxide-semiconductor (MOS) transistors have been scaled down to 10-nm technology nodes, outperforming silicon PMOS 4,5 and potentially enabling a thousand-fold performance boost of chips through 3D integration 6,7 . One of the cornerstones to realize SWCNTs’ potential in the post-Moore era is the uniformity of SWCNT properties. However, the as-synthesized SWCNT mixtures are composed of SWCNTs with diverse electrical and optical properties due to varying structures. In the past decade, post-synthesis processes that extract the target nanotubes from the as-synthesized SWCNT mixture have yielded high-purity semiconducting SWCNTs, supporting the researches on high-performance SWCNT transistors and integrated circuits (ICs) 4–7 . However, chirality-dependent band structures of different semiconducting (n, m) species vary considerably, resulting in marked differences in on-state current and mobility, reaching an order of magnitude 8 . Especially in large-scale logic systems, the inhomogeneity of mixed-chirality SWCNT properties becomes a major concern, as the devices downsizing 5 . To improve the performance and uniformity of SWCNT-based devices, it is crucial not only to enhance the purity of semiconducting SWCNTs but also to obtain high-purity single-chirality SWCNTs. In recent decades, chiral selective growth has made remarkable progress 9,10 , but synthesis of single-chirality SWCNTs for device applications remains a worldwide challenge. For this, multiple liquid-phase separation methods have been developed 11,12 . These methods primarily revolve around the surface coating of SWCNTs by surfactants 13–25 , DNA 26,27 or conjugated polymers 28–30 . The essence of these three categories lies in the structure-dependent surface coating of different SWCNTs by dispersants. Among these dispersants, the surfactant coatings onto SWCNT are relatively easily manipulated by varying surfactant types 13 , concentrations 14 , temperatures 15,16 , pH 17 , redox 18 and mixed surfactants 16,19–22 . These strategies enlarge the difference in surface coatings of various (n, m) species, leading to different buoyant density, hydrophilicity and interaction with gel medium for each (n, m) species. Consequently, these property differences of SWCNT-dispersant hybrids were recognized by appropriately designed methods, such as gel chromatography 14,21–23 , density gradient ultracentrifugation (DGU) 19,24 and aqueous two-phase extraction (ATPE) 18,25 . Owing to the precise tuning of surfactant coating onto SWCNTs, more than a dozen of high-purity single-chirality species has been separated 16,20,21 . Some of them even have been produced on milligram scale 16,22 . On the other hand, fluorene-, carbazoles- and thiophene-based conjugated polymers effectively wrap semiconducting SWCNTs through π–π stacking and van der Waals interactions and selectively disperse them in aromatic organic solutions such as toluene and p -xylene, providing a more straightforward separation procedure 28–30 . The polymers’ strong recognition of the electronic type of large-diameter (1.0-1.7 nm) SWCNTs grants them the potential for single-chirality separation of SWCNTs with diameters larger than 1 nm 31–33 . Moreover, compared with those dispersed in aqueous solutions, polymer-wrapped SWCNTs are easier to process into uniform and oriented thin films for transistors (TFTs) 4–7,34 , and exhibit higher process compatibility for organic electronic devices fabrication 34,35 . However, the chiral purity of SWCNTs separated in organic system is markedly lower than that of surfactant- and DNA-based methods 13–22,26,27 , which is the major drawback of polymer-based method. Therefore, achieving single-chirality is essential for polymer wrapping techniques. In the past decade, the community has explored multiple polymers for the separation of semiconducting SWCNTs and even near single-chirality species 36–39 . Strategies similar to those used in surfactant-based methods have been adopted to refine polymer wrapping, including adjusting polymer concentrations 40 , molecular weights 41 , solution temperatures 30 , acidity 42 , solvents 43 , dispersion techniques 44 and employing mixed polymers 45 , to enhance the coating differences of various species. However, compared with separation in aqueous systems, these strategies are less effective in organic systems. And, the coating differences cannot be recognized through the traditional selective dispersion processes, thus failing in single-chirality separation. Recently, intensive ultracentrifugation 29,32 , filtration 46 and ATPE 33 were combined with selective dispersion to further increase the chiral resolution of separation. This emphasizes the need to both enlarge and recognize the coating differences. Yet, multiple single-chirality species with purities above 90% have not been achieved in polymer systems. The conformation of polymers in solution, which is crucial for selectively dispersing SWCNTs, is dominated by solvent properties. A less compatible solvent for solubilizing polymer leads to a coating change on SWCNTs’ surfaces and affects the selectivity of dispersion 43 . Alcohols strongly affect the behaviors of dispersants in solutions and reduce the surface coating of SWCNTs 47,48 . Ethanol is a non-aromatic solvent. Its dielectric constant (25.3) is significantly higher than that of toluene (2.4). Employing ethanol could tune the polymer wrapping on SWCNTs by changing the solution environment, potentially enlarging the coating differences among various SWCNTs. This is supposed to facilitate spontaneous selective aggregation, increasing separation resolution. Thus, we propose enlarging the coating differences of various (n, m) species with ethanol and a simple strategy to boost the selectivity of reaggregation to recognize these differences. In this work, we report a straightforward strategy to achieve multiple high-purity single-chirality (n, m) species in different polymer systems by introducing ethanol and undispersed SWCNTs. Ethanol induced a reduction in polymer coating on the SWCNTs, resulting in spontaneous selective reaggregation over time. The undispersed SWCNTs were introduced to SWCNT dispersions to anchor the SWCNTs with relatively loose surface coating, improving the selectivity and efficiency of reaggregation. With this technique, single-chirality SWCNTs including ( 6 , 5 ), ( 7 , 5 ), ( 7 , 6 ), ( 8 , 6 ), ( 8 , 7 ), ( 9 , 7 ), ( 10 , 5 ) and ( 10 , 6 ) were successfully separated. The purities of ( 6 , 5 ), ( 7 , 5 ), ( 7 , 6 ), ( 9 , 7 ), ( 10 , 5 ) were calculated to be > 90%. Moreover, we distinctly increased the purities of large-diameter semiconducting SWCNT while narrowing the structural distribution. This technique is universal for different polymer systems and straightforward, requiring neither iterative separation in aqueous system nor additional equipment. By detecting the surface coating of ( 7 , 5 ) and ( 7 , 6 ) SWCNTs, we demonstrate that the coating differences on various (n, m) species are enlarged and tuned by ethanol. Thus, the successful single-chirality separation is ascribed to the high-resolution recognition to the ethanol-induced coating differences of various (n, m) species by undispersed SWCNTs. Our present strategy significantly improves the chiral resolution of polymer-wrapping separation method and have potential impacts on SWCNT separation in new polymer systems in the future. This work could also benefit SWCNT applications in carbon-based transistors, ICs and photoelectronics. 2. Results and Discussion Tuning the polymer wrapping for selective reaggregation HiPco SWCNTs separated by traditional method, where raw SWCNTs were dispersed with poly(9,9-dioctylfluorenyl-2,7-diyl) (PFO) in toluene, followed by centrifugation at 8500 g for 30 min to eliminate the undispersed SWCNTs. The concentration of SWCNT and polymer was 0.3 mg/ml and 1 mg/ml, respectively. To verify ethanol’s effect, different amounts of ethanol were added to the supernatants. After 48 hours of standing, these dispersions were centrifuged at 8500 g for 5 min to remove the reaggregated SWCNTs (Fig. 1 a). Upon adding ethanol, flocculent agglomerates emerged over time without noticeable polymer precipitation (Supplementary Fig. 1). The reaggregation of SWCNTs changed the concentration and structural distribution of SWCNTs in solutions (Fig. 1 b and c). Especially, the relative content of ( 7 , 6 ), ( 8 , 6 ) and ( 9 , 7 ) in SWCNT dispersions distinctly decreased, indicating the selective reaggregation of these (n, m) species. As a result, ( 7 , 5 ) and ( 8 , 7 ) SWCNTs were enriched. At the ethanol/toluene ratio of 0.02:1, variations in SWCNT concentration and chiral distribution remained relatively minor compared with the traditional method (Fig. 1 c). Each (n, m) species reaggregated, albeit with a slight increase in the relative content of ( 7 , 5 ) and ( 8 , 7 ) SWCNTs. Increasing ethanol concentration significantly enhanced selective reaggregation of ( 7 , 6 ), ( 8 , 6 ) and ( 9 , 7 ). Meanwhile, a large portion of ( 8 , 7 ) SWCNTs also reaggregated, further enriching ( 7 , 5 ) SWCNTs in the solutions. This demonstrates the high sensitivity of polymer wrappings to the ethanol concentration. Notably, without ethanol, the SWCNT reaggregation over time is subtle (Supplementary Fig. 2). Although ethanol induced selective reaggregation, single-chirality separation was not achieved by simply increasing ethanol concentration and standing time. As the ethanol was further increased to 0.12:1 (ethanol/toluene), excess ethanol excessively affected polymers’ coating on SWCNTs, resulting in intensive reaggregation and a reduction in chiral selectivity (Supplementary Fig. 1). Moreover, Supplementary Fig. 3 exhibits the varying concentrations of different SWCNTs over time. Increasing standing time indeed favor ( 7 , 5 ) enrichment over ( 8 , 7 ). However, after 48 hours, although the enrichment towards ( 7 , 5 ) still slightly increases, the rate of change is very slow. Considering that the number of SWCNT remaining in solutions decreases with standing time, it is reasonable that the decrease rate in SWCNT concentration slows down gradually. However, upon adding ethanol, the concentration decrease rate initially increases and then decreases (Supplementary Fig. 3). Meanwhile, we noticed that flocculent agglomerates formed within 3 h after adding ethanol. The separation resolution and efficiency were reduced when these agglomerates were removed (Supplementary Fig. 4). So, the enhanced reaggregation rate is ascribed to these agglomerates composing of undispersed SWCNTs. Therefore, we intentionally introduced the undispersed SWCNT (Fig. 1 d). During the sonication process, undispersed SWCNTs containing various (n, m) species exist as agglomerates in the dispersion. After centrifugation, they settle as pellet. The difficulty in individualizing these SWCNTs stems from two factors: firstly, low polymer affinity of some (n, m) species 28 . Secondly, large bundles that are difficult to detach effectively 22 . These agglomerates are expected to have loose polymer coatings, exposing SWCNT sidewalls to the dispersion medium. This configuration increases surface area for tube-tube interactions, facilitating the reaggregation process. Standing time after introducing undispersed SWCNTs is quite important, because the reaggregation process is dynamic. Four HiPco dispersions were prepared using the traditional method, and the undispersed SWCNTs were added back to them. After standing for 12 h, 24 h, 36 h and 48 h, these dispersions were centrifugated at 8500 g for 30 min. The structural distribution of SWCNTs narrowed over time (Fig. 1 e and Supplementary Fig. 5). Besides, the amount of undispersed SWCNTs affect the rate of reaggregation. However, as the amount increasing, the reaggregation rate rapidly reaches a plateau (Supplementary Fig. 6). Since there were no environmental changes in the dispersion, the selective reaggregation originated from the small differences in the interactions between different SWCNTs, rather than drastic changes in the polymer wrapping properties. Figure 1 e suggests that ( 7 , 5 ) and ( 8 , 7 ) are more stable than ( 8 , 6 ) and ( 7 , 6 ) in solutions due to denser coating. It fits well with the previous study on the (n, m)-variant surface PFO coating 40 , where the saturated coverages of PFO on ( 7 , 5 ), ( 8 , 7 ) and ( 8 , 6 ) progressively decreases. Despite the difficulty in distinguishing ( 7 , 5 ) and ( 8 , 7 ), undispersed SWCNTs contribute to recognizing the coating difference between ( 7 , 5 )/( 8 , 7 ) and ( 7 , 6 )/( 8 , 6 ). Comparing Fig. 1 c and f, the chiral selectivity induced by undispersed SWCNTs differed from that observed with ethanol addition. Specifically, the absorbance of ( 8 , 7 ) maintained approximately 2-fold higher than that of ( 7 , 5 ) over time. It implies that although the selective reaggregation shown in Fig. 1 b partially originates from the agglomerates, the role of ethanol differs from undispersed SWCNTs in selective reaggregation. And, their combination may lead to increased chiral resolution. Hence, we sonicated raw SWCNT powders in mixtures containing individualized SWCNTs and undispersed SWCNTs with polymers. Then, ethanol was added. The mixtures were allowed to stand for several hours before centrifugation to remove the undispersed SWCNTs along with the reaggregated nanotubes, as exhibited in Fig. 2 a. We investigated the process of spontaneous enhancement of chiral purity during selective reaggregation. HiPco SWCNTs were dispersed with PFO and left to stand for 0–48 h in the presence of ethanol (0.08:1) and undispersed SWCNTs, followed by centrifugation. The results are exhibited in Fig. 2 b and Supplementary