Non-solvent Induced Phase Separation Technique Research Articles

High performance gel polymer electrolyte based on P(MMA-co-Sty) and PVDF blend for fast-charging lithium metal batteries with extended cycle life

In the quest for high-energy-density lithium metal batteries (LMBs), the stabilization of lithium (Li) metal anodes during fast charging remains a formidable challenge. In this study, a novel copolymer, Poly(methyl methacrylate-co-styrene) (namely PMS) is synthesized and blended with Poly(vinylidene fluoride) to fabricate a porous gel polymer electrolyte (GPE, namely PMS-PVDF) through the nonsolvent-induced phase separation technique, which significantly enhances the electrochemical stability and fast-charging capabilities of LMBs. The developed GPE exhibits a high ionic conductivity of 5.62 mS cm−1, thereby reducing the formation of detrimental Li dendrites and leading to over 400 h stripping/plating process at 0.5 mA cm−2. Extensive electrochemical tests show that the LMBs with the obtained PMS-PVDF GPE achieve exceptional cycle stability over 600 and 1000 cycles at the C-rates of 0.5 and 3 C, respectively, outperforming traditional electrolytes. Furthermore, the ultra-stability of the quasi-solid-state electrolyte is demonstrated in a 375 mAh pouch cell setup, suggesting an essential trait for the practical application of high-power devices. This work marks a pivotal contribution to the field of energy storage, delivering insights and a clear methodology that pave the way for the development of next-generation LMBs poised for commercial viability.

Temperature and photosensitive PVDF-g-PNIPAAm/GPE-PDA@ZnO composite membranes with efficient dyes separation capability and light-cleaning function

In this paper, PVDF-g-PNIPAAm/GEP-PDA@ZnO composite membranes that can undergo light-induced structural response and photodegradation to achieve self-cleaning have been designed and applied to the separation and purification of dye wastewater. The membranes were prepared by blending graphene (GPE)-polydopamine (PDA)-coated zinc oxide (ZnO) core–shell particles into the PVDF-g-PNIPAAm matrix with a non-solvent induced phase separation technique. The GPE and ZnO are tightly bonded by highly adhesive PDA to form a “strawberry-like” core–shell structure. GPE absorbs light energy and converts it into heat, resulting in changes in PNIPAAm chain segments to expand the pore size for self-cleaning. While the membrane is warming up, GPE further promotes the activation of active groups on the surface of PDA@ZnO at high temperature, resulting in unique and excellent photothermal catalytic activity. As a result, the membrane achieves both self-cleaning and pollutant degradation, which results in an FRR of 99.6% after light cleaning. Moreover, the GPE-PDA@ZnO nanoparticle-modified PVDF-g-PNIPAAm membranes exhibit excellent cycling stability with a degradation flux recovery rate of more than 97% even after multiple UV cleaning. Thus, PVDF-g-PNIPAAm/GPE-PDA@ZnO composite membranes extend the versatility of PVDF-based membranes and show extraordinary potential for application in wastewater treatment.

Investigating the impact of stormwater fouling on polysulfone ultrafiltration membranes modified with deep eutectic solvents

In this study, we evaluate the performance of modified polysulfone (PSF) ultrafiltration (UF) membranes, which incorporate deep eutectic solvents (DES), in treating stormwater laden with natural organic matter e.g. chemical oxygen demand (COD) and total suspended solids (TSS). We also aim to understand how these organic substances, e.g. COD, TSS, from the water source contribute to the fouling of the synthesized membranes. PSF membranes were synthesized using a non-solvent induced phase separation technique and integrated with varying concentrations of ChCl:FR (Choline Chloride: D-(−)-Fructose) 1:1 DES. The surface and porous structures of the membranes were characterized through Fourier-transform infrared spectroscopy (FTIR), atomic force microscopy (AFM), contact angle measurements, scanning electron microscopy (SEM), and mechanical testing. The UF performance of these membranes was assessed and compared with different commercially available UF flat sheet membranes in terms of pure water permeability and antifouling behavior against collected stormwater from a sedimentation pond. Furthermore, the study evaluated the quality of the permeate based on parameters such as COD, turbidity, TSS, pH, and conductivity and compared the permeate quality of a pilot-scale ceramic UF membrane unit. The findings indicate that the inclusion of DES in the polysulfone membrane structure enhances the membranes' antifouling properties and permeability. This research offers valuable insights into the role of DES in the formation of polysulfone UF membranes and their potential for practical use e.g. sedimented stormwater.

