Printable Newtonian fluid photocatalysts for scale-up solar CO2 conversion

Printable Newtonian fluid photocatalysts for scale-up solar CO2 conversion | 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 Printable Newtonian fluid photocatalysts for scale-up solar CO 2 conversion Kan Zhang, Ziyang Lu, Yu Cheng, Yangrui Xu, Liguang Tang, Hongping Li, and 2 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7844074/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 20 Mar, 2026 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Abstract Photocatalysis is a green and sustainable process for fuel and chemical synthesis, while the photocatalysts are in powder form, leading to a significant challenge in scale-up technology. Here, we report a flowing viscous Newtonian fluid photocatalyst, which consists of an internal nano-hollow imidazole framework (PIL) and an external light-excitable liquid chain (EY[M]) striking a pose on the stage. Due to the significant steric hindrance effect and intermolecular interaction at the solid-liquid interface, the Newtonian fluid catalyst with higher surface tension can firmly adhere to any kind of scaffold via a simple printing or spraying, such as curved surfaces, inclined walls, and grids, where powder materials are difficult to load. In addition to the easier scale-up, the pore structure of frameworks favors faster CO 2 mass transfer, and the liquid chain with a co-catalytic effect serves as the electron donor for efficient CO 2 photoreduction. As a result, the PIL-EY[M] achieved a 100% selective CO overflow efficiency, which is 57.8 times higher than that of the PIL, with a stable performance under long-time and large-scale solar radiation. By utilizing the structural characteristics of imidazole cationic solid and anionic liquid ends, a series of Newtonian fluid photocatalysts, such as TiO 2 -EY[M] and C 3 N 4 -EY[M], can be readily synthesized. The viscous Newtonian fluid photocatalysts enable a chance for commercial feasibility at an affordable cost. Physical sciences/Chemistry/Catalysis/Photocatalysis Physical sciences/Materials science/Materials for energy and catalysis/Photocatalysis Printable catalyst Newtonian fluid Scaling up photocatalysis CO2 reduction Figures Figure 1 Figure 2 Figure 3 Figure 4 Introduction Photocatalysis is a green and sustainable manner for converting solar energy into high-value chemicals, which has the potential to become an important tool for addressing climate change and environmental crises 1,2 , 3,4 . In the past few decades, various semiconductor photocatalysts have been developed, including nanotubes 5 , nanosheets 6 , amorphous nanoparticles 7 , alloys 8 , and so on 4,9 , dedicated to improving the intrinsic catalytic activity during the reaction process. Although significant progress has been made in the performance of photocatalysts and the exploration of reaction mechanisms, the demand for suitable large-scale reactions has not been well explored. The amplification of photocatalytic systems needs to consider the practicality of catalysts beyond their performance 10 . At present, immobilized photocatalyst reactors are the main form for achieving large-scale photocatalysis, where photocatalysts are fixed to a matrix to prevent loss of catalysts in outdoor reaction environments 11,12 . For example, Wang et al. prepared a porous hydrogel nanocomposite photocatalysis platform with an area of 1m 2 by embedding a large number of photocatalysts into the hydrogel macroporous matrix 13 ; Zhu et al. prepared a 1600cm 2 photocatalytic hydrogen production platform by immobilizing powder photocatalysts on a super-hydrophilic wood fiber matrix using gradient alignment theory 14 . Although these scaled-up methods have broad applicability in accommodating various types of nanoscale photocatalytic fillers, the matrix of the encapsulated photocatalyst interrupts the active material conduction chain between the catalysts and the effective charge transfer between the catalyst and reactants (such as small gas molecules) at the catalytic interface. Therefore, it is required to design a photocatalyst that can achieve simple amplification without the need for a large matrix. Newtonian liquid is an ideal viscous liquid proposed by Newton in 1687, whose viscosity remains constant regardless of the shear rate. This characteristic makes it a stable coating material that can be easily coated on flat surfaces. Compared with embedding a large amount of catalyst into the matrix, the method of expanding the photocatalytic reaction scale by simply coating and brushing to increase the reaction area can not only improve performance, but also eliminate the cumbersome "matrix-catalyst" binding relationship and additional pre-operation costs. The stable and uniform liquid catalyst formed by grafting liquid ends on the surface of microporous nanoparticles has been proven to have promising prospects in the field of photocatalysis 15,16 , 17 . However, these liquid catalysts lack viscosity due to weak surface tension, making it difficult to stably coat them on steep slopes, grilles, or in strong wind environments. It is considered that the intramolecular interaction of the solvent or the solvent and solute causes the liquid to generate resistance in the flow, which increases the surface tension of the liquid and thus produces viscosity 18 . Inspired by this, the liquid chain with a large steric hindrance is spatially confined around its side chains, and then grafted with microporous nano-semiconductors through weak molecular forces, such as electrostatic action, to form a strong viscous Newtonian fluid that responds to non-horizontal or open natural conditions 19,20 . Unfortunately, since the liquid chain cannot be photoexcited, the internal catalyst surface radiation is attenuated, giving fluidity while sacrificing photocatalytic activity. Therefore, a rational design of high-performance and strong surface tension liquid catalysts would hold further interest. In this study, we propose a viscous Newtonian fluid catalyst composed of internal microporous nano-hollow spheres with positive potential and external negative potential assisted catalytic liquid chains for simple scaling up of photocatalysis. Due to the electrostatic interactions between the inner and outer components and the significant steric hindrance effect of the liquid chains, the Newtonian fluid catalyst exhibits robust flow resistance, making it easy to apply and stabilize loads in strong winds and non-horizontal environments such as grids, slopes, and even downward orientations. On the other hand, the liquid chain that can be light-excited was designed as an electron donor to improve the electron enrichment degree of internal nano-hollow spheres, thereby promoting reactant adsorption and rapid light conversion. Theoretical and experimental verification have demonstrated the practical advantages of Newtonian fluid catalysts in photocatalysis. The structure of Newtonian fluid photocatalysts To achieve the viscous and flowing effect of Newtonian fluids while maintaining photocatalytic performance, we divide the catalyst into two parts: an inner and an outer part. The microporous nano-hollow spheres, serving as the inner part, act as the primary catalytic contributor. In this regard, the polymerization of imidazolium (PIL) rings, which possess a strong positive potential and an electron-enriched site, can serve as the adsorption and conversion sites of reactants. The outer parts are long polymer liquid chains (EY[M]) grafted by Eosin Y (EY) and Polyether amine (M2070), which can ionize anions EY[M] ∙‑ for combining with PIL from electrostatic attraction and act as electron donors. Schematic (Fig.1a) and optical images show the main preparation process. Firstly, the PIL was synthesized by the polymerization of divinylbenzene and 1-vinylimidazole on the surface of the PS sphere as templates (Fig.S1). Then, by etching templates, PIL forms the hollow states and micropore surface. The optical images show that the PIL is a white powder. The EY[M] is formed by the dehydration condensation reaction (Fig.S2). EY[M] appears as a dark red semi-translucent liquid. Finally, PIL and EY[M] are self-assembled by electrostatic action to form a viscous fluid catalyst (PIL-EY[M]). The molecular structure is shown in Fig.1a. The fluid rheology experimental results of PIL-EY[M] show that the ratio of shear stress to shear rate is a constant (Fig.1b). Therefore, the viscosity of PIL-EY[M] does not change with the change of shear rate, which belongs to a Newtonian fluid 19 , the viscosity of PIL-EY[M] is 6386.21 mPa∙s. Subsequently, a series of characterizations were conducted to demonstrate the structure of PIL-EY[M]. The morphology of PIL is spherical with a hollow diameter of around 370 nm inside (Fig.1c, Fig.S3), and there are positive potential (+32.6 mV) multiple microporous structures on its surface (Fig.S4, Tab.S1). These hollow and microporous materials are used to increase reactant mass transfer inside the Newtonian fluid photocatalyst. The 13 C Solid State Nuclear Magnetic Resonance (SSNMR) was used to demonstrate the composition of PIL (Fig.1d). The peaks at 138 ppm and 128 ppm belong to the imidazole carbon 21 , the peaks around 145 ppm and 113 ppm are attributable to the phenyl carbon 22 , and the other peaks belong to the carbon chain. Two broad diffraction peaks at 13.3° and 27.5° were observed in the X-ray diffraction (XRD) pattern of PIL (Fig.S5), attributed to the planar stacking of imidazole rings and the interlayer stacking of aromatic rings, respectively. The PIL-EY[M] did not detect the above two peaks, and their signals were completely covered by the EY[M], showing a peak located at 21.6°, which belongs to the amorphous diffraction of M2070 23 . The X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared (FTIR) spectroscopy further confirmed the detailed information of the PIL (Fig.1e and Fig.S6). In the TEM image of EY[M], small negatively charged (-32.3 mV) nanoclusters (<5 nm) can be observed (Fig.S7), which are formed due to the monomers and dimer-aggregates of EY 24 (Fig.S8). These nanoclusters serve as the “head” for binding with PIL. In the FTIR spectrum of EY[M], there is an added peak at 1670 cm -1 (Fig.1e), which represents the -NH- groups formed by the dehydration condensation of EY and M2070. The PIL-EY[M] still maintains the nanosphere morphology. TEM and mapping images indicate that EY[M] is wrapped around the outer surface of PIL (Fig.S9-S10). Characterization of Newtonian fluid photocatalysts The stable fluidity and viscosity of the catalyst at room temperature are expected to yield unique features that are advantageous for the scale-up of photocatalysis. To achieve a coating effect, a viscous and slowly flowing Newtonian fluid photocatalyst can be controlled by adjusting the synthesis ratio of the inner and outer parts. In the optical images (Fig.2a), it can be observed that when flipping the bottle containing PIL-EY[M], the PIL-EY[M] flows slowly downwards under the influence of gravity. By