Fig. 7. The chiral distribution changes over time revealed a rapid decrease in ( 7 , 6 ) content (Fig. 2 c). Despite initially being the most abundant species, ( 7 , 6 ) SWCNTs disappeared after 48 hours. Similarly, the content of ( 8 , 6 ) and ( 9 , 7 ) decreased at a slower rate and eventually disappeared. In contrast, the concentrations of ( 7 , 5 ) SWCNTs were difficultly affected by the ethanol and undispersed SWCNTs. Due to the slower concentration decrease, the relative content of ( 7 , 5 ) and ( 8 , 7 ) increased within 24 hours. Yet, the concentration of ( 8 , 7 ) decreased faster than that of ( 7 , 5 ), evidenced by the reductions of 80% and 50% respectively within 24 hours, eventually leading to a single-chirality ( 7 , 5 ) dispersion. This result clearly elucidates the stability of various SWCNTs, ranked as ( 7 , 5 ) > ( 8 , 7 ) > ( 8 , 6 )/( 9 , 7 ) > ( 7 , 6 ), in the given solution. The chiral selectivity could be finely tuned by varying ethanol concentration in the presence of undispersed SWCNTs. Adding ethanol to a SWCNT dispersion containing undispersed SWCNTs at an ethanol/toluene ratio of 0.02:1 significantly enriched ( 8 , 7 ) after standing for 48 hours, as shown in Fig. 2 d and Supplementary Fig. 7. While, as ethanol concentration further increasing to 0.08:1, the chiral selectivity shifted from ( 8 , 7 ) to ( 7 , 5 ) SWCNTs (Fig. 2 d). Obtaining two types of single-chirality SWCNTs from HiPco SWCNTs in the PFO system provides solid evidence of fine-tuning of polymer wrapping and recognition of different (n, m) species. Separation of multiple single-chirality species from different polymer systems To verify the universality of the above separation protocol, SWCNTs were separated with different polymers. The generalized process is proposed to achieve multiple single-chirality species (Fig. 2 a). Briefly, raw SWCNT powders were sonicated into mixtures containing individualized SWCNTs and undispersed SWCNTs with polymers. Then, ethanol was added, and the dispersions were allowed to stand for a duration. Eventually, the dispersions were centrifuged to eliminate the undispersed SWCNTs and reaggregated nanotubes. This simple process was applied to various polymer systems including PFO, poly[(9,9-dioctylfluorenyl-2,7-diyl)-alt-co-(6,6′-{2,2′-bipyridine})] (PFO-BPy), poly[(9,9-di-n-octylfuorenyl-2,7-diyl)-alt-(benzo-[2,1,3]thiadiazol-4,8-diyl)] (F8BT), poly[(9,9-didodecylfuorenyl-2,7-diyl)] (PFDD), and poly[9-(1-octylonoyl)-9H-carbazole-2,7-diyl] (PCz), as depicted in Supplementary Fig. 8. Compared with the traditional selective dispersion method, the present method significantly increased the purities of single-chirality SWCNTs (Fig. 3 and Supplementary Fig. 9). The separation parameters are present in the Methods section and Table S1 . Raw SWCNTs with different structural distributions were employed. The diameter distributions of CoMoCAT( 6 , 5 ), CoMoCAT( 7 , 6 ) and HiPco-SWCNTs are < 1.2 nm, featured with S 11 and S 22 absorption peaks at 850–1400 nm and 500–800 nm, respectively. Traditionally separated SWCNTs showed multiple peaks in both regions regardless of the polymer types, indicating relatively low chiral purities. Even ( 6 , 5 ) SWCNT dispersions show two peaks of undesired nanotubes (Fig. 3 a). In contrast, the resultant ( 6 , 5 ), ( 7 , 5 ), ( 7 , 6 ), ( 8 , 7 ) and ( 10 , 5 ) dispersions achieved by the present technique exhibit isolate S 11 and S 22 peaks. Plasma-SWCNTs (0.9–1.7 nm) exhibit S 22 peaks at 800–1100 nm. Due to PFO’s poor selectivity and wrapping profile for large-diameter SWCNTs (1.0-1.7 nm) 38 , a small quantity of large-diameter SWCNTs were dispersed along with ( 9 , 7 ) SWCNTs by tradition method (Fig. 3 f). With the present method, high-purity ( 9 , 7 ) was achieved by incorporating an additional step (Supplementary Figs. 10 and 11). The SWCNTs that were selectively dispersed using PFO-BPy from HiPco contained multiple (n, m) species with large chiral angles. By employing the present method, ( 8 , 6 ) and ( 10 , 6 ) were highly enriched, providing ideal starting materials for iterative separation, as shown in Fig. 3 g. Multistep rinse eliminated most of the PFO-BPy 47 , enabling the redispersion of ( 8 , 6 ) using PFO and subsequent redispersion of ( 10 , 6 ) using PFO-BPy (details in Supplementary Fig. 12). The purities of each separated (n, m) species were calculated in Supplementary Fig. 13 according to their S 11 peak areas 14,22 . The chiral purities of ( 6 , 5 ), ( 7 , 5 ), ( 7 , 6 ), ( 9 , 7 ) and ( 10 , 5 ) exceed 90%. Notably, the purity of ( 6 , 5 ) increased from 95% to approximately 99%. Moreover, the separation of ( 8 , 6 ), ( 8 , 7 ) and ( 10 , 6 ) using polymers is reported for the first time (Figs. 4 a and b). Figure 4 c highlights the significant improvement in the polymer wrapping method, making it comparable to DNA- and surfactant-based methods in terms of chiral purity. Separation of high-purity large-diameter semiconducting We also investigated the effect of ethanol on the separation purity of large-diameter SWCNTs. We introduced different amounts of ethanol to semiconducting arc-discharge SWCNT (AP-SWCNT) dispersions separated through the traditional method using PFO-BPy, and let the dispersions stand for 6 h. The concentrations of SWCNT and PFO-BPy were 0.3 mg/ml and 0.5 mg/ml, respectively. Results are shown in Fig. 5 a and Supplementary Fig. 14. For the AP-SWCNTs (1.2–1.6 nm), the absorbance in 600–800 nm and 800–1200 nm ranges corresponds to M 11 and S 22 peaks, respectively. Increasing ethanol concentration significantly decreased the M 11 peaks, indicating the enhanced semiconducting SWCNT purity. At an ethanol/toluene ratio of 0.06:1, M 11 peaks became undetectable. Further increasing the ethanol concentration to 0.08:1 led to a decrease in the absorbance in the range of 600–800 nm, reflecting a reduction in background. Compared with the small-diameter SWCNTs, large-diameter SWCNTs seem more sensitive to ethanol, evidenced by the fast reaggregation within 6 h. To quantitatively assess the semiconducting purity of large-diameter SWCNTs, \(\varphi = {\text{A}}_{\text{C}\text{N}\text{T}}/({\text{A}}_{\text{C}\text{N}\text{T}}+{\text{A}}_{\text{B}})\) was employed, where \({\text{A}}_{\text{C}\text{N}\text{T}}\) is the area of S 22 and M 11 regions enclosed by a linear baseline, and \({\text{A}}_{\text{B}}\) is the background 49,50 . Metallic tubes, amorphous carbon and bundles exhibit stronger absorption at shorter wavelengths than semiconducting SWCNTs, contributing more to the background 49,51 . Hence, an increase in the \(\varphi\) value signifies an enhancement in the purity and quality of semiconducting tubes (Fig. 5 b). We attempted to enhance the effect of ethanol through optimizing the mass ratio of SWCNT/polymer and the standing time. The results are exhibited in Fig. 5 c and Supplementary Fig. 15. The purity of semiconducting SWCNT increased with the SWCNT/polymer ratio. However, the quantity of SWCNTs remaining in the dispersion decreased faster at high SWCNT/polymer ratios, leading to a lower yield as shown in Supplementary Fig. 16. At the 0.5/0.5 SWCNT/polymer ratio, after standing for 24 h with ethanol, the intensity in the range of 600–800 nm was even lower than that in 1200–1400 nm wavelength range, suggesting a remarkably high semiconducting SWCNT purity. The \(\varphi\) value also demonstrated the high level of semiconducting SWCNT purity (Fig. 5 d). Raman spectra further confirmed the enhanced purity of semiconducting SWCNTs (Fig. 5 e). The peaks corresponding to M 11 in RBM region disappeared following ethanol addition. A decrease in the D/G ratio, suggesting fewer defects in SWCNTs, was also observed (Supplementary Fig. 17). Then, undispersed SWCNTs and ethanol were employed cooperatively. The separation results are shown in Fig. 5 f and Supplementary Fig. 18. The structural distribution is narrowed compared with that achieved by solely employing ethanol, as evidenced by the reduced S 22 peaks at 910 nm, 1007 nm and 1060 nm. However, distinct enhancement in chiral selectivity was not achieved. We noticed that the reaggregation process was significantly accelerated in the presence of undispersed SWCNTs, leading to the rapid precipitation of most of the nanotubes. It implies that the large-diameter SWCNTs are readily affected by the changes in solution environment. However, the polymers used in this work exhibit minimal molecular recognition for chirality of large-diameter SWCNTs, making it difficult to finely tune their surface coatings. Effect of ethanol on structure-dependent surface coating and mechanism of single-chirality separation In a specific polymer system, the solution environment, such as polarity, aromaticity and architecture of solvents, dominates the dispersion of SWCNTs 43 . Polymer aggregation varies in different solvents 52 . Less compatible solutions lead to polymer folding, thus affecting their wrapping on SWCNTs 43 . This results in enhanced competitive coating of polymers on different SWCNTs, which is crucial for chiral selectivity. Due to the high dielectric constants, alcohols were reported to induce a collapsed coil conformation of chains in polymers with aromatic backbone and slightly polar alkoxy side chains, and decrease the polymer solubility 54 . As a poor solvent for PFO, ethanol induces the conversion of PFO conformation from the \(\alpha\) phase to the \(\beta\) phase in solutions by promoting mesoscopic aggregation 53 . This results in the swelling of polymer wrapping on SWCNTs 54 , which could cause detachment of polymer from SWCNTs and inter-polymer aggregations. The changes in surface coating may vary among SWCNTs with different structures due to different polymer affinities. To verify the structure-dependent impacts of ethanol, we carried out X-ray photoelectron spectroscopy (XPS) on single-chirality ( 7 , 5 ) and ( 7 , 6 ) SWCNTs (Fig. 6 ). Single-chirality ( 7 , 5 ) and ( 7 , 6 ) were dispersed with PFO. After adding ethanol (0.12:1), they were deposited on silicon substrates by immersing the substrates in SWCNT dispersions. Excess PFO was washed away with an ethanol/toluene solution. For comparison, ( 7 , 5 ) and ( 7 , 6 ) SWCNT dispersions without ethanol were deposited in the same manner, and then rinsed with neat toluene. The polymer wrapping on SWCNTs cannot be eliminated by rinsing 55 . The C-C at 285 eV is derived from polymers, while the C-C (graphite) bond at 284.4 eV originates from both SWCNTs and polymers 56,57 . The peak area ratios of C-C bond and C-C (graphite) bond reflect the relative content of SWCNT and polymers. Introduction of ethanol reduced the surface coating on ( 7 , 5 ) and ( 7 , 6 ), leading to the decreased C-C/C-C (graphite) bond ratios from 0.46 to 0.33 for ( 7 , 5 ) and from 0.38 to 0.18 for ( 7 , 6 ), as shown in Fig. 6 e. After adding ethanol, the C-C/C-C (graphite) ratios of ( 7 , 5 ) and ( 7 , 6 ) decreased by 28% and 52%, respectively. The more pronounced reduction in the C-C bond representing PFO indicates that ethanol impacts the surface coating more significantly in ( 7 , 6 ). Notably, C-C bonds in XPS results may stem from contamination and residual polymers on the substrate, and may overlap with the C-H bonds in contaminants. To further confirm the reductions of polymers on ( 7 , 5 ) and ( 7 , 6 ), we removed excess polymers using vacuum filtration. Single-chirality ( 7 , 5 ) and ( 7 , 6 ) SWCNTs that were separated using PFO were divided into two groups. Ethanol was added to one of the two groups at ethanol/toluene ratio of 0.12:1, while an equal volume of toluene was added to the control group. Then, the two groups of solutions were filtered. SWCNTs on membranes extracted from the two groups were rinsed with neat toluene and ethanol/toluene (0.12:1), respectively. After removing the excess polymer, the SWCNTs were redispersed in neat toluene and characterized by optical absorption to verify the remaining polymer on SWCNT sidewalls (Fig. 6 f-h). In the absence of the excess polymers, the absorbance contributed by polymers significantly decreased, changing the solution color from green to bluish-green (Fig. 6 g and h). The peak intensity ratios of PFO (I 380 nm ) and S 11 of single-chirality ( 7 , 5 ) and ( 7 , 6 ) (I 11, (7,5) and I 11, (7,6) ) are exhibited in Fig. 6 f. Without ethanol, the I 380 nm /I 11 ratios of ( 7 , 5 ) and ( 7 , 6 ) were 2.42 and 2.06, respectively. After ethanol was employed, the I 380 nm /I 11, (7,5) decreased to 1.58, while that of ( 7 , 6 ) SWCNTs reduced to 0.90, indicating a polymer wrapping reduction for both species. The I 380 nm /I 11, (7,5) and I 380 nm /I 11, (7,6) decreases by about 35% and 56%, respectively. The degree of polymer density reduction on ( 7 , 6 ) surfaces increased to a greater extent, enlarging the coating difference between the two species. Therefore, the ( 7 , 6 ) species were easier to reaggregate. Clearly, ethanol induced detachment of polymers from SWCNTs’ surfaces, with varying effects on different (n, m) species. Those (n, m) species with relatively lower polymer affinity or unstable coating configurations tend to expose more of their surface, increasing the chance of forming bundles 58 . The (n, m) species with the well-packed coating are least affected by solution environment. Among the (n, m) species dispersed by PFO, coating structure of ( 7 , 5 ) is the most stable in ethanol/toluene solutions, likely due to the smallest wrapping angle of PFO on ( 7 , 5 ) among various species 40 , indicating a more parallel alignment of PFO backbone with the axis of SWCNTs. A linearly aligned configuration of PFO on nanotubes is more stable than helical wrapping 59 . This renders ( 7 , 5 ) SWCNTs less sensitive to the solution