Novel TFC membrane with PMIA thin-film as active layer fabricated by the T-FLO technique for dye desalination

Poly (m-phenylene isophthalamide) (PMIA) generally is employed in a thin-film composite (TFC) membrane as the porous substrate via the non-solvent induced phase separation technique. Relatively little research has been done on PMIA thin-films. Here, dense PMIA thin-film was deposited via the cast-coating coupled solvent evaporation and was modified systematically. The ion permeance of PMIA thin-film has been explored for the first time. Furthermore, the novel TFC membrane with PMIA active layer (TFC-P10) was successfully fabricated for the first time via the thin-film liftoff (T-FLO) technique. The mechanism of applying PMIA thin-film as the active layer was illustrated by SEM, FTIR and XPS as the secondary amine group of PMIA reacted with the epoxide group of the epoxy layer. TFC-P10 performed remarkable dye desalination. Specifically, Congo red (CR) rejection of 99.55 % (50 mg L−1), NaCl rejection of 7.34 % (1000 mg L−1), high-temperature resistance under 90 °C, good antifouling with FRR > 90 %, and 96 h long-term stability. Besides, the dye/salt selectivity coefficient α of TFC-P10 was 207.9. This work endows a guideline for in-situ dye effluent treatment and the novel TFC membrane fabrication.

Closed-loop recyclable membranes enabled by covalent adaptable networks for water purification

In the state-of-the-art membrane industry, membranes have linear life cycles and are commonly disposed of by landfill or incineration, sacrificing their sustainability. To date, little or no thought is given in the design phase to the end-of-life management of membranes. For the first time, we have innovated high-performance sustainable membranes, which can be closed-loop recycled after long-term usage for water purification. By synergizing membrane technology and dynamic covalent chemistry, covalent adaptable networks (CANs) with thermally reversible Diels-Alder (DA) adducts were synthesized and employed to fabricate integrally skinned asymmetric membranes via the nonsolvent-induced phase separation technique. Due to the stable and reversible features of CAN, the closed-loop recyclable membranes exhibit excellent mechanical properties and thermal and chemical stabilities as well as separation performance, which are comparable to or even higher than the state-of-the-art nonrecyclable membranes. Moreover, the used membranes can be closed-loop recycled with consistent properties and separation performance by depolymerization to remove contaminants, followed by refabrication into new membranes through the dissociation and reformation of DA adducts. This study may fill in the gaps in closed-loop recycling of membranes and inspire the advancement of sustainable membranes for a green membrane industry.

Polyetherimide membrane with tunable porous morphology for safe lithium metal-based batteries

The separator is critical in ensuring the safety and improving the electrochemical performance of lithium metal batteries (LMBs). However, the weak thermal stability, common mechanical strength and the poor wettability towards electrolyte of the commercial polyolefin separator severely hamper its application in high-performance LMBs. Herein, a simple phase inversion technique could be used to design and scalably fabricate porous polyetherimide (PEI) membranes, which was used as LMB separators for the first time. The final morphology of PEI membranes can be finely tuned from finger-like voids to sponge-like pores by selecting an appropriate non-solvent. Combining experiments and density functional theory (DFT) simulations, it reveals that the optimal PEI membrane shows a sponge-like pore structure, which can induce the genuine deposition of the Li metal due to the homogeneously distributed pores in high density on the membrane and its good affinity towards the electrolytes. Consequently, the PEI based LMB show better performance than the commercial polypropylene (PP) based LMB. More importantly, the optimal PEI membrane shows a better mechanical strength and thermal stability than the PP membrane at the same thickness, which can ensure a higher safety for real applications. Since the non-solvent induced phase separation technique used to prepare PEI membrane is scalable in low cost, this work provides insightful route to overcome one of the main challenges, i.e. lack of high performance and high safety separator, for practical LMB application.

Flexural strength and elastic modulus of gradient structured YSZ membranes with multi-scale pores

3 mol% yttria-stabilized zirconia membranes prepared by a non-solvent induced phase separation technique can balance the performance between robust mechanics and high porosity, because of having a multi-scale porous microstructure. However, the fracture mechanism of membranes with multi-scale pores is incomplete due to the nonlinear structure, which limits its performance optimization. In this study, effects of the various pores on stress distributions and related mechanical properties were experimentally studied and simulated. The gradient diameter of the macro-channels led to a loading direction dependent flexural strength. Meanwhile, no strength degradation was found when penetration depths of these macro-channels increased from 70% to 80% of the membrane thickness, because the channel tails hardly caused interference to the maximum bending stress. The flexural strength was determined by the cellular structure surrounding the macro-channels, and its bimodal porosity distribution reduced the elastic modulus, which might favor an improvement of strain tolerance.

