Water-based UV-ozone activation enables aggregation-free processing of MFI nanosheets for membrane fabrication

Water-based UV-ozone activation enables aggregation-free processing of MFI nanosheets for membrane fabrication | 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 Water-based UV-ozone activation enables aggregation-free processing of MFI nanosheets for membrane fabrication Kemal Celebi, Pingping Li, Ming Zhang, Yubin Hu, Xiangcheng Dai, and 2 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7510110/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted You are reading this latest preprint version Abstract Zeolite nanosheets offer promising opportunities to fabricate ultrathin molecular sieving platforms for energy-efficient and cost-effective gas separation. However, activating these nanosheets requires a high-temperature calcination process that opens the pores, causing drying and subsequent irreversible aggregation. Once aggregated, most nanosheets cannot be well-aligned to form a continuous thin membrane, which is a persistent bottleneck for mixed matrix membrane fabrication. In this study, we present a facile ultraviolet (UV)-ozone treatment that activates MFI zeolite nanosheets in aqueous solution. This treatment prevents the drying and aggregation of the nanosheets, thereby ensuring high yields of solvent dispersion for open-pore MFI nanosheets. Furthermore, the UV-ozone treatment also introduces hydroxyl groups on the nanosheet surface that enhance both CO 2 adsorption and interfacial compatibility with the polymer matrix. The activated nanosheets are then used to fabricate micrometer-thick, highly b -oriented MFI mixed matrix membranes on polymer substrates via solution casting. These membranes demonstrate high CO 2 /N 2 selectivity of 40 ± 6, with permeances of 194 ± 50 GPU (at 25℃, ambient pressure). This method is thus substantiated as an effective and scalable approach for activating zeolite nanosheets and can be a cost-efficient approach for the fabrication of thin, flexible zeolite-nanosheet-based gas separation membranes. Physical sciences/Chemistry/Chemical engineering Physical sciences/Materials science/Nanoscale materials/Two-dimensional materials Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Introduction The development of high-performance membranes for gas separation, particularly for hydrocarbon separation, has garnered significant attention in recent years due to the pressing need for energy-efficient and scalable separation technologies 1 . MFI zeolite membranes have demonstrated considerable potential in the field of gas separation, particularly in ultra-thin configurations with vertical channels along the b -axis ( b -oriented). This configuration offers reduced transport pathways and substantial mitigation of diffusion resistance, thereby accelerating gas diffusion processes 2 – 4 . It has been widely recognized that nanometer-thick b -oriented MFI nanosheets (NSs) have considerable potential as building blocks for the fabrication of highly b -oriented MFI membranes 5 – 7 . With cross-sectional dimensions of 5.6×5.3 Å for the channel along the b -axis (Fig. 1 ) and CO 2 -affinity, b -oriented MFI is an attractive option for practical CO 2 separation from gas mixtures, such as CO 2 /H 2 8,9 , CO 2 /CH 4 10,11 , CO 2 /N 2 12,13 . MFI inorganic membranes are among the most commonly fabricated membranes due to their excellent gas permeation flux, which is often significantly higher than that of polymer membranes 9 , 14 . However, conventional calcination for pore activation to remove organic templates inside the channels often induces cracks and grain boundaries, compromising membrane integrity 15 . Beyond this challenge, purely inorganic MFI membranes also suffer from inherent brittleness, the need for expensive ceramic substrates, and difficulties in large-scale fabrication, all of which hinder their broader industrial implementation 16 , 17 . In contrast, mixed matrix membranes (MMMs) incorporate zeolite fillers within a polymer matrix, offering a promising alternative by combining the advantages of molecular sieving with enhanced mechanical flexibility and scalable processability 13 , 18 – 20 . However, a significant challenge arises from the substantial aggregation of two-dimensional NSs during processing, which compromises membrane uniformity and reduces NS utilization, consequently diminishing separation performance 18 – 21 . This aggregation mainly originates from the zeolite activation step, where organic structure-directing agents (OSDAs) must be removed to open micropores prior to membrane fabrication. Conventional activation by calcination at ~ 500°C in air efficiently eliminates OSDAs but simultaneously induces irreversible wrinkling and aggregation of NSs, drastically lowering their solvent-dispersion yields and impairing both processability and membrane performance 18 – 20 . Alternatively, low-temperature ozone activation can also decompose the organic template under milder conditions (~ 200°C) by flowing ozone (generated from high-purity O 2 ) through the zeolite powder. However, this method cannot avoid the irreversible aggregation problem, as the powder is already in dried form 22 . Post-calcination processes can be applied to mitigate aggregation, such as ball milling, yielding modest improvement, with dispersion yields after calcination remaining below 10% 20,23 . This is primarily because NSs tend to form tightly bound aggregates upon drying, making subsequent redispersion highly challenging. Another way to avoid the aggregation problem is to fabricate a membrane using the as-synthesized nanosheets and then removing the OSDA by ultraviolet (UV)-ozone treatment in air 20 , 24 . However, this activation has been carried out on pre-formed, dried membranes rather than in the liquid phase, requiring at least six days of UV exposure to achieve complete template removal. This method is therefore time-consuming and limited on UV-resistant substrates, making it unsuitable for scalable processing. The limitations of existing activation methods have motivated efforts to remove OSDA while maintaining the NSs in a dispersed state, thereby avoiding aggregation during solvent processing. Piranha treatment, a liquid-phase activation strategy, has been investigated as a means of enhancing the solvent dispersion yield of MFI NS 25 . However, this approach has significant drawbacks, including safety hazards and requirement for multiple treatment rounds, which render it impractical for large-scale implementation. Therefore, developing a mild, liquid-phase UV activation strategy that can activate zeolite NSs in a dispersed state is crucial if zeolite NSs are to be utilized in membrane fabrication and other applications that require ordered assembly of the NSs. In this study, we present a liquid-based template removal strategy for activating the microporous MFI NSs dispersed in aqueous media using UV-ozone treatment (Fig. 1 ). For zeolite NSs, this method offers a distinct advantage of mitigating aggregation, thereby enhancing their dispersibility and usability. Utilizing this activation approach, we have fabricated micrometer-thick, highly b -oriented MFI MMMs on polyvinylidene fluoride (PVDF) substrates via solution casting. The UV-treatment also enriches the NSs with hydroxyl (-OH) groups, possibly enhancing CO 2 affinity and improving the interfacial compatibility between Pebax 1074 and NSs. The integration of well-aligned NSs within the Pebax matrix has been shown to enhance gas separation performance, achieving a CO 2 /N 2 selectivity of 40 ± 6 and a CO 2 permeance of 194 ± 50 gas permeation units (GPU) at 25℃ under ambient pressure. This methodology has been demonstrated to facilitate the activation process while concomitantly addressing the long-standing challenges associated with NS aggregation and the low solvent-dispersion yield of NSs in conventional calcination. These findings offer a promising foundation for the cost-effective fabrication of MFI or other zeolite-NS-based membranes, as well as for a range of industrial applications of zeolite NSs. Results Organic template removal in aqueous media under UV-ozone irradiation. We compare three methods for removing the organic template occluded in the MFI NSs. Conventionally, template removal is accomplished through high-temperature calcination in air, whereby the NSs are gradually heated to 550°C and maintained at this temperature for an extended period to facilitate the combustion of the organic template molecules. A chemical alternative to calcination involves piranha treatment, in which the NSs are dispersed in concentrated sulfuric acid and hydrogen peroxide mixtures at 120°C, with periodic replenishment of the oxidant to fully decompose the template. As the third method we present a milder approach by dispersing the NSs in aqueous solution and exposing them to UV light coupled with ozone. This allows for the gradual decomposition of the template. This decomposition occurs at moderate temperatures and does not require aggressive thermal or chemical conditions. To confirm the effectiveness of aqueous UV-ozone treatment in activating MFI NSs, we conducted a series of structural and compositional analyses. It is important to note that the organic template in this work refers to bis-1,5 (tripropyl ammonium) pentamethylene diiodide (dC5) (Fig. S1 , chemical structure). First, N 2 adsorption-desorption measurements verify the complete removal of the organic template, as the isotherms of both UV-ozone-treated NSs (Fig. 2 a, purple circle) and calcined NSs (Fig. 2 a, pink square) exhibited a typical open-pore structure with a surface area of ~ 416 m 2 /g, calculated by Brunauer-Emmett-Teller (BET) method. However, piranha-treated NSs and as-synthesized NSs exhibit a smaller surface area, measuring 158 cm 2 /g and 57 cm 2 /g, respectively, implying incomplete activation. Furthermore, pore size distribution analysis demonstrates the presence of micropores in the 0.5–0.6 nm range for UV-ozone treated NSs (Fig. S2, purple circle), which is similar to the calcined sample (Fig. S2, pink square). In contrast, piranha-treated NSs and as-synthesized NSs (green and black triangle) do not exhibit similar micropores, confirming incomplete activation. Further evidence of the efficacy of UV-ozone treatment is provided by chemical composition analysis. As shown in Fig. 2 b, Fourier transform infrared spectroscopy (FTIR) data of the as-synthesized NSs with the organic templates present peaks at 2850–2970 cm − 1 and 1560 cm − 1 , attributed to C-H vibrations, and 1469 cm − 1 belonging to C-N vibrations. However, both UV-ozone-treated NSs (Fig. 2 b, purple curve) and calcined NSs (Fig. 2 b, pink curve) demonstrate the elimination of C-H and C-N vibrations, thereby confirming complete template removal. In contrast, as-synthesized NSs and piranha-treated NSs exhibit weak C-H peaks and a prominent C-N peak, suggesting incomplete template removal. Furthermore, the UV-ozone treatment results in the introduction of -OH groups on the NSs surface. As shown in Fig. 2 b, the FTIR spectrum of UV-ozone treated NS exhibited a broad peak at 3000–3500 cm − 1 and a peak at 1629 cm − 1 , which are attributed to -OH and silanol (Si-OH), respectively. This finding indicates that UV-ozone treatment enhances surface hydrophilicity while removing organic species. Thermogravimetry analysis (TGA) results (Fig. 2 c and Table S1 ) provide further insight into the effectiveness of template removal. At around 130°C, both UV-ozone-treated and calcined NSs exhibit approximately 6% weight loss, which is primarily attributed to the desorption of physically adsorbed water or gas molecules from the internal pores and external surfaces. In contrast, as-synthesized and piranha-treated NSs show significantly lower weight losses of only 1–2% in this temperature range. At elevated temperatures, more distinct differences emerge. Between 400 and 600°C, the UV-ozone-treated NSs (purple curve) exhibit a modest 3.2% weight loss, which can be attributed to the condensation and dehydration of terminal silanol groups 26 , 27 . Notably, no significant weight loss is observed for calcined NSs in this range, suggesting the silanol condensation to be specific to the UV-ozone-modified surface chemistry. By contrast, both as-synthesized and piranha-treated NSs exhibit substantial weight losses of 17.1% and 15.6%, respectively, at around 600°C. These losses are consistent with the decomposition of retained organic templates (e.g., dC5), confirming incomplete template removal in these samples. Moreover, X-ray photoelectron spectroscopy (XPS) (Fig. 2 d, e) provides additional evidence for the above discussion. For both UV-ozone-treated and calcined NSs, the characteristic peak at ~ 402 eV, corresponding to C-N bonds from the dC5, completely disappears, confirming the successful elimination of residual organics. This finding aligns with the TGA and FTIR results, indicating efficient template removal by UV-ozone treatment. Furthermore, energy-dispersive X-ray spectroscopy (EDS) exhibits consistent results. Figure 2 f-j and Fig. S3 show TEM-EDS (UV-ozone treated NSs) and SEM-EDS results (as-synthesized and UV-ozone treated NSs), respectively, which reveal the near-negligible amount about of nitrogen in UV-ozone-treated NSs, while Si and O are present as expected. Besides, XRD analysis (Fig. 2 k) confirms that the crystallinity of UV-ozone-treated NSs remains identical to that of calcined samples, demonstrating that the treatment does not compromise structural integrity. The crystallinity can be further assessed via TEM imaging and SAED (Fig. 2 l,m), which confirm that UV-ozone-treated NSs retain their crystalline structure without signs of degradation, consistent with XRD results. Overall, UV-ozone treatment effectively removes organic templates from NSs, as confirmed by above analyses. Time-dependent decomposition of dC5 under UV-ozone treatment. To better understand how UV-ozone treatment enables effective template removal without damaging the NS structure, we further investigated the time-dependent degradation pathway of the dC5. Based on combined FTIR and XPS analyses, we propose a possible UV-ozone degradation mechanism for the dC5 (Fig. 3 a,b). In the early stages of irradiation, reactive oxidative species such as hydroxyl radicals (•OH) initially attack the terminal CH 2 and CH 3 groups exposed at the pore openings, leading to the formation of CO 2 , NO x , and other volatile byproducts (Fig. 1 and Fig. S4) 28 . This initial step is structurally supported by density functional theory (DFT) simulations of MFI/dC5 systems (Fig. 3 b, along b and c axis), which reveal that several dC5 molecules partially extend beyond the zeolite pore openings, making their terminal groups accessible to oxidative species, as shown in Fig. 3 a and 3 b 29 . As the exposure progresses, increased molecular mobility facilitates the