environment and maintains their dispersion in the presence of ethanol. Although ethanol alters the polymer wrapping on different (n, m) species, achieving single-chirality separation merely by tuning ethanol concentration is difficult (Fig. 1 b). Because selective reaggregation relying only on the tube-tube attraction of loosely coated SWCNTs to self-assemble and precipitate is low efficient. Moreover, previous works have shown that some undesired (n, m) species were dispersed in form of small bundles by polymers. However, these bundles are difficult to induce selective reaggregation, leading to a poor chiral selectivity in the rebundling process 41 . They can only be effectively eliminated via intensive ultracentrifugation and filtration, thus enhancing the chiral purity of SWCNTs remaining in the solutions 32,46 . Introducing undispersed SWCNTs significantly accelerates the reaggregation and improves the chiral selectivity (Fig. 2 c and d). The undispersed SWCNTs provide large exposed surface areas with abundant binding sites, aiding in anchoring (n, m) species with loose polymer coating. By combining undispersed SWCNTs with ethanol, the coating differences between ( 7 , 5 ) and ( 7 , 6 ) were efficiently recognized. As demonstrated in a different separation route in Supplementary Figs. 10 and 11, most of ( 7 , 6 ) disappeared from the SWCNT-PFO dispersions and emerged in the undispersed SWCNTs, leaving ( 7 , 5 ) species in the supernatant. It unambiguously demonstrates the selective anchoring of ( 7 , 6 ) to undispersed SWCNTs. Besides, the length distribution of SWCNT is minorly affected by the selective reaggregation, indicating that the chiral separation is ascribed to coating differences rather than length difference (Supplementary Fig. 19). A phase diagram showing the effect of ethanol and undispersed SWCNTs is exhibited in Fig. 7 a. The molecular recognition zone above the dashed line represents the successful differentiation of two species. In this work, single-chirality separation was achieved through two processes: (i) ethanol increases the coating differences between different (n, m) species; (ii) undispersed SWNTs greatly enhanced the resolution of separation. As for ( 7 , 5 )/( 7 , 6 ), the addition of ethanol enlarges their coating differences. The undispersed SWCNTs significantly reduced the threshold for recognizing the coating differences in a separation strategy. As ethanol concentration increasing, the coating difference increases above the dashed line, which represents the recognition capability of undispersed SWCNTs. Thus, ( 7 , 5 )/( 7 , 6 ) SWCNTs, which cannot be distinguished by selective dispersion, were separated by the present method. Compared with ( 7 , 5 )/( 7 , 6 ), to distinguish ( 7 , 5 ) and ( 8 , 7 ) is much more difficult, as evidenced in Fig. 1 . In the absence of ethanol, the coating difference between ( 7 , 5 ) and ( 8 , 7 ) is much smaller than that between ( 7 , 5 ) and ( 7 , 6 ) 40 . The ratio of ( 7 , 5 ) and ( 8 , 7 ) contents barely changes over time, indicating that they cannot be differentiated by undispersed SWCNTs (Fig. 1 f). By combining ethanol and undispersed SWCNTs, ( 7 , 5 ) and ( 8 , 7 ) were achieved at different ethanol concentrations (Fig. 2 d). At low ethanol concentrations, a small amount of ethanol does not reduce the stability of ( 8 , 7 ) and ( 7 , 5 ), yet facilitates the reaggregation of ( 7 , 6 ), ( 8 , 6 ) and ( 9 , 7 ) in the presence of undispersed SWCNTs. During the selective dispersion stage of HiPco-SWCNT, ( 8 , 7 ) predominates over ( 7 , 5 ) in the solution, and their mass ratio maintained during the subsequent reaggregation. Thus, after eliminating other undesired SWCNTs, a single-chirality ( 8 , 7 ) solution with minor ( 7 , 5 ) content was achieved (Figs. 2 d and 3 d). At high ethanol concentrations, the coating differences of ( 8 , 7 )/( 7 , 5 ) were significantly enlarged, and these differences were successfully recognized by undispersed SWCNTs, as shown in Fig. 7 a. Owing to the differentiation of enlarged coating differences between ( 7 , 5 )/( 7 , 6 ) and between ( 7 , 5 )/( 8 , 7 ), ( 7 , 5 ) SWCNTs were separated from the ( 7 , 6 )/( 8 , 7 )/( 7 , 5 ) mixtures. The selective reaggregation process is exhibited in Fig. 7 b. Initially, despite minimal coating differences, ( 7 , 5 ), ( 7 , 6 ) and ( 8 , 7 ) were dispersed and stably maintained in the solution. Then, ethanol addition reduced the density or number of polymer molecules on SWCNTs, with varying degrees of impact on different (n, m) species, granting them larger differences in surface coatings. The ethanol concentration is vital for determining the degree of surface coating reduction and the coating differences variations. Consequently, the most impacted (n, m) species, such as ( 7 , 6 ), tend to reaggregate more easily. ( 8 , 7 ) SWCNTs exposed a part of their sidewalls as the ethanol concentration increasing. The relatively stable coating configuration of ( 7 , 5 ) preserves the surface coating from impact of environmental changes. Introducing undispersed SWCNTs rapidly anchors those with looser surface coating, significantly improving the separation resolution and efficiency, resulting in the predominance of ( 7 , 5 ) in the dispersion. 3. Conclusion We developed a method to finely tune polymer wrapping and recognize the coating differences of various (n, m) species. Introducing ethanol successfully enlarges coating differences of different SWCNTs. The undispersed SWCNTs efficiently enhance the selective reaggregation. By combining ethanol and undispersed SWCNTs, eight types of high-purity single-chirality SWCNTs, including ( 6 , 5 ), ( 7 , 5 ), ( 7 , 6 ), ( 8 , 6 ) ( 8 , 7 ), ( 10 , 5 ), ( 10 , 6 ) and ( 9 , 7 ), were achieved through a simple spontaneous selective reaggregation process. The current method also yields a significant increase in semiconducting purity of large-diameter SWCNTs. We further explored the impact of ethanol and demonstrated the varying degree of surface coating reduction of ( 7 , 5 ) and ( 7 , 6 ). Undispersed SWCNTs selectively anchor SWCNTs with loose surface coatings via interaction between exposed surfaces, leaving single-chirality SWCNTs in the dispersion. We believe that the present method provides an effective pathway for increasing the separation resolution in polymer systems. Furthermore, multiple single-chirality (n, m) species achieved from organic system promote the applications of SWCNTs in the fields of nanoelectronics, optoelectronics, sensors and organic photovoltaics. Methods Materials : Raw CoMoCAT ( 6 , 5 ) (purity ≥ 95%) and CoMoCAT ( 7 , 6 ) (purity ≥ 77%) were purchased from Sigma-Aldrich. HiPco- (Fluffy Powder, Catalyst :< 35%) and Plasma-SWCNTs (RN-220) (Carbon purity 85%-90%) were purchased from Nanointegris, Inc. AP-SWCNTs (Carbon purity 60%-70%) were purchased from Carbon Solution, Inc. PFO (M w ≥ 20k) and F8BT (M n ≤ 25k, Mw/Mn ≤ 3) were purchased from Sigma-Aldrich. PFO-BPy (purity > 98%) was purchased from Konosclence. PCz (purity 95% M w 10k-100k) was purchased from Xi’an Qiyue Biotechnology co., Ltd. PFDD (M w > 50k) was purchased from Derthon Optoelectronics Materials Science Technology Co. Ethanol (> 99.7 wt%) was purchased from Sigma-Aldrich. Toluene (> 99.5 wt%) was purchased from Damao Chemical Reagent Factory. Separation of single-chirality SWCNTs : Different raw SWCNTs and polymers were used to separate different (n, m) species. The detailed information was exhibited in Table S1 . Typically, raw SWCNT materials were dispersed at the initial SWCNT concentration of 0.3 mg/ml with corresponding polymers in toluene using a 0.5-inch tip homogenizer for 2 h at 30% power in an ice-water bath. Then, different quantities of ethanol were added to the mixture of dispersion. The dispersions were allowed to stand for 3–48 h with the undispersed SWCNTs. Eventually, the dispersions were centrifuged for 30 min at 8500 g, and the upper 80% supernatants were collected as the separated SWCNT dispersions. Specifically, to achieve high-purity of ( 8 , 7 ), the polymer concentration was set to 1.3 mg/ml to increase the proportion of ( 8 , 7 ) to ( 7 , 5 ) obtained through selective dispersion (details in Supplementary Table 1). To enhance the purities of ( 7 , 6 ) and ( 9 , 7 ) SWCNTs, a different route was employed, as shown in Supplementary Fig. 10. CoMoCAT( 7 , 6 ) and Plasma-SWCNTs were used as the raw materials for separation of ( 7 , 6 ) and ( 9 , 7 ) SWCNTs respectively. After the sonication, the dispersions were centrifuged for 2 h at 26000 g to remove the undispersed CoMoCAT( 7 , 6 ) and Plasma-SWCNTs. Then undispersed AP-SWCNTs and ethanol was added to the dispersions. After standing for 3–6 hours, the dispersions were centrifuged for 30 min at 8500 g, and the supernatants were completely removed. The pellets were collected and redispersed with 0.1-mg/ml PFO toluene solutions. Again, after centrifugation for 2 h at 26000 g, the final upper 80% supernatants were collected as single-chirality ( 7 , 6 ) and ( 9 , 7 ) dispersions. Besides, single-chirality ( 7 , 6 ) can also be obtained via the procedure in Fig. 2 a when applying ethanol and undispersed SWCNTs to PFDD-dispersed CoMoCAT( 7 , 6 ). To achieve ( 8 , 6 ) and ( 10 , 6 ), 0.3-mg/ml HiPco were dispersed with PFO-BPy (0.3 mg/ml). After adding ethanol (0.04:1) and standing with undispersed SWCNTs for 24 h, the dispersion was centrifuged for 30 min at 8500 g to collect the supernatant enriched in ( 8 , 6 ) and ( 10 , 6 ). Then, the PFO-BPy in this sample was removed as much as possible by employing high-concentration ethanol (0.2:1). Subsequently, SWCNTs were redispersed with PFO to achieve ( 8 , 6 ) SWCNTs, and the undispersed fractions were redispersed with PFO-BPy to obtain ( 10 , 6 ) SWCNTs (see details in Supplementary Fig. 12). Separation of large-diameter semiconducting SWCNTs : 3, 4, and 5 mg of AP-SWCNTs were dispersed in 10 ml of toluene (≥ 99.5%) with PFO-BPy fixed at 0.5 mg/ml. The three dispersions were respectively sonicated for 2 h at 30% power in an ice-water bath using a 0.5-inch tip homogenizer (SFX550, Branson), followed by centrifugation for 30 min at 8500 g. Then, each of the three dispersions was divided into several aliquots. Then, different quantities of ethanol were added to these dispersions at the volume ratio of ethanol/toluene of 0.02:1, 0.04:1, 0.06:1, 0.08:1 and 0.12:1. After standing for 3–48 hours, these dispersions were centrifugated for 5 min at 8500 g to remove the reaggregated SWCNTs. Notably, after each centrifugation, the upper 80% supernatants were collected. To further narrow the structure distributions, the dispersed large-diameter SWCNTs were mixed with ethanol (0.08:1) without removing undispersed SWCNTs. After 48 hours, the sample was centrifuged for 30 min at 8500 g to eliminate the undispersed SWCNTs and reaggregated nanotubes. The upper 80% dispersion was collected. Characterization Optical absorption spectra were obtained using a UV-vis-NIR spectrophotometer (Lambda 950, PerkinElmer). The SWCNTs dispersed in toluene were recorded from 400 to 1400 nm. Raman spectra were measured by a confocal Raman microscope (HR Evolution, Horiba) from 100 to 2800 cm − 1 at integral time of 3s. The length of SWCNTs were characterized by a field emission scanning electron microscope (Nova NanoSEM450, FEI). X-ray photoelectron spectroscopy (ESCALAB 250Xi, ThermoFisher) was carried out in ultrahigh-vacuum conditions (base pressure of 1 × 10 − 9 mbar) using an Al Kα X-ray source (15kV, 10mA, 500 µm spot size). Declarations Acknowledgments This work was financially supported by the National Key Research and Development Program of China (grant nos. 2020YFA0714700), the National Natural Science Foundation of China (grant nos. 62274054), the Strategic Priority Research Program of Chinese Academy of Sciences (grant no. XDB33030100), the Key Research Program of Frontier Sciences, CAS (grant no. QYZDBSSW-SYS028), Hebei province Science Foundation for Distinguished Young Scholars (F2021201035), “333 project” of Hebei Province (C20221014). The Central Guidance on Local Science and Technology Development Fund Project of Hebei Province (No. 236Z4307G). Data availability The key data generated in this study are provided in the Supplementary Information. Source data are provided. References Javey A, Guo J, Wang Q, Lundstorm M, Dai H (2003) Ballistic carbon nanotube field-effect transistors. Nature 424:654–657 He X, Htoon H et al (2018) Carbon nanotubes as emerging quantum-light sources. 