pressing the PIL-EY[M] in the syringe, it can drip (Fig.2b). By dipping the needle into the PIL-EY[M] and applying an upward force, the PIL adheres to the needle and exhibits strong upward flow resistance. These indicate that the PIL-EY[M] takes into account both viscosity and fluidity at room temperature and can be coated onto a carrier using a brush, greatly improving efficiency compared to the matrix preparation and catalyst embedding processes in conventional photocatalytic amplification platforms. There properties make it suitable for brush coating on various carriers (such as plastic, wood, metal, et al.) and even grids (Fig.2c). In contrast, the powder photocatalysts are limited to planar carriers in sealed conditions, as powder are difficult to fix under non-horizontal plane environments such as inclined plain or facing downwards, and are also prone to mass loss due to being blown away in open air. In a simulated open environment with a wind speed of 18m/s (equivalent to an 8-level typhoon) for 20 min (Fig.2d), the PIL-EY[M] has no significant photocatalyst mass loss (Fig.S11), and it can maintain stability in non-horizontal planes or even vertically downward states for 180 days. Despite all this, strong viscosity does not mean difficult to recycle, the PIL-EY[M] can be removed from the carrier using organic solvents such as N,N-Dimethylformamide and ethanol, and can be recovered by washing with these solvents (Fig.2e). The thermal decomposition temperature and melting temperature of PIL-EY[M] are 235 °C and -40 °C (Fig.2g, Fig.S12), respectively, which indicate that it can remain the fluidity and viscosity for most climate environments on Earth. Weak intermolecular forces, such as electrostatic interactions, can cause the flow resistance, which is one of the reasons for the PIL-EY[M] viscosity. Reduced Density Gradient (RDG) and Independent Gradient Model (IGM) analysis were used to evaluate the weak intermolecular forces between PIL and EY[M] (Fig.S13). The RDG analysis results confirmed the existence of a prominent weak interaction force (blue iso surface) between PIL and EY[M], which can be reasonably inferred as an electrostatic force between them (Fig.2h). As shown in Fig.S14, the black and red dots are defined as intramolecular and intermolecular forces. The IGM analysis results clearly indicate the intermolecular forces between PIL and EY[M]. After eliminating the interference of atomic density gradients, IGM analysis visualizes the real binding environment. The results reveal an ideal intermolecular interaction between PIL and EY[M] (Fig.2i), where the blue surface is attributed to electrostatic binding force, while the green surface reflects the spatial potential resistance and dispersion effect with low electron density 25 . It is worth noting that the length and width of EY[M] reach 22.97 Å and 21.22 Å, respectively (Fig.2j). Such a large-sized EY[M] cannot pass through the micropores on the PIL surface or enter the hollow structure. The micropores of PIL are well preserved for enhancing the adsorption and mass transfer of reactants in photocatalytic reactions. The photocatalytic advantages and mechanism of Newtonian fluid photocatalysis The photocatalytic CO 2 conversion reaction is one of the most common reactions in the field of photocatalysis, and the unique advantages of Newtonian fluid photocatalysts in practical applications are analyzed through CO 2 reduction reactions. The detailed description and light source information of the photocatalytic CO 2 reduction measurement experiment are provided in Fig.S15. The performance testing was conducted under gas-solid conditions, where the PIL-EY[M] was coated onto a carrier film, and the PIL is dispersed on the carrier with the same area for detection. Optical images indicate that compared to powder catalysts, Newtonian fluid photocatalysts can be coated more uniformly on the surface of the carrier with less mass (Fig.S16), which greatly saves catalyst usage and maximizes the reaction contact area between the catalytic surface and CO 2 . After five hours of simulated light reaction, CO was the only product in all samples. The results showed that the CO yield of PIL, EY, and EY[M] were 21.24 μmol h -1 m -2 , 87.82 μmol h -1 m -2 and 80.83 μmol h -1 m -2 , respectively (Fig.3a). In contrast, the CO evolution rates of PIL-EY[M] reached 1228.68 μmol h -1 m -2 , which was 57.84, 13.99 and 15.20 times of PIL, EY and EY[M], respectively. The long-term reaction test of the photocatalysts showed that the yield of PIL and EY gradually decreased after stable for 10 hours during the continuous reaction of 25 hours (Fig.3b). The CO yield of PIL-EY[M] remained stable, with an average yield of 1206.28 μmol h -1 m -2 over 25 hours, which was 58.61 times and 58.99 times higher than PIL and EY, respectively. Compared with the same type of imidazole photocatalysts, ion composite photocatalysts, and different types of photocatalysts (Tab.S2-S3), PIL-EY[M] has outstanding performance increased multiplier factors, emphasizing the advantages of Newtonian fluid photocatalysts in photocatalytic systems (Fig.3c). The FT-IR and XPS characterization confirmed that there were no functional or structural changes observed after the PIL-EY[M] reaction (Fig.S17-S18). Subsequently, the isotopic 13 CO 2 experiment and a series of comparative experiments were conducted to demonstrate the photocatalytic activity of the product derived from Newtonian fluids (Fig.3d, Fig.S19). Explain the advantages of Newtonian fluids in photocatalytic reactions from a mechanistic perspective. The UV absorption spectrum of PIL-EY[M] showed stronger absorption than EY[M], which may be due to the charge transfer (CT) state between PIL and EY[M] (Fig. 3e). As the reaction time increases, the peak at 516nm and 480nm strengthens, indicating an enhanced π/π* transition in PIL-EY[M]. In contrast, the absorption spectrum of EY decreases significantly with reaction time. By performing time-dependent density functional theory (TDDFT) calculations on the optimized structure of PIL-EY[M], it was found that the distance between the centers of mass of holes and electrons was as high as 3.69 Å at S0-S1 (Fig.3f, Fig.S20), corresponding to the contribution of charge-transfer excitation as the lowest energy excited state of PIL-EY[M], indicating a high degree of separation between electrons and holes 26 . It can be reasonably inferred that it belongs to π/π* charge transfer excitation in the EY to PIL direction. The charge difference calculation of PIL-EY[M] proves that the excited electrons gather on EY and are consumed on PIL, indicating that EY[M] can serve as an electron donor and PIL as an acceptor. A larger dipole moment of the excited state is more conducive to the charge transfer from the lowest excited state of EY[M] to PIL (Fig.S20). In addition, PIL-EY[M] has a larger ground state dipole moment (19.34 D) compared to PIL (1.63 D) and EY[M] (8.32 D), indicating that PIL-EY[M] is more conducive to photogenerated charge separation 27 , which is consistent with the results of weaker emission intensity, better electrochemical properties, and charge transfer density (Fig. S21-S22). To gain a deeper understanding of the excited-state dynamics between EY[M] and PIL. Immediately, femtosecond transient absorption spectroscopy (TAS) was conducted on PIL-EY[M] after excitation by a 420 nm laser pulse, the spectrum displayed a strong broad bleach centered at 538 nm, attributed to the singlet excited state absorption of EY[M] (Fig.S23). The 420 nm - 490 nm range exhibited the characteristic absorption of the EY radical anion in ET[M], reaching a maximum at 440 nm. The mono-exponential fit of PIL-EY[M] dynamics at 440 nm resulted in a lifetime of only 857.3 ps (Fig.3g), indicating that exciton energy has been transferred from EY[M] radical anions to PIL, directly demonstrating effective electron transfer between EY[M] and PIL 28,29 . The availability of reactants and stable adsorption at catalyst sites are key steps in the photocatalytic reduction process. The weak adsorption capacity of CO 2 without porosity limits the development of liquid catalysts. The presence of permanent hollow pores in porous Newtonian fluid photocatalysts is expected to facilitate reactants diffusion and transfer without resistance. PIL-EY[M] exhibits a 3 times higher adsorption rate of CO 2 compared to EY[M] (Fig.S24), improving the mass transfer of the CO 2 reduction reaction. In addition, we monitored the color change of the PIL-EY[M] in a solution containing alkaline phenolphthalein exposed to the CO 2 environment. The color of phenolphthalein fades due to the consumption of hydroxide ions (OH - ) dissolved in CO 2 in the presence of carbonic acid. Therefore, the length of fading time can be used to reflect the diffusion rate of CO 2 in the catalyst solutions 30 . It is worth noting that the micropores of PIL are extremely hydrophobic (Fig.S25), which allows their pores to be well preserved in aqueous solutions. To prevent color overlap of the orange PIL-EY[M] and EY[M] aqueous solution, the thymolphthalein, which appears blue under alkaline conditions, is replaced by the red phenolphthalein (Fig. S26). At the same CO 2 flow rate, the color change of PIL-EY[M] is more pronounced than that of EY[M] and PIL (Fig. 4a). The complete faded solution in PIL, EY[M] and PIL-EY[M] takes about 126s, 93s and 57s, respectively. This indicates that the permanent porosity in the Newtonian fluid photocatalyst makes gas mass transfer no longer the limiting step of liquid catalysts. However, due to the easy aggregation of powdered catalysts, the contact area between CO 2 and PIL is limited, leading to a hard diffusion in the aqueous phase with the slowest mass transfer time. Further in-situ infrared spectroscopy was used to detect the adsorption vibration changes of CO 2 intermediates (Fig.4b). The signal intensity of PIL-EY[M] is significantly stronger than that of PIL. The reaction intermediates in PIL showed a linear adsorption state dominated by *C-O, with a peak at 2263 cm -1 , which may be attributed to *CO 2 and *COOH combinations. The wide peaks were observed at 2137 cm -1 , 2069 cm -1 , and 1997 cm -1 , which overlapped and belonged to the bridged adsorption of *C-O in PIL imidazole sites (Fig.S27). The bridged adsorption mode is generally considered to be a more stable chemical adsorption than linear adsorption 31 . Bridged adsorption peaks of PIL-EY[M] gradually become dominant compared to PIL during the 0-20 minutes reaction process, which is attributed to the formation of CO 2 intermediates adsorption at the interface between PIL and EY[M]. The DFT theoretical calculation results indicate that CO 2 intermediates adsorbed at the interface between PIL and EY[M] have more advantageous adsorption energy (Fig. S28). Their advantages are manifested in more electron-enriched sites, faster adsorption kinetics and lower thermodynamic reaction energy barriers (Fig.S29-S31). Therefore, the interaction between the solid-liquid interface of Newtonian