migration of residual organics out of the pores or enables deeper penetration of oxidants, resulting in further decomposition of the internal (the dC5 fading progress is shown in Fig. 3 b, along b and c axis). As supported by FTIR spectra in Fig. 3 c, the NSs exposed to UV-ozone for 0, 12, 36, 60, and 72 hours exhibit a gradual disappearance of CH 2 and CH 3 peaks (2850–2970 cm − 1 and 1560 cm − 1 ). Notably, the C-H signal declines sharply within the first 12 hours, consistent with the early removal of aliphatic groups from external surfaces (Fig. 3 a). However, the C-N peak (1469 cm − 1 ), which is more representative of the internal template within the zeolite channels, persists until 36 hours and disappears after 60 hours. This time lag indicates the diffusion-limited access of oxidants into the internal pore network. Besides, the FTIR spectra show a gradual increase in the -OH stretching band (~ 3400 cm − 1 ) with prolonged UV-ozone exposure, indicating the formation of surface hydroxyl groups during template degradation. XPS analysis further substantiates this temporal degradation profile (Fig. 3 b). The N1s survey signal (Fig. 3 d) diminishes progressively with irradiation time, confirming the continuous loss of nitrogen-containing organic residues. A residual N signal after 72 hours (Fig. 3 d) is likely attributable to adventitious nitrogen adsorbed from ambient air, rather than incomplete decomposition. High-resolution C1s spectra (Fig. 3 e) show a consistent decline in the integrated intensity of C-C (285 eV) and C-N (286 eV) bonds, alongside a slight rightward shift, indicative of oxidation to more electronegative environments. Consequently, the N1s peak at 402 eV (C-N) in Fig. 3 f persists until 36 hours and disappears after 60 hours, perfectly aligning with the FTIR observations. These results confirm that UV-ozone treatment achieves complete removal of dC5 templates via a gradual, depth-dependent oxidative mechanism, avoiding structural damage. The combined spectroscopic trends provide compelling evidence for both the efficacy and gentleness of this approach. Enhanced interfacial compatibility of MFI NSs in Pebax-based MMMs. The conventional high-temperature calcination leads to severe aggregation and loss of structural integrity (Fig. 4 a). The solvent-dispersion yield can be decreased to less than 10%, even after making more efforts such as tip sonication and ball-milling 20 , 23 . In contrast, the dispersibility of the NSs after UV-ozone-treatment is confirmed by SEM, displaying well-aligned NS without aggregations (Fig. 4 b). In order to gain initial insight into the stacking behavior of UV-ozone-treated MFI NSs, we first fabricated NS membranes by vacuum filtration. Despite the SEM of the resulting membranes showing well-aligned NS stacking (Fig. 4 c), significant interlayer voids are also present (Fig. 4 d), suggesting incomplete packing. This void formation can be attributed to the inherent morphological thickness nonuniformity of the MFI NSs. As atomic force microscopy (AFM) analysis reveal (Fig. 4 e), the seed-like central domains reach ~ 30 nm thickness (Fig. 4 f). Still, the majority of the NS area exhibits a uniform thickness of 6–7 nm (Fig. 4 g). These bulky centers have been shown to originate from secondary ad-layer growth during the synthesis process 6 , 30 , 31 . Such local thickening disrupts the NSs stacking during vacuum filtration and gives rise to the observed voids. Therefore, a critical challenge lies in the removal or minimization of these central domains to produce thickness-homogeneous NSs suitable for dense membrane assembly. Addressing this issue, we subsequently applied post-treatment strategies to fragment the NSs into more uniform NSs, which were then used for the following MMM fabrication. The activated MFI NSs were processed by tip sonication and centrifugation, effectively removing the thicker ad-layer regions at the NS centers, which results in flat and well-dispersed fragments (Fig. 4 h, as indicated by yellow dotted line). These NS fragments exhibit excellent dispersibility in water and ethanol, enabling their incorporation into a Pebax® 1074 solution for MMM fabrication. It is acknowledged that achieving uniform and defect-free dispersion of NSs within polymer matrices persists as a formidable challenge, particularly due to interfacial incompatibility 18 – 21 . The enhanced hydrophilicity of the UV-ozone-treated MFI NSs, attributable to the presence of hydroxyl groups, leads to significant improvement in their dispersion within the hydrophilic Pebax® 1074 block copolymer, comprising polyether (PEO) and polyamide (PA) segments (Fig. 5 a). As confirmed by FTIR and TGA analysis (Fig. 2 b,c), the UV-ozone treatment introduces abundant surface hydroxyl groups (Fig. 5 b). Further evidence from the O1s XPS spectrum demonstrates enhanced signals corresponding to -OH and Si-O species (Fig. 5 c), thereby validating the occurrence of ozone-induced hydrolysis. These chemical alterations result in a substantial increase in hydrophilicity, as evidenced by a decrease in the water contact angle from 46.1° (pristine NSs) to 11.7° following the UV-ozone treatment (Fig. 5 d). The enhanced hydrophilicity can lead to better compatibility with the Pebax® 1074 matrix by improving surface energy matching. These NSs with -OH groups present a more polar surface, which facilitates stronger interfacial interactions, such as hydrogen bonding and dipole-dipole interactions, with the polar groups (ether oxygens and amide functionalities) in Pebax chains (Fig. 5 b) 18 , 32 – 34 . The MMMs were prepared by drop-casting the homogeneous NS-polymer mixture onto glass petri dishes and covering them with 25 mm PVDF in diameter substrates to form ultrathin films. The MFI content in the MMMs was measured precisely by TGA, revealing 4 wt.% and 1.6 wt.% weight percentage in different MMM samples (Fig. 5 e). The fabricated MMMs have NS alignment in (0 2 0) plane as shown by the XRD analysis (Fig. 5 f). This alignment is reinforced by the shear forces during the solvent evaporation 35 , 36 . After removing the solvents at 80°C for 2h, the membranes were peeled off by soaking in water and tweezers, after that vacuum drying overnight at 80°C was conducted. The top-view and the cross-section of the MMMs are shown by the SEM images (Fig. 5 g-l), displaying excellent dispersibility and interfacial adhesion of NSs within the Pebax matrix. Even at high NS loadings (> 10 wt.%), no aggregation can be observed, with the NSs exhibiting a well-aligned b -orientation, as indicated by the yellow arrows (Fig. 5 g). However, at high loadings, voids can be observed in the membrane structure (Fig. S5), due to incomplete polymer infiltration. Reduced loading can also enable significant thinning down of the MMMs (~ 1 µm, Fig. 5 k and l) with reduced voids and more homogeneous NS distribution (Fig. 5 h,i), attributed to improved polymer infiltration and reduced crowding. Overall, surface functionalization through UV-ozone activation significantly enhances the interfacial compatibility between NSs and the polymer, leading to improved dispersibility and uniform distribution of the NSs in the MMMs. Thin zeolite MMMs for CO 2 /N 2 separation with enhanced selectivity. Recent advances in the fabrication of MMMs have primarily focused on membranes with thicknesses in the range of tens to hundreds of micrometers, typically produced via solution casting techniques 37 , 38 . However, the development of "thin MMMs" with sub-2-µm thicknesses, represents both a technical challenge and a promising direction for high-performance gas separation 39 . In this study, the MMMs can be classified within this emerging category, with thicknesses of approximately 1 µm. In order to accurately assess and present the separation performance of thin membranes, it is imperative to report the gas transport data in terms of permeance, rather than permeability. While the latter is a valuable metric for comparing membrane materials due to its correlation with membrane thickness, it may overestimate the membrane performance, as they exclude any detrimental issues associated with membrane thinning. Conversely, permeance directly reflects the flux performance normalized by pressure difference, offering a more practical and consistent metric for evaluating thin membranes. MMMs on PVDF substrates with 25 mm-diameter are used for gas separation characterization (Fig. 6a). The effective gas permeation area was 1.33 cm 2 , defined by the o-ring in the membrane fixture. The CO 2 /N 2 separation measurements were done under ambient conditions using an equimolar binary gas mixture (Fig. 6b and Fig. S6). The permeance-selectivity results in Fig. 6b indicate that both CO 2 permeance and CO 2 /N 2 selectivity exhibit a strong dependence on the MFI NS loading. The separation performance improves with increasing filler content, reaching the maximum CO 2 /N 2 selectivity of 40 ± 6 at 1.6 wt.% NS loading. This is ~ 20 times higher than that of Pebax matrix, while the CO 2 permeance (194 ± 50 GPU) is slightly lower than the Pebax matrix. However, further increasing the loading to 4 wt.% leads to a slight decline in the selectivity (25 ± 3). At an even higher loading of 10 wt.%, the selectivity drops significantly to 4 ± 3 (Table S2). This deterioration suggests that the presence of a residual ad-layer hinders the alignment of NSs within the MMMs (Fig. 4 e), leading to void formation. Furthermore, the permeability values for the MMMs with varying loadings have been calculated. Fig. S7 shows the permeabilities of MMMs identical to Fig. 6b, which monotonically increase with MFI NS loadings. This might give a misleading impression that higher loadings are better for the overall performance, thus confirming our initial reasoning that permeance values should be compared. To ensure the reproducibility of our findings, we conducted batch-to-batch variation tests on MMMs with an optimal NS loading of 1.6 wt.% (Fig. 6c and Table S3). The four independent batches (M1-M4) demonstrate highly consistent CO 2 /N 2 separation performance (CO 2 permeance of 194 ± 7 GPU and selectivity of 40 ± 4 on average), thereby substantiating the reliability of our fabrication approach. Furthermore, long-term stability tests were performed over a 22-hour period under continuous CO 2 exposure. As shown in Fig. 6d, both CO 2 permeance and selectivity remained nearly constant throughout the testing period, demonstrating excellent durability. Besides the excellent interfacing of the NSs and the polymer matrix, the CO 2 /N 2 selectivity enhancement can also be attributed to the increased number of hydroxyl groups on the NSs. CO 2 adsorption-desorption measurements at room temperature (Fig. 6e) indicate a slightly higher CO 2 adsorption capacity (42.6 cm 3 /g) for the UV-ozone-treated NSs compared to the calcined NSs (39.6 cm 3 /g). Considering their similar pore structures, this higher capacity can be attributed not to the increased porosity, but rather to the introduction of hydroxyl groups, which offers stronger interactions with CO 2 molecules (Fig. 5 b). Further supporting this, the UV-ozone-treated NSs also showed a significantly slower desorption rate (Fig. 6e, purple triangle with solid dot), probably due to the CO 2 interaction with NSs or the inter-nanosheet gaps caused by enriched hydroxyl groups. These stronger interactions can be attributed to hydrogen bonding and dipole-quadrupole interactions between CO 2 and the polar -OH groups 40 . Most importantly, these hydroxyl groups provide more energetically favorable adsorption sites for CO 2 , directly validating the role of functional groups in enhancing selective adsorption. Specifically, CO 2 exhibits a significantly higher adsorption enthalpy (27.5–50 kJ/mol) on the MFI framework compared to N 2 (13.8 kJ/mol) 41 . The presence of polar hydroxyl groups further amplifies this disparity, enabling preferential adsorption of CO 2 , while N 2 , with its lower affinity and non-polar nature, is more readily excluded, thereby increasing CO 2 /N 2 selectivity 40 , 42 , 43 . While UV-ozone-treated NSs provide strong CO 2 affinity at low pressure due to abundant surface hydroxyl groups, the preferential adsorption advantage is gradually offset at higher pressures by higher N 2 flux and competitive site occupation. As the feed pressure increased, both CO 2 permeance and selectivity declined (Fig. 6f). This can be attributed to the saturation of surface adsorption sites and a shift in transport mechanism from adsorption-dominated to more diffusion-governed. Moreover, polymer chain compression and reduced interfacial porosity may contribute to the overall decline in gas permeance. These observations indicate that the selectivity enhancement from surface functionalization is most effective under moderate-pressure conditions where adsorption-driven transport is dominant. Discussion This study demonstrates that UV-ozone treatment in an aqueous medium offers an effective low-temperature strategy to activate MFI NSs while preventing aggregations and simultaneously enhancing their structural and interfacial properties. This enables the fabrication of high-performance thin membranes. In comparison with thermal activation, which frequently results in irreversible aggregation and compromises NS alignment, the non-thermal UV-ozone method preserves the NSs in a dispersed, open-pore state, thereby markedly enhancing their utilization efficiency in membrane fabrication. Beyond the opening of micropores and the prevention of aggregation, the UV-ozone treatment introduces hydroxyl groups, which serve to enhance the hydrophilicity and dispersion of NSs in the Pebax matrix. Additionally, these hydroxyl groups modulate gas transport behavior. A schematic representation of the CO 2 /N 2 separation mechanism through the resulting MMMs, consisting of UV-ozone-activated MFI NSs, is presented in Fig. 7a. The NS-aligned structure provides a selective pathway and strong interaction for CO 2 molecules while effectively hindering the transport of less soluble N 2 , resulting in enhanced separation performance. We have benchmarked our MMMs against literature-reported zeolite-based MMMs (Fig. 7b, Table S4). The membranes in this study exhibit two orders of magnitude higher CO 2 permeance in comparison to hundred-micrometer-thick MMMs, while maintaining competitive selectivity. This significant enhancement can be attributed to a synergistic effect, whereby two factors contribute to the observed outcome. Firstly, the enhanced dispersibility and interfacial compatibility of the NSs within the polymer matrix effectively suppress aggregation. Secondly, the reduced membrane thickness on a micron scale significantly lowers the diffusion resistance for gas molecules, thereby boosting overall separation performance. Compared to our previously-reported platelike MFI MMMs (< 5 µm), the MMMs here achieves a fivefold increase in CO 2 permeance and a 2.4-fold improvement in CO 2 /N 2 selectivity 13 . Furthermore, this low filler loading membrane has two notable benefits. First, it substantially reduces material cost. Second, it enhances processability while maintaining membrane flexibility and structural integrity. Conversely, the utilization of excessive filler loadings in conventional MMMs frequently results in filler agglomeration, interfacial voids, and augmented membrane brittleness, collectively leading to a deterioration in separation performance. Hence, a meticulously designed polymer-filler interface has the potential to achieve high efficiency even at low filler loadings. In summary, the UV-ozone treatment method presented here facilitates the drying-free activation of zeolite NSs in an aqueous environment, thereby eliminating the necessity for high-temperature calcination. Consequently, this approach enables the scalable production of flexible and thin membranes with enhanced selectivity, thereby paving the way for energy-efficient CO 2 separation technologies. The ultrathin and well-aligned morphology of the MMM, in conjunction with its excellent interfacial matching and hydroxyl functionalization, yields exceptional performance even with a filler loading as low as 1.6 wt.