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ACS Nano 9:9012–9019 Additional Declarations There is NO Competing Interest. Supplementary Files SupplementaryinformationYang.docx Cite Share Download PDF Status: Posted Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-4431799","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":305636711,"identity":"587aa275-8d27-4b5a-bd3b-1bd3c6f202ff","order_by":0,"name":"Dehua Yang","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAxUlEQVRIiWNgGAWjYBACef7mA8Y/DNjs5NkbiNRiOONYQjFDBV+yYc8BYq05kGPwmeGMHGPDjQQidTA2HDDcXNhmxsw48/HGGww1NtEEtbAzNyQbz2xL42OXTiu2YDiWlttAhC3HDHjbjjEzzs4xk2BsOExYC8OBxPYfvG3/GRtuniFaSzKDMc8ZNqD3eYjUAgxkIK5gAwYy0C8JxPhFnr//g8EHcFQe3njjQ40NEQ5DAgYSCaQoh2ghVccoGAWjYBSMDAAAELdBn+JC5n4AAAAASUVORK5CYII=","orcid":"https://orcid.org/0000-0002-0567-9118","institution":"Heibei University","correspondingAuthor":true,"prefix":"","firstName":"Dehua","middleName":"","lastName":"Yang","suffix":""},{"id":305636712,"identity":"b93f6056-aed0-4232-b56e-547f46438adc","order_by":1,"name":"Xuan Chang","email":"","orcid":"","institution":"Hebei University","correspondingAuthor":false,"prefix":"","firstName":"Xuan","middleName":"","lastName":"Chang","suffix":""},{"id":305636713,"identity":"bf3232bb-ac27-454d-875b-39d890ef22fd","order_by":2,"name":"Xiaoyang Yuan","email":"","orcid":"","institution":"Hebei University","correspondingAuthor":false,"prefix":"","firstName":"Xiaoyang","middleName":"","lastName":"Yuan","suffix":""},{"id":305636714,"identity":"1526ade7-5922-45f5-9e48-88c095465664","order_by":3,"name":"Xiaofei Yang","email":"","orcid":"","institution":"Hebei University","correspondingAuthor":false,"prefix":"","firstName":"Xiaofei","middleName":"","lastName":"Yang","suffix":""},{"id":305636715,"identity":"16832b2e-bde8-4bb8-98bd-283d2bccfa88","order_by":4,"name":"Linhai Li","email":"","orcid":"https://orcid.org/0000-0003-2302-231X","institution":"Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China","correspondingAuthor":false,"prefix":"","firstName":"Linhai","middleName":"","lastName":"Li","suffix":""},{"id":305636716,"identity":"15a6844c-dcbf-49d1-a80b-48c7c9429202","order_by":5,"name":"Wei Xi","email":"","orcid":"","institution":"University of Chinese Academy of Sciences","correspondingAuthor":false,"prefix":"","firstName":"Wei","middleName":"","lastName":"Xi","suffix":""},{"id":305636717,"identity":"8b64f408-d2a0-4fdc-a9e6-e6d99fed9e56","order_by":6,"name":"Huaping Liu","email":"","orcid":"https://orcid.org/0000-0001-7017-4127","institution":"Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences","correspondingAuthor":false,"prefix":"","firstName":"Huaping","middleName":"","lastName":"Liu","suffix":""},{"id":305636718,"identity":"7b1b9c54-3571-440e-ae46-6de6dc6795bd","order_by":7,"name":"Jianhui Chen","email":"","orcid":"","institution":"Hebei University","correspondingAuthor":false,"prefix":"","firstName":"Jianhui","middleName":"","lastName":"Chen","suffix":""}],"badges":[],"createdAt":"2024-05-16 14:40:18","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-4431799/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-4431799/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":56983469,"identity":"6b42955d-c134-4f85-b27c-e97dc3eb16c2","added_by":"auto","created_at":"2024-05-23 04:25:48","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":151359,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eChiral enhancement induced by ethanol and undispersed SWCNTs.\u003c/strong\u003e a) Schematic diagram of reaggregation induced by adding ethanol. b) Normalized optical absorption spectra of the remaining SWCNTs in solutions after the addition of varying ethanol concentrations and subsequent 48-hour standing, followed by the removal of reaggregated SWCNTs. The separation results of traditional method were achieved without ethanol and standing. c) Relative contents of different (n, m) species as a function of ethanol/toluene ratio. The standing time after adding ethanol was fixed at 48 h. d) Schematic diagram of chiral resolution enhancement by employing undispersed SWCNTs. e) Normalized optical absorption spectra of SWCNTs in the solution after mixing with undispersed SWCNTs for different durations, followed by centrifugation to remove the aggregated SWCNTs. f) Variation of relative contents of different SWCNTs with standing time at fixed ethanol concentration. “Eth.” and “tol.” are abbreviation of “ethanol” and “toluene”, respectively.\u003c/p\u003e","description":"","filename":"1.png","url":"https://assets-eu.researchsquare.com/files/rs-4431799/v1/b9ce43bc36da16cc0d38164c.png"},{"id":56984020,"identity":"0ce61109-b73f-4064-98a2-761150909c8f","added_by":"auto","created_at":"2024-05-23 04:33:48","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":120553,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eSelective reaggregation through combining ethanol and undispersed SWCNTs.\u003c/strong\u003e a) Separation procedure of selective reaggregation. b) Normalized optical absorption spectra of SWCNT dispersions standing with undispersed SWCNTs in ethanol/toluene (0.08:1) for different durations. c) Variation of relative contents of each (n, m) species in SWCNT dispersions with standing times. d) Normalized optical absorption spectra of SWCNTs separated by combining ethanol and undispersed SWCNTs at different ethanol concentrations.\u003c/p\u003e","description":"","filename":"2.png","url":"https://assets-eu.researchsquare.com/files/rs-4431799/v1/b21af01f37adb4197f967d58.png"},{"id":56983470,"identity":"e77e648f-ffd9-4862-b40f-30e5e9060468","added_by":"auto","created_at":"2024-05-23 04:25:48","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":156169,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eNormalized optical spectra of separation results using the traditional method and the present method. \u003c/strong\u003ea) Separated (6, 5) SWCNTs using CoMoCAT(6, 5) and PFO-BPy. The stars in a) mark the two SWCNT peaks arising from impurity SWCNTs. b) Separation results using CoMoCAT(6, 5) in PCz system. c) Separation of (7, 6) using CoMoCAT(7, 6) in PFO system. d) (8, 7) SWCNTs separated using HiPco and PFO. e) (10, 5) separated using HiPco and F8BT. f) Separation results using Plasma and PFO. g) Separation results using HiPco and PFO-BPy. h) (8, 6) SWCNTs achieved by Iterative separation of (10, 6)/(8, 6)-enriched sample corresponding to g). i) (10, 6) SWCNTs achieved by Iterative separation of (10, 6)/(8, 6)-enriched sample corresponding to g). The black lines represent the pristine CoMoCAT(6, 5), CoMoCAT(7, 6), HiPco and Plasma SWCNTs dispersed in sodium cholate (SC) aqueous solutions.\u003c/p\u003e","description":"","filename":"3.png","url":"https://assets-eu.researchsquare.com/files/rs-4431799/v1/467381fc738324a38faa3936.png"},{"id":56983473,"identity":"eb36d387-7d77-4b6c-b226-d528dc724afc","added_by":"auto","created_at":"2024-05-23 04:25:48","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":79572,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ePurity of single-chirality SWCNTs achieved by the present method.\u003c/strong\u003e a) Normalized optical absorption spectra of separated single-chirality SWCNTs using the present method. b) Comparison of the purities of chiral separation with the previous works using polymer wrapping. c) Comparison with separation techniques in aqueous systems on the purities of chiral separation. The purities of gel chromatography, DNA wrapping and DGU are obtained from reported results in Ref.13, 16, 24, 26. Notably, ATPE also provided various single-chirality SWCNTs with high purities, but their specific calculated chiral purities were not disclosed. So, they were not displayed in this figure.\u003c/p\u003e","description":"","filename":"4.png","url":"https://assets-eu.researchsquare.com/files/rs-4431799/v1/0a0b93cd5e61252d021c5744.png"},{"id":56983474,"identity":"595dde66-decd-45c7-a718-07250ee024ab","added_by":"auto","created_at":"2024-05-23 04:25:48","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":140206,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eSeparation of large-diameter SWCNTs.\u003c/strong\u003e a) Normalized optical absorption spectra of the SWCNTs remaining in dispersions after removing the reaggregated SWCNTs under different ethanol/toluene ratios. b) Variation of \u0026nbsp;and \u0026nbsp;with ethanol content. \u0026nbsp;and \u0026nbsp;denote the peak area of SWCNT and the ratio of SWCNT peak area to background in the S\u003csub\u003e22\u003c/sub\u003e and M\u003csub\u003e11\u003c/sub\u003e region. c) Normalized optical absorption spectra of the remained SWCNTs in dispersions after removing selectively reaggregated SWCNTs under the SWCNT/polymer ratio of 0.5/0.5. The as-prepared SWCNT dispersions were allowed to stand for 0-36 h after adding ethanol (0.08:1). The insert shows the decrease in absorbance with standing time in the M\u003csub\u003e11\u003c/sub\u003e region. d) Relationship between standing time after adding ethanol and \u0026nbsp;of separated SWCNTs at different SWCNT/polymer ratios. e) RBM band of Raman spectra of SWCNT dispersions corresponding to c). The spectra were excited at a wavelength of 633 nm. For each sample, spectra were taken in 5 random positions of the SWCNT film. f) Normalized absorbance of the large-diameter SWCNTs separated by combining ethanol and undispersed SWCNTs.\u003c/p\u003e","description":"","filename":"5.png","url":"https://assets-eu.researchsquare.com/files/rs-4431799/v1/b7fd43e55dc9b078a6692e81.png"},{"id":56983472,"identity":"2fb0d4c6-5418-41ad-8662-ae48d291a51a","added_by":"auto","created_at":"2024-05-23 04:25:48","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":251843,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eVariation of SWCNT surface coating. \u003c/strong\u003eX-ray photoelectron spectra (XPS) of a) C 1s peaks of (7, 5) deposited without ethanol and b) from ethanol/toluene solution. c) C 1s peaks of (7, 6) deposited without ethanol and d) with ethanol. Note that excess polymers were washed away by solvents. e) Peak area ratios of C-C and C-C (graphite) bonds of (7, 5) and (7, 6) SWCNTs with/without ethanol. f) Absorbance peak intensity ratios of PFO (I\u003csub\u003e380 nm\u003c/sub\u003e) and S\u003csub\u003e11\u003c/sub\u003e of SWCNTs (I\u003csub\u003e11\u003c/sub\u003e) with/without ethanol. g) Optical absorption spectra of (7, 5) after removing excess polymers by vacuum filtration with/without adding ethanol. h) Optical absorption spectra of (7, 6) after removing excess polymers by vacuum filtration with/without adding ethanol. The insert photography shows the (7, 5) and (7, 6) solutions before and after removing excess PFO.\u003c/p\u003e","description":"","filename":"6.png","url":"https://assets-eu.researchsquare.com/files/rs-4431799/v1/9f79d82ce4ad398cac1c07ed.png"},{"id":56983475,"identity":"b71c572e-2c38-4792-977b-530016c82365","added_by":"auto","created_at":"2024-05-23 04:25:48","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":172772,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eDiagram of separation mechanism. \u003c/strong\u003ea) Phase diagram of single-chirality separation basing on molecular recognition. b) Schematic illustration of selective reaggregation for single-chirality separation by employing ethanol and undispersed SWCNTs.\u003c/p\u003e","description":"","filename":"7.png","url":"https://assets-eu.researchsquare.com/files/rs-4431799/v1/3a46e9212510def0060ddd95.png"},{"id":66964039,"identity":"40e55af9-c7b9-491f-94b8-bb8daaa6ea5b","added_by":"auto","created_at":"2024-10-18 13:26:56","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":1702639,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-4431799/v1/1ac3f6be-da02-4f32-9054-819ebb4cc39d.pdf"},{"id":56983476,"identity":"f81d6f33-b5a8-4b8d-b259-a2b04239a831","added_by":"auto","created_at":"2024-05-23 04:25:48","extension":"docx","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":51614525,"visible":true,"origin":"","legend":"","description":"","filename":"SupplementaryinformationYang.docx","url":"https://assets-eu.researchsquare.com/files/rs-4431799/v1/708dde1d69443e4ec45364c2.docx"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Ethanol selectively inducing the separation of single-chirality carbon nanotubes from polymer-dispersed mixture","fulltext":[{"header":"1. Introduction","content":"\u003cp\u003eSingle-wall carbon nanotubes (SWCNTs) stand out due to their ultrahigh carrier mobility and structure-dependent optical transitions\u003csup\u003e1\u0026ndash;3\u003c/sup\u003e. Recently, SWCNT-based metal-oxide-semiconductor (MOS) transistors have been scaled down to 10-nm technology nodes, outperforming silicon PMOS\u003csup\u003e4,5\u003c/sup\u003e and potentially enabling a thousand-fold performance boost of chips through 3D integration\u003csup\u003e6,7\u003c/sup\u003e. One of the cornerstones to realize SWCNTs\u0026rsquo; potential in the post-Moore era is the uniformity of SWCNT properties. However, the as-synthesized SWCNT mixtures are composed of SWCNTs with diverse electrical and optical properties due to varying structures. In the past decade, post-synthesis processes that extract the target nanotubes from the as-synthesized SWCNT mixture have yielded high-purity semiconducting SWCNTs, supporting the researches on high-performance SWCNT transistors and integrated circuits (ICs)\u003csup\u003e4\u0026ndash;7\u003c/sup\u003e. However, chirality-dependent band structures of different semiconducting (n, m) species vary considerably, resulting in marked differences in on-state current and mobility, reaching an order of magnitude\u003csup\u003e8\u003c/sup\u003e. Especially in large-scale logic systems, the inhomogeneity of mixed-chirality SWCNT properties becomes a major concern, as the devices downsizing\u003csup\u003e5\u003c/sup\u003e. To improve the performance and uniformity of SWCNT-based devices, it is crucial not only to enhance the purity of semiconducting SWCNTs but also to obtain high-purity single-chirality SWCNTs.