fluid photocatalysts is also crucial for the improved photocatalytic performance. Large-scale application characteristics of Newtonian fluid photocatalyst As Newtonian fluid photocatalysts with fluidity and viscosity having application advantages in amplification reactions, The PIL-EY[M] can be uniformly coated on the inner surface of the bottom of a 36L square glass reactor, and a 0.6m*0.6m quartz cover plate was sealed on the top to form a scale-up solar CO 2 reduction device (Fig.4c). The CO 2 was continuously introduced for two hours to fill the reduction device for outdoor testing, and 10ml of water was added as the proton donor. The reaction was conducted from 11:00 to 16:00 every day (Fig.4d). Under an average sunlight intensity of 35 mW/cm 2 in outdoor testing, the CO production rate in five hours was 613.51 μmol/m 2 (Fig.4e). Comparison of CO evolution performance on day 1, day 4 and day 7 confirms its long-term stability (Fig.S32). Compared to simulated light sources, the light intensity under real sunlight is reduced by a maximum of 39.5 times, but the performance is only reduced by a maximum of 10.1 times. Therefore, the performance of the photocatalyst did not decrease, and the decrease in yield may only be related to the light intensity. Currently, attempts to scale up reaction systems in the field of photocatalysis are still limited by the difficulty of immobilizing powder state, and can only be conducted by laying the devices horizontally 32,33 . The variation in solar elevation angle alters the solar radiation intensity, impacting the surface photon absorption rate of the catalysts and consequently leading to the performance decline in horizontal conditions (Fig.S33). The Newtonian fluid photocatalyst can adjust the carrier tilt angle by changing the incident solar elevation angle to increase the production rate without catalyst consumption. In addition, the preparation strategy of Newtonian fluid catalysts can be extended to various photocatalysts. Taking typical powder organic photocatalyst carbon nitride (C 3 N 4 ) and inorganic photocatalyst titanium dioxide (TiO 2 ) as examples. By coating a Polyimidazolium layer on the surface of TiO 2 and C 3 N 4 , and then grafting liquid end EY[M] onto the surfaces, Newtonian fluid photocatalysts TiO 2 PIL-EY[M] and C 3 N 4 PIL-EY[M] can be formed in a state similar to PIL-EY[M]. They also exhibit fluidity, uniformity, viscosity, and paintability (Fig.4f, Fig. S34, Video 1 and 2). At the same time, Newtonian fluids TiO 2 PIL-EY[M] and C 3 N 4 PIL-EY[M] also showed improved CO 2 reduction ability (Fig.S35). However, when removing the Polyimidazolium layer or EY from TiO 2 PIL-EY[M] and C 3 N 4 PIL-EY[M], the TiO 2 and C 3 N 4 will separate (Fig.4f, Fig. S34), ultimately preventing the formation of Newtonian fluids. Therefore, the electrostatic interaction between the solid and liquid ends is the key to the formation of this type of Newtonian fluid photocatalyst. The construction strategy of solid-liquid interaction can achieve universal synthesis of various Newtonian fluid photocatalysts. Methods Materials Deionized water (DI water) was employed in all experiments. Sodium dodecyl benzene sulfonate (SDBS, A.R.), Potassium persulfate (KPS, A.R.), Styrene (St, A.R.), Divinylbenzene (DVB, A.R.), 1-Vinylimidazole (VIM, A.R.), tetrahydrofuran (THF, A.R.), Polyether amine (M2070), 1,6-Diaminohexane (A.R.), acetic acid (A.R.), formaldehyde (A.R.), methylglyoxal (A.R.) were obtained from Sinopharm Chemical Reagent Co., Ltd. INHONG GAS Company supplied carbon dioxide (CO 2 ) and nitrogen (N 2 ). Synthesis of polystyrene (PS) microspheres The PS microspheres were synthesized by emulsion polymerization, using SDBS as an emulsifier and KPS as an anionic initiator. The reaction was conducted under a nitrogen atmosphere, and 200 mL of DI water and 50 mL of ethanol were added into a 500 mL three-necked flask containing 0.5 g of SDBS. After adequately dispersing the SDBS, 12.5 mL of St, 3 mL DVB, and 0.25 g KPS were added into the reactor. Then, the polymerization was conducted in an oil bath at 80 °C, with shaking at 300 rpm, for 12 h. Eventually, the PS microspheres were collected by high-speed centrifugation at 10,000 r/min, and finally vacuum dried at 50 °C for further use. Synthesis of PIL The PIL hollow spheres were obtained by combining the template strategy. Specifically, 0.05g of the as-prepared PS microspheres was added to 37.5 mL DI water in a flask under stirring. In this state, 1 mL DVB and 2 mL VIM were added to the flask with continuous agitation for 1 h. Then, 6 mL KPS solution (0.5 wt%) was added to this system at 75 °C. After keeping stirring for 24 h at this temperature, the precursor of PIL spheres was obtained. Then, the PIL hollow spheres were obtained by etching the PS core with THF and separating by high-speed centrifugation at 10000 r/min. Synthesis of PIL-EY[M] PIL-EY[M] were prepared by electrostatic self-assembly of PIL hollow spheres and EY[M]. The PIL hollow spheres (0.1g) were dispersed in 15 mL DI water, a specified amount of EY was added to the PIL hollow spheres suspension. After stirring for 1 h at 60 °C, M2070 in the same amount as EY was slowly added to the mixture solution, stirred at 70 °C until it turned into a red viscous liquid. Synthesis of EY[M] A specified amount of EY was added to the PIL hollow spheres suspension. After stirring for 1 h at 60 °C, M2070 in the same amount as EY was slowly added to the mixture solution, stirred at 70 °C until it turned into a red viscous liquid. Synthesis of TiO 2 and C 3 N 4 covered with the imidazole cation layer 0.5g TiO 2 or C 3 N 4 , DI water (10mL),1,6-Diaminohexane (0.5mL), acetic acid (2mL) were sequentially added to a round bottom flask and sonicated for 0.5 hours. After that, formaldehyde (0.71mL) and methylglyoxal (1.47mL) were added and stirred at room temperature for 24 hours. The final product is washed with water and ethanol. Synthesis of TiO 2 -EY[M] and C 3 N 4 -EY[M] Similar to the PIL-EY[M] synthesis process, the difference is that TiO 2 and C 3 N 4 covered with the imidazole cation layer were used instead of PIL Photocatalysis experiments The entire photocatalytic CO 2 reduction reaction was carried out in a gas-solid mode in a 250 mL quartz glass device with good translucency. The PIL-EY[M] were painted on a poly (vinylidene fluoride) membrane with a radius of 25mm while weighing the weight of the PIL-EY[M] load, and the membrane coated with the photocatalyst was put on the platform in the reaction device. The water vapor environment was constructed by the introduction of 1 mL of water. A low-energy 360 nm LED visible light source was 5 cm away from the membrane. The detailed schematic diagram of the device is shown in Fig. S17. Before turning on the light, breathe with high-purity CO 2 gas for 15 min to eliminate other gases, and maintain the reaction temperature at room temperature by flowing water. During light irradiation, the gas products were analyzed by a Tetchrom gas chromatograph (GC2030) with a flame ionization detector (FID) and thermal conductivity detector (TCD). TA spectroscopy Time-resolved experiments were carried out on laser-based spectroscopy, with laser powers equating to less than one photon absorption per particle. Samples for transient absorption experiments were kept in dark between each measurement. A Coherent Legend Ti: Sapphire amplifier (800 nm, 100 fs pulse length, 3 kHz repetition rate) was used. The output is split to pump and probe beams. Excitation pulses at the wavelength of 450 nm were acquired using an optical parametric amplifier (Topas C, Light Conversion). The probe pulses (a broad supercontinuum spectrum) were generated from the 800-nm pulses in a CaF 2 crystal and split by a beam splitter into a probe pulse and a reference pulse. The probe pulse and the reference pulse were dispersed in a spectrograph and detected by a diode array. Instrumental response time is ∼100 fs. Characterization Power X-ray diffraction (XRD) was performed by a 9 kW Rigaku Smartlab X-ray diffractometer with Cu Kα radiation. The morphology and element distribution were characterized by high-resolution transmission electron microscopy (FEI TALOS F200X) and scanning electron microscope (Regulus 8100) with energy dispersive spectroscopy. XPS was implemented on an X-ray photoelectron spectrum (Thermo SCIENTIFIC ESCALAB Xi+), and C 1s 284.8 eV as reference. The element-selective X-ray absorption fine structure measurements were performed on the Shanghai Synchrotron Radiation Facility, and the data were analyzed by Athena software. The optical absorption properties were measured over a UV-2600 UV-vis DRS spectrophotometer with BaSO 4 powder as a reference. 13 C-isotopic tracer was investigated through gas chromatography-mass spectrometry (Shimadzu GC-MSQP2020). Brunauer-Emmett-Teller (BET) specific surface areas were recorded on a Micromeritics TriStar Ⅱ 3020M instrument. CO 2 adsorption was analyzed by the QUADRASORB evo instrument. The gas products were detected by a gas chromatography-mass spectrometer (GC-MS, Agilent Technologies) in the isotopic 13 CO 2 experiment. In-situ FT-IR experiments were recorded on a Thermo Scientific Nicolet iS50 FTIR with drift accessory. First, the material is loaded into the reaction chamber and paved, and the sample position is located below the center of three windows, including a quartz window and two infrared-transparent windows. Then, high-purity nitrogen containing water vapor is run through the reaction tank to keep the signal stable under dark conditions for 60 min. Subsequently, infrared data of CO 2 adsorption on the catalyst began to be recorded under a continuous flow of high-purity CO 2 gas. After the signal is stabilized, turn on the LED light and record the infrared data during the CO 2 photoreduction process. Photoelectrochemical measurements Photoelectrochemical tests were performed on a three-electrode system using a CH660E electrochemical workstation. Pt and Ag/AgCl electrodes were used as counter and reference electrodes, respectively. The saturated calomel electrode, Pt wire, and FTO were used as the reference electrode, counter electrode, and working electrode. The catalyst (1 mg) was added into 1 mL of ethanol, ultrasonic for 30 min, and uniformly added to an area of 1 cm × 1 cm on FTO. Mott-Schottky and photocurrent measurements were carried out in 0.5 M sodium sulfate solution. Electrochemical impedance spectroscopy properties were tested in potassium ferricyanide solution. DFT calculations The geometry optimization and excited-state calculations were performed by B3LYP-D3BJ exchange-correlation functional with the 6-311G(d) basis set based on the Gaussian 16 C.01 code. Frequency calculations were performed to ensure that the stability configuration has no imaginary frequency. Independent gradient model (IGM) 34,35 , Reduced density gradient (RGD), Frontier molecular orbital, the distribution of electrons and holes in the electron excitation process 35 , and interfragmentary charge transfer were calculated