% (for ~ 1 µm-thick membranes: CO 2 /N 2 selectivity = 40 ± 6; CO 2 permeance = 194 ± 50 GPU at 25°C, ambient pressure). These MMMs exhibit high performance that surpasses most zeolite-based MMMs reported in the literature. Subsequent endeavors would center on decreasing the membrane thickness to the hundred-nanometer range, optimizing flatter NSs synthesis, and enhancing NS alignment to promote advancements in industrial applications. Methods Chemicals. Tetraethoxysilane (TEOS, Macklin) and silicic acid (H 4 SiO 4 , Aladdin) were used as silicon sources. Tetrapropylammonium hydroxide (TPAOH, 25 wt.% aqueous solution, Aladdin) served as the structure-directing agent. Potassium hydroxide (KOH, ≥ 85%, pellet) was bought from China National Pharmaceutical Group Chemical Reagent Co., Ltd. Organic compounds including 1,5-diaminopentane (Macklin), 1-iodopropane (J&K), and butanone (SCR) were employed as reactants and solvents for dC5 template synthesis. N, N-Dimethylformamide (DMF, SCR) was also used as a dispersing solvent. For membrane fabrication, Pebax 1074 (Arkema) was used as the polymer matrix. Hydrophilic PVDF (0.45 µm pore size (BS-PVDF-45), Merck Millipore) was used for membrane fabrication. Preparation of MFI NSs. The MFI NSs were synthesized using a two-step process as described in the previous report 6 , 29 . In brief, the synthesis involved initial fragment growth and secondary growth, using molar ratios of 80 TEOS: 3.75 dC5: 20 KOH: 9500 H 2 O: 320 ethanol. The fragment synthesis was conducted at 155°C for 3 days with rotary stirring at 60 rpm, followed by secondary growth under identical conditions. This process yielded high-aspect-ratio NSs with excellent dispersion, suitable for membrane fabrication. MFI NS fragments were initially synthesized through rotational intergrowth triggered by nanocrystals as seeds, using the dC5 template, as previously described by Tsapatsis 29 . Firstly, the seed crystals (~ 30 nm), were prepared using a molar ratio of 10 SiO 2 : 2.4 TPAOH: 0.87 NaOH: 114 H 2 O 66 . by mixing 1.096 g NaOH, 61.39 g TPAOH (25 wt.% aqueous), and 18.607 g deionized water, stirring for 15 min at room temperature. Subsequently, 18.90 g of solid H 4 SiO 4 was added, and the precursor was stirred overnight for hydrolysis. The mixture was then heated in a 50°C-oil bath for 6 days with stirring at 1000 rpm, followed by a filtration using a 0.45 µm GHP syringe filter to remove any aggregates. The filtrate was further heated in a 100°C-oil bath for 3 days without stirring. The resulting nanocrystals were purified by centrifugation at 11,000 revolutions per minute (rpm) for 1 h, followed by rinsing with deionized water. The centrifugation and rinsing processes were repeated twice, and the final product was diluted to 0.48 wt.% with water. Next, the dC5 template was synthesized through exhaustive alkylation of 1,5-diaminopentane with 1-iodopropane, following the procedure outlined by Bonilla et al 67 . Its purity was confirmed by proton nuclear magnetic resonance ( 1 H NMR), as shown in Fig. S1 . For MFI NS fragments synthesis, 0.31 g KOH, 4.0 g TEOS, 0.549 g dC5 (as-synthesized), and 41.04 g deionized water were thoroughly mixed and hydrolyzed at 30°C for 16 h, with pH 10.4. The dust and impurities were removed by vacuum filtration, followed by adding 0.3 g of 0.48 wt.% nanocrystal seed. This mixture was then transferred to an autoclave with Teflon beads to promote fragment formation. The autoclaves were then subjected to a preheated oven at 155℃ for 3 days, rotating at 60 rpm. These NS fragments were separated by a combination of 2-min tip sonication and 30-s centrifugation (5000 relative centrifugal force (RCF)) without rinsing, maintaining a pH of 10.4. For the secondary growth of NSs, the same precursor molar ratio and procedures were used. The hydrolyzed precursor was mixed with NS fragments 1.5:1 (weight ratio, e.g., 18 g precursor solution to 12 g fragments solution) and then loaded into an autoclave with an internal volume of 100 mL, which was subjected to 155℃ for 3 days at 60 rpm. After synthesis, the NSs were extracted by centrifugation at 5000 RCF for 30 s. The high-aspect-ratio NSs were dispersed at the top of the solution and were collected at 11,000 rpm for 10 min, followed by rinsing with deionized water. This rinsing process was repeated three to four times, after which the slurry was dispersed into water. To increase the crystallization speed, a fast synthetic strategy (FSS) was used. Cleaning of the reactors and loading of precursors followed previously reported procedures 68 . As a result, the large, rectangle-shaped NSs (2.02 × 1.64 µm) are produced at 155℃ for 30 hours. UV-Ozone Activation of MFI NSs in Aqueous Solution. The as-synthesized NSs were dispersed aqueous solution and exposed to UV light to remove the dC5 occluded in the pores by using a Cnlight UV (23 W ultraviolet light ranging from 185 to 254 nm coupled with ozone) for 12, 36, 60, and 72 h. The maximum temperature of the aqueous solution with a UV chamber inserted was ~ 58°C. To compare the effects of both UV-ozone-activation and thermal calcination, another batch of NSs was calcined by a traditional procedure. NSs were heated to 550°C with a heating and cooling rate of 1°C min − 1 and kept at 500°C for 6 h. Piranha treatment for MFI NSs. After synthesis, the MFI NSs were centrifuged several times to remove unreacted precursors before undergoing piranha treatment for template removal. The collected NSs were first mixed with concentrated sulfuric acid, followed by vortexing to ensure uniform dispersion. Subsequently, hydrogen peroxide solution (H 2 O 2 , 30%) was added slowly in a volume ratio of 1:3 (H 2 O 2 to H 2 SO 4 ) to generate the piranha solution directly in a glass container. Extreme caution was exercised during this step due to the highly corrosive and exothermic nature of the mixture, and appropriate personal protective equipment (PPE) was used at all times. The reaction vessel was then placed on a hotplate at 120°C and loosely covered with a watch glass to minimize rapid gas release and prevent liquid splashing. After overnight reaction, additional H 2 O 2 was added to replenish the oxidant and maintain reaction efficacy; this step was repeated 5–6 times. Upon completion, the mixture was diluted and washed thoroughly with deionized water until a neutral pH was reached. The final product was redispersed in aqueous solution for further use. Preparation of MFI membrane. As-filtered membranes were prepared by vacuum filtration on PVDF substrates. To reduce the cave and void formation, the UV-ozone-NSs were broken by tip sonication for 40 min to remove the crystals at the thicker ad-layer of the NSs. A homogeneous dispersion of MFI fragments and Pebax 1074 was prepared by thoroughly mixing the components in 70% ethanol. The MFI MMMs were fabricated using a solution casting method. In brief, the mixture was drop-cast in the glass petri dish as reported before 13 , covered by a PVDF substrate to obtain ultra-thin MMMs and ensure uniform deposition of the NS-polymer composite. The membrane was dried under vacuum overnight at 80°C to remove residual solvent. For peeling off the membrane, membranes were immersed in water for 0.5-1 h, and then taken off carefully with tweezers. Characterizations and measurements. XRD was performed by a LabX XRD-6100 X-ray diffractometer equipped with Cu Kα radiation (λ = 1.5418 Å) within the 5–50 ° range at a scan rate of 2 ° /min. SEM images of the zeolite samples were captured with a Zeiss MINI 300 at an accelerating voltage of 3.0 kV. High-resolution transmission electron microscopy (HR-TEM), along with electron diffraction and EDS mapping, was performed on a JEOL JEM-2100F microscope operating at 200 kV. Nitrogen adsorption-desorption isotherms at 77 K and CO 2 adsorption-desorption isotherms at 283 K were obtained using an ASAP 2460 analyzer. The height profiles of the MFI NSs were recorded using an Oxford Asylum Research Cypher ES AFM operating in AC mode (tapping), and image processing was carried out with Gwyddion software. FTIR spectroscopy was performed using a Thermo Fisher Scientific Nicolet iS20 spectrometer. TGA was conducted using a Discovery TGA 55 analyzer (TA Instruments, USA). XPS measurements were carried out using a Thermo Scientific K-Alpha instrument. The binding energy range from 0 to 1350 eV was scanned to capture the relevant elements, including Si, C, N, and O. Calibration of the binding energy scale was done by setting the C 1s peak at 284.8 eV to account for charging effects. Water contact angle measurements were conducted using a Theta Flex goniometer from Biolin Scientific. Sample Preparation for SEM and AFM. SEM and AFM samples were prepared by LB deposition. To be specific, the NSs were first dispersed in a solvent mixture of water and DMF at a 5:1 v/v ratio, followed by 60 min of bath sonication. 0.3 mL of the dispersion was injected onto the surface of the water and spread for 1 h before being transferred vertically onto a 1 × 1 cm Si/SiO 2 wafer and air-dried at ambient conditions. The Si/SiO 2 substrate was then heated at 500°C for 8 hours in a furnace to remove organic impurities. Sample preparation for nitrogen adsorption-desorption isotherms. The as-synthesized NSs were calcinated at 500℃ for 8 h in air, with a heating rate of 1℃/min. NSs treated with piranha solution were rinsed with fresh DI water and dried at 150℃ overnight. The NSs exposed to UV-ozone treatment were filtered, washed with DI water, and dried at 150℃ overnight. These NSs were degassed at 200℃ for 6 h before measurement. XPS sample preparation. The samples were prepared by dispersing the NSs in DI water and drop-casting 0.4 mL of the dispersion onto a 5 mm × 5 mm substrate. The DI water was allowed to evaporate at ambient conditions, leaving behind a thin film of the NSs on the substrate surface. The samples analyzed included as-synthesized NSs, calcined NSs, NSs treated with piranha solution, and NSs subjected to different UV-ozone exposure times. CO 2 /N 2 separation performance test. Gas separation experiments were conducted using a membrane sample with an effective area of 1.3 cm in diameter. An equimolar mixture of CO 2 /N 2 (10 standard cubic centimeters per minute (sccm) each, total 20 sccm) was introduced to the feed side of the membrane module, while helium (He) was continuously supplied to the permeate side at a flow rate of 20 sccm as a sweep gas. The experiments were conducted using the Wicke-Kallenbach method under controlled conditions of 1 bar pressure and room temperature. The feed gas was introduced on the upstream side of the membrane, while He swept the permeate side. Gas composition was analyzed using a Shimadzu GC-2014C gas chromatograph with a thermal conductivity detector (TCD). Steady-state conditions were established before collecting data to ensure reliable results. The permeance of a gas through a membrane is a key parameter that quantifies the intrinsic ability of the membrane to allow the passage of a specific gas under a given pressure difference. It is defined as the molar flux of the gas per unit area, per unit time, and per unit pressure difference. The permeance Π of gas component i is given by the following expression: Π i = N i /( A ∙ t ∙ Δp ), where N i represents the amount of gas component i that has permeated through the membrane, expressed in moles (mol). A is the effective area of the membrane, in square meters (m 2 ), through which the gas is permeating. t is the elapsed time during which the permeation is measured, in seconds (s). Δp is the pressure difference across the membrane, expressed in Pascals (Pa), which acts as the driving force for the permeation process. For practical purposes, the permeance is often expressed in gas permeation units (GPU), where 1 GPU is equivalent to 10 − 6 cm 3 (STP) / (cm 2 ·s·cmHg) or 3.35×10 − 10 mol / (m 2 ∙s∙Pa). The permeability in Barrer can be calculated via multiplying the permeance (in GPU) by the thickness (µm). Declarations Acknowledgments We sincerely thank Xiaokun Ding and Xiangcheng Dai for providing technical support in TEM characterization, including high-resolution imaging, selected area electron diffraction (SAED), and EDS mapping, for the as-synthesized and UV-ozone-treated MFI NS samples. Funding: National Natural Science Foundation of China (grant no: 52270108) National Natural Science Foundation of China Research Fund for International Scientists (grant no: W2432010) Author contributions: Conceptualization: PL, KC Methodology: PL, MZ, YH, XD Investigation: PL, MZ, YH Visualization: PL, KC Supervision: KC Writing - original draft: PL Writing - discussion and editing: PL, MZ, YH, JZ, DK, KC Competing interests: All other authors declare they have no competing interests. Data and materials availability: All data are available in the main text or the supplementary materials. 