Cyclic olefin polymer membrane as an emerging material for CO2 capture in gas-liquid membrane contactor

Porous flat sheet membranes were prepared with a commercial grade of cyclic olefin polymer (COP) for CO2 capture using membrane contactor (MC). The membranes were prepared via non-solvent induced phase separation technique using different types of additives, namely, polyvinylpyrrolidone (PVP), polyethylene glycol (PEG400) and sorbitan monooleate (Span 80), and coagulants (acetone and 70/30 wt% acetone/water mixture) were investigated. The prepared membranes were characterized in terms of the thickness (70–85 µm), porosity (50–80%), mean pore size (158–265 nm), bubble pore size (~ 0.6–12 µm), liquid entry pressure (1.67–4.55 bar), water contact angle (~ 94° - 111°), monoethanolamine (MEA) contact angle (~ 67° - 73°) and mechanical properties (tensile strength: 4.53 – 5.15 MPa, elongation at break: 4 – 8% and Young´s modulus: 190 – 232 MPa). The thermodynamic study of COP membranes proved that a fast phase inversion of the proposed system resulted in a more porous structure. The addition of PEG400 and Span 80 caused delayed demixing and influenced the morphological structure and MC performance. The structural and topographical characteristics of the membranes were also studied. The CO2 absorption test performed at 27 °C showed that the maximum CO2 absorption flux was around 16 × 10−5 mol/m2.s using 1 M MEA aqueous solution as absorbent with fixed liquid and gas flow rates at 150 L/h and 8.4 L/h, respectively. It was found that the considered additives enhanced the MC performance and affected the CO2 absorption flux.

A Single Step Preparation of Photothermally Active Polyvinylidene Fluoride Membranes Using Triethyl Phosphate as a Green Solvent for Distillation Applications.

Membrane distillation is a growing technology that can address the growing problem of water shortage. The implementation of renewable energy and a reduction in the environmental impact of membrane production could improve the sustainability of this process. With this perspective, porous hydrophobic polyvinylidene fluoride (PVDF) membranes were prepared using triethyl phosphate (TEP) as a green solvent, using the non-solvent induced phase separation technique. Different amounts of carbon black were added to dope solutions to improve the photothermal properties of the membranes and to enable direct heating by solar energy. By optimizing the preparation conditions, membranes with porosity values as high as 87% were manufactured. Vacuum membrane distillation tests carried out using a concentrated NaCl solution at 50 °C showed distillate fluxes of up to 36 L/m2 h and a complete salt rejection. Some preliminary studies on the photothermal performance were also conducted and highlighted the possibility of using such membranes in a direct solar membrane distillation configuration.

A combined physical blending and surface grafting strategy for hydrophilic modification of polyethersulfone membrane toward oil/water separation

The block copolymer, Pluronic F127-block-poly(acrylic acid) (PAA-b-F127-b-PAA) was firstly synthesized via RAFT polymerization. Then, the copolymer was utilized as the blending modifier for fabricate polyethersulfone (PES)/PAA-b-F127-b-PAA composite membrane by nonsolvent induced phase separation technique. The hydrophilic PAA segments were concentrated onto the membrane surface due to the surface segregation phenomenon in the membrane formation process, which improved the hydrophilicity of the membrane surface and provided active sites for further surface grafting modification. Subsequently, the amine-terminated poly(sulfobetaine methacrylate) (NH2-PSBMA) was prepared through ARGET ATRP and used as surface modifier to fabricate PES/PAA-b-F127-b-PAA/PSBMA composite membrane by amination reaction. The composite membrane exhibited the highest pure water flux and oil flux around 358.25 and 217.53 L m−2 h−1, which equal to 5.6 times and 19.6 times of unmodified PES membrane respectively. The flux recovery rate increased from 45.74% to 94.64%, suggesting the fouling-resistance of the composite membranes was greatly improved. The hydrophobic PPO segments of PAA-b-F127-b-PAA used as anchor segments and amalgamated with PES molecular by hydrophobic interaction and physical intertwisting, resulting in the PAA-b-F127-b-PAA was firmly embedded in the membrane. Moreover, the PSBMA segments were grafted onto the membrane surface by forming strong chemical bonds, exhibiting excellent stability. It shows that this membrane material prepared by physical blending and surface grafting has a good application prospect in oil/water separation.