with Multiwfn 3.8 (dev) 36 . Molecular dynamics simulation, conducted using CP2K software. All structures and isosurfaces images were visualized by VMD 1.9.3. and VESTA. The single-point energy was calculated by M06-2X/def2-TZVPP level. The adsorption energy (E ads ) of CO 2 (Equation 1). E ads (CO 2 ) = E(*CO 2 ) - E(*) - E(CO 2 ) (1) Where E(*CO 2 ), E(*) and E(CO 2 ) were the total energy of samples with CO 2 adsorbed on the surface, the energy of the pristine sample surface and CO 2 , respectively. At room temperature, the Gibbs free energy for each model was calculated by the following equation (Equation 2): G(T) = E ele + G corr (T) = E ele + ZPE + ΔG 0→T (2) Where E ele , G corr (T), ZPE and ΔG 0→T were electronic energy, thermal corrections to Gibbs free energy, zero-point energy and contribution by heating the system from 0 K to 298.15 K, respectively. Conclusion In summary, we have synthesized a flowing viscous Newtonian fluid material, which is grafted from internal hollow spheres and external liquid chains, for more convenient material applications and more efficient photocatalytic conversion. Experimental results show that, compared to powder catalytic systems, Newtonian fluid photocatalysts can be more uniformly and stably painted on non-planar surfaces, which enables the catalyst to cope with the effects of wind speed and solar altitude angle under natural conditions. At the same time, the permanent porosity and the solid-liquid interface of a Newtonian fluid enable better adsorption, mass transfer, and conversion. In the application of photocatalytic reduction of CO 2 , the PIL-EY[M] achieved a 100% selective CO overflow efficiency, which is 57.8 times higher than that of the PIL, with a stable performance under long-time and large-scale solar radiation. Viscous Newtonian fluid photocatalysts have shown potential for commercial feasibility by expanding the application scope of photocatalysis. In addition, by taking the most commonly used inorganic and organic photocatalysts TiO 2 and C 3 N 4 as examples, Newtonian fluid photocatalysts TiO 2 PIL-EY[M] and C 3 N 4 PIL-EY[M] with similar viscosity and fluidity were synthesized, demonstrating the universal synthesis of this type of Newtonian fluid photocatalysts. Declarations Competing interests The authors declare no competing interests. Author contributions Z.Y.L., Y.C. and Y.R.X. performed the experiments, data analysis and wrote the paper. L.G.T. and H.P.L. performed the computer simulations. T.H.Z., K.Z and W.D.S conceived the ideas and designed the experiments. Acknowledgements This work was supported by the National Natural Science Foundation of China (22225808, U24A20551, 22278190), Qing Lan Project of Jiangsu Province (2023), Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment, Jiangsu Graduate Research Innovation Program (KYCX25_4257), Open Project of State Key Laboratory of Structural Chemistry (20230022). Data availability Source data are provided with this paper. All other data that support this study are available from the corresponding authors upon reasonable request. References Li, J. , et al. Molecular-scale CO spillover on a dual-site electrocatalyst enhances methanol production from CO 2 reduction. Nat. Nanotechnol. , 10.1038/s41565-025-01866-8, (2025). Ye, J. , et al. Hydrogenation of CO 2 for sustainable fuel and chemical production. Science 387 , eadn9388 (2025). Yin, S. , et al. Boosting water decomposition by sulfur vacancies for efficient CO 2 photoreduction. Energy Environ. 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Supplementary Files SupportingInformation.docx Supporting information Video1.mp4 fluidity, uniformity and viscosity exhibition Video2.mp4 paintability exhibition Cite Share Download PDF Status: Published Journal Publication published 20 Mar, 2026 Read the published version in Nature Communications → 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. 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1","display":"","copyAsset":false,"role":"figure","size":510373,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ea,\u003c/strong\u003e Schematic and optical images of the fabrication process. \u003cstrong\u003eb,\u003c/strong\u003e Rheological experiment of PIL-EY[M]. \u003cstrong\u003ec, \u003c/strong\u003eHigh-resolution TEM images of PIL. \u003cstrong\u003ed,\u003c/strong\u003e Solid-state \u003csup\u003e13\u003c/sup\u003eC NMR of PIL. \u0026nbsp;\u003cstrong\u003ee,\u003c/strong\u003e FTIR spectroscopy of PIL, EY and PIL-EY[M].\u003c/p\u003e","description":"","filename":"1.png","url":"https://assets-eu.researchsquare.com/files/rs-7844074/v1/6d2c58563e5f88e40a7b8ae0.png"},{"id":94160964,"identity":"6d6a10a7-767d-4282-b980-af24e751ce74","added_by":"auto","created_at":"2025-10-23 04:42:07","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":679582,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ea,\u003c/strong\u003e Fluidity of Newtonian fluid photocatalysts. \u003cstrong\u003eb, \u003c/strong\u003eViscosity of Newtonian fluid photocatalysts. \u003cstrong\u003ec,\u003c/strong\u003e Printing coating on various carriers. \u003cstrong\u003ed,\u003c/strong\u003e Newtonian fluids facing strong wind conditions. \u003cstrong\u003ee, \u003c/strong\u003eNewtonian fluid photocatalysts applied face down. \u003cstrong\u003ef,\u003c/strong\u003e Easily erasable Newtonian fluid. \u003cstrong\u003eg, \u003c/strong\u003eMelting point and flow stability of Newtonian fluid photocatalysts. \u003cstrong\u003eh,\u003c/strong\u003e The RDG analysis of PIL and EY[M].\u003cstrong\u003e i, \u003c/strong\u003eThe IGM analysis of PIL and EY[M].\u003cstrong\u003e j, \u003c/strong\u003eSimulated size\u003cstrong\u003e \u003c/strong\u003eof EY[M].\u003c/p\u003e","description":"","filename":"2.png","url":"https://assets-eu.researchsquare.com/files/rs-7844074/v1/a3ea68e9bba7ce115fd83ce2.png"},{"id":94160556,"identity":"b3b397ae-0e1c-4a13-8254-ae2a5bc34b84","added_by":"auto","created_at":"2025-10-23 04:34:07","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":447042,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ea,\u003c/strong\u003e Photocatalytic CO\u003csub\u003e2\u003c/sub\u003e reduction production of CO. \u003cstrong\u003eb,\u003c/strong\u003e 25 hours CO\u003csub\u003e2\u003c/sub\u003e reduction production of CO. \u003cstrong\u003ec,\u003c/strong\u003e The CO\u003csub\u003e2 \u003c/sub\u003ereduction performance of different catalysts (The corresponding information is presented in Tab.S2). \u003cstrong\u003ed, \u003c/strong\u003eIsotopic \u003csup\u003e13\u003c/sup\u003eCO\u003csub\u003e2\u003c/sub\u003e experiment. \u003cstrong\u003ee,\u003c/strong\u003e UV-vis spectra before and after reaction of PIL-EY[M] and EY. \u003cstrong\u003ef,\u003c/strong\u003e The TDDFT calculations at the lowest energy excited state and the differential charge density of PIL-EY[M]. \u003cstrong\u003eg, \u003c/strong\u003eThe mono-exponential fit of PIL-EY[M] dynamics at 440 nm.\u003c/p\u003e","description":"","filename":"3.png","url":"https://assets-eu.researchsquare.com/files/rs-7844074/v1/06a52e45999ee6acd5a29da6.png"},{"id":94160965,"identity":"db67edd3-a3d6-4343-aad2-c0a221aea0f1","added_by":"auto","created_at":"2025-10-23 04:42:07","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":845060,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ea, \u003c/strong\u003eCO\u003csub\u003e2\u003c/sub\u003e mass transfer experiments of PIL-EY[M], EY[M] and PIL. \u003cstrong\u003eb,\u003c/strong\u003e In-situ infrared spectroscopy of PIL and PIL-EY[M]. \u003cstrong\u003ec, \u003c/strong\u003eSchematic of the overview of a 0.6*0.6*0.1 m\u003csup\u003e2\u003c/sup\u003e-scale CO production facility\u003cstrong\u003e. d, \u003c/strong\u003eOptical image of scale-up reaction under sunlight. \u003cstrong\u003ee, \u003c/strong\u003ePhotocatalytic CO\u003csub\u003e2\u003c/sub\u003e reduction production of CO in scale-up reaction under sunlight.\u0026nbsp; \u003cstrong\u003ef, \u003c/strong\u003eOptical image of Newtonian fluid photocatalysts TiO­\u003csub\u003e2\u003c/sub\u003ePIL-EY[M].\u003c/p\u003e","description":"","filename":"4.png","url":"https://assets-eu.researchsquare.com/files/rs-7844074/v1/ad1069e9ba1f4ae36baf90d5.png"},{"id":109158086,"identity":"e5634a02-c554-4b4c-8ae1-9a32647da1ca","added_by":"auto","created_at":"2026-05-13 07:07:24","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2942876,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7844074/v1/cddb75f1-2545-4ce3-a351-1e149c16a73f.pdf"},{"id":94160560,"identity":"a412fbfa-95e5-48cc-b110-2eac5e9493e0","added_by":"auto","created_at":"2025-10-23 04:34:07","extension":"docx","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":7214739,"visible":true,"origin":"","legend":"Supporting information","description":"","filename":"SupportingInformation.docx","url":"https://assets-eu.researchsquare.com/files/rs-7844074/v1/f6cc5c7a5161e5c396cfe504.docx"},{"id":94160573,"identity":"a51477d6-d886-4786-b25a-61dd998664f7","added_by":"auto","created_at":"2025-10-23 04:34:08","extension":"mp4","order_by":2,"title":"","display":"","copyAsset":false,"role":"supplement","size":50091507,"visible":true,"origin":"","legend":"\u003cp\u003efluidity, uniformity and viscosity exhibition\u003c/p\u003e","description":"","filename":"Video1.mp4","url":"https://assets-eu.researchsquare.com/files/rs-7844074/v1/bf570bcead1b6ba9941aca9c.mp4"},{"id":94160569,"identity":"5aa3939a-7f0e-4444-ae42-6c7d84300bc6","added_by":"auto","created_at":"2025-10-23 04:34:07","extension":"mp4","order_by":3,"title":"","display":"","copyAsset":false,"role":"supplement","size":11839747,"visible":true,"origin":"","legend":"\u003cp\u003epaintability exhibition\u003c/p\u003e","description":"","filename":"Video2.mp4","url":"https://assets-eu.researchsquare.com/files/rs-7844074/v1/699596d8716e784ed7bdabbd.mp4"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"\u003cp\u003ePrintable Newtonian fluid photocatalysts for scale-up solar CO\u003csub\u003e2\u003c/sub\u003e conversion\u003c/p\u003e","fulltext":[{"header":"Introduction","content":"\u003cp\u003ePhotocatalysis is a green and sustainable manner for converting solar energy into high-value chemicals, which has the potential to become an important tool for addressing climate change and environmental crises\u003csup\u003e1,2\u003c/sup\u003e\u003csup\u003e,\u003c/sup\u003e\u003csup\u003e3,4\u003c/sup\u003e. In the past few decades, various semiconductor photocatalysts have been developed, including nanotubes\u003csup\u003e5\u003c/sup\u003e, nanosheets\u003csup\u003e6\u003c/sup\u003e, amorphous nanoparticles\u003csup\u003e7\u003c/sup\u003e, alloys\u003csup\u003e8\u003c/sup\u003e, and so on\u003csup\u003e4,9\u003c/sup\u003e, dedicated to improving the intrinsic catalytic activity during the reaction process. Although significant progress has been made in the performance of photocatalysts and the exploration of reaction mechanisms, the demand for suitable large-scale reactions has not been well explored. The amplification of photocatalytic systems needs to consider the practicality of catalysts beyond their performance\u003csup\u003e10\u003c/sup\u003e. At present, immobilized photocatalyst reactors are the main form for achieving large-scale photocatalysis, where photocatalysts are fixed to a matrix to prevent loss of catalysts in outdoor reaction environments\u003csup\u003e11,12\u003c/sup\u003e. For example, Wang et al. prepared a porous hydrogel nanocomposite photocatalysis platform with an area of 1m\u003csup\u003e2\u003c/sup\u003e by embedding a large number of photocatalysts into the hydrogel macroporous matrix\u003csup\u003e13\u003c/sup\u003e; Zhu et al. prepared a 1600cm\u003csup\u003e2\u003c/sup\u003e photocatalytic hydrogen production platform by immobilizing powder photocatalysts on a super-hydrophilic wood fiber matrix using gradient alignment theory\u003csup\u003e14\u003c/sup\u003e. Although these scaled-up methods have broad applicability in accommodating various types of nanoscale photocatalytic fillers, the matrix of the encapsulated photocatalyst interrupts the active material conduction chain between the catalysts and the effective charge transfer between the catalyst and reactants (such as small gas molecules) at the catalytic interface. Therefore, it is required to design a photocatalyst that can achieve simple amplification without the need for a large matrix.