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Supplementary Files tableS4.xlsx dataset 1 Supplementary.pdf Water-based UV-ozone activation enables aggregation-free processing of MFI nanosheets for membrane fabrication Cite Share Download PDF Status: Under Review 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-7510110","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":521121252,"identity":"b253d607-501c-42f7-8e6c-543a3b4ff6b9","order_by":0,"name":"Kemal 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05:13:36","extension":"png","order_by":17,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":72992,"visible":true,"origin":"","legend":"","description":"","filename":"Onlinefloatimage7.png","url":"https://assets-eu.researchsquare.com/files/rs-7510110/v1/70250ea8fdfdee708b3e2712.png"},{"id":92376323,"identity":"8968e081-4d92-4c15-a770-2bc1580246a8","added_by":"auto","created_at":"2025-09-29 05:05:36","extension":"xml","order_by":18,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":150017,"visible":true,"origin":"","legend":"","description":"","filename":"NCOMMS25693880structuring.xml","url":"https://assets-eu.researchsquare.com/files/rs-7510110/v1/706d0de432143caa03ba1384.xml"},{"id":92376321,"identity":"a2c0457d-f8ad-47ab-b2c2-cf83f8893d48","added_by":"auto","created_at":"2025-09-29 05:05:36","extension":"html","order_by":19,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":158262,"visible":true,"origin":"","legend":"","description":"","filename":"earlyproof.html","url":"https://assets-eu.researchsquare.com/files/rs-7510110/v1/a7bc6c4b69d1585fbfec464e.html"},{"id":92376316,"identity":"57997e0e-7059-4925-9429-b6e63cbcfdc7","added_by":"auto","created_at":"2025-09-29 05:05:36","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":405850,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eSchematic diagram for the activation of MFI NSs by UV-ozone treatment in aqueous solution, enabling efficient OSDA removal from NS micropores in liquid. a\u003c/strong\u003e, A lamp irradiates UV light between 185-254 nm in an aqueous solution containing MFI NSs, generating ozone and reactive oxygen species (e.g., •OH radicals). These oxidizing species progressively degrade the dC5 confined in the micropores, which is decomposed into gaseous products (e.g., CO\u003csub\u003e2\u003c/sub\u003e, NO\u003csub\u003ex\u003c/sub\u003e), leading to bubble generation. Meanwhile, the NS surface is functionalized with hydroxyl groups (-OH) after the UV-ozone treatment. \u003cstrong\u003eb\u003c/strong\u003e, Illustration of the OSDA (dC5) degradation process: MFI NS micropores are initially filled with dC5 molecules (left), which are gradually decomposed and emptied after UV-ozone treatment, yielding fully activated MFI NSs with open pores (right).\u003c/p\u003e","description":"","filename":"image1.png","url":"https://assets-eu.researchsquare.com/files/rs-7510110/v1/24041d98291ac98a7e294b9c.png"},{"id":92376313,"identity":"8d25986c-8ed5-48bc-9567-f97ca6deb308","added_by":"auto","created_at":"2025-09-29 05:05:36","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":848281,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eValidation of effective dC5 removal via UV-ozone irradiation in liquid media. a\u003c/strong\u003e, N\u003csub\u003e2\u003c/sub\u003e adsorption-desorption isotherms comparing the three methods (conventional thermal calcination, piranha treatment, and UV-ozone-activation), showing that micropore surface area of UV-treated NSs is comparable to calcined NSs. \u003cstrong\u003eb\u003c/strong\u003e, FTIR spectra illustrating effective degradation of dC5 in UV-ozone-treated and calcined NSs, whereas piranha-treated NSs remain largely unchanged. \u003cstrong\u003ec\u003c/strong\u003e, TGA analysis quantifying template removal efficiency across the three strategies (summarized in Table S1), indicating the UV-ozone activation matches the calcination efficiency. \u003cstrong\u003ed\u003c/strong\u003e, \u003cstrong\u003ee\u003c/strong\u003e, XPS spectra highlighting the loss of organic constituents (C, N) in UV-ozone-treated and calcined NSs relative to as-synthesized samples. \u003cstrong\u003ef\u003c/strong\u003e-\u003cstrong\u003ej\u003c/strong\u003e EDS elemental mapping revealing near-complete elimination of nitrogen following UV-ozone exposure. \u003cstrong\u003ek\u003c/strong\u003e, XRD patterns confirming preservation of NSs crystallinity after treatment. \u003cstrong\u003el\u003c/strong\u003e, TEM image and (\u003cstrong\u003em\u003c/strong\u003e) SAED pattern of UV-ozone-treated NSs, showing the crystallinity of NSs after UV-ozone treatment.\u003c/p\u003e","description":"","filename":"image2.png","url":"https://assets-eu.researchsquare.com/files/rs-7510110/v1/ffdc7b659b442549528238ac.png"},{"id":92376318,"identity":"ed67e2db-26a9-440e-bba9-c1498c2457f5","added_by":"auto","created_at":"2025-09-29 05:05:36","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":724852,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eCharacterization of decomposition of dC5.\u003c/strong\u003e \u003cstrong\u003ea\u003c/strong\u003e, Schematic of dC5 decomposition under UV ozone treatment, hydrogen atoms are omitted. \u003cstrong\u003eb\u003c/strong\u003e, The step-by-step dC5 degradation under UV-ozone irradiation. The view of the MFI framework is along the \u003cem\u003ec\u003c/em\u003e axis (top) and \u003cem\u003eb\u003c/em\u003e axis (bottom), respectively. \u003cstrong\u003ec\u003c/strong\u003e, FTIR spectra for NSs treated for 0, 12, 36, 60, and 72 hours, showed the degradation of CH\u003csub\u003e2\u003c/sub\u003e and CH\u003csub\u003e3\u003c/sub\u003e groups with increasing UV-ozone exposure time and increased hydrophilicity of UV-ozone-treated NSs. \u003cstrong\u003ed\u003c/strong\u003e-\u003cstrong\u003ef\u003c/strong\u003e, XPS spectra after varying UV-ozone treatment time, indicate reduced C-N and C-C signals/integral area due to dC5 removal.\u003c/p\u003e","description":"","filename":"image3.png","url":"https://assets-eu.researchsquare.com/files/rs-7510110/v1/d6e0b28619d2034507d83d67.png"},{"id":92376329,"identity":"cb46a7fd-ae3b-4afb-ac83-112b5b944c5c","added_by":"auto","created_at":"2025-09-29 05:05:37","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":724228,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eDispersibility of activated MFI NSs and membrane fabrication optimization.\u003c/strong\u003e \u003cstrong\u003ea\u003c/strong\u003e, Photograph of calcined NSs showing irreversible aggregation. \u003cstrong\u003eb\u003c/strong\u003e, SEM image of NSs obtained after UV-ozone activation, showing high dispersibility. \u003cstrong\u003ec\u003c/strong\u003e, Cross-sectional SEM of a vacuum-filtrated membrane showing well-aligned NS stacking. \u003cstrong\u003ed\u003c/strong\u003e, Enlarged SEM image revealing interlayer voids caused by NS thickness mismatch. \u003cstrong\u003ee\u003c/strong\u003e, AFM images and (\u003cstrong\u003ef\u003c/strong\u003e, \u003cstrong\u003eg\u003c/strong\u003e) height profiles of NSs showing flat regions, and thickened centers (~30 nm) due to ad-layer growth (6-7 nm). \u003cstrong\u003eh\u003c/strong\u003e, SEM image of the NS fragments after the thickened centers removed by tip sonication. The shape of the broken NS is highlighted by yellow dotted lines. These uniform NS fragments were subsequently applied for the following MMM fabrication\u003c/p\u003e","description":"","filename":"image4.png","url":"https://assets-eu.researchsquare.com/files/rs-7510110/v1/a358209a9321e13ba1ed6cdc.png"},{"id":92376308,"identity":"aaedd3d3-2fad-4e4e-9b37-b77666c768b8","added_by":"auto","created_at":"2025-09-29 05:05:35","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":1319017,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eEnhanced interfacial compatibility by integrating hydrophilic and well-dispersed NS in Pebax-based MMMs. a\u003c/strong\u003e, The structure of the Pebax 1074 chain. \u003cstrong\u003eb\u003c/strong\u003e, The schematic of MFI NSs with enriched hydroxyl groups. The green lines indicate the interaction between Pebax chain and hydroxyl-riched NSs MFI NS. \u003cstrong\u003ec,\u003c/strong\u003e XPS spectra of O1safter varying UV-ozone treatment time, indicating the enhancement of Si-O or OH peaks\u003cstrong\u003e. d\u003c/strong\u003e, Water contact angle measurements before (left) and after (right) UV-ozone treatment, confirming increased hydrophilicity after the UV treatment. \u003cstrong\u003ee\u003c/strong\u003e, TGA results of MMMs with different MFI loadings.\u003cstrong\u003ef\u003c/strong\u003e,XRD patterns of MMMs with different MFI loadings, indicating highly \u003cem\u003eb\u003c/em\u003e-orientated morphology. \u003cstrong\u003eg\u003c/strong\u003e-\u003cstrong\u003ei\u003c/strong\u003e, SEM images of MMMs with different MFI loadings. The yellow arrows indicate the location of NSs on the surface of MMMs. \u003cstrong\u003ej\u003c/strong\u003e-\u003cstrong\u003el\u003c/strong\u003e, Cross-sectional images of MMMs with varying MFI loadings. The yellow arrows show highly aligned morphology and reduced layer spacing.\u003c/p\u003e","description":"","filename":"image5.png","url":"https://assets-eu.researchsquare.com/files/rs-7510110/v1/241ed07aed2d26ede0beada6.png"},{"id":92376328,"identity":"cca9392a-5a8d-4e75-9244-bcd15a020527","added_by":"auto","created_at":"2025-09-29 05:05:37","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":386024,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eCO\u003c/strong\u003e\u003csub\u003e\u003cstrong\u003e2\u003c/strong\u003e\u003c/sub\u003e\u003cstrong\u003e/N\u003c/strong\u003e\u003csub\u003e\u003cstrong\u003e2\u003c/strong\u003e\u003c/sub\u003e\u003cstrong\u003e separation performance for thin MFI MMMs.\u003c/strong\u003e \u003cstrong\u003ea\u003c/strong\u003e, Digital photo of an MMM prepared on a 25 mm PVDF substrate. The orange circle represents the effective area for the membrane measurement in the following gas separation measurements. \u003cstrong\u003eb\u003c/strong\u003e, CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e separation as a function of MFI NS loading, showing that both CO\u003csub\u003e2\u003c/sub\u003e permeance and selectivity increase with filler content, reaching optimal performance at 1.6 wt.% NSs. \u003cstrong\u003ec\u003c/strong\u003e, Batch-to-batch reproducibility for MMMs with 1.6 wt.% NSs, demonstrating consistent CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e permeance and selectivity. \u003cstrong\u003ed\u003c/strong\u003e, Long-term stability of the optimal MMM (1.6 wt.%) under continuous CO\u003csub\u003e2\u003c/sub\u003e exposure for 22 h, showing negligible decline, highlighting the robustness of NS-polymer interfacing. \u003cstrong\u003ee\u003c/strong\u003e, CO\u003csub\u003e2\u003c/sub\u003e isotherms at room temperature for calcined and UV-ozone-treated NSs, indicating slightly higher CO\u003csub\u003e2\u003c/sub\u003e uptake and slower desorption for treated NSs, possibly due to the enriched surface hydroxyl groups, which enhance CO\u003csub\u003e2\u003c/sub\u003e affinity.\u003cstrong\u003e f\u003c/strong\u003e, CO\u003csub\u003e2\u003c/sub\u003e permeance under varying feed pressures, illustrating adsorption-dominated transport at low pressures and gradual decline at higher pressures due to site saturation and diffusion effects, where the 1.6 wt.% MMM was tested.\u003c/p\u003e","description":"","filename":"image6.png","url":"https://assets-eu.researchsquare.com/files/rs-7510110/v1/0b0a8384875e2663cfe8e79c.png"},{"id":92376306,"identity":"fcedb77c-a322-4161-8d6a-b0da4532516e","added_by":"auto","created_at":"2025-09-29 05:05:35","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":210529,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eCO\u003c/strong\u003e\u003csub\u003e\u003cstrong\u003e2\u003c/strong\u003e\u003c/sub\u003e\u003cstrong\u003e permeance and selectivity of MMMs compared to literature-reported zeolite MMMs. a\u003c/strong\u003e, Schematic illustration of CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e separation through MMM consisting of hydroxyl-enriched MFI NSs, which facilitate selective CO\u003csub\u003e2\u003c/sub\u003e adsorption via hydrogen bonding (green line).\u003cstrong\u003e b\u003c/strong\u003e, CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e separation performance benchmarked against literature-reported zeolite MMMs\u003csup\u003e37,44-65\u003c/sup\u003e (summarized in Table S4).\u003c/p\u003e","description":"","filename":"image7.png","url":"https://assets-eu.researchsquare.com/files/rs-7510110/v1/3d28c920d587267aa78c54b1.png"},{"id":92391469,"identity":"3bf21d89-ef50-4047-aac0-e3f20e327149","added_by":"auto","created_at":"2025-09-29 08:40:59","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":5744722,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7510110/v1/325786a5-b053-4825-8e96-1a2ffc9f8492.pdf"},{"id":92376304,"identity":"927ee370-ffa1-4438-a762-2cd67c91e3f2","added_by":"auto","created_at":"2025-09-29 05:05:35","extension":"xlsx","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":33494,"visible":true,"origin":"","legend":"dataset 1","description":"","filename":"tableS4.xlsx","url":"https://assets-eu.researchsquare.com/files/rs-7510110/v1/7c445614cf490d2d75188f6e.xlsx"},{"id":92376326,"identity":"a48f24d0-a3cd-484f-b7e3-16bf8a719954","added_by":"auto","created_at":"2025-09-29 05:05:36","extension":"pdf","order_by":2,"title":"","display":"","copyAsset":false,"role":"supplement","size":1206490,"visible":true,"origin":"","legend":"Water-based UV-ozone activation enables aggregation-free processing of MFI nanosheets for membrane fabrication","description":"","filename":"Supplementary.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7510110/v1/3ad81f405b01740b7fbe2d19.pdf"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Water-based UV-ozone activation enables aggregation-free processing of MFI nanosheets for membrane fabrication","fulltext":[{"header":"Introduction","content":"\u003cp\u003eThe development of high-performance membranes for gas separation, particularly for hydrocarbon separation, has garnered significant attention in recent years due to the pressing need for energy-efficient and scalable separation technologies\u003csup\u003e\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u003c/sup\u003e. MFI zeolite membranes have demonstrated considerable potential in the field of gas separation, particularly in ultra-thin configurations with vertical channels along the \u003cem\u003eb\u003c/em\u003e-axis (\u003cem\u003eb\u003c/em\u003e-oriented). This configuration offers reduced transport pathways and substantial mitigation of diffusion resistance, thereby accelerating gas diffusion processes\u003csup\u003e\u003cspan additionalcitationids=\"CR3\" citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e\u003c/sup\u003e. It has been widely recognized that nanometer-thick \u003cem\u003eb\u003c/em\u003e-oriented MFI nanosheets (NSs) have considerable potential as building blocks for the fabrication of highly \u003cem\u003eb\u003c/em\u003e-oriented MFI membranes\u003csup\u003e\u003cspan additionalcitationids=\"CR6\" citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e\u003c/sup\u003e. With cross-sectional dimensions of 5.6\u0026times;5.3 \u0026Aring; for the channel along the \u003cem\u003eb\u003c/em\u003e-axis (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e) and CO\u003csub\u003e2\u003c/sub\u003e-affinity, \u003cem\u003eb\u003c/em\u003e-oriented MFI is an attractive option for practical CO\u003csub\u003e2\u003c/sub\u003e separation from gas mixtures, such as CO\u003csub\u003e2\u003c/sub\u003e/H\u003csub\u003e2\u003c/sub\u003e\u003csup\u003e8,9\u003c/sup\u003e, CO\u003csub\u003e2\u003c/sub\u003e/CH\u003csub\u003e4\u003c/sub\u003e\u003csup\u003e10,11\u003c/sup\u003e, CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e\u003csup\u003e12,13\u003c/sup\u003e.