\u003c/p\u003e \u003cp\u003eIn recent decades, chiral selective growth has made remarkable progress\u003csup\u003e9,10\u003c/sup\u003e, but synthesis of single-chirality SWCNTs for device applications remains a worldwide challenge. For this, multiple liquid-phase separation methods have been developed\u003csup\u003e11,12\u003c/sup\u003e. These methods primarily revolve around the surface coating of SWCNTs by surfactants\u003csup\u003e13\u0026ndash;25\u003c/sup\u003e, DNA\u003csup\u003e26,27\u003c/sup\u003e or conjugated polymers\u003csup\u003e28\u0026ndash;30\u003c/sup\u003e. The essence of these three categories lies in the structure-dependent surface coating of different SWCNTs by dispersants. Among these dispersants, the surfactant coatings onto SWCNT are relatively easily manipulated by varying surfactant types\u003csup\u003e13\u003c/sup\u003e, concentrations\u003csup\u003e14\u003c/sup\u003e, temperatures\u003csup\u003e15,16\u003c/sup\u003e, pH\u003csup\u003e17\u003c/sup\u003e, redox\u003csup\u003e18\u003c/sup\u003e and mixed surfactants\u003csup\u003e16,19\u0026ndash;22\u003c/sup\u003e. These strategies enlarge the difference in surface coatings of various (n, m) species, leading to different buoyant density, hydrophilicity and interaction with gel medium for each (n, m) species. Consequently, these property differences of SWCNT-dispersant hybrids were recognized by appropriately designed methods, such as gel chromatography\u003csup\u003e14,21\u0026ndash;23\u003c/sup\u003e, density gradient ultracentrifugation (DGU)\u003csup\u003e19,24\u003c/sup\u003e and aqueous two-phase extraction (ATPE)\u003csup\u003e18,25\u003c/sup\u003e. Owing to the precise tuning of surfactant coating onto SWCNTs, more than a dozen of high-purity single-chirality species has been separated\u003csup\u003e16,20,21\u003c/sup\u003e. Some of them even have been produced on milligram scale\u003csup\u003e16,22\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eOn the other hand, fluorene-, carbazoles- and thiophene-based conjugated polymers effectively wrap semiconducting SWCNTs through π\u0026ndash;π stacking and van der Waals interactions and selectively disperse them in aromatic organic solutions such as toluene and \u003cem\u003ep\u003c/em\u003e-xylene, providing a more straightforward separation procedure\u003csup\u003e28\u0026ndash;30\u003c/sup\u003e. The polymers\u0026rsquo; strong recognition of the electronic type of large-diameter (1.0-1.7 nm) SWCNTs grants them the potential for single-chirality separation of SWCNTs with diameters larger than 1 nm\u003csup\u003e31\u0026ndash;33\u003c/sup\u003e. Moreover, compared with those dispersed in aqueous solutions, polymer-wrapped SWCNTs are easier to process into uniform and oriented thin films for transistors (TFTs)\u003csup\u003e4\u0026ndash;7,34\u003c/sup\u003e, and exhibit higher process compatibility for organic electronic devices fabrication\u003csup\u003e34,35\u003c/sup\u003e. However, the chiral purity of SWCNTs separated in organic system is markedly lower than that of surfactant- and DNA-based methods\u003csup\u003e13\u0026ndash;22,26,27\u003c/sup\u003e, which is the major drawback of polymer-based method. Therefore, achieving single-chirality is essential for polymer wrapping techniques.\u003c/p\u003e \u003cp\u003eIn the past decade, the community has explored multiple polymers for the separation of semiconducting SWCNTs and even near single-chirality species\u003csup\u003e36\u0026ndash;39\u003c/sup\u003e. Strategies similar to those used in surfactant-based methods have been adopted to refine polymer wrapping, including adjusting polymer concentrations\u003csup\u003e40\u003c/sup\u003e, molecular weights\u003csup\u003e41\u003c/sup\u003e, solution temperatures\u003csup\u003e30\u003c/sup\u003e, acidity\u003csup\u003e42\u003c/sup\u003e, solvents\u003csup\u003e43\u003c/sup\u003e, dispersion techniques\u003csup\u003e44\u003c/sup\u003e and employing mixed polymers\u003csup\u003e45\u003c/sup\u003e, to enhance the coating differences of various species. However, compared with separation in aqueous systems, these strategies are less effective in organic systems. And, the coating differences cannot be recognized through the traditional selective dispersion processes, thus failing in single-chirality separation. Recently, intensive ultracentrifugation\u003csup\u003e29,32\u003c/sup\u003e, filtration\u003csup\u003e46\u003c/sup\u003e and ATPE\u003csup\u003e33\u003c/sup\u003e were combined with selective dispersion to further increase the chiral resolution of separation. This emphasizes the need to both enlarge and recognize the coating differences. Yet, multiple single-chirality species with purities above 90% have not been achieved in polymer systems.\u003c/p\u003e \u003cp\u003eThe conformation of polymers in solution, which is crucial for selectively dispersing SWCNTs, is dominated by solvent properties. A less compatible solvent for solubilizing polymer leads to a coating change on SWCNTs\u0026rsquo; surfaces and affects the selectivity of dispersion\u003csup\u003e43\u003c/sup\u003e. Alcohols strongly affect the behaviors of dispersants in solutions and reduce the surface coating of SWCNTs\u003csup\u003e47,48\u003c/sup\u003e. Ethanol is a non-aromatic solvent. Its dielectric constant (25.3) is significantly higher than that of toluene (2.4). Employing ethanol could tune the polymer wrapping on SWCNTs by changing the solution environment, potentially enlarging the coating differences among various SWCNTs. This is supposed to facilitate spontaneous selective aggregation, increasing separation resolution. Thus, we propose enlarging the coating differences of various (n, m) species with ethanol and a simple strategy to boost the selectivity of reaggregation to recognize these differences.\u003c/p\u003e \u003cp\u003eIn this work, we report a straightforward strategy to achieve multiple high-purity single-chirality (n, m) species in different polymer systems by introducing ethanol and undispersed SWCNTs. Ethanol induced a reduction in polymer coating on the SWCNTs, resulting in spontaneous selective reaggregation over time. The undispersed SWCNTs were introduced to SWCNT dispersions to anchor the SWCNTs with relatively loose surface coating, improving the selectivity and efficiency of reaggregation. With this technique, single-chirality SWCNTs including (\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e), (\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e), (\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) were successfully separated. The purities of (\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), (\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e), (\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) were calculated to be \u0026gt;\u0026thinsp;90%. Moreover, we distinctly increased the purities of large-diameter semiconducting SWCNT while narrowing the structural distribution. This technique is universal for different polymer systems and straightforward, requiring neither iterative separation in aqueous system nor additional equipment. By detecting the surface coating of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) SWCNTs, we demonstrate that the coating differences on various (n, m) species are enlarged and tuned by ethanol. Thus, the successful single-chirality separation is ascribed to the high-resolution recognition to the ethanol-induced coating differences of various (n, m) species by undispersed SWCNTs. Our present strategy significantly improves the chiral resolution of polymer-wrapping separation method and have potential impacts on SWCNT separation in new polymer systems in the future. This work could also benefit SWCNT applications in carbon-based transistors, ICs and photoelectronics.\u003c/p\u003e"},{"header":"2. Results and Discussion","content":"\u003cp\u003e \u003cb\u003eTuning the polymer wrapping for selective reaggregation\u003c/b\u003e \u003c/p\u003e \u003cp\u003eHiPco SWCNTs separated by traditional method, where raw SWCNTs were dispersed with poly(9,9-dioctylfluorenyl-2,7-diyl) (PFO) in toluene, followed by centrifugation at 8500 g for 30 min to eliminate the undispersed SWCNTs. The concentration of SWCNT and polymer was 0.3 mg/ml and 1 mg/ml, respectively. To verify ethanol\u0026rsquo;s effect, different amounts of ethanol were added to the supernatants. After 48 hours of standing, these dispersions were centrifuged at 8500 g for 5 min to remove the reaggregated SWCNTs (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ea). Upon adding ethanol, flocculent agglomerates emerged over time without noticeable polymer precipitation (Supplementary Fig.\u0026nbsp;1). The reaggregation of SWCNTs changed the concentration and structural distribution of SWCNTs in solutions (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003eb and c). Especially, the relative content of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and (\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) in SWCNT dispersions distinctly decreased, indicating the selective reaggregation of these (n, m) species. As a result, (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) SWCNTs were enriched.\u003c/p\u003e \u003cp\u003eAt the ethanol/toluene ratio of 0.02:1, variations in SWCNT concentration and chiral distribution remained relatively minor compared with the traditional method (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ec). Each (n, m) species reaggregated, albeit with a slight increase in the relative content of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) SWCNTs. Increasing ethanol concentration significantly enhanced selective reaggregation of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and (\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e). Meanwhile, a large portion of (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) SWCNTs also reaggregated, further enriching (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) SWCNTs in the solutions. This demonstrates the high sensitivity of polymer wrappings to the ethanol concentration. Notably, without ethanol, the SWCNT reaggregation over time is subtle (Supplementary Fig.\u0026nbsp;2).\u003c/p\u003e \u003cp\u003eAlthough ethanol induced selective reaggregation, single-chirality separation was not achieved by simply increasing ethanol concentration and standing time. As the ethanol was further increased to 0.12:1 (ethanol/toluene), excess ethanol excessively affected polymers\u0026rsquo; coating on SWCNTs, resulting in intensive reaggregation and a reduction in chiral selectivity (Supplementary Fig.\u0026nbsp;1). Moreover, Supplementary Fig.\u0026nbsp;3 exhibits the varying concentrations of different SWCNTs over time. Increasing standing time indeed favor (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) enrichment over (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e). However, after 48 hours, although the enrichment towards (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) still slightly increases, the rate of change is very slow.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eConsidering that the number of SWCNT remaining in solutions decreases with standing time, it is reasonable that the decrease rate in SWCNT concentration slows down gradually. However, upon adding ethanol, the concentration decrease rate initially increases and then decreases (Supplementary Fig.\u0026nbsp;3). Meanwhile, we noticed that flocculent agglomerates formed within 3 h after adding ethanol. The separation resolution and efficiency were reduced when these agglomerates were removed (Supplementary Fig.\u0026nbsp;4). So, the enhanced reaggregation rate is ascribed to these agglomerates composing of undispersed SWCNTs.\u003c/p\u003e \u003cp\u003eTherefore, we intentionally introduced the undispersed SWCNT (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ed). During the sonication process, undispersed SWCNTs containing various (n, m) species exist as agglomerates in the dispersion. After centrifugation, they settle as pellet. The difficulty in individualizing these SWCNTs stems from two factors: firstly, low polymer affinity of some (n, m) species\u003csup\u003e28\u003c/sup\u003e. Secondly, large bundles that are difficult to detach effectively\u003csup\u003e22\u003c/sup\u003e. These agglomerates are expected to have loose polymer coatings, exposing SWCNT sidewalls to the dispersion medium. This configuration increases surface area for tube-tube interactions, facilitating the reaggregation process.\u003c/p\u003e \u003cp\u003eStanding time after introducing undispersed SWCNTs is quite important, because the reaggregation process is dynamic. Four HiPco dispersions were prepared using the traditional method, and the undispersed SWCNTs were added back to them. After standing for 12 h, 24 h, 36 h and 48 h, these dispersions were centrifugated at 8500 g for 30 min. The structural distribution of SWCNTs narrowed over time (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ee and Supplementary Fig.\u0026nbsp;5). Besides, the amount of undispersed SWCNTs affect the rate of reaggregation. However, as the amount increasing, the reaggregation rate rapidly reaches a plateau (Supplementary Fig.\u0026nbsp;6).\u003c/p\u003e \u003cp\u003eSince there were no environmental changes in the dispersion, the selective reaggregation originated from the small differences in the interactions between different SWCNTs, rather than drastic changes in the polymer wrapping properties. Figure\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ee suggests that (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) are more stable than (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) in solutions due to denser coating. It fits well with the previous study on the (n, m)-variant surface PFO coating\u003csup\u003e40\u003c/sup\u003e, where the saturated coverages of PFO on (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) and (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) progressively decreases. Despite the difficulty in distinguishing (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e), undispersed SWCNTs contribute to recognizing the coating difference between (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e)/(\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e)/(\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e). Comparing Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ec and f, the chiral selectivity induced by undispersed SWCNTs differed from that observed with ethanol addition. Specifically, the absorbance of (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) maintained approximately 2-fold higher than that of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) over time. It implies that although the selective reaggregation shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003eb partially originates from the agglomerates, the role of ethanol differs from undispersed SWCNTs in selective reaggregation. And, their combination may lead to increased chiral resolution.