\u0026nbsp;\u003c/p\u003e\n\u003cp\u003eNewtonian liquid is an ideal viscous liquid proposed by Newton in 1687, whose viscosity remains constant regardless of the shear rate. This characteristic makes it a stable coating material that can be easily coated on flat surfaces. Compared with embedding a large amount of catalyst into the matrix, the method of expanding the photocatalytic reaction scale by simply coating and brushing to increase the reaction area can not only improve performance, but also eliminate the cumbersome \u0026quot;matrix-catalyst\u0026quot; binding relationship and additional pre-operation costs. The stable and uniform liquid catalyst formed by grafting liquid ends on the surface of microporous nanoparticles has been proven to have promising prospects in the field of photocatalysis\u003csup\u003e15,16\u003c/sup\u003e\u003csup\u003e,\u003c/sup\u003e\u003csup\u003e17\u003c/sup\u003e. However, these liquid catalysts lack viscosity due to weak surface tension, making it difficult to stably coat them on steep slopes, grilles, or in strong wind environments.\u0026nbsp;It is considered that the intramolecular interaction of the solvent or the solvent and solute causes the liquid to generate resistance in the flow, which increases the surface tension of the liquid and thus produces viscosity\u003csup\u003e18\u003c/sup\u003e. Inspired by this, the liquid chain with a large steric hindrance is spatially confined around its side chains, and then grafted with microporous nano-semiconductors through weak molecular forces, such as electrostatic action, to form a strong viscous Newtonian fluid that responds to non-horizontal or open natural conditions\u003csup\u003e19,20\u003c/sup\u003e. Unfortunately, since the liquid chain cannot be photoexcited, the internal catalyst surface radiation is attenuated, giving fluidity while sacrificing photocatalytic activity. Therefore, a rational design of high-performance and strong surface tension liquid catalysts would hold further interest.\u003c/p\u003e\n\u003cp\u003eIn this study, we propose a viscous Newtonian fluid catalyst composed of internal microporous nano-hollow spheres with positive potential and external negative potential assisted catalytic liquid chains for simple scaling up of photocatalysis. Due to the electrostatic interactions between the inner and outer components and the significant steric hindrance effect of the liquid chains, the Newtonian fluid catalyst exhibits robust flow resistance, making it easy to apply and stabilize loads in strong winds and non-horizontal environments such as grids, slopes, and even downward orientations. On the other hand, the liquid chain that can be light-excited was designed as an electron donor to improve the electron enrichment degree of internal nano-hollow spheres, thereby promoting reactant adsorption and rapid light conversion.\u0026nbsp;Theoretical and experimental verification have demonstrated the practical advantages of Newtonian fluid catalysts in photocatalysis.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eThe structure of Newtonian fluid photocatalysts\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eTo achieve the viscous and flowing effect of Newtonian fluids while maintaining photocatalytic performance, we divide the catalyst into two parts: an inner and an outer part. The microporous nano-hollow spheres, serving as the inner part, act as the primary catalytic contributor. In this regard, the polymerization of imidazolium (PIL) rings, which possess a strong positive potential and an electron-enriched site, can serve as the adsorption and conversion sites of reactants. The outer parts are long polymer liquid chains (EY[M]) grafted by Eosin Y (EY) and Polyether amine (M2070), which can ionize anions EY[M]\u003csup\u003e∙‑\u003c/sup\u003e for combining with PIL from electrostatic attraction and act as electron donors. Schematic (Fig.1a) and optical images show the main preparation process. Firstly, the PIL was synthesized by the polymerization of divinylbenzene and 1-vinylimidazole on the surface of the PS sphere as templates (Fig.S1). Then, by etching templates, PIL forms the hollow states and micropore surface. The optical images show that the PIL is a white powder. The EY[M] is formed by the dehydration condensation reaction (Fig.S2). EY[M] appears as a dark red semi-translucent liquid. Finally, PIL and EY[M] are self-assembled by electrostatic action to form a viscous fluid catalyst (PIL-EY[M]). The molecular structure is shown in Fig.1a. The fluid rheology experimental results of PIL-EY[M] show that the ratio of shear stress to shear rate is a constant (Fig.1b). Therefore, the viscosity of PIL-EY[M] does not change with the change of shear rate, which belongs to a Newtonian fluid\u003csup\u003e19\u003c/sup\u003e, the viscosity of PIL-EY[M] is 6386.21 mPa∙s.\u003c/p\u003e\n\u003cp\u003eSubsequently, a series of characterizations were conducted to demonstrate the structure of PIL-EY[M]. The morphology of PIL is spherical with a hollow diameter of around 370 nm inside (Fig.1c, Fig.S3), and there are positive potential (+32.6 mV) multiple microporous structures on its surface (Fig.S4, Tab.S1). These hollow and microporous materials are used to increase reactant mass transfer inside the Newtonian fluid photocatalyst. The \u003csup\u003e13\u003c/sup\u003eC Solid State Nuclear Magnetic Resonance (SSNMR) was used to demonstrate the composition of PIL (Fig.1d). The peaks at 138 ppm and 128 ppm belong to the imidazole carbon\u003csup\u003e21\u003c/sup\u003e, the peaks around 145 ppm and 113 ppm are attributable to the phenyl carbon\u003csup\u003e22\u003c/sup\u003e, and the other peaks belong to the carbon chain. Two broad diffraction peaks at 13.3\u0026deg; and 27.5\u0026deg; were observed in the X-ray diffraction (XRD) pattern of PIL (Fig.S5), attributed to the planar stacking of imidazole rings and the interlayer stacking of aromatic rings, respectively. The PIL-EY[M] did not detect the above two peaks, and their signals were completely covered by the EY[M], showing a peak located at 21.6\u0026deg;, which belongs to the amorphous diffraction of M2070\u003csup\u003e23\u003c/sup\u003e. The X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared (FTIR) spectroscopy further confirmed the detailed information of the PIL (Fig.1e and Fig.S6). In the TEM image of EY[M], small negatively charged (-32.3 mV) nanoclusters (\u0026lt;5 nm) can be observed (Fig.S7), which are formed due to the monomers and dimer-aggregates of EY\u003csup\u003e24\u003c/sup\u003e (Fig.S8). These nanoclusters serve as the \u0026ldquo;head\u0026rdquo; for binding with PIL. In the FTIR spectrum of EY[M], there is an added peak at 1670 cm\u003csup\u003e-1\u0026nbsp;\u003c/sup\u003e(Fig.1e), which represents the -NH- groups formed by the dehydration condensation of EY and M2070. The PIL-EY[M] still maintains the nanosphere morphology. TEM and mapping images indicate that EY[M] is wrapped around the outer surface of PIL (Fig.S9-S10).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eCharacterization of Newtonian fluid photocatalysts\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe stable fluidity and viscosity of the catalyst at room temperature are expected to yield unique features that are advantageous for the scale-up of photocatalysis. To achieve a coating effect, a viscous and slowly flowing Newtonian fluid photocatalyst can be controlled by adjusting the synthesis ratio of the inner and outer parts. In the optical images (Fig.2a), it can be observed that when flipping the bottle containing PIL-EY[M], the PIL-EY[M] flows slowly downwards under the influence of gravity. By pressing the PIL-EY[M] in the syringe, it can drip (Fig.2b). By dipping the needle into the PIL-EY[M] and applying an upward force, the PIL adheres to the needle and exhibits strong upward flow resistance. These indicate that the PIL-EY[M] takes into account both viscosity and fluidity at room temperature and can be coated onto a carrier using a brush, greatly improving efficiency compared to the matrix preparation and catalyst embedding processes in conventional photocatalytic amplification platforms. There properties make it suitable for brush coating on various carriers (such as plastic, wood, metal, et al.) and even grids (Fig.2c). In contrast, the powder photocatalysts are limited to planar carriers in sealed conditions, as powder are difficult to fix under non-horizontal plane environments such as inclined plain or facing downwards, and are also prone to mass loss due to being blown away in open air. In a simulated open environment with a wind speed of 18m/s (equivalent to an 8-level typhoon) for 20 min (Fig.2d), the PIL-EY[M] has no significant photocatalyst mass loss (Fig.S11), and it can maintain stability in non-horizontal planes or even vertically downward states for 180 days. Despite all this, strong viscosity does not mean difficult to recycle, the PIL-EY[M] can be removed from the carrier using organic solvents such as N,N-Dimethylformamide and ethanol, and can be recovered by washing with these solvents (Fig.2e). The thermal decomposition temperature and melting temperature of PIL-EY[M] are 235 \u0026deg;C and -40 \u0026deg;C (Fig.2g, Fig.S12), respectively, which indicate that it can remain the fluidity and viscosity for most climate environments on Earth.