\u003c/p\u003e\u003cp\u003eMFI inorganic membranes are among the most commonly fabricated membranes due to their excellent gas permeation flux, which is often significantly higher than that of polymer membranes\u003csup\u003e\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e,\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e\u003c/sup\u003e. However, conventional calcination for pore activation to remove organic templates inside the channels often induces cracks and grain boundaries, compromising membrane integrity\u003csup\u003e\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e\u003c/sup\u003e. Beyond this challenge, purely inorganic MFI membranes also suffer from inherent brittleness, the need for expensive ceramic substrates, and difficulties in large-scale fabrication, all of which hinder their broader industrial implementation\u003csup\u003e\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e,\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e\u003c/sup\u003e.\u003c/p\u003e\u003cp\u003eIn contrast, mixed matrix membranes (MMMs) incorporate zeolite fillers within a polymer matrix, offering a promising alternative by combining the advantages of molecular sieving with enhanced mechanical flexibility and scalable processability\u003csup\u003e\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e,\u003cspan additionalcitationids=\"CR19\" citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e\u003c/sup\u003e. However, a significant challenge arises from the substantial aggregation of two-dimensional NSs during processing, which compromises membrane uniformity and reduces NS utilization, consequently diminishing separation performance\u003csup\u003e\u003cspan additionalcitationids=\"CR19 CR20\" citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e\u003c/sup\u003e. This aggregation mainly originates from the zeolite activation step, where organic structure-directing agents (OSDAs) must be removed to open micropores prior to membrane fabrication. Conventional activation by calcination at ~\u0026thinsp;500\u0026deg;C in air efficiently eliminates OSDAs but simultaneously induces irreversible wrinkling and aggregation of NSs, drastically lowering their solvent-dispersion yields and impairing both processability and membrane performance\u003csup\u003e\u003cspan additionalcitationids=\"CR19\" citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e\u003c/sup\u003e. Alternatively, low-temperature ozone activation can also decompose the organic template under milder conditions (~\u0026thinsp;200\u0026deg;C) by flowing ozone (generated from high-purity O\u003csub\u003e2\u003c/sub\u003e) through the zeolite powder. However, this method cannot avoid the irreversible aggregation problem, as the powder is already in dried form\u003csup\u003e\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e\u003c/sup\u003e.\u003c/p\u003e\u003cp\u003ePost-calcination processes can be applied to mitigate aggregation, such as ball milling, yielding modest improvement, with dispersion yields after calcination remaining below 10%\u003csup\u003e20,23\u003c/sup\u003e. This is primarily because NSs tend to form tightly bound aggregates upon drying, making subsequent redispersion highly challenging. Another way to avoid the aggregation problem is to fabricate a membrane using the as-synthesized nanosheets and then removing the OSDA by ultraviolet (UV)-ozone treatment in air\u003csup\u003e\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e,\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e\u003c/sup\u003e. However, this activation has been carried out on pre-formed, dried membranes rather than in the liquid phase, requiring at least six days of UV exposure to achieve complete template removal. This method is therefore time-consuming and limited on UV-resistant substrates, making it unsuitable for scalable processing.\u003c/p\u003e\u003cp\u003eThe limitations of existing activation methods have motivated efforts to remove OSDA while maintaining the NSs in a dispersed state, thereby avoiding aggregation during solvent processing. Piranha treatment, a liquid-phase activation strategy, has been investigated as a means of enhancing the solvent dispersion yield of MFI NS\u003csup\u003e\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e\u003c/sup\u003e. However, this approach has significant drawbacks, including safety hazards and requirement for multiple treatment rounds, which render it impractical for large-scale implementation. Therefore, developing a mild, liquid-phase UV activation strategy that can activate zeolite NSs in a dispersed state is crucial if zeolite NSs are to be utilized in membrane fabrication and other applications that require ordered assembly of the NSs.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eIn this study, we present a liquid-based template removal strategy for activating the microporous MFI NSs dispersed in aqueous media using UV-ozone treatment (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e). For zeolite NSs, this method offers a distinct advantage of mitigating aggregation, thereby enhancing their dispersibility and usability. Utilizing this activation approach, we have fabricated micrometer-thick, highly \u003cem\u003eb\u003c/em\u003e-oriented MFI MMMs on polyvinylidene fluoride (PVDF) substrates via solution casting. The UV-treatment also enriches the NSs with hydroxyl (-OH) groups, possibly enhancing CO\u003csub\u003e2\u003c/sub\u003e affinity and improving the interfacial compatibility between Pebax 1074 and NSs. The integration of well-aligned NSs within the Pebax matrix has been shown to enhance gas separation performance, achieving a CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e selectivity of 40\u0026thinsp;\u0026plusmn;\u0026thinsp;6 and a CO\u003csub\u003e2\u003c/sub\u003e permeance of 194\u0026thinsp;\u0026plusmn;\u0026thinsp;50 gas permeation units (GPU) at 25℃ under ambient pressure. This methodology has been demonstrated to facilitate the activation process while concomitantly addressing the long-standing challenges associated with NS aggregation and the low solvent-dispersion yield of NSs in conventional calcination. These findings offer a promising foundation for the cost-effective fabrication of MFI or other zeolite-NS-based membranes, as well as for a range of industrial applications of zeolite NSs.\u003c/p\u003e"},{"header":"Results","content":"\u003cp\u003e\u003cb\u003eOrganic template removal in aqueous media under UV-ozone irradiation.\u003c/b\u003e We compare three methods for removing the organic template occluded in the MFI NSs. Conventionally, template removal is accomplished through high-temperature calcination in air, whereby the NSs are gradually heated to 550\u0026deg;C and maintained at this temperature for an extended period to facilitate the combustion of the organic template molecules. A chemical alternative to calcination involves piranha treatment, in which the NSs are dispersed in concentrated sulfuric acid and hydrogen peroxide mixtures at 120\u0026deg;C, with periodic replenishment of the oxidant to fully decompose the template. As the third method we present a milder approach by dispersing the NSs in aqueous solution and exposing them to UV light coupled with ozone. This allows for the gradual decomposition of the template. This decomposition occurs at moderate temperatures and does not require aggressive thermal or chemical conditions.\u003c/p\u003e\u003cp\u003eTo confirm the effectiveness of aqueous UV-ozone treatment in activating MFI NSs, we conducted a series of structural and compositional analyses. It is important to note that the organic template in this work refers to bis-1,5 (tripropyl ammonium) pentamethylene diiodide (dC5) (Fig. \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e, chemical structure). First, N\u003csub\u003e2\u003c/sub\u003e adsorption-desorption measurements verify the complete removal of the organic template, as the isotherms of both UV-ozone-treated NSs (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea, purple circle) and calcined NSs (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea, pink square) exhibited a typical open-pore structure with a surface area of ~\u0026thinsp;416 m\u003csup\u003e2\u003c/sup\u003e/g, calculated by Brunauer-Emmett-Teller (BET) method. However, piranha-treated NSs and as-synthesized NSs exhibit a smaller surface area, measuring 158 cm\u003csup\u003e2\u003c/sup\u003e/g and 57 cm\u003csup\u003e2\u003c/sup\u003e/g, respectively, implying incomplete activation. Furthermore, pore size distribution analysis demonstrates the presence of micropores in the 0.5\u0026ndash;0.6 nm range for UV-ozone treated NSs (Fig. S2, purple circle), which is similar to the calcined sample (Fig. S2, pink square). In contrast, piranha-treated NSs and as-synthesized NSs (green and black triangle) do not exhibit similar micropores, confirming incomplete activation.\u003c/p\u003e\u003cp\u003eFurther evidence of the efficacy of UV-ozone treatment is provided by chemical composition analysis. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb, Fourier transform infrared spectroscopy (FTIR) data of the as-synthesized NSs with the organic templates present peaks at 2850\u0026ndash;2970 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 1560 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, attributed to C-H vibrations, and 1469 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e belonging to C-N vibrations. However, both UV-ozone-treated NSs (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb, purple curve) and calcined NSs (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb, pink curve) demonstrate the elimination of C-H and C-N vibrations, thereby confirming complete template removal. In contrast, as-synthesized NSs and piranha-treated NSs exhibit weak C-H peaks and a prominent C-N peak, suggesting incomplete template removal. Furthermore, the UV-ozone treatment results in the introduction of -OH groups on the NSs surface. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb, the FTIR spectrum of UV-ozone treated NS exhibited a broad peak at 3000\u0026ndash;3500 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and a peak at 1629 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, which are attributed to -OH and silanol (Si-OH), respectively. This finding indicates that UV-ozone treatment enhances surface hydrophilicity while removing organic species.\u003c/p\u003e\u003cp\u003eThermogravimetry analysis (TGA) results (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec and Table \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e) provide further insight into the effectiveness of template removal. At around 130\u0026deg;C, both UV-ozone-treated and calcined NSs exhibit approximately 6% weight loss, which is primarily attributed to the desorption of physically adsorbed water or gas molecules from the internal pores and external surfaces. In contrast, as-synthesized and piranha-treated NSs show significantly lower weight losses of only 1\u0026ndash;2% in this temperature range. At elevated temperatures, more distinct differences emerge. Between 400 and 600\u0026deg;C, the UV-ozone-treated NSs (purple curve) exhibit a modest 3.2% weight loss, which can be attributed to the condensation and dehydration of terminal silanol groups\u003csup\u003e\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e,\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e\u003c/sup\u003e. Notably, no significant weight loss is observed for calcined NSs in this range, suggesting the silanol condensation to be specific to the UV-ozone-modified surface chemistry. By contrast, both as-synthesized and piranha-treated NSs exhibit substantial weight losses of 17.1% and 15.6%, respectively, at around 600\u0026deg;C. These losses are consistent with the decomposition of retained organic templates (e.g., dC5), confirming incomplete template removal in these samples.\u003c/p\u003e\u003cp\u003eMoreover, X-ray photoelectron spectroscopy (XPS) (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed, e) provides additional evidence for the above discussion. For both UV-ozone-treated and calcined NSs, the characteristic peak at ~\u0026thinsp;402 eV, corresponding to C-N bonds from the dC5, completely disappears, confirming the successful elimination of residual organics. This finding aligns with the TGA and FTIR results, indicating efficient template removal by UV-ozone treatment. Furthermore, energy-dispersive X-ray spectroscopy (EDS) exhibits consistent results. Figure\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ef-j and Fig. S3 show TEM-EDS (UV-ozone treated NSs) and SEM-EDS results (as-synthesized and UV-ozone treated NSs), respectively, which reveal the near-negligible amount about of nitrogen in UV-ozone-treated NSs, while Si and O are present as expected. Besides, XRD analysis (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ek) confirms that the crystallinity of UV-ozone-treated NSs remains identical to that of calcined samples, demonstrating that the treatment does not compromise structural integrity. The crystallinity can be further assessed via TEM imaging and SAED (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003el,m), which confirm that UV-ozone-treated NSs retain their crystalline structure without signs of degradation, consistent with XRD results. Overall, UV-ozone treatment effectively removes organic templates from NSs, as confirmed by above analyses.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003e\u003cb\u003eTime-dependent decomposition of dC5 under UV-ozone treatment.