Inhibition of algae-induced membrane fouling by in-situ formed hydrophilic micropillars on ultrafiltration membrane surface

Inhibiting algae-induced membrane fouling has become an extremely challenging work in algae-laden water treatment. In this study, we developed a novel Polyvinylidene Fluoride (PVDF) ultrafiltration membrane to inhibit algal fouling by in-situ formed four-arms star poly(styrene)-block-poly(ethylene oxide)monomethacrylate (FAS-PS-b-PEGMA) micropillars on membrane surface via nonsolvent induced phase separation technique. Morphology characterization revealed that the protruding micropillars were formed on membrane surface after the addition of FAS-PS-b-PEGMA. The formation of micropillars affected phase separation behaviors, resulting in more porous membrane structure. Surface analyses suggested that the hydrophilic PEGMA chains of the amphiphilic copolymers were enriched onto the surfaces of micropillars, and endowed the modified membranes with higher hydrophilicity and lower electronegativity. The excellent permeability and antifouling properties of the modified membranes were demonstrated by gravity-driven filtration of Microcystis aeruginosa solution. Especially for M5 membrane, the stable permeation flux was more than 5 times than that of the control membrane. The flux decline ratio was only 51.3%, which was much lower than the control membrane (80.1%). Furthermore, the analyses of fouling layer further confirmed that the micropillars could inhibit the accumulation of algae cells on the membrane surface. This study provides a one-step strategy on the modulation of ultrafiltration membrane preparation, modification and performance for algae-laden water treatment.

Fabrication of mesoporous TiO2/PVDF photocatalytic membranes for efficient photocatalytic degradation of synthetic dyes

Water recovery and reuse are the two best alternatives to assuage the growing water scarcity. Mixed matrix membranes (MMMs) incorporated with heterogeneous photocatalysts have been proven to be efficient in the degradation of toxic organic compounds, particularly dyes. In this study, a mesoporous photocatalyst, titanium dioxide, was prepared using two different routes: (1) Solution combustion synthesis using different organic fuels such as (TiO2-U), (TiO2-G), (TiO2-A), (TiO2-H), and (TiO2-HM); (2) Modified hydrothermal method using an abundantly available polysaccharide starch (TiO2-S). These photocatalysts were exhaustively characterized to study their physicochemical and structural properties using XRD, UV-DRS, FT-Raman, BET, PL Spectra, XPS, HR-SEM, HR-TEM and EDX. The mesoporous TiO2 nanoparticles incorporated mixed matrix PVDF membranes were synthesized by the facile non-solvent induced phase separation technique. The photocatalytic activity of the synthesized catalysts and the MMMs were evaluated using two different dyes such as Congo Red (CR) and Reactive Yellow 145 (RY 145). As far as the catalyst embedded membranes are concerned, they also show a similar trend but slightly reduced photocatalytic activity. Among the MMMs, TiO2–S/PVDF showed higher photocatalytic activity. The percentage decolourization/mineralization of CR and RY 145 over were determined to be 84%/71% and 100%/87% respectively. Kinetic studies revealed that among the synthesized catalysts, TiO2-S/PVDF showed the highest kapp and the lowest t1/2 values – CR – 0.0061 min−1 and 113 min; RY 145 – 0.0134 min−1 and 51.71 min. The PVDF MMMs were also found to be thermally stable with excellent recyclability and long-term activity.

Fabrication of porous polymer membrane from polysulfone grafted with acid ionic liquid and the catalytic property for inulin hydrolysis