\u003c/p\u003e\n\u003cp\u003eWeak intermolecular forces, such as electrostatic interactions, can cause the\u0026nbsp;flow resistance, which is one of the reasons for the\u0026nbsp;PIL-EY[M]\u0026nbsp;viscosity. Reduced Density Gradient (RDG)\u0026nbsp;and Independent Gradient Model (IGM) analysis were used to evaluate the weak intermolecular forces between PIL and EY[M] (Fig.S13). The RDG analysis results confirmed the existence of a prominent weak interaction force (blue iso surface) between PIL and EY[M], which can be reasonably inferred as an electrostatic force between them (Fig.2h). As shown in Fig.S14, the black and red dots are defined as intramolecular and intermolecular forces. The IGM analysis results clearly indicate the intermolecular forces between PIL and EY[M]. After eliminating the interference of atomic density gradients, IGM analysis visualizes the real binding environment. The results reveal an ideal intermolecular interaction between PIL and EY[M] (Fig.2i), where the blue surface is attributed to electrostatic binding force, while the green surface reflects the spatial potential resistance and dispersion effect with low electron density\u003csup\u003e25\u003c/sup\u003e. It is worth noting that the length and width of EY[M] reach 22.97 \u0026Aring; and 21.22 \u0026Aring;, respectively (Fig.2j). Such a large-sized EY[M] cannot pass through the micropores on the PIL surface or enter the hollow structure. The micropores of PIL are well preserved for enhancing the adsorption and mass transfer of reactants in photocatalytic reactions.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eThe photocatalytic advantages and mechanism of Newtonian fluid photocatalysis\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe photocatalytic CO\u003csub\u003e2\u003c/sub\u003e conversion reaction is one of the most common reactions in the field of photocatalysis, and the unique advantages of Newtonian fluid photocatalysts in practical applications are analyzed through CO\u003csub\u003e2\u003c/sub\u003e reduction reactions. The detailed description and light source information of the photocatalytic CO\u003csub\u003e2\u003c/sub\u003e reduction measurement experiment are provided in Fig.S15. The performance testing was conducted under gas-solid conditions, where the PIL-EY[M] was coated onto a carrier film, and the PIL is dispersed on the carrier with the same area for detection. Optical images indicate that compared to powder catalysts, Newtonian fluid photocatalysts can be coated more uniformly on the surface of the carrier with less mass (Fig.S16), which greatly saves catalyst usage and maximizes the reaction contact area between the catalytic surface and CO\u003csub\u003e2\u003c/sub\u003e. After five hours of simulated light reaction, CO was the only product in all samples. The results showed that the CO yield of PIL, EY, and EY[M] were 21.24 \u0026mu;mol h\u003csup\u003e-1\u003c/sup\u003e m\u003csup\u003e-2\u003c/sup\u003e, 87.82 \u0026mu;mol h\u003csup\u003e-1\u003c/sup\u003e m\u003csup\u003e-2\u003c/sup\u003e and 80.83 \u0026mu;mol h\u003csup\u003e-1\u003c/sup\u003e m\u003csup\u003e-2\u003c/sup\u003e, respectively\u0026nbsp;(Fig.3a). In contrast, the CO evolution rates of PIL-EY[M] reached 1228.68 \u0026mu;mol h\u003csup\u003e-1\u003c/sup\u003e m\u003csup\u003e-2\u003c/sup\u003e, which was 57.84, 13.99 and 15.20 times of PIL, EY and EY[M], respectively. The long-term reaction test of the photocatalysts showed that the yield of PIL and EY gradually decreased after stable for 10 hours during the continuous reaction of 25 hours (Fig.3b). The CO yield of PIL-EY[M] remained stable, with an average yield of 1206.28 \u0026mu;mol h\u003csup\u003e-1\u003c/sup\u003e m\u003csup\u003e-2\u003c/sup\u003e over 25 hours, which was 58.61 times and 58.99 times higher than PIL and EY, respectively. Compared with the same type of imidazole photocatalysts, ion composite photocatalysts, and\u0026nbsp;different types of photocatalysts (Tab.S2-S3), PIL-EY[M] has outstanding performance increased multiplier factors, emphasizing the advantages of Newtonian fluid photocatalysts in photocatalytic systems (Fig.3c). The FT-IR and XPS characterization confirmed that there were no functional or structural changes observed after the PIL-EY[M] reaction (Fig.S17-S18). Subsequently, the isotopic \u003csup\u003e13\u003c/sup\u003eCO\u003csub\u003e2\u003c/sub\u003e experiment and a series of comparative experiments were conducted to demonstrate the photocatalytic activity of the product derived from Newtonian fluids (Fig.3d, Fig.S19).\u003c/p\u003e\n\u003cp\u003eExplain the advantages of Newtonian fluids in photocatalytic reactions from a mechanistic perspective. The UV absorption spectrum of PIL-EY[M] showed stronger absorption than EY[M], which may be due to the charge transfer (CT) state between PIL and EY[M] (Fig. 3e). As the reaction time increases, the peak at 516nm and 480nm strengthens, indicating an enhanced \u0026pi;/\u0026pi;* transition in PIL-EY[M]. In contrast, the absorption spectrum of EY decreases significantly with reaction time. By performing time-dependent density functional theory (TDDFT) calculations on the optimized structure of PIL-EY[M], it was found that the distance between the centers of mass of holes and electrons was as high as 3.69 \u0026Aring; at S0-S1 (Fig.3f, Fig.S20), corresponding to the contribution of charge-transfer excitation as the lowest energy excited state of PIL-EY[M], indicating a high degree of separation between electrons and holes\u003csup\u003e26\u003c/sup\u003e. It can be reasonably inferred that it belongs to \u0026pi;/\u0026pi;* charge transfer excitation in the EY to PIL direction. The charge difference calculation of PIL-EY[M] proves that the excited electrons gather on EY and are consumed on PIL, indicating that EY[M] can serve as an electron donor and PIL as an acceptor. A larger dipole moment of the excited state is more conducive to the charge transfer from the lowest excited state of EY[M] to PIL (Fig.S20). In addition, PIL-EY[M] has a larger ground state dipole moment (19.34 D) compared to PIL (1.63 D) and EY[M] (8.32 D), indicating that PIL-EY[M] is more conducive to photogenerated charge separation\u003csup\u003e27\u003c/sup\u003e, which is consistent with the results of weaker emission intensity, better electrochemical properties, and charge transfer density (Fig. S21-S22).\u0026nbsp;To gain a deeper understanding of the excited-state dynamics between EY[M] and PIL.\u0026nbsp;Immediately, femtosecond transient absorption spectroscopy (TAS) was conducted on PIL-EY[M] after excitation by a 420 nm laser pulse, the spectrum displayed a strong broad bleach centered at 538 nm, attributed to the singlet excited state absorption of EY[M]\u0026nbsp;(Fig.S23). The 420 nm - 490 nm range exhibited the characteristic absorption of the EY radical anion in ET[M], reaching a maximum at 440 nm.\u0026nbsp;The mono-exponential fit of PIL-EY[M] dynamics at 440 nm resulted in a lifetime of only 857.3 ps\u0026nbsp;(Fig.3g), indicating that exciton energy has been transferred from EY[M] radical anions to PIL, directly demonstrating effective electron transfer between EY[M] and PIL\u003csup\u003e28,29\u003c/sup\u003e.\u003c/p\u003e\n\u003cp\u003eThe availability of reactants and stable adsorption at catalyst sites are key steps in the photocatalytic reduction process. The weak adsorption capacity of CO\u003csub\u003e2\u003c/sub\u003e without porosity limits the development of liquid catalysts. The presence of permanent hollow pores in porous Newtonian fluid photocatalysts is expected to facilitate reactants\u003csub\u003e\u0026nbsp;\u003c/sub\u003ediffusion and transfer without resistance. PIL-EY[M] exhibits a 3 times higher adsorption rate of CO\u003csub\u003e2\u003c/sub\u003e compared to EY[M] (Fig.S24), improving the mass transfer of the CO\u003csub\u003e2\u003c/sub\u003e reduction reaction. In addition, we monitored the color change of the PIL-EY[M] in a solution containing alkaline phenolphthalein exposed to the CO\u003csub\u003e2\u0026nbsp;\u003c/sub\u003eenvironment. The color of phenolphthalein fades due to the consumption of hydroxide ions (OH\u003csup\u003e-\u003c/sup\u003e) dissolved in CO\u003csub\u003e2\u003c/sub\u003e in the presence of carbonic acid. Therefore, the length of fading time can be used to reflect the diffusion rate of CO\u003csub\u003e2\u003c/sub\u003e in the catalyst solutions\u003csup\u003e30\u003c/sup\u003e. It is worth noting that the micropores of PIL are extremely hydrophobic (Fig.S25), which allows their pores to be well preserved in aqueous solutions. To prevent color overlap of the orange PIL-EY[M] and EY[M] aqueous solution, the thymolphthalein, which appears blue under alkaline conditions, is replaced by the red phenolphthalein (Fig. S26). At the same CO\u003csub\u003e2\u003c/sub\u003e flow rate, the color change of PIL-EY[M] is more pronounced than that of EY[M] and PIL (Fig. 4a). The complete faded solution in PIL, EY[M] and PIL-EY[M] takes about 126s, 93s and 57s, respectively. This indicates that the permanent porosity in the Newtonian fluid photocatalyst makes gas mass transfer no longer the limiting step of liquid catalysts. However, due to the easy aggregation of powdered catalysts, the contact area between CO\u003csub\u003e2\u003c/sub\u003e and PIL is limited, leading to a hard diffusion in the aqueous phase with the slowest mass transfer time. Further in-situ infrared spectroscopy was used to detect the adsorption vibration changes of CO\u003csub\u003e2\u003c/sub\u003e intermediates (Fig.4b). The signal intensity of PIL-EY[M] is significantly stronger than that of PIL. The reaction intermediates in PIL showed a linear adsorption state dominated by *C-O, with a peak at 2263 cm\u003csup\u003e-1\u003c/sup\u003e, which may be attributed to *CO\u003csub\u003e2\u003c/sub\u003e and *COOH combinations. The wide peaks were observed at 2137 cm\u003csup\u003e-1\u003c/sup\u003e, 2069 cm\u003csup\u003e-1\u003c/sup\u003e, and 1997 cm\u003csup\u003e-1\u003c/sup\u003e, which overlapped and belonged to the bridged adsorption of *C-O in PIL imidazole sites (Fig.S27). The bridged adsorption mode is generally considered to be a more stable chemical adsorption than linear adsorption\u003csup\u003e31\u003c/sup\u003e. Bridged adsorption peaks of PIL-EY[M] gradually become dominant compared to PIL during the 0-20 minutes reaction process, which is attributed to the formation of CO\u003csub\u003e2\u003c/sub\u003e intermediates adsorption at the interface between PIL and EY[M]. The DFT theoretical calculation results indicate that CO\u003csub\u003e2\u003c/sub\u003e intermediates adsorbed at the interface between PIL and EY[M] have more advantageous adsorption energy (Fig. S28). Their advantages are manifested in more electron-enriched sites, faster adsorption kinetics and lower thermodynamic reaction energy barriers (Fig.S29-S31). Therefore, the interaction between the solid-liquid interface of Newtonian fluid photocatalysts is also crucial for the improved photocatalytic performance.