\u003c/b\u003e To better understand how UV-ozone treatment enables effective template removal without damaging the NS structure, we further investigated the time-dependent degradation pathway of the dC5. Based on combined FTIR and XPS analyses, we propose a possible UV-ozone degradation mechanism for the dC5 (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea,b). In the early stages of irradiation, reactive oxidative species such as hydroxyl radicals (\u0026bull;OH) initially attack the terminal CH\u003csub\u003e2\u003c/sub\u003e and CH\u003csub\u003e3\u003c/sub\u003e groups exposed at the pore openings, leading to the formation of CO\u003csub\u003e2\u003c/sub\u003e, NO\u003csub\u003ex\u003c/sub\u003e, and other volatile byproducts (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e and Fig. S4)\u003csup\u003e\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e\u003c/sup\u003e. This initial step is structurally supported by density functional theory (DFT) simulations of MFI/dC5 systems (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb, along \u003cem\u003eb\u003c/em\u003e and \u003cem\u003ec\u003c/em\u003e axis), which reveal that several dC5 molecules partially extend beyond the zeolite pore openings, making their terminal groups accessible to oxidative species, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea and \u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb\u003csup\u003e\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e\u003c/sup\u003e. As the exposure progresses, increased molecular mobility facilitates the migration of residual organics out of the pores or enables deeper penetration of oxidants, resulting in further decomposition of the internal (the dC5 fading progress is shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb, along \u003cem\u003eb\u003c/em\u003e and \u003cem\u003ec\u003c/em\u003e axis). As supported by FTIR spectra in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ec, the NSs exposed to UV-ozone for 0, 12, 36, 60, and 72 hours exhibit a gradual disappearance of CH\u003csub\u003e2\u003c/sub\u003e and CH\u003csub\u003e3\u003c/sub\u003e peaks (2850\u0026ndash;2970 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and 1560 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e). Notably, the C-H signal declines sharply within the first 12 hours, consistent with the early removal of aliphatic groups from external surfaces (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea). However, the C-N peak (1469 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e), which is more representative of the internal template within the zeolite channels, persists until 36 hours and disappears after 60 hours. This time lag indicates the diffusion-limited access of oxidants into the internal pore network. Besides, the FTIR spectra show a gradual increase in the -OH stretching band (~\u0026thinsp;3400 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e) with prolonged UV-ozone exposure, indicating the formation of surface hydroxyl groups during template degradation.\u003c/p\u003e\u003cp\u003eXPS analysis further substantiates this temporal degradation profile (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb). The N1s survey signal (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ed) diminishes progressively with irradiation time, confirming the continuous loss of nitrogen-containing organic residues. A residual N signal after 72 hours (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ed) is likely attributable to adventitious nitrogen adsorbed from ambient air, rather than incomplete decomposition. High-resolution C1s spectra (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ee) show a consistent decline in the integrated intensity of C-C (285 eV) and C-N (286 eV) bonds, alongside a slight rightward shift, indicative of oxidation to more electronegative environments. Consequently, the N1s peak at 402 eV (C-N) in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ef persists until 36 hours and disappears after 60 hours, perfectly aligning with the FTIR observations. These results confirm that UV-ozone treatment achieves complete removal of dC5 templates via a gradual, depth-dependent oxidative mechanism, avoiding structural damage. The combined spectroscopic trends provide compelling evidence for both the efficacy and gentleness of this approach.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003e\u003cb\u003eEnhanced interfacial compatibility of MFI NSs in Pebax-based MMMs.\u003c/b\u003e The conventional high-temperature calcination leads to severe aggregation and loss of structural integrity (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea). The solvent-dispersion yield can be decreased to less than 10%, even after making more efforts such as tip sonication and ball-milling\u003csup\u003e\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e,\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e\u003c/sup\u003e. In contrast, the dispersibility of the NSs after UV-ozone-treatment is confirmed by SEM, displaying well-aligned NS without aggregations (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb).\u003c/p\u003e\u003cp\u003eIn order to gain initial insight into the stacking behavior of UV-ozone-treated MFI NSs, we first fabricated NS membranes by vacuum filtration. Despite the SEM of the resulting membranes showing well-aligned NS stacking (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ec), significant interlayer voids are also present (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ed), suggesting incomplete packing. This void formation can be attributed to the inherent morphological thickness nonuniformity of the MFI NSs. As atomic force microscopy (AFM) analysis reveal (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ee), the seed-like central domains reach\u0026thinsp;~\u0026thinsp;30 nm thickness (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ef). Still, the majority of the NS area exhibits a uniform thickness of 6\u0026ndash;7 nm (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eg). These bulky centers have been shown to originate from secondary ad-layer growth during the synthesis process\u003csup\u003e\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e,\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e,\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e\u003c/sup\u003e. Such local thickening disrupts the NSs stacking during vacuum filtration and gives rise to the observed voids. Therefore, a critical challenge lies in the removal or minimization of these central domains to produce thickness-homogeneous NSs suitable for dense membrane assembly.\u003c/p\u003e\u003cp\u003eAddressing this issue, we subsequently applied post-treatment strategies to fragment the NSs into more uniform NSs, which were then used for the following MMM fabrication. The activated MFI NSs were processed by tip sonication and centrifugation, effectively removing the thicker ad-layer regions at the NS centers, which results in flat and well-dispersed fragments (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eh, as indicated by yellow dotted line). These NS fragments exhibit excellent dispersibility in water and ethanol, enabling their incorporation into a Pebax\u0026reg; 1074 solution for MMM fabrication.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eIt is acknowledged that achieving uniform and defect-free dispersion of NSs within polymer matrices persists as a formidable challenge, particularly due to interfacial incompatibility\u003csup\u003e\u003cspan additionalcitationids=\"CR19 CR20\" citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e\u003c/sup\u003e. The enhanced hydrophilicity of the UV-ozone-treated MFI NSs, attributable to the presence of hydroxyl groups, leads to significant improvement in their dispersion within the hydrophilic Pebax\u0026reg; 1074 block copolymer, comprising polyether (PEO) and polyamide (PA) segments (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea). As confirmed by FTIR and TGA analysis (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb,c), the UV-ozone treatment introduces abundant surface hydroxyl groups (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eb). Further evidence from the O1s XPS spectrum demonstrates enhanced signals corresponding to -OH and Si-O species (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ec), thereby validating the occurrence of ozone-induced hydrolysis. These chemical alterations result in a substantial increase in hydrophilicity, as evidenced by a decrease in the water contact angle from 46.1\u0026deg; (pristine NSs) to 11.7\u0026deg; following the UV-ozone treatment (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ed). The enhanced hydrophilicity can lead to better compatibility with the Pebax\u0026reg; 1074 matrix by improving surface energy matching. These NSs with -OH groups present a more polar surface, which facilitates stronger interfacial interactions, such as hydrogen bonding and dipole-dipole interactions, with the polar groups (ether oxygens and amide functionalities) in Pebax chains (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eb) \u003csup\u003e\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e,\u003cspan additionalcitationids=\"CR33\" citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e\u003c/sup\u003e.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eThe MMMs were prepared by drop-casting the homogeneous NS-polymer mixture onto glass petri dishes and covering them with 25 mm PVDF in diameter substrates to form ultrathin films. The MFI content in the MMMs was measured precisely by TGA, revealing 4 wt.% and 1.6 wt.% weight percentage in different MMM samples (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ee). The fabricated MMMs have NS alignment in (0 \u003cem\u003e2\u003c/em\u003e 0) plane as shown by the XRD analysis (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ef). This alignment is reinforced by the shear forces during the solvent evaporation\u003csup\u003e\u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e,\u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e\u003c/sup\u003e. After removing the solvents at 80\u0026deg;C for 2h, the membranes were peeled off by soaking in water and tweezers, after that vacuum drying overnight at 80\u0026deg;C was conducted. The top-view and the cross-section of the MMMs are shown by the SEM images (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eg-l), displaying excellent dispersibility and interfacial adhesion of NSs within the Pebax matrix. Even at high NS loadings (\u0026gt;\u0026thinsp;10 wt.%), no aggregation can be observed, with the NSs exhibiting a well-aligned \u003cem\u003eb\u003c/em\u003e-orientation, as indicated by the yellow arrows (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eg). However, at high loadings, voids can be observed in the membrane structure (Fig. S5), due to incomplete polymer infiltration. Reduced loading can also enable significant thinning down of the MMMs (~\u0026thinsp;1 \u0026micro;m, Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ek and l) with reduced voids and more homogeneous NS distribution (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eh,i), attributed to improved polymer infiltration and reduced crowding. Overall, surface functionalization through UV-ozone activation significantly enhances the interfacial compatibility between NSs and the polymer, leading to improved dispersibility and uniform distribution of the NSs in the MMMs.\u003c/p\u003e\u003cp\u003e\u003cb\u003eThin zeolite MMMs for CO\u003c/b\u003e\u003csub\u003e\u003cb\u003e2\u003c/b\u003e\u003c/sub\u003e\u003cb\u003e/N\u003c/b\u003e\u003csub\u003e\u003cb\u003e2\u003c/b\u003e\u003c/sub\u003e \u003cb\u003eseparation with enhanced selectivity.\u003c/b\u003e Recent advances in the fabrication of MMMs have primarily focused on membranes with thicknesses in the range of tens to hundreds of micrometers, typically produced via solution casting techniques\u003csup\u003e\u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e,\u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e\u003c/sup\u003e. However, the development of \"thin MMMs\" with sub-2-\u0026micro;m thicknesses, represents both a technical challenge and a promising direction for high-performance gas separation\u003csup\u003e\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e\u003c/sup\u003e. In this study, the MMMs can be classified within this emerging category, with thicknesses of approximately 1 \u0026micro;m.\u003c/p\u003e\u003cp\u003eIn order to accurately assess and present the separation performance of thin membranes, it is imperative to report the gas transport data in terms of permeance, rather than permeability. While the latter is a valuable metric for comparing membrane materials due to its correlation with membrane thickness, it may overestimate the membrane performance, as they exclude any detrimental issues associated with membrane thinning. Conversely, permeance directly reflects the flux performance normalized by pressure difference, offering a more practical and consistent metric for evaluating thin membranes.\u003c/p\u003e\u003cp\u003eMMMs on PVDF substrates with 25 mm-diameter are used for gas separation characterization (Fig.\u0026nbsp;6a). The effective gas permeation area was 1.33 cm\u003csup\u003e\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e\u003c/sup\u003e, defined by the o-ring in the membrane fixture. The CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e separation measurements were done under ambient conditions using an equimolar binary gas mixture (Fig.\u0026nbsp;6b and Fig. S6). The permeance-selectivity results in Fig.\u0026nbsp;6b indicate that both CO\u003csub\u003e2\u003c/sub\u003e permeance and CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e selectivity exhibit a strong dependence on the MFI NS loading. The separation performance improves with increasing filler content, reaching the maximum CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e selectivity of 40\u0026thinsp;\u0026plusmn;\u0026thinsp;6 at 1.6 wt.% NS loading. This is ~\u0026thinsp;20 times higher than that of Pebax matrix, while the CO\u003csub\u003e2\u003c/sub\u003e permeance (194\u0026thinsp;\u0026plusmn;\u0026thinsp;50 GPU) is slightly lower than the Pebax matrix. However, further increasing the loading to 4 wt.% leads to a slight decline in the selectivity (25\u0026thinsp;\u0026plusmn;\u0026thinsp;3). At an even higher loading of 10 wt.%, the selectivity drops significantly to 4\u0026thinsp;\u0026plusmn;\u0026thinsp;3 (Table S2). This deterioration suggests that the presence of a residual ad-layer hinders the alignment of NSs within the MMMs (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ee), leading to void formation. Furthermore, the permeability values for the MMMs with varying loadings have been calculated. Fig. S7 shows the permeabilities of MMMs identical to Fig.\u0026nbsp;6b, which monotonically increase with MFI NS loadings. This might give a misleading impression that higher loadings are better for the overall performance, thus confirming our initial reasoning that permeance values should be compared.\u003c/p\u003e\u003cp\u003eTo ensure the reproducibility of our findings, we conducted batch-to-batch variation tests on MMMs with an optimal NS loading of 1.6 wt.% (Fig.\u0026nbsp;6c and Table S3). The four independent batches (M1-M4) demonstrate highly consistent CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e separation performance (CO\u003csub\u003e2\u003c/sub\u003e permeance of 194\u0026thinsp;\u0026plusmn;\u0026thinsp;7 GPU and selectivity of 40\u0026thinsp;\u0026plusmn;\u0026thinsp;4 on average), thereby substantiating the reliability of our fabrication approach. Furthermore, long-term stability tests were performed over a 22-hour period under continuous CO\u003csub\u003e2\u003c/sub\u003e exposure. As shown in Fig.