\u003c/p\u003e \u003cp\u003eHence, we sonicated raw SWCNT powders in mixtures containing individualized SWCNTs and undispersed SWCNTs with polymers. Then, ethanol was added. The mixtures were allowed to stand for several hours before centrifugation to remove the undispersed SWCNTs along with the reaggregated nanotubes, as exhibited in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eWe investigated the process of spontaneous enhancement of chiral purity during selective reaggregation. HiPco SWCNTs were dispersed with PFO and left to stand for 0\u0026ndash;48 h in the presence of ethanol (0.08:1) and undispersed SWCNTs, followed by centrifugation. The results are exhibited in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb and Supplementary Fig.\u0026nbsp;7. The chiral distribution changes over time revealed a rapid decrease in (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) content (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec). Despite initially being the most abundant species, (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) SWCNTs disappeared after 48 hours. Similarly, the content of (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and (\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) decreased at a slower rate and eventually disappeared. In contrast, the concentrations of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) SWCNTs were difficultly affected by the ethanol and undispersed SWCNTs. Due to the slower concentration decrease, the relative content of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) increased within 24 hours. Yet, the concentration of (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) decreased faster than that of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), evidenced by the reductions of 80% and 50% respectively within 24 hours, eventually leading to a single-chirality (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) dispersion. This result clearly elucidates the stability of various SWCNTs, ranked as (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) \u0026gt; (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) \u0026gt; (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e)/(\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) \u0026gt; (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), in the given solution.\u003c/p\u003e \u003cp\u003eThe chiral selectivity could be finely tuned by varying ethanol concentration in the presence of undispersed SWCNTs. Adding ethanol to a SWCNT dispersion containing undispersed SWCNTs at an ethanol/toluene ratio of 0.02:1 significantly enriched (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) after standing for 48 hours, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed and Supplementary Fig.\u0026nbsp;7. While, as ethanol concentration further increasing to 0.08:1, the chiral selectivity shifted from (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) to (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) SWCNTs (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed). Obtaining two types of single-chirality SWCNTs from HiPco SWCNTs in the PFO system provides solid evidence of fine-tuning of polymer wrapping and recognition of different (n, m) species.\u003c/p\u003e \u003cp\u003e \u003cb\u003eSeparation of multiple single-chirality species from different polymer systems\u003c/b\u003e \u003c/p\u003e \u003cp\u003eTo verify the universality of the above separation protocol, SWCNTs were separated with different polymers. The generalized process is proposed to achieve multiple single-chirality species (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea). Briefly, raw SWCNT powders were sonicated into mixtures containing individualized SWCNTs and undispersed SWCNTs with polymers. Then, ethanol was added, and the dispersions were allowed to stand for a duration. Eventually, the dispersions were centrifuged to eliminate the undispersed SWCNTs and reaggregated nanotubes. This simple process was applied to various polymer systems including PFO, poly[(9,9-dioctylfluorenyl-2,7-diyl)-alt-co-(6,6\u0026prime;-{2,2\u0026prime;-bipyridine})] (PFO-BPy), poly[(9,9-di-n-octylfuorenyl-2,7-diyl)-alt-(benzo-[2,1,3]thiadiazol-4,8-diyl)] (F8BT), poly[(9,9-didodecylfuorenyl-2,7-diyl)] (PFDD), and poly[9-(1-octylonoyl)-9H-carbazole-2,7-diyl] (PCz), as depicted in Supplementary Fig.\u0026nbsp;8.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eCompared with the traditional selective dispersion method, the present method significantly increased the purities of single-chirality SWCNTs (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e and Supplementary Fig.\u0026nbsp;9). The separation parameters are present in the Methods section and Table \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e. Raw SWCNTs with different structural distributions were employed. The diameter distributions of CoMoCAT(\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), CoMoCAT(\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and HiPco-SWCNTs are \u0026lt;\u0026thinsp;1.2 nm, featured with S\u003csub\u003e11\u003c/sub\u003e and S\u003csub\u003e22\u003c/sub\u003e absorption peaks at 850\u0026ndash;1400 nm and 500\u0026ndash;800 nm, respectively. Traditionally separated SWCNTs showed multiple peaks in both regions regardless of the polymer types, indicating relatively low chiral purities. Even (\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) SWCNT dispersions show two peaks of undesired nanotubes (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea). In contrast, the resultant (\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) and (\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) dispersions achieved by the present technique exhibit isolate S\u003csub\u003e11\u003c/sub\u003e and S\u003csub\u003e22\u003c/sub\u003e peaks. Plasma-SWCNTs (0.9\u0026ndash;1.7 nm) exhibit S\u003csub\u003e22\u003c/sub\u003e peaks at 800\u0026ndash;1100 nm. Due to PFO\u0026rsquo;s poor selectivity and wrapping profile for large-diameter SWCNTs (1.0-1.7 nm)\u003csup\u003e38\u003c/sup\u003e, a small quantity of large-diameter SWCNTs were dispersed along with (\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) SWCNTs by tradition method (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ef). With the present method, high-purity (\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) was achieved by incorporating an additional step (Supplementary Figs.\u0026nbsp;10 and 11). The SWCNTs that were selectively dispersed using PFO-BPy from HiPco contained multiple (n, m) species with large chiral angles. By employing the present method, (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and (\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) were highly enriched, providing ideal starting materials for iterative separation, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eg. Multistep rinse eliminated most of the PFO-BPy\u003csup\u003e47\u003c/sup\u003e, enabling the redispersion of (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) using PFO and subsequent redispersion of (\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) using PFO-BPy (details in Supplementary Fig.\u0026nbsp;12).\u003c/p\u003e \u003cp\u003eThe purities of each separated (n, m) species were calculated in Supplementary Fig.\u0026nbsp;13 according to their S\u003csub\u003e11\u003c/sub\u003e peak areas\u003csup\u003e14,22\u003c/sup\u003e. The chiral purities of (\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), (\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) and (\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) exceed 90%. Notably, the purity of (\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) increased from 95% to approximately 99%. Moreover, the separation of (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) and (\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) using polymers is reported for the first time (Figs.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea and b). Figure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ec highlights the significant improvement in the polymer wrapping method, making it comparable to DNA- and surfactant-based methods in terms of chiral purity.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003cb\u003eSeparation of high-purity large-diameter semiconducting\u003c/b\u003e \u003c/p\u003e \u003cp\u003eWe also investigated the effect of ethanol on the separation purity of large-diameter SWCNTs. We introduced different amounts of ethanol to semiconducting arc-discharge SWCNT (AP-SWCNT) dispersions separated through the traditional method using PFO-BPy, and let the dispersions stand for 6 h. The concentrations of SWCNT and PFO-BPy were 0.3 mg/ml and 0.5 mg/ml, respectively. Results are shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea and Supplementary Fig.\u0026nbsp;14. For the AP-SWCNTs (1.2\u0026ndash;1.6 nm), the absorbance in 600\u0026ndash;800 nm and 800\u0026ndash;1200 nm ranges corresponds to M\u003csub\u003e11\u003c/sub\u003e and S\u003csub\u003e22\u003c/sub\u003e peaks, respectively. Increasing ethanol concentration significantly decreased the M\u003csub\u003e11\u003c/sub\u003e peaks, indicating the enhanced semiconducting SWCNT purity. At an ethanol/toluene ratio of 0.06:1, M\u003csub\u003e11\u003c/sub\u003e peaks became undetectable. Further increasing the ethanol concentration to 0.08:1 led to a decrease in the absorbance in the range of 600\u0026ndash;800 nm, reflecting a reduction in background. Compared with the small-diameter SWCNTs, large-diameter SWCNTs seem more sensitive to ethanol, evidenced by the fast reaggregation within 6 h.\u003c/p\u003e \u003cp\u003eTo quantitatively assess the semiconducting purity of large-diameter SWCNTs, \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\varphi = {\\text{A}}_{\\text{C}\\text{N}\\text{T}}/({\\text{A}}_{\\text{C}\\text{N}\\text{T}}+{\\text{A}}_{\\text{B}})\\)\u003c/span\u003e\u003c/span\u003e was employed, where \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({\\text{A}}_{\\text{C}\\text{N}\\text{T}}\\)\u003c/span\u003e\u003c/span\u003e is the area of S\u003csub\u003e22\u003c/sub\u003e and M\u003csub\u003e11\u003c/sub\u003e regions enclosed by a linear baseline, and \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\({\\text{A}}_{\\text{B}}\\)\u003c/span\u003e\u003c/span\u003e is the background\u003csup\u003e49,50\u003c/sup\u003e. Metallic tubes, amorphous carbon and bundles exhibit stronger absorption at shorter wavelengths than semiconducting SWCNTs, contributing more to the background\u003csup\u003e49,51\u003c/sup\u003e. Hence, an increase in the \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\varphi\\)\u003c/span\u003e\u003c/span\u003e value signifies an enhancement in the purity and quality of semiconducting tubes (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eb).\u003c/p\u003e \u003cp\u003eWe attempted to enhance the effect of ethanol through optimizing the mass ratio of SWCNT/polymer and the standing time. The results are exhibited in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ec and Supplementary Fig.\u0026nbsp;15. The purity of semiconducting SWCNT increased with the SWCNT/polymer ratio. However, the quantity of SWCNTs remaining in the dispersion decreased faster at high SWCNT/polymer ratios, leading to a lower yield as shown in Supplementary Fig.\u0026nbsp;16. At the 0.5/0.5 SWCNT/polymer ratio, after standing for 24 h with ethanol, the intensity in the range of 600\u0026ndash;800 nm was even lower than that in 1200\u0026ndash;1400 nm wavelength range, suggesting a remarkably high semiconducting SWCNT purity. The \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\varphi\\)\u003c/span\u003e\u003c/span\u003e value also demonstrated the high level of semiconducting SWCNT purity (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ed). Raman spectra further confirmed the enhanced purity of semiconducting SWCNTs (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ee). The peaks corresponding to M\u003csub\u003e11\u003c/sub\u003e in RBM region disappeared following ethanol addition. A decrease in the D/G ratio, suggesting fewer defects in SWCNTs, was also observed (Supplementary Fig.\u0026nbsp;17).\u003c/p\u003e \u003cp\u003eThen, undispersed SWCNTs and ethanol were employed cooperatively. The separation results are shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ef and Supplementary Fig.\u0026nbsp;18. The structural distribution is narrowed compared with that achieved by solely employing ethanol, as evidenced by the reduced S\u003csub\u003e22\u003c/sub\u003e peaks at 910 nm, 1007 nm and 1060 nm. However, distinct enhancement in chiral selectivity was not achieved. We noticed that the reaggregation process was significantly accelerated in the presence of undispersed SWCNTs, leading to the rapid precipitation of most of the nanotubes. It implies that the large-diameter SWCNTs are readily affected by the changes in solution environment. However, the polymers used in this work exhibit minimal molecular recognition for chirality of large-diameter SWCNTs, making it difficult to finely tune their surface coatings.