Catalytically active membranes are the core components of the membrane reactors. Polysulfone (PSF) grafted with ionic liquids (ILs), PSF-DG-ILs, was prepared via introducing chloromethyl group into benzene ring of PSF, then grafting ILs, imidazolyl acid ILs ([(CH2)3SO3HVIm]HSO4), by chemical bonding. Then PSF-DG-ILs membranes were prepared by non-solvent induced phase separation technique for hydrolysis of inulin. The effects of coagulation bath, grafting degree, and various dope blending on structure, physico-chemical characters, and catalytic performance of membranes were evaluated. And results revealed that catalytic performance could be efficiently enhanced by choosing ethanol as coagulation compared with ethyl acetate, which was mainly attributed to surface segregation. Membrane mechanical strength decreased with the enhancing ILs grafting degree, while the catalytic performance increased. However, PSF-DG-ILs with high degree of ILs grafting lost its membrane-forming property. The mechanical and catalytic properties of the membrane were synergistically enhanced by blending PSF-DG-ILs polymers with high and low ILs grafting degree, then the resulting membranes broke the trade-off effect between mechanical strength and catalytic ability. Specifically, membrane fabricated by mixing the polymers with ILs grafting degree of 0.31 and 0.59 integrates optimized mechanical property and catalysis performance. The strength and strain of this blending membrane are 3.17 MPa and 14.10%. The average pore size and porosity are 215.5 nm and 46.2%. The yield of inulin hydrolysis can reach 88.22% with 20 wt% concentration of inulin at 75 °C using a flux of 23.4 L/(m2·h). Therefore, the PSF-DG-ILs membrane displayed promising potential for the application in biomass conversion.

Single-walled carbon nanotubes grafted with dextran as additive to improve separation performance of polymer membranes

Permeability and selectivity are two important parameters for evaluating membrane separation performance. In this work, the functionalized single-walled carbon nanotubes (DexDTM-g-SCNT) is fabricated by non-covalent interaction using dextran-based macro-chain transfer agent, and used as an additive to blend with polyethersulfone to prepare ultrafiltration membranes via a non-solvent induced phase separation technique. DexDTM-g-SCNT modified membrane has excellent anti-fouling properties, good permeability, and excellent separation performance. Typically, the hydrophilicity of the modified membrane is significantly improved, when the content of additive is 3 wt%. The modified membrane shows high pure water flux of up to 223.3 L m−2h−1, and high rejection ratio for bovine serum albumin, and congo red of 98.5 and 98.8%, respectively. The strategy has great potential for practical applications in water purification and other separation fields.

Porous composites based on cellulose acetate and alfa-hematite with optical and antimicrobial properties

Polymer nanoparticles (NPs) composites are rapidly gaining attention due to their high potential for application in several technological fields. On one hand, polymers contribute to balance the attractive magnetic and van der Waals forces that act on NPs and thus reduce their agglomeration. On the other hand, NPs can bring into the composites their inherent properties as nanosized objects. In this work, hematite NPs were blended with cellulose acetate (CA) polymer and thin nanocomposite films were produced by the non-solvent induced phase separation technique. A full physicochemical characterization of these composite materials confirmed its superior character in terms of structure, thermal stability, electronic/optical and antibacterial properties when compared to the polymer on its own and opens the door to its further validation in adsorptive and photocatalytic applications.

Development of underwater superoleophobic polyamide-imide (PAI) microfiltration membranes for oil/water emulsion separation

Fouling of microfiltration membranes by the adhesion of oil onto the membrane surface and/or penetration into its pores is a major challenge for effective treatment of oily wastewater. In this study, polyamide-imide (PAI) was used to make hydrophilic and underwater superoleophobic microfiltration membranes via non-solvent induced phase separation technique. Membranes were modified with hydrophilic additives, including polyethylene glycol (PEG, 0.4 and 6 kDa) and polyvinylpyrrolidone (PVP, 10 and 360 kDa) to improve their hydrophilicity further. Oil rejection experiments were conducted for three consecutive cycles at a very low transmembrane pressure (0.5 bar) to evaluate the reusability of the synthesized membranes. The use of additives resulted in a wide range of membrane morphology, porosity, pore size, and surface chemical property, which affected the permeation rate and flux recovery. However, all synthesized membranes showed > 98% oil rejection with permeation rate as high as 210 Lm−2 h−1. Membranes modified with PEG 0.4 kDa, PEG 6 kDa, and PVP 10 kDa had underwater oil contact angle (OCA) above 150° and showed almost 98% flux recovery ratio. In the case of PVP 360 kDa, a lower flux recovery was observed due to a reduced oleophobic property (OCA = 124°). This study proposes a facile approach for the production of high-performance oil-rejecting membranes without employing complex surface modification methods.

Textile waste, dyes/inorganic salts separation of cerium oxide-loaded loose nanofiltration polyethersulfone membranes

Poly(ether sulfone) (PES) loose nanofiltration nanocomposite membranes were prepared by incorporating cerium oxide (CeO2) nanoparticles (NPs) via a non-solvent induced phase separation technique. The influence of NPs on thermodynamic and kinetic aspects of phase separation was studied by phase diagram construction and viscosity measurement. FESEM images exhibited asymmetric structure of the membranes with a dense top layer, while contact angle measurements confirmed improved membrane hydrophilicity. The performances of the membranes were tested by aqueous dye solutions viz., Direct Red 23, Congo Red, and Direct Red 243 as well as real textile wastewater. Low rejection rates were observed for different aqueous salt solutions following the sequence: MgSO4 (4.1%) > Na2SO4 (3.3%) > MgCl2 (1.8%) > NaCl (1.2%). The nanocomposites exhibit remarkable antifouling properties compared to the pristine membrane.