\u0026nbsp;6d, both CO\u003csub\u003e2\u003c/sub\u003e permeance and selectivity remained nearly constant throughout the testing period, demonstrating excellent durability.\u003c/p\u003e\u003cp\u003eBesides the excellent interfacing of the NSs and the polymer matrix, the CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e selectivity enhancement can also be attributed to the increased number of hydroxyl groups on the NSs. CO\u003csub\u003e2\u003c/sub\u003e adsorption-desorption measurements at room temperature (Fig.\u0026nbsp;6e) indicate a slightly higher CO\u003csub\u003e2\u003c/sub\u003e adsorption capacity (42.6 cm\u003csup\u003e3\u003c/sup\u003e/g) for the UV-ozone-treated NSs compared to the calcined NSs (39.6 cm\u003csup\u003e3\u003c/sup\u003e/g). Considering their similar pore structures, this higher capacity can be attributed not to the increased porosity, but rather to the introduction of hydroxyl groups, which offers stronger interactions with CO\u003csub\u003e2\u003c/sub\u003e molecules (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eb). Further supporting this, the UV-ozone-treated NSs also showed a significantly slower desorption rate (Fig.\u0026nbsp;6e, purple triangle with solid dot), probably due to the CO\u003csub\u003e2\u003c/sub\u003e interaction with NSs or the inter-nanosheet gaps caused by enriched hydroxyl groups. These stronger interactions can be attributed to hydrogen bonding and dipole-quadrupole interactions between CO\u003csub\u003e2\u003c/sub\u003e and the polar -OH groups\u003csup\u003e\u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e40\u003c/span\u003e\u003c/sup\u003e.\u003c/p\u003e\u003cp\u003eMost importantly, these hydroxyl groups provide more energetically favorable adsorption sites for CO\u003csub\u003e2\u003c/sub\u003e, directly validating the role of functional groups in enhancing selective adsorption. Specifically, CO\u003csub\u003e2\u003c/sub\u003e exhibits a significantly higher adsorption enthalpy (27.5\u0026ndash;50 kJ/mol) on the MFI framework compared to N\u003csub\u003e2\u003c/sub\u003e (13.8 kJ/mol)\u003csup\u003e41\u003c/sup\u003e. The presence of polar hydroxyl groups further amplifies this disparity, enabling preferential adsorption of CO\u003csub\u003e2\u003c/sub\u003e, while N\u003csub\u003e2\u003c/sub\u003e, with its lower affinity and non-polar nature, is more readily excluded, thereby increasing CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e selectivity\u003csup\u003e\u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e40\u003c/span\u003e,\u003cspan citationid=\"CR42\" class=\"CitationRef\"\u003e42\u003c/span\u003e,\u003cspan citationid=\"CR43\" class=\"CitationRef\"\u003e43\u003c/span\u003e\u003c/sup\u003e.\u003c/p\u003e\u003cp\u003eWhile UV-ozone-treated NSs provide strong CO\u003csub\u003e2\u003c/sub\u003e affinity at low pressure due to abundant surface hydroxyl groups, the preferential adsorption advantage is gradually offset at higher pressures by higher N\u003csub\u003e2\u003c/sub\u003e flux and competitive site occupation. As the feed pressure increased, both CO\u003csub\u003e2\u003c/sub\u003e permeance and selectivity declined (Fig.\u0026nbsp;6f). This can be attributed to the saturation of surface adsorption sites and a shift in transport mechanism from adsorption-dominated to more diffusion-governed. Moreover, polymer chain compression and reduced interfacial porosity may contribute to the overall decline in gas permeance. These observations indicate that the selectivity enhancement from surface functionalization is most effective under moderate-pressure conditions where adsorption-driven transport is dominant.\u003c/p\u003e"},{"header":"Discussion","content":"\u003cp\u003eThis study demonstrates that UV-ozone treatment in an aqueous medium offers an effective low-temperature strategy to activate MFI NSs while preventing aggregations and simultaneously enhancing their structural and interfacial properties. This enables the fabrication of high-performance thin membranes. In comparison with thermal activation, which frequently results in irreversible aggregation and compromises NS alignment, the non-thermal UV-ozone method preserves the NSs in a dispersed, open-pore state, thereby markedly enhancing their utilization efficiency in membrane fabrication. Beyond the opening of micropores and the prevention of aggregation, the UV-ozone treatment introduces hydroxyl groups, which serve to enhance the hydrophilicity and dispersion of NSs in the Pebax matrix. Additionally, these hydroxyl groups modulate gas transport behavior.\u003c/p\u003e\u003cp\u003eA schematic representation of the CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e separation mechanism through the resulting MMMs, consisting of UV-ozone-activated MFI NSs, is presented in Fig.\u0026nbsp;7a. The NS-aligned structure provides a selective pathway and strong interaction for CO\u003csub\u003e2\u003c/sub\u003e molecules while effectively hindering the transport of less soluble N\u003csub\u003e2\u003c/sub\u003e, resulting in enhanced separation performance. We have benchmarked our MMMs against literature-reported zeolite-based MMMs (Fig.\u0026nbsp;7b, Table S4). The membranes in this study exhibit two orders of magnitude higher CO\u003csub\u003e2\u003c/sub\u003e permeance in comparison to hundred-micrometer-thick MMMs, while maintaining competitive selectivity. This significant enhancement can be attributed to a synergistic effect, whereby two factors contribute to the observed outcome. Firstly, the enhanced dispersibility and interfacial compatibility of the NSs within the polymer matrix effectively suppress aggregation. Secondly, the reduced membrane thickness on a micron scale significantly lowers the diffusion resistance for gas molecules, thereby boosting overall separation performance. Compared to our previously-reported platelike MFI MMMs (\u0026lt;\u0026thinsp;5 \u0026micro;m), the MMMs here achieves a fivefold increase in CO\u003csub\u003e2\u003c/sub\u003e permeance and a 2.4-fold improvement in CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e selectivity\u003csup\u003e\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e\u003c/sup\u003e. Furthermore, this low filler loading membrane has two notable benefits. First, it substantially reduces material cost. Second, it enhances processability while maintaining membrane flexibility and structural integrity. Conversely, the utilization of excessive filler loadings in conventional MMMs frequently results in filler agglomeration, interfacial voids, and augmented membrane brittleness, collectively leading to a deterioration in separation performance. Hence, a meticulously designed polymer-filler interface has the potential to achieve high efficiency even at low filler loadings.\u003c/p\u003e\u003cp\u003eIn summary, the UV-ozone treatment method presented here facilitates the drying-free activation of zeolite NSs in an aqueous environment, thereby eliminating the necessity for high-temperature calcination. Consequently, this approach enables the scalable production of flexible and thin membranes with enhanced selectivity, thereby paving the way for energy-efficient CO\u003csub\u003e2\u003c/sub\u003e separation technologies. The ultrathin and well-aligned morphology of the MMM, in conjunction with its excellent interfacial matching and hydroxyl functionalization, yields exceptional performance even with a filler loading as low as 1.6 wt.% (for ~\u0026thinsp;1 \u0026micro;m-thick membranes: CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e selectivity\u0026thinsp;=\u0026thinsp;40\u0026thinsp;\u0026plusmn;\u0026thinsp;6; CO\u003csub\u003e2\u003c/sub\u003e permeance\u0026thinsp;=\u0026thinsp;194\u0026thinsp;\u0026plusmn;\u0026thinsp;50 GPU at 25\u0026deg;C, ambient pressure). These MMMs exhibit high performance that surpasses most zeolite-based MMMs reported in the literature. Subsequent endeavors would center on decreasing the membrane thickness to the hundred-nanometer range, optimizing flatter NSs synthesis, and enhancing NS alignment to promote advancements in industrial applications.\u003c/p\u003e"},{"header":"Methods","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e\u003cp\u003e\u003cb\u003eChemicals.\u003c/b\u003e Tetraethoxysilane (TEOS, Macklin) and silicic acid (H\u003csub\u003e4\u003c/sub\u003eSiO\u003csub\u003e4\u003c/sub\u003e, Aladdin) were used as silicon sources. Tetrapropylammonium hydroxide (TPAOH, 25 wt.% aqueous solution, Aladdin) served as the structure-directing agent. Potassium hydroxide (KOH, \u0026ge;\u0026thinsp;85%, pellet) was bought from China National Pharmaceutical Group Chemical Reagent Co., Ltd. Organic compounds including 1,5-diaminopentane (Macklin), 1-iodopropane (J\u0026amp;K), and butanone (SCR) were employed as reactants and solvents for dC5 template synthesis. N, N-Dimethylformamide (DMF, SCR) was also used as a dispersing solvent.\u003c/p\u003e\u003cp\u003eFor membrane fabrication, Pebax 1074 (Arkema) was used as the polymer matrix. Hydrophilic PVDF (0.45 \u0026micro;m pore size (BS-PVDF-45), Merck Millipore) was used for membrane fabrication.\u003c/p\u003e\u003cp\u003e\u003cb\u003ePreparation of MFI NSs.\u003c/b\u003e The MFI NSs were synthesized using a two-step process as described in the previous report\u003csup\u003e\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e,\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e\u003c/sup\u003e. In brief, the synthesis involved initial fragment growth and secondary growth, using molar ratios of 80 TEOS: 3.75 dC5: 20 KOH: 9500 H\u003csub\u003e2\u003c/sub\u003eO: 320 ethanol. The fragment synthesis was conducted at 155\u0026deg;C for 3 days with rotary stirring at 60 rpm, followed by secondary growth under identical conditions. This process yielded high-aspect-ratio NSs with excellent dispersion, suitable for membrane fabrication.\u003c/p\u003e\u003cp\u003eMFI NS fragments were initially synthesized through rotational intergrowth triggered by nanocrystals as seeds, using the dC5 template, as previously described by Tsapatsis\u003csup\u003e\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e\u003c/sup\u003e. Firstly, the seed crystals (~\u0026thinsp;30 nm), were prepared using a molar ratio of 10 SiO\u003csub\u003e2\u003c/sub\u003e: 2.4 TPAOH: 0.87 NaOH: 114 H\u003csub\u003e2\u003c/sub\u003eO\u003csup\u003e\u003cspan citationid=\"CR66\" class=\"CitationRef\"\u003e66\u003c/span\u003e\u003c/sup\u003e. by mixing 1.096 g NaOH, 61.39 g TPAOH (25 wt.% aqueous), and 18.607 g deionized water, stirring for 15 min at room temperature. Subsequently, 18.90 g of solid H\u003csub\u003e4\u003c/sub\u003eSiO\u003csub\u003e4\u003c/sub\u003e was added, and the precursor was stirred overnight for hydrolysis. The mixture was then heated in a 50\u0026deg;C-oil bath for 6 days with stirring at 1000 rpm, followed by a filtration using a 0.45 \u0026micro;m GHP syringe filter to remove any aggregates. The filtrate was further heated in a 100\u0026deg;C-oil bath for 3 days without stirring. The resulting nanocrystals were purified by centrifugation at 11,000 revolutions per minute (rpm) for 1 h, followed by rinsing with deionized water. The centrifugation and rinsing processes were repeated twice, and the final product was diluted to 0.48 wt.% with water.\u003c/p\u003e\u003cp\u003eNext, the dC5 template was synthesized through exhaustive alkylation of 1,5-diaminopentane with 1-iodopropane, following the procedure outlined by Bonilla et al\u003csup\u003e\u003cspan citationid=\"CR67\" class=\"CitationRef\"\u003e67\u003c/span\u003e\u003c/sup\u003e. Its purity was confirmed by proton nuclear magnetic resonance (\u003csup\u003e\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u003c/sup\u003eH NMR), as shown in Fig. \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e.\u003c/p\u003e\u003cp\u003eFor MFI NS fragments synthesis, 0.31 g KOH, 4.0 g TEOS, 0.549 g dC5 (as-synthesized), and 41.04 g deionized water were thoroughly mixed and hydrolyzed at 30\u0026deg;C for 16 h, with pH 10.4. The dust and impurities were removed by vacuum filtration, followed by adding 0.3 g of 0.48 wt.% nanocrystal seed. This mixture was then transferred to an autoclave with Teflon beads to promote fragment formation. The autoclaves were then subjected to a preheated oven at 155℃ for 3 days, rotating at 60 rpm. These NS fragments were separated by a combination of 2-min tip sonication and 30-s centrifugation (5000 relative centrifugal force (RCF)) without rinsing, maintaining a pH of 10.4.\u003c/p\u003e\u003cp\u003eFor the secondary growth of NSs, the same precursor molar ratio and procedures were used. The hydrolyzed precursor was mixed with NS fragments 1.5:1 (weight ratio, e.g., 18 g precursor solution to 12 g fragments solution) and then loaded into an autoclave with an internal volume of 100 mL, which was subjected to 155℃ for 3 days at 60 rpm. After synthesis, the NSs were extracted by centrifugation at 5000 RCF for 30 s. The high-aspect-ratio NSs were dispersed at the top of the solution and were collected at 11,000 rpm for 10 min, followed by rinsing with deionized water. This rinsing process was repeated three to four times, after which the slurry was dispersed into water.\u003c/p\u003e\u003cp\u003eTo increase the crystallization speed, a fast synthetic strategy (FSS) was used. Cleaning of the reactors and loading of precursors followed previously reported procedures\u003csup\u003e\u003cspan citationid=\"CR68\" class=\"CitationRef\"\u003e68\u003c/span\u003e\u003c/sup\u003e. As a result, the large, rectangle-shaped NSs (2.02 \u0026times; 1.64 \u0026micro;m) are produced at 155℃ for 30 hours.\u003c/p\u003e\u003cp\u003e\u003cb\u003eUV-Ozone Activation of MFI NSs in Aqueous Solution.\u003c/b\u003e The as-synthesized NSs were dispersed aqueous solution and exposed to UV light to remove the dC5 occluded in the pores by using a Cnlight UV (23 W ultraviolet light ranging from 185 to 254 nm coupled with ozone) for 12, 36, 60, and 72 h. The maximum temperature of the aqueous solution with a UV chamber inserted was ~\u0026thinsp;58\u0026deg;C. To compare the effects of both UV-ozone-activation and thermal calcination, another batch of NSs was calcined by a traditional procedure. NSs were heated to 550\u0026deg;C with a heating and cooling rate of 1\u0026deg;C min\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e and kept at 500\u0026deg;C for 6 h.\u003c/p\u003e\u003cp\u003e\u003cb\u003ePiranha treatment for MFI NSs.