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eLarge-scale application characteristics of Newtonian fluid photocatalyst\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eAs Newtonian fluid photocatalysts with fluidity and viscosity having application advantages in amplification reactions, The PIL-EY[M] can be uniformly coated on the inner surface of the bottom of a 36L square glass reactor, and a 0.6m*0.6m quartz cover plate was sealed on the top to form a scale-up solar CO\u003csub\u003e2\u003c/sub\u003e reduction device (Fig.4c). The CO\u003csub\u003e2\u003c/sub\u003e was continuously introduced for two hours to fill the reduction device for outdoor testing, and 10ml of water was added as the proton donor. The reaction was conducted from 11:00 to 16:00 every day (Fig.4d). Under an average sunlight intensity of 35 mW/cm\u003csup\u003e2\u0026nbsp;\u003c/sup\u003ein outdoor testing, the CO production rate in five hours was 613.51 \u0026mu;mol/m\u003csup\u003e2\u0026nbsp;\u003c/sup\u003e(Fig.4e). Comparison of CO evolution performance on day 1, day 4 and day 7 confirms its long-term stability (Fig.S32). Compared to simulated light sources, the light intensity under real sunlight is reduced by a maximum of 39.5 times, but the performance is only reduced by a maximum of 10.1 times. Therefore, the performance of the photocatalyst did not decrease, and the decrease in yield may only be related to the light intensity. Currently, attempts to scale up reaction systems in the field of photocatalysis are still limited by the difficulty of immobilizing powder state, and can only be conducted by laying the devices horizontally\u003csup\u003e32,33\u003c/sup\u003e. The variation in solar elevation angle alters the solar radiation intensity, impacting the surface photon absorption rate of the catalysts and consequently leading to the performance decline in horizontal\u003cstrong\u003e\u0026nbsp;\u003c/strong\u003econditions (Fig.S33).\u0026nbsp;The Newtonian fluid photocatalyst can adjust the carrier tilt angle by changing the incident solar elevation angle to increase the production rate without catalyst consumption. In addition, the preparation strategy of Newtonian fluid catalysts can be extended to various photocatalysts. Taking typical powder organic photocatalyst carbon nitride (C\u003csub\u003e3\u003c/sub\u003eN\u003csub\u003e4\u003c/sub\u003e) and inorganic photocatalyst titanium dioxide (TiO\u003csub\u003e2\u003c/sub\u003e) as examples. By coating a Polyimidazolium layer on the surface of TiO\u003csub\u003e2\u003c/sub\u003e and C\u003csub\u003e3\u003c/sub\u003eN\u003csub\u003e4\u003c/sub\u003e, and then grafting liquid end EY[M] onto the surfaces, Newtonian fluid photocatalysts TiO\u003csub\u003e2\u003c/sub\u003ePIL-EY[M] and C\u003csub\u003e3\u003c/sub\u003eN\u003csub\u003e4\u003c/sub\u003ePIL-EY[M] can be formed in a state similar to PIL-EY[M]. They also exhibit fluidity, uniformity, viscosity, and paintability (Fig.4f, Fig. S34, Video 1 and 2). At the same time, Newtonian fluids TiO\u003csub\u003e2\u003c/sub\u003ePIL-EY[M] and C\u003csub\u003e3\u003c/sub\u003eN\u003csub\u003e4\u003c/sub\u003ePIL-EY[M] also showed improved CO\u003csub\u003e2\u003c/sub\u003e reduction ability (Fig.S35). However, when removing the Polyimidazolium layer or EY from TiO\u003csub\u003e2\u003c/sub\u003ePIL-EY[M] and C\u003csub\u003e3\u003c/sub\u003eN\u003csub\u003e4\u003c/sub\u003ePIL-EY[M], the TiO\u003csub\u003e2\u003c/sub\u003e and C\u003csub\u003e3\u003c/sub\u003eN\u003csub\u003e4\u003c/sub\u003e will separate (Fig.4f, Fig. S34), ultimately preventing the formation of Newtonian fluids. Therefore, the electrostatic interaction between the solid and liquid ends is the key to the formation of this type of Newtonian fluid photocatalyst. The construction strategy of solid-liquid interaction can achieve universal synthesis of various Newtonian fluid photocatalysts.\u003c/p\u003e"},{"header":"Methods","content":"\u003cp\u003e\u003cstrong\u003eMaterials\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eDeionized water (DI water) was employed in all experiments. Sodium dodecyl benzene sulfonate (SDBS, A.R.), Potassium persulfate (KPS, A.R.), Styrene (St, A.R.), Divinylbenzene (DVB, A.R.), 1-Vinylimidazole (VIM, A.R.), tetrahydrofuran (THF, A.R.), Polyether amine (M2070), 1,6-Diaminohexane (A.R.), acetic acid (A.R.), formaldehyde (A.R.), methylglyoxal (A.R.) were obtained from Sinopharm Chemical Reagent Co., Ltd. INHONG GAS Company supplied carbon dioxide (CO\u003csub\u003e2\u003c/sub\u003e) and nitrogen (N\u003csub\u003e2\u003c/sub\u003e).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eSynthesis of polystyrene (PS) microspheres\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe PS microspheres were synthesized by emulsion polymerization, using SDBS as an emulsifier and KPS as an anionic initiator. The reaction was conducted under a nitrogen atmosphere, and 200 mL of DI water and 50 mL of ethanol were added into a 500 mL three-necked flask containing 0.5 g of SDBS. After adequately dispersing the SDBS, 12.5 mL of St, 3 mL DVB, and 0.25 g KPS were added into the reactor. Then, the polymerization was conducted in an oil bath at 80 \u0026deg;C, with shaking at 300 rpm, for 12 h. Eventually, the PS microspheres were collected by high-speed centrifugation at 10,000 r/min, and finally vacuum dried at 50 \u0026deg;C for further use.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eSynthesis of PIL\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe PIL hollow spheres were obtained by combining the template strategy. Specifically, 0.05g of the as-prepared PS microspheres was added to 37.5 mL DI water in a flask under stirring. In this state, 1 mL DVB and 2 mL VIM were added to the flask with continuous agitation for 1 h. Then, 6 mL KPS solution (0.5 wt%) was added to this system at 75 \u0026deg;C. After keeping stirring for 24 h at this temperature, the precursor of PIL spheres was obtained. Then, the PIL hollow spheres were obtained by etching the PS core with THF and separating by high-speed centrifugation at 10000 r/min.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eSynthesis of PIL-EY[M]\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003ePIL-EY[M] were prepared by electrostatic self-assembly of PIL hollow spheres and EY[M]. The PIL hollow spheres (0.1g) were dispersed in 15 mL DI water, a specified amount of EY was added to the PIL hollow spheres suspension. After stirring for 1 h at 60 \u0026deg;C, M2070 in the same amount as EY was slowly added to the mixture solution, stirred at 70 \u0026deg;C until it turned into a red viscous liquid.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eSynthesis of EY[M]\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eA specified amount of EY was added to the PIL hollow spheres suspension. After stirring for 1 h at 60 \u0026deg;C, M2070 in the same amount as EY was slowly added to the mixture solution, stirred at 70 \u0026deg;C until it turned into a red viscous liquid.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eSynthesis of TiO\u003csub\u003e2\u003c/sub\u003e and C\u003csub\u003e3\u003c/sub\u003eN\u003csub\u003e4\u003c/sub\u003e covered with the imidazole cation layer\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e0.5g TiO\u003csub\u003e2\u003c/sub\u003e or C\u003csub\u003e3\u003c/sub\u003eN\u003csub\u003e4\u003c/sub\u003e, DI water (10mL),1,6-Diaminohexane (0.5mL), acetic acid (2mL) were sequentially added to a round bottom flask and sonicated for 0.5 hours. After that, formaldehyde (0.71mL) and methylglyoxal (1.47mL) were added and stirred at room temperature for 24 hours. The final product is washed with water and ethanol.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eSynthesis of TiO\u003csub\u003e2\u003c/sub\u003e-EY[M] and C\u003csub\u003e3\u003c/sub\u003eN\u003csub\u003e4\u003c/sub\u003e-EY[M]\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eSimilar to the PIL-EY[M] synthesis process, the difference is that TiO\u003csub\u003e2\u003c/sub\u003e and C\u003csub\u003e3\u003c/sub\u003eN\u003csub\u003e4\u003c/sub\u003e covered with the imidazole cation layer were used instead of PIL\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003ePhotocatalysis experiments\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe entire photocatalytic CO\u003csub\u003e2\u003c/sub\u003e reduction reaction was carried out in a gas-solid mode in a 250 mL quartz glass device with good translucency. The PIL-EY[M] were painted on a poly (vinylidene fluoride) membrane with a radius of 25mm while weighing the weight of the PIL-EY[M] load, and the membrane coated with the photocatalyst was put on the platform in the reaction device. The water vapor environment was constructed by the introduction of 1 mL of water. A low-energy 360 nm LED visible light source was 5 cm away from the membrane. The detailed schematic diagram of the device is shown in Fig. S17. Before turning on the light, breathe with high-purity CO\u003csub\u003e2\u003c/sub\u003e gas for 15 min to eliminate other gases, and maintain the reaction temperature at room temperature by flowing water. During light irradiation, the gas products were analyzed by a Tetchrom gas chromatograph (GC2030) with a flame ionization detector (FID) and thermal conductivity detector (TCD).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eTA spectroscopy\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eTime-resolved experiments were carried out on laser-based spectroscopy, with laser powers equating to less than one photon absorption per particle. Samples for transient absorption experiments were kept in dark between each measurement. A Coherent Legend Ti: Sapphire amplifier (800 nm, 100 fs pulse length, 3 kHz repetition rate) was used.\u003c/p\u003e\n\u003cp\u003eThe output is split to pump and probe beams. Excitation pulses at the wavelength of 450 nm were acquired using an optical parametric amplifier (Topas C, Light Conversion). The probe pulses (a broad supercontinuum spectrum) were generated from the 800-nm pulses in a CaF\u003csub\u003e2\u0026nbsp;\u003c/sub\u003ecrystal and split by a beam splitter into a probe pulse and a reference pulse. The probe pulse and the reference pulse were dispersed in a spectrograph and detected by a diode array. Instrumental response time is \u0026sim;100 fs.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eCharacterization\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003ePower X-ray diffraction (XRD) was performed by a 9 kW Rigaku Smartlab X-ray diffractometer with Cu K\u0026alpha; radiation. The morphology and element distribution were characterized by high-resolution transmission electron microscopy (FEI TALOS F200X) and scanning electron microscope (Regulus 8100) with energy dispersive spectroscopy. XPS was implemented on an X-ray photoelectron spectrum (Thermo SCIENTIFIC ESCALAB Xi+), and C 1s 284.8 eV as reference. The element-selective X-ray absorption fine structure measurements were performed on the Shanghai Synchrotron Radiation Facility, and the data were analyzed by Athena software. The optical absorption properties were measured over a UV-2600 UV-vis DRS spectrophotometer with BaSO\u003csub\u003e4\u003c/sub\u003e powder as a reference. \u003csup\u003e13\u003c/sup\u003eC-isotopic tracer was investigated through gas chromatography-mass spectrometry (Shimadzu GC-MSQP2020). Brunauer-Emmett-Teller (BET) specific surface areas were recorded on a Micromeritics TriStar Ⅱ 3020M instrument. CO\u003csub\u003e2\u003c/sub\u003e adsorption was analyzed by the QUADRASORB evo instrument. The gas products were detected by a gas chromatography-mass spectrometer (GC-MS, Agilent Technologies) in the isotopic \u003csup\u003e13\u003c/sup\u003eCO\u003csub\u003e2\u003c/sub\u003e experiment.