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003cb\u003eEffect of ethanol on structure-dependent surface coating and mechanism of single-chirality separation\u003c/b\u003e \u003c/p\u003e \u003cp\u003eIn a specific polymer system, the solution environment, such as polarity, aromaticity and architecture of solvents, dominates the dispersion of SWCNTs\u003csup\u003e43\u003c/sup\u003e. Polymer aggregation varies in different solvents\u003csup\u003e52\u003c/sup\u003e. Less compatible solutions lead to polymer folding, thus affecting their wrapping on SWCNTs\u003csup\u003e43\u003c/sup\u003e. This results in enhanced competitive coating of polymers on different SWCNTs, which is crucial for chiral selectivity. Due to the high dielectric constants, alcohols were reported to induce a collapsed coil conformation of chains in polymers with aromatic backbone and slightly polar alkoxy side chains, and decrease the polymer solubility\u003csup\u003e54\u003c/sup\u003e. As a poor solvent for PFO, ethanol induces the conversion of PFO conformation from the \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\alpha\\)\u003c/span\u003e\u003c/span\u003e phase to the \u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\beta\\)\u003c/span\u003e\u003c/span\u003e phase in solutions by promoting mesoscopic aggregation\u003csup\u003e53\u003c/sup\u003e. This results in the swelling of polymer wrapping on SWCNTs\u003csup\u003e54\u003c/sup\u003e, which could cause detachment of polymer from SWCNTs and inter-polymer aggregations. The changes in surface coating may vary among SWCNTs with different structures due to different polymer affinities.\u003c/p\u003e \u003cp\u003eTo verify the structure-dependent impacts of ethanol, we carried out X-ray photoelectron spectroscopy (XPS) on single-chirality (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) SWCNTs (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003e). Single-chirality (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) were dispersed with PFO. After adding ethanol (0.12:1), they were deposited on silicon substrates by immersing the substrates in SWCNT dispersions. Excess PFO was washed away with an ethanol/toluene solution. For comparison, (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) SWCNT dispersions without ethanol were deposited in the same manner, and then rinsed with neat toluene. The polymer wrapping on SWCNTs cannot be eliminated by rinsing\u003csup\u003e55\u003c/sup\u003e. The C-C at 285 eV is derived from polymers, while the C-C (graphite) bond at 284.4 eV originates from both SWCNTs and polymers\u003csup\u003e56,57\u003c/sup\u003e. The peak area ratios of C-C bond and C-C (graphite) bond reflect the relative content of SWCNT and polymers. Introduction of ethanol reduced the surface coating on (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), leading to the decreased C-C/C-C (graphite) bond ratios from 0.46 to 0.33 for (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and from 0.38 to 0.18 for (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ee. After adding ethanol, the C-C/C-C (graphite) ratios of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) decreased by 28% and 52%, respectively. The more pronounced reduction in the C-C bond representing PFO indicates that ethanol impacts the surface coating more significantly in (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e).\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eNotably, C-C bonds in XPS results may stem from contamination and residual polymers on the substrate, and may overlap with the C-H bonds in contaminants. To further confirm the reductions of polymers on (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), we removed excess polymers using vacuum filtration. Single-chirality (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) SWCNTs that were separated using PFO were divided into two groups. Ethanol was added to one of the two groups at ethanol/toluene ratio of 0.12:1, while an equal volume of toluene was added to the control group. Then, the two groups of solutions were filtered. SWCNTs on membranes extracted from the two groups were rinsed with neat toluene and ethanol/toluene (0.12:1), respectively. After removing the excess polymer, the SWCNTs were redispersed in neat toluene and characterized by optical absorption to verify the remaining polymer on SWCNT sidewalls (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ef-h). In the absence of the excess polymers, the absorbance contributed by polymers significantly decreased, changing the solution color from green to bluish-green (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003eg and h).\u003c/p\u003e \u003cp\u003eThe peak intensity ratios of PFO (I\u003csub\u003e380 nm\u003c/sub\u003e) and S\u003csub\u003e11\u003c/sub\u003e of single-chirality (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) (I\u003csub\u003e11, (7,5)\u003c/sub\u003e and I\u003csub\u003e11, (7,6)\u003c/sub\u003e) are exhibited in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ef. Without ethanol, the I\u003csub\u003e380 nm\u003c/sub\u003e/I\u003csub\u003e11\u003c/sub\u003e ratios of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) were 2.42 and 2.06, respectively. After ethanol was employed, the I\u003csub\u003e380 nm\u003c/sub\u003e/I\u003csub\u003e11, (7,5)\u003c/sub\u003e decreased to 1.58, while that of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) SWCNTs reduced to 0.90, indicating a polymer wrapping reduction for both species. The I\u003csub\u003e380 nm\u003c/sub\u003e/I\u003csub\u003e11, (7,5)\u003c/sub\u003e and I\u003csub\u003e380 nm\u003c/sub\u003e/I\u003csub\u003e11, (7,6)\u003c/sub\u003e decreases by about 35% and 56%, respectively. The degree of polymer density reduction on (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) surfaces increased to a greater extent, enlarging the coating difference between the two species. Therefore, the (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) species were easier to reaggregate.\u003c/p\u003e \u003cp\u003eClearly, ethanol induced detachment of polymers from SWCNTs\u0026rsquo; surfaces, with varying effects on different (n, m) species. Those (n, m) species with relatively lower polymer affinity or unstable coating configurations tend to expose more of their surface, increasing the chance of forming bundles\u003csup\u003e58\u003c/sup\u003e. The (n, m) species with the well-packed coating are least affected by solution environment. Among the (n, m) species dispersed by PFO, coating structure of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) is the most stable in ethanol/toluene solutions, likely due to the smallest wrapping angle of PFO on (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) among various species\u003csup\u003e40\u003c/sup\u003e, indicating a more parallel alignment of PFO backbone with the axis of SWCNTs. A linearly aligned configuration of PFO on nanotubes is more stable than helical wrapping\u003csup\u003e59\u003c/sup\u003e. This renders (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) SWCNTs less sensitive to the solution environment and maintains their dispersion in the presence of ethanol.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eAlthough ethanol alters the polymer wrapping on different (n, m) species, achieving single-chirality separation merely by tuning ethanol concentration is difficult (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003eb). Because selective reaggregation relying only on the tube-tube attraction of loosely coated SWCNTs to self-assemble and precipitate is low efficient. Moreover, previous works have shown that some undesired (n, m) species were dispersed in form of small bundles by polymers. However, these bundles are difficult to induce selective reaggregation, leading to a poor chiral selectivity in the rebundling process\u003csup\u003e41\u003c/sup\u003e. They can only be effectively eliminated via intensive ultracentrifugation and filtration, thus enhancing the chiral purity of SWCNTs remaining in the solutions\u003csup\u003e32,46\u003c/sup\u003e. Introducing undispersed SWCNTs significantly accelerates the reaggregation and improves the chiral selectivity (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec and d). The undispersed SWCNTs provide large exposed surface areas with abundant binding sites, aiding in anchoring (n, m) species with loose polymer coating. By combining undispersed SWCNTs with ethanol, the coating differences between (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) were efficiently recognized. As demonstrated in a different separation route in Supplementary Figs.\u0026nbsp;10 and 11, most of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) disappeared from the SWCNT-PFO dispersions and emerged in the undispersed SWCNTs, leaving (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) species in the supernatant. It unambiguously demonstrates the selective anchoring of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) to undispersed SWCNTs. Besides, the length distribution of SWCNT is minorly affected by the selective reaggregation, indicating that the chiral separation is ascribed to coating differences rather than length difference (Supplementary Fig.\u0026nbsp;19).\u003c/p\u003e \u003cp\u003eA phase diagram showing the effect of ethanol and undispersed SWCNTs is exhibited in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ea. The molecular recognition zone above the dashed line represents the successful differentiation of two species. In this work, single-chirality separation was achieved through two processes: (i) ethanol increases the coating differences between different (n, m) species; (ii) undispersed SWNTs greatly enhanced the resolution of separation. As for (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e)/(\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), the addition of ethanol enlarges their coating differences. The undispersed SWCNTs significantly reduced the threshold for recognizing the coating differences in a separation strategy. As ethanol concentration increasing, the coating difference increases above the dashed line, which represents the recognition capability of undispersed SWCNTs. Thus, (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e)/(\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) SWCNTs, which cannot be distinguished by selective dispersion, were separated by the present method.\u003c/p\u003e \u003cp\u003eCompared with (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e)/(\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), to distinguish (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) is much more difficult, as evidenced in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. In the absence of ethanol, the coating difference between (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) is much smaller than that between (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e)\u003csup\u003e40\u003c/sup\u003e. The ratio of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) contents barely changes over time, indicating that they cannot be differentiated by undispersed SWCNTs (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ef). By combining ethanol and undispersed SWCNTs, (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) were achieved at different ethanol concentrations (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed). At low ethanol concentrations, a small amount of ethanol does not reduce the stability of (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), yet facilitates the reaggregation of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and (\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) in the presence of undispersed SWCNTs. During the selective dispersion stage of HiPco-SWCNT, (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) predominates over (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) in the solution, and their mass ratio maintained during the subsequent reaggregation. Thus, after eliminating other undesired SWCNTs, a single-chirality (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) solution with minor (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) content was achieved (Figs.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed and \u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ed). At high ethanol concentrations, the coating differences of (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e)/(\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) were significantly enlarged, and these differences were successfully recognized by undispersed SWCNTs, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ea. Owing to the differentiation of enlarged coating differences between (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e)/(\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and between (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e)/(\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e), (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) SWCNTs were separated from the (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e)/(\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e)/(\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) mixtures.