\u003c/b\u003e After synthesis, the MFI NSs were centrifuged several times to remove unreacted precursors before undergoing piranha treatment for template removal. The collected NSs were first mixed with concentrated sulfuric acid, followed by vortexing to ensure uniform dispersion. Subsequently, hydrogen peroxide solution (H\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e2\u003c/sub\u003e, 30%) was added slowly in a volume ratio of 1:3 (H\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e2\u003c/sub\u003e to H\u003csub\u003e2\u003c/sub\u003eSO\u003csub\u003e4\u003c/sub\u003e) to generate the piranha solution directly in a glass container. Extreme caution was exercised during this step due to the highly corrosive and exothermic nature of the mixture, and appropriate personal protective equipment (PPE) was used at all times. The reaction vessel was then placed on a hotplate at 120\u0026deg;C and loosely covered with a watch glass to minimize rapid gas release and prevent liquid splashing. After overnight reaction, additional H\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e2\u003c/sub\u003e was added to replenish the oxidant and maintain reaction efficacy; this step was repeated 5\u0026ndash;6 times. Upon completion, the mixture was diluted and washed thoroughly with deionized water until a neutral pH was reached. The final product was redispersed in aqueous solution for further use.\u003c/p\u003e\u003cp\u003e\u003cb\u003ePreparation of MFI membrane.\u003c/b\u003e As-filtered membranes were prepared by vacuum filtration on PVDF substrates. To reduce the cave and void formation, the UV-ozone-NSs were broken by tip sonication for 40 min to remove the crystals at the thicker ad-layer of the NSs. A homogeneous dispersion of MFI fragments and Pebax 1074 was prepared by thoroughly mixing the components in 70% ethanol. The MFI MMMs were fabricated using a solution casting method. In brief, the mixture was drop-cast in the glass petri dish as reported before\u003csup\u003e\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e\u003c/sup\u003e, covered by a PVDF substrate to obtain ultra-thin MMMs and ensure uniform deposition of the NS-polymer composite. The membrane was dried under vacuum overnight at 80\u0026deg;C to remove residual solvent. For peeling off the membrane, membranes were immersed in water for 0.5-1 h, and then taken off carefully with tweezers.\u003c/p\u003e\u003cp\u003e\u003cb\u003eCharacterizations and measurements.\u003c/b\u003e XRD was performed by a LabX XRD-6100 X-ray diffractometer equipped with Cu Kα radiation (λ\u0026thinsp;=\u0026thinsp;1.5418 \u0026Aring;) within the 5\u0026ndash;50\u003csup\u003e\u0026deg;\u003c/sup\u003e range at a scan rate of 2\u003csup\u003e\u0026deg;\u003c/sup\u003e/min. SEM images of the zeolite samples were captured with a Zeiss MINI 300 at an accelerating voltage of 3.0 kV. High-resolution transmission electron microscopy (HR-TEM), along with electron diffraction and EDS mapping, was performed on a JEOL JEM-2100F microscope operating at 200 kV. Nitrogen adsorption-desorption isotherms at 77 K and CO\u003csub\u003e2\u003c/sub\u003e adsorption-desorption isotherms at 283 K were obtained using an ASAP 2460 analyzer. The height profiles of the MFI NSs were recorded using an Oxford Asylum Research Cypher ES AFM operating in AC mode (tapping), and image processing was carried out with Gwyddion software. FTIR spectroscopy was performed using a Thermo Fisher Scientific Nicolet iS20 spectrometer. TGA was conducted using a Discovery TGA 55 analyzer (TA Instruments, USA). XPS measurements were carried out using a Thermo Scientific K-Alpha instrument. The binding energy range from 0 to 1350 eV was scanned to capture the relevant elements, including Si, C, N, and O. Calibration of the binding energy scale was done by setting the C 1s peak at 284.8 eV to account for charging effects. Water contact angle measurements were conducted using a Theta Flex goniometer from Biolin Scientific.\u003c/p\u003e\u003cp\u003e\u003cb\u003eSample Preparation for SEM and AFM.\u003c/b\u003e SEM and AFM samples were prepared by LB deposition. To be specific, the NSs were first dispersed in a solvent mixture of water and DMF at a 5:1 v/v ratio, followed by 60 min of bath sonication. 0.3 mL of the dispersion was injected onto the surface of the water and spread for 1 h before being transferred vertically onto a 1 \u0026times; 1 cm Si/SiO\u003csub\u003e2\u003c/sub\u003e wafer and air-dried at ambient conditions. The Si/SiO\u003csub\u003e2\u003c/sub\u003e substrate was then heated at 500\u0026deg;C for 8 hours in a furnace to remove organic impurities.\u003c/p\u003e\u003cp\u003e\u003cb\u003eSample preparation for nitrogen adsorption-desorption isotherms.\u003c/b\u003e The as-synthesized NSs were calcinated at 500℃ for 8 h in air, with a heating rate of 1℃/min. NSs treated with piranha solution were rinsed with fresh DI water and dried at 150℃ overnight. The NSs exposed to UV-ozone treatment were filtered, washed with DI water, and dried at 150℃ overnight. These NSs were degassed at 200℃ for 6 h before measurement.\u003c/p\u003e\u003cp\u003e\u003cb\u003eXPS sample preparation.\u003c/b\u003e The samples were prepared by dispersing the NSs in DI water and drop-casting 0.4 mL of the dispersion onto a 5 mm \u0026times; 5 mm substrate. The DI water was allowed to evaporate at ambient conditions, leaving behind a thin film of the NSs on the substrate surface. The samples analyzed included as-synthesized NSs, calcined NSs, NSs treated with piranha solution, and NSs subjected to different UV-ozone exposure times.\u003c/p\u003e\u003cp\u003e\u003cb\u003eCO\u003c/b\u003e\u003csub\u003e\u003cb\u003e2\u003c/b\u003e\u003c/sub\u003e\u003cb\u003e/N\u003c/b\u003e\u003csub\u003e\u003cb\u003e2\u003c/b\u003e\u003c/sub\u003e \u003cb\u003eseparation performance test.\u003c/b\u003e Gas separation experiments were conducted using a membrane sample with an effective area of 1.3 cm in diameter. An equimolar mixture of CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e (10 standard cubic centimeters per minute (sccm) each, total 20 sccm) was introduced to the feed side of the membrane module, while helium (He) was continuously supplied to the permeate side at a flow rate of 20 sccm as a sweep gas. The experiments were conducted using the Wicke-Kallenbach method under controlled conditions of 1 bar pressure and room temperature. The feed gas was introduced on the upstream side of the membrane, while He swept the permeate side. Gas composition was analyzed using a Shimadzu GC-2014C gas chromatograph with a thermal conductivity detector (TCD). Steady-state conditions were established before collecting data to ensure reliable results.\u003c/p\u003e\u003cp\u003eThe permeance of a gas through a membrane is a key parameter that quantifies the intrinsic ability of the membrane to allow the passage of a specific gas under a given pressure difference. It is defined as the molar flux of the gas per unit area, per unit time, and per unit pressure difference. The permeance \u003cem\u003eΠ\u003c/em\u003e of gas component \u003cem\u003ei\u003c/em\u003e is given by the following expression: \u003cem\u003eΠ\u003c/em\u003e\u003csub\u003e\u003cem\u003ei\u003c/em\u003e\u003c/sub\u003e\u0026thinsp;=\u0026thinsp;\u003cem\u003eN\u003c/em\u003e\u003csub\u003e\u003cem\u003ei\u003c/em\u003e\u003c/sub\u003e/(\u003cem\u003eA\u003c/em\u003e∙\u003cem\u003et\u003c/em\u003e∙\u003cem\u003eΔp\u003c/em\u003e), where N\u003csub\u003e\u003cem\u003ei\u003c/em\u003e\u003c/sub\u003e represents the amount of gas component \u003cem\u003ei\u003c/em\u003e that has permeated through the membrane, expressed in moles (mol). \u003cem\u003eA\u003c/em\u003e is the effective area of the membrane, in square meters (m\u003csup\u003e\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e\u003c/sup\u003e), through which the gas is permeating. \u003cem\u003et\u003c/em\u003e is the elapsed time during which the permeation is measured, in seconds (s). \u003cem\u003eΔp\u003c/em\u003e is the pressure difference across the membrane, expressed in Pascals (Pa), which acts as the driving force for the permeation process.\u003c/p\u003e\u003cp\u003eFor practical purposes, the permeance is often expressed in gas permeation units (GPU), where 1 GPU is equivalent to 10\u003csup\u003e\u0026minus;\u0026thinsp;6\u003c/sup\u003e cm\u003csup\u003e3\u003c/sup\u003e(STP) / (cm\u003csup\u003e2\u003c/sup\u003e\u0026middot;s\u0026middot;cmHg) or 3.35\u0026times;10\u003csup\u003e\u0026minus;\u0026thinsp;10\u003c/sup\u003e mol / (m\u003csup\u003e2\u003c/sup\u003e∙s∙Pa). The permeability in Barrer can be calculated via multiplying the permeance (in GPU) by the thickness (\u0026micro;m).\u003c/p\u003e\u003c/div\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eAcknowledgments\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eWe sincerely thank Xiaokun Ding and Xiangcheng Dai\u0026nbsp;for providing technical support in TEM characterization, including high-resolution imaging, selected area electron diffraction (SAED), and EDS mapping, for the as-synthesized and UV-ozone-treated MFI NS samples.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eFunding:\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eNational Natural Science Foundation of China (grant no: 52270108)\u003c/p\u003e\n\u003cp\u003eNational Natural Science Foundation of China Research Fund for International Scientists (grant no: W2432010)\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAuthor contributions:\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eConceptualization: PL, KC\u003c/p\u003e\n\u003cp\u003eMethodology: PL, MZ, YH, XD\u003c/p\u003e\n\u003cp\u003eInvestigation: PL, MZ, YH\u003c/p\u003e\n\u003cp\u003eVisualization: PL, KC\u003c/p\u003e\n\u003cp\u003eSupervision: KC\u003c/p\u003e\n\u003cp\u003eWriting - original draft: PL\u003c/p\u003e\n\u003cp\u003eWriting - discussion and editing: PL, MZ, YH, JZ, DK, KC\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eCompeting interests:\u003c/strong\u003e All other authors declare they have no competing interests.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eData and materials availability:\u003c/strong\u003e All data are available in the main text or the supplementary materials.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eDai Z, Deng L (2023) Membranes for CO\u003csub\u003e2\u003c/sub\u003e capture and separation: Progress in research and development for industrial applications. 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Fuel Process Technol 118:125\u0026ndash;132\u003c/span\u003e\u003c/li\u003e\u003cli\u003e\u003cspan\u003eKhan AL, Klaysom C, Gahlaut A, Khan AU, Vankelecom IF (2013) Mixed matrix membranes comprising of Matrimid and\u0026ndash;SO\u003csub\u003e3\u003c/sub\u003eH functionalized mesoporous MCM-41 for gas separation. J Membr Sci 447:73\u0026ndash;79\u003c/span\u003e\u003c/li\u003e\u003cli\u003e\u003cspan\u003eYu Y, Zhang C, Fan J, Liu D, Meng J (2022) A mixed matrix membrane for enhanced CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e separation via aligning hierarchical porous zeolite with a polyethersulfone based comb-like polymer. J Taiwan Inst Chem Eng 132:104132\u003c/span\u003e\u003c/li\u003e\u003cli\u003e\u003cspan\u003eZhang Y, Balkus Jr KJ, Musselman IH, Ferraris JP (2008) Mixed-matrix membranes composed of Matrimid\u0026reg; and mesoporous ZSM-5 nanoparticles. 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Sep Purif Technol 148:38\u0026ndash;48\u003c/span\u003e\u003c/li\u003e\u003cli\u003e\u003cspan\u003ede Moor P-PE, Beelen TP, van Santen RA (1999) In situ observation of nucleation and crystal growth in zeolite synthesis. A small-angle X-ray scattering investigation on Si-TPA-MFI. J Phys Chem B 103:1639\u0026ndash;1650\u003c/span\u003e\u003c/li\u003e\u003cli\u003e\u003cspan\u003eBonilla G et al (2004) Zeolite (MFI) crystal morphology control using organic structure-directing agents. Chem Mater 16:5697\u0026ndash;5705\u003c/span\u003e\u003c/li\u003e\u003cli\u003e\u003cspan\u003eLi P, Han L, Kim D, Celebi K (2024) A fast synthetic strategy for quick preparation and optimization of platelike MFI crystals. Microporous Mesoporous Mater 365:112905. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1016/j.micromeso.2023.112905\u003c/span\u003e\u003cspan address=\"10.1016/j.micromeso.2023.112905\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"nature-portfolio","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"","title":"Nature Portfolio","twitterHandle":"","acdcEnabled":false,"dfaEnabled":false,"editorialSystem":"ejp","reportingPortfolio":"","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"","lastPublishedDoi":"10.21203/rs.3.rs-7510110/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-7510110/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eZeolite nanosheets offer promising opportunities to fabricate ultrathin molecular sieving platforms for energy-efficient and cost-effective gas separation. However, activating these nanosheets requires a high-temperature calcination process that opens the pores, causing drying and subsequent irreversible aggregation. Once aggregated, most nanosheets cannot be well-aligned to form a continuous thin membrane, which is a persistent bottleneck for mixed matrix membrane fabrication. In this study, we present a facile ultraviolet (UV)-ozone treatment that activates MFI zeolite nanosheets in aqueous solution. This treatment prevents the drying and aggregation of the nanosheets, thereby ensuring high yields of solvent dispersion for open-pore MFI nanosheets. Furthermore, the UV-ozone treatment also introduces hydroxyl groups on the nanosheet surface that enhance both CO\u003csub\u003e2\u003c/sub\u003e adsorption and interfacial compatibility with the polymer matrix. The activated nanosheets are then used to fabricate micrometer-thick, highly \u003cem\u003eb\u003c/em\u003e-oriented MFI mixed matrix membranes on polymer substrates via solution casting. These membranes demonstrate high CO\u003csub\u003e2\u003c/sub\u003e/N\u003csub\u003e2\u003c/sub\u003e selectivity of 40\u0026thinsp;\u0026plusmn;\u0026thinsp;6, with permeances of 194\u0026thinsp;\u0026plusmn;\u0026thinsp;50 GPU (at 25℃, ambient pressure). This method is thus substantiated as an effective and scalable approach for activating zeolite nanosheets and can be a cost-efficient approach for the fabrication of thin, flexible zeolite-nanosheet-based gas separation membranes.\u003c/p\u003e","manuscriptTitle":"Water-based UV-ozone activation enables aggregation-free processing of MFI nanosheets for membrane fabrication","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-09-29 05:05:30","doi":"10.21203/rs.3.rs-7510110/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":"204c33c9-d65c-4620-ba47-58f0bc2f858a","owner":[],"postedDate":"September 29th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[{"id":55396645,"name":"Physical sciences/Chemistry/Chemical engineering"},{"id":55396646,"name":"Physical sciences/Materials science/Nanoscale materials/Two-dimensional materials"}],"tags":[],"updatedAt":"2026-03-24T17:40:43+00:00","versionOfRecord":[],"versionCreatedAt":"2025-09-29 05:05:30","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-7510110","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-7510110","identity":"rs-7510110","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}