\u003c/p\u003e\n\u003cp\u003eIn-situ FT-IR experiments were recorded on a Thermo Scientific Nicolet iS50 FTIR with drift accessory. First, the material is loaded into the reaction chamber and paved, and the sample position is located below the center of three windows, including a quartz window and two infrared-transparent windows. Then, high-purity nitrogen containing water vapor is run through the reaction tank to keep the signal stable under dark conditions for 60 min. Subsequently, infrared data of CO\u003csub\u003e2\u003c/sub\u003e adsorption on the catalyst began to be recorded under a continuous flow of high-purity CO\u003csub\u003e2\u003c/sub\u003e gas. After the signal is stabilized, turn on the LED light and record the infrared data during the CO\u003csub\u003e2\u003c/sub\u003e photoreduction process.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003ePhotoelectrochemical measurements\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003ePhotoelectrochemical tests were performed on a three-electrode system using a CH660E electrochemical workstation. Pt and Ag/AgCl electrodes were used as counter and reference electrodes, respectively. The saturated calomel electrode, Pt wire, and FTO were used as the reference electrode, counter electrode, and working electrode. The catalyst (1 mg) was added into 1 mL of ethanol, ultrasonic for 30 min, and uniformly added to an area of 1 cm \u0026times; 1 cm on FTO. Mott-Schottky and photocurrent measurements were carried out in 0.5 M sodium sulfate solution. Electrochemical impedance spectroscopy properties were tested in potassium ferricyanide solution.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eDFT calculations\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe geometry optimization and excited-state calculations were performed by B3LYP-D3BJ exchange-correlation functional with the 6-311G(d) basis set based on the Gaussian 16 C.01 code. Frequency calculations were performed to ensure that the stability configuration has no imaginary frequency. Independent gradient model (IGM)\u003csup\u003e34,35\u003c/sup\u003e, Reduced density gradient (RGD), Frontier molecular orbital, the distribution of electrons and holes in the electron excitation process\u003csup\u003e35\u003c/sup\u003e, and interfragmentary charge transfer were calculated with Multiwfn 3.8 (dev)\u003csup\u003e36\u003c/sup\u003e. Molecular dynamics simulation, conducted using CP2K software. All structures and isosurfaces images were visualized by VMD 1.9.3. and VESTA. The single-point energy was calculated by M06-2X/def2-TZVPP level. The adsorption energy (E\u003csub\u003eads\u003c/sub\u003e) of CO\u003csub\u003e2\u003c/sub\u003e (Equation 1).\u003c/p\u003e\n\u003cp\u003eE\u003csub\u003eads\u003c/sub\u003e(CO\u003csub\u003e2\u003c/sub\u003e) = E(*CO\u003csub\u003e2\u003c/sub\u003e) - E(*) - E(CO\u003csub\u003e2\u003c/sub\u003e) \u0026nbsp; \u0026nbsp; \u0026nbsp; (1)\u003c/p\u003e\n\u003cp\u003eWhere E(*CO\u003csub\u003e2\u003c/sub\u003e), E(*) and E(CO\u003csub\u003e2\u003c/sub\u003e) were the total energy of samples with CO\u003csub\u003e2\u003c/sub\u003e adsorbed on the surface, the energy of the pristine sample surface and CO\u003csub\u003e2\u003c/sub\u003e, respectively.\u003c/p\u003e\n\u003cp\u003eAt room temperature, the Gibbs free energy for each model was calculated by the following equation (Equation 2):\u003c/p\u003e\n\u003cp\u003eG(T) = E\u003csub\u003eele\u003c/sub\u003e + G\u003csub\u003ecorr\u003c/sub\u003e(T) = E\u003csub\u003eele\u003c/sub\u003e + ZPE + \u0026Delta;G\u003csub\u003e0\u0026rarr;T\u003c/sub\u003e\u0026nbsp; \u0026nbsp; \u0026nbsp; \u0026nbsp;(2)\u003c/p\u003e\n\u003cp\u003eWhere E\u003csub\u003eele\u003c/sub\u003e, G\u003csub\u003ecorr\u003c/sub\u003e(T), ZPE and \u0026Delta;G\u003csub\u003e0\u0026rarr;T\u003c/sub\u003e were electronic energy, thermal corrections to Gibbs free energy, zero-point energy and contribution by heating the system from 0 K to 298.15 K, respectively.\u003c/p\u003e"},{"header":"Conclusion","content":"\u003cp\u003eIn summary, we have synthesized a flowing viscous Newtonian fluid material, which is grafted from internal hollow spheres and external liquid chains, for more convenient material applications and more efficient photocatalytic conversion. Experimental results show that, compared to powder catalytic systems, Newtonian fluid photocatalysts can be more uniformly and stably painted on non-planar surfaces, which enables the catalyst to cope with the effects of wind speed and solar altitude angle under natural conditions. At the same time, the permanent porosity and the solid-liquid interface of a Newtonian fluid enable better adsorption, mass transfer, and conversion. In the application of photocatalytic reduction of CO\u003csub\u003e2\u003c/sub\u003e, the PIL-EY[M] achieved a 100% selective CO overflow efficiency, which is 57.8 times higher than that of the PIL, with a stable performance under long-time and large-scale solar radiation. Viscous Newtonian fluid photocatalysts have shown potential for commercial feasibility by expanding the application scope of photocatalysis. In addition, by taking the most commonly used inorganic and organic photocatalysts TiO\u003csub\u003e2\u003c/sub\u003e and C\u003csub\u003e3\u003c/sub\u003eN\u003csub\u003e4\u003c/sub\u003e as examples, Newtonian fluid photocatalysts TiO\u003csub\u003e2\u003c/sub\u003ePIL-EY[M] and C\u003csub\u003e3\u003c/sub\u003eN\u003csub\u003e4\u003c/sub\u003ePIL-EY[M] with similar viscosity and fluidity were synthesized, demonstrating the universal synthesis of this type of Newtonian fluid photocatalysts.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003ch2\u003eCompeting interests\u003c/h2\u003e\u003cp\u003eThe authors declare no competing interests.\u003c/p\u003e\u003c/p\u003e\u003ch2\u003eAuthor contributions\u003c/h2\u003e\u003cp\u003eZ.Y.L., Y.C. and Y.R.X. performed the experiments, data analysis and wrote the paper. L.G.T. and H.P.L. performed the computer simulations. T.H.Z., K.Z and W.D.S conceived the ideas and designed the experiments.\u003c/p\u003e\u003ch2\u003eAcknowledgements\u003c/h2\u003e\u003cp\u003eThis work was supported by the National Natural Science Foundation of China (22225808, U24A20551, 22278190), Qing Lan Project of Jiangsu Province (2023), Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment, Jiangsu Graduate Research Innovation Program (KYCX25_4257), Open Project of State Key Laboratory of Structural Chemistry (20230022).\u003c/p\u003e\u003ch2\u003eData availability\u003c/h2\u003e\u003cp\u003eSource data are provided with this paper. All other data that support this study are available from the corresponding authors upon reasonable request.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003eLi, J.\u003cem\u003e, et al.\u003c/em\u003e Molecular-scale CO spillover on a dual-site electrocatalyst enhances methanol production from CO\u003csub\u003e2\u003c/sub\u003e reduction. \u003cem\u003eNat. Nanotechnol.\u003c/em\u003e, 10.1038/s41565-025-01866-8, (2025).\u003c/li\u003e\n\u003cli\u003eYe, J.\u003cem\u003e, et al.\u003c/em\u003e Hydrogenation of CO\u003csub\u003e2\u003c/sub\u003e for sustainable fuel and chemical production. \u003cem\u003eScience\u003c/em\u003e \u003cstrong\u003e387\u003c/strong\u003e, eadn9388 (2025).\u003c/li\u003e\n\u003cli\u003eYin, S.\u003cem\u003e, et al.\u003c/em\u003e Boosting water decomposition by sulfur vacancies for efficient CO\u003csub\u003e2\u003c/sub\u003e photoreduction. \u003cem\u003eEnergy Environ. 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Here, we report a flowing viscous Newtonian fluid photocatalyst, which consists of an internal nano-hollow imidazole framework (PIL) and an external light-excitable liquid chain (EY[M]) striking a pose on the stage. Due to the significant steric hindrance effect and intermolecular interaction at the solid-liquid interface, the Newtonian fluid catalyst with higher surface tension can firmly adhere to any kind of scaffold via a simple printing or spraying, such as curved surfaces, inclined walls, and grids, where powder materials are difficult to load. In addition to the easier scale-up, the pore structure of frameworks favors faster CO\u003csub\u003e2\u003c/sub\u003e mass transfer, and the liquid chain with a co-catalytic effect serves as the electron donor for efficient CO\u003csub\u003e2\u003c/sub\u003e photoreduction. As a result, the PIL-EY[M] achieved a 100% selective CO overflow efficiency, which is 57.8 times higher than that of the PIL, with a stable performance under long-time and large-scale solar radiation. By utilizing the structural characteristics of imidazole cationic solid and anionic liquid ends, a series of Newtonian fluid photocatalysts, such as TiO\u003csub\u003e2\u003c/sub\u003e-EY[M] and C\u003csub\u003e3\u003c/sub\u003eN\u003csub\u003e4\u003c/sub\u003e-EY[M], can be readily synthesized. The viscous Newtonian fluid photocatalysts enable a chance for commercial feasibility at an affordable cost.\u003c/p\u003e","manuscriptTitle":"Printable Newtonian fluid photocatalysts for scale-up solar CO2 conversion","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-10-23 04:34:02","doi":"10.21203/rs.3.rs-7844074/v1","editorialEvents":[],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"nature-communications","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"NCOMMS","sideBox":"Learn more about [Nature Communications](http://www.nature.com/ncomms/)","snPcode":"","submissionUrl":"https://mts-ncomms.nature.com/","title":"Nature Communications","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"Nature Communications","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"8a2021a3-92b3-4437-b74b-60f3d1153324","owner":[],"postedDate":"October 23rd, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[{"id":56741822,"name":"Physical sciences/Chemistry/Catalysis/Photocatalysis"},{"id":56741823,"name":"Physical sciences/Materials science/Materials for energy and catalysis/Photocatalysis"}],"tags":[],"updatedAt":"2026-05-13T07:07:18+00:00","versionOfRecord":{"articleIdentity":"rs-7844074","link":"https://doi.org/10.1038/s41467-026-70819-z","journal":{"identity":"nature-communications","isVorOnly":false,"title":"Nature Communications"},"publishedOn":"2026-03-20 04:00:00","publishedOnDateReadable":"March 20th, 2026"},"versionCreatedAt":"2025-10-23 04:34:02","video":"","vorDoi":"10.1038/s41467-026-70819-z","vorDoiUrl":"https://doi.org/10.1038/s41467-026-70819-z","workflowStages":[]},"version":"v1","identity":"rs-7844074","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-7844074","identity":"rs-7844074","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}