\u003c/p\u003e \u003cp\u003eThe selective reaggregation process is exhibited in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003eb. Initially, despite minimal coating differences, (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) were dispersed and stably maintained in the solution. Then, ethanol addition reduced the density or number of polymer molecules on SWCNTs, with varying degrees of impact on different (n, m) species, granting them larger differences in surface coatings. The ethanol concentration is vital for determining the degree of surface coating reduction and the coating differences variations. Consequently, the most impacted (n, m) species, such as (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), tend to reaggregate more easily. (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) SWCNTs exposed a part of their sidewalls as the ethanol concentration increasing. The relatively stable coating configuration of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) preserves the surface coating from impact of environmental changes. Introducing undispersed SWCNTs rapidly anchors those with looser surface coating, significantly improving the separation resolution and efficiency, resulting in the predominance of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) in the dispersion.\u003c/p\u003e"},{"header":"3. Conclusion","content":"\u003cp\u003eWe developed a method to finely tune polymer wrapping and recognize the coating differences of various (n, m) species. Introducing ethanol successfully enlarges coating differences of different SWCNTs. The undispersed SWCNTs efficiently enhance the selective reaggregation. By combining ethanol and undispersed SWCNTs, eight types of high-purity single-chirality SWCNTs, including (\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e), (\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), (\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and (\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e), were achieved through a simple spontaneous selective reaggregation process. The current method also yields a significant increase in semiconducting purity of large-diameter SWCNTs. We further explored the impact of ethanol and demonstrated the varying degree of surface coating reduction of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e). Undispersed SWCNTs selectively anchor SWCNTs with loose surface coatings via interaction between exposed surfaces, leaving single-chirality SWCNTs in the dispersion. We believe that the present method provides an effective pathway for increasing the separation resolution in polymer systems. Furthermore, multiple single-chirality (n, m) species achieved from organic system promote the applications of SWCNTs in the fields of nanoelectronics, optoelectronics, sensors and organic photovoltaics.\u003c/p\u003e "},{"header":"Methods","content":" \u003cp\u003e \u003cb\u003eMaterials\u003c/b\u003e: Raw CoMoCAT (\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) (purity\u0026thinsp;\u0026ge;\u0026thinsp;95%) and CoMoCAT (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) (purity\u0026thinsp;\u0026ge;\u0026thinsp;77%) were purchased from Sigma-Aldrich. HiPco- (Fluffy Powder, Catalyst :\u0026lt; 35%) and Plasma-SWCNTs (RN-220) (Carbon purity 85%-90%) were purchased from Nanointegris, Inc. AP-SWCNTs (Carbon purity 60%-70%) were purchased from Carbon Solution, Inc. PFO (M\u003csub\u003ew\u003c/sub\u003e \u0026ge; 20k) and F8BT (M\u003csub\u003en\u003c/sub\u003e \u0026le; 25k, Mw/Mn\u0026thinsp;\u0026le;\u0026thinsp;3) were purchased from Sigma-Aldrich. PFO-BPy (purity\u0026thinsp;\u0026gt;\u0026thinsp;98%) was purchased from Konosclence. PCz (purity 95% M\u003csub\u003ew\u003c/sub\u003e 10k-100k) was purchased from Xi\u0026rsquo;an Qiyue Biotechnology co., Ltd. PFDD (M\u003csub\u003ew\u003c/sub\u003e \u0026gt; 50k) was purchased from Derthon Optoelectronics Materials Science Technology Co. Ethanol (\u0026gt;\u0026thinsp;99.7 wt%) was purchased from Sigma-Aldrich. Toluene (\u0026gt;\u0026thinsp;99.5 wt%) was purchased from Damao Chemical Reagent Factory.\u003c/p\u003e \u003cp\u003e \u003cb\u003eSeparation of single-chirality SWCNTs\u003c/b\u003e: Different raw SWCNTs and polymers were used to separate different (n, m) species. The detailed information was exhibited in Table \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e. Typically, raw SWCNT materials were dispersed at the initial SWCNT concentration of 0.3 mg/ml with corresponding polymers in toluene using a 0.5-inch tip homogenizer for 2 h at 30% power in an ice-water bath. Then, different quantities of ethanol were added to the mixture of dispersion. The dispersions were allowed to stand for 3\u0026ndash;48 h with the undispersed SWCNTs. Eventually, the dispersions were centrifuged for 30 min at 8500 g, and the upper 80% supernatants were collected as the separated SWCNT dispersions. Specifically, to achieve high-purity of (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e), the polymer concentration was set to 1.3 mg/ml to increase the proportion of (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) to (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) obtained through selective dispersion (details in Supplementary Table\u0026nbsp;1). To enhance the purities of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and (\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) SWCNTs, a different route was employed, as shown in Supplementary Fig.\u0026nbsp;10. CoMoCAT(\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and Plasma-SWCNTs were used as the raw materials for separation of (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and (\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) SWCNTs respectively. After the sonication, the dispersions were centrifuged for 2 h at 26000 g to remove the undispersed CoMoCAT(\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and Plasma-SWCNTs. Then undispersed AP-SWCNTs and ethanol was added to the dispersions. After standing for 3\u0026ndash;6 hours, the dispersions were centrifuged for 30 min at 8500 g, and the supernatants were completely removed. The pellets were collected and redispersed with 0.1-mg/ml PFO toluene solutions. Again, after centrifugation for 2 h at 26000 g, the final upper 80% supernatants were collected as single-chirality (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and (\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e) dispersions. Besides, single-chirality (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) can also be obtained via the procedure in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea when applying ethanol and undispersed SWCNTs to PFDD-dispersed CoMoCAT(\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e). To achieve (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and (\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), 0.3-mg/ml HiPco were dispersed with PFO-BPy (0.3 mg/ml). After adding ethanol (0.04:1) and standing with undispersed SWCNTs for 24 h, the dispersion was centrifuged for 30 min at 8500 g to collect the supernatant enriched in (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) and (\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e). Then, the PFO-BPy in this sample was removed as much as possible by employing high-concentration ethanol (0.2:1). Subsequently, SWCNTs were redispersed with PFO to achieve (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) SWCNTs, and the undispersed fractions were redispersed with PFO-BPy to obtain (\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e) SWCNTs (see details in Supplementary Fig.\u0026nbsp;12).\u003c/p\u003e \u003cp\u003e \u003cb\u003eSeparation of large-diameter semiconducting SWCNTs\u003c/b\u003e: 3, 4, and 5 mg of AP-SWCNTs were dispersed in 10 ml of toluene (\u0026ge;\u0026thinsp;99.5%) with PFO-BPy fixed at 0.5 mg/ml. The three dispersions were respectively sonicated for 2 h at 30% power in an ice-water bath using a 0.5-inch tip homogenizer (SFX550, Branson), followed by centrifugation for 30 min at 8500 g. Then, each of the three dispersions was divided into several aliquots. Then, different quantities of ethanol were added to these dispersions at the volume ratio of ethanol/toluene of 0.02:1, 0.04:1, 0.06:1, 0.08:1 and 0.12:1. After standing for 3\u0026ndash;48 hours, these dispersions were centrifugated for 5 min at 8500 g to remove the reaggregated SWCNTs. Notably, after each centrifugation, the upper 80% supernatants were collected. To further narrow the structure distributions, the dispersed large-diameter SWCNTs were mixed with ethanol (0.08:1) without removing undispersed SWCNTs. After 48 hours, the sample was centrifuged for 30 min at 8500 g to eliminate the undispersed SWCNTs and reaggregated nanotubes. The upper 80% dispersion was collected.\u003c/p\u003e \u003cp\u003e \u003cstrong\u003eCharacterization\u003c/strong\u003e \u003cp\u003eOptical absorption spectra were obtained using a UV-vis-NIR spectrophotometer (Lambda 950, PerkinElmer). The SWCNTs dispersed in toluene were recorded from 400 to 1400 nm. Raman spectra were measured by a confocal Raman microscope (HR Evolution, Horiba) from 100 to 2800 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e at integral time of 3s. The length of SWCNTs were characterized by a field emission scanning electron microscope (Nova NanoSEM450, FEI). X-ray photoelectron spectroscopy (ESCALAB 250Xi, ThermoFisher) was carried out in ultrahigh-vacuum conditions (base pressure of 1 \u0026times; 10\u0026thinsp;\u0026minus;\u0026thinsp;9 mbar) using an Al Kα X-ray source (15kV, 10mA, 500 \u0026micro;m spot size).\u003c/p\u003e"},{"header":"Declarations","content":"\u003ch2\u003eAcknowledgments\u003c/h2\u003e \u003cp\u003eThis work was financially supported by the National Key Research and Development Program of China (grant nos. 2020YFA0714700), the National Natural Science Foundation of China (grant nos. 62274054), the Strategic Priority Research Program of Chinese Academy of Sciences (grant no. XDB33030100), the Key Research Program of Frontier Sciences, CAS (grant no. QYZDBSSW-SYS028), Hebei province Science Foundation for Distinguished Young Scholars (F2021201035), \u0026ldquo;333 project\u0026rdquo; of Hebei Province (C20221014). The Central Guidance on Local Science and Technology Development Fund Project of Hebei Province (No. 236Z4307G).\u003c/p\u003e\u003ch2\u003eData availability\u003c/h2\u003e \u003cp\u003eThe key data generated in this study are provided in the Supplementary Information. Source data are provided.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eJavey A, Guo J, Wang Q, Lundstorm M, Dai H (2003) Ballistic carbon nanotube field-effect transistors. Nature 424:654\u0026ndash;657\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eHe X, Htoon H et al (2018) Carbon nanotubes as emerging quantum-light sources. Nat Mater 17:663\u0026ndash;670\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eNanot S, H\u0026aacute;roz EH, Kim J-H, Hauge RH, Kono J (2012) Optoelectronic properties of single-wall carbon nanotubes. 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ACS Nano 9:9012\u0026ndash;9019\u003c/span\u003e\u003c/li\u003e\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":true,"highlight":"","institution":"","isAcceptedByJournal":false,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true},"keywords":"","lastPublishedDoi":"10.21203/rs.3.rs-4431799/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-4431799/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eStructural separation of single-wall carbon nanotubes (SWCNTs) is crucial for high-performance SWCNT-based devices. Compared with separation methods in aqueous systems, SWCNTs separated via polymer wrapping are more conducive to being processed into uniform and well-oriented films for high-speed nanoelectronic devices. However, high-purity separation of multiple single-chirality SWCNTs in organic systems remains a challenge due to the limited chiral resolution of polymer-based methods. Herein, we develop a straightforward technique to enlarge the polymer coating differences of different SWCNT species by employing ethanol and precisely recognize the various (n, m) species by introducing undispersed SWCNTs to induce a spontaneous chiral selective reaggregation. With this technique, we obtained eight types of single-chirality SWCNTs in organic systems, including (\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e), (\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), (\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e), (\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e), (\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e) and (\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e), with purities higher than 90% in five of them. Ethanol also induces the reaggregation of metallic SWCNTs, increasing the purity of large-diameter semiconducting SWCNTs. This technique makes significant progress in the polymer-based method for achieving single-chirality separation. We believe that this work promotes the SWCNT-based electronics.\u003c/p\u003e","manuscriptTitle":"Ethanol selectively inducing the separation of single-chirality carbon nanotubes from polymer-dispersed mixture","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2024-05-23 04:25:43","doi":"10.21203/rs.3.rs-4431799/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"fb9d73e3-f682-4328-8bde-405b3f035e15","owner":[],"postedDate":"May 23rd, 2024","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[{"id":32275958,"name":"Physical sciences/Materials science/Nanoscale materials/Carbon nanotubes and fullerenes"},{"id":32275959,"name":"Physical sciences/Materials science/Nanoscale materials/Electronic properties and materials"}],"tags":[],"updatedAt":"2025-10-14T09:25:54+00:00","versionOfRecord":[],"versionCreatedAt":"2024-05-23 04:25:43","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-4431799","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-4431799","identity":"rs-4431799","version":["v1"]},"buildId":"qtupq5eGEP_6zYnWcrvyt","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}