Superior fouling resistant PVDF membrane with enhanced filtration performance fabricated by combined blending and the self-polymerization approach of dopamine

This work presents a new and simple modification approach to fabricate a Polyvinylidene Fluoride membrane with superior permeation, separation, and antifouling performance. Dopamine was introduced by blending into the membrane casting solution and the membrane was prepared using a classic non-solvent induced phase separation technique. The prepared flat-sheet membrane was then dipped into a Tris-HCl buffer solution with a pH of 8.5 to trigger the polymerization of dopamine into polydopamine. The effects of the modification on the membrane characteristics were analyzed in terms of a change in the chemical components, hydrophilicity, surface porosity, and mechanical strength. In addition, the permeation, separation, and fouling resistant performance were studied by means of a filtration experiment using deionized water and humic acid solution as feeds. The results revealed that the addition of dopamine successfully increased the porosity by 300%, hydrophilicity by 180%, and water flux performance by 600% compared to the original membrane. Polymerization of dopamine into the polydopamine layer recovered the loss of rejection due to pore enlargement by dopamine blending from 91 to 93%. In addition, the blended and polymerized membrane successfully recovered up to 92% of pure water flux after backwash, which indicates the superior antifouling performance. It can be concluded that this new technique can be a potential approach to produce membranes for the water treatment process with overall excellent performance.

Amine wetting evaluation on hydrophobic silane modified polyvinylidene fluoride/silicoaluminophosphate zeolite membrane for membrane gas absorption

Membrane wetting in membrane gas absorption is undesirable as it reduces the gas transfer in wet pores. This work aims to understand the improvement of membrane hydrophobicity using fluoroalkyl silane and its effects on membrane properties, separation performance and membrane wetting by amine. Polyvinylidene fluoride/silicoaluminophosphate zeolite membranes were prepared using non-solvent induced phase separation technique and then immersed into a mixture of (3,3,3-trifluoropropyl) trimethoxysilane and ethanol solution (volume ratio of 1: 100) for 20 min. The post-modification resulted in a slight improvement of water contact angle and liquid entry pressure. Hence, the highest CO2 absorption flux of 4.48 ± 0.36 × 10−4 mol.m−2. s−1 was achieved using silanated membrane, about 25 % of improvement in comparison to the neat membrane. The absorption flux of humid gas was slightly reduced (-16 %) due to pore wetting. Fluoroalkyl silane could be used to prevent water wetting, resulting improvement of CO2 absorption. The membranes were immersed in diethanolamine solution (2 M) for 50 h before characterization using goniometer, Fourier transform infrared spectroscopy and scanning electron microscope. The incorporation of zeolite reduced membrane wetting because membrane swelling could be prevented. The unfavorable interaction between fluoroalkyl and amine groups induced severe membrane wetting by amine.

Development of 3D-printed polymer-zeolite composite monoliths for gas separation

Organic-inorganic materials have emerged as promising candidates for use in various gas separation processes due to the beneficial synergistic effect of both constituents. Herein, we report a novel and facile approach for fabrication of composite monoliths consisting of Torlon polymer and 13X and 5A zeolites via 3D printing technique for the removal of CO2 from flue gas. The physical and structural properties of 3D-printed composite monoliths were systematically evaluated and compared with their pristine powders. The formation of monoliths was facilitated through nonsolvent-induced phase separation technique. By the incorporation of ∼31 wt% zeolite particles into the polymer matrix, the obtained monoliths displayed CO2 capture capacities proportional to the zeolite loading. Most importantly, both 3D-printed Torlon-zeolite monoliths exhibited high compressive strengths of approximately 210 MPa, which was significantly higher than that of 3D-printed zeolite monoliths developed in our previous work. These results demonstrate the superiority of polymer-zeolite composite monoliths, formulated by 3D printing technique as robust structures with outstanding mechanical integrity and comparable adsorption capacity for various adsorption-based gas separation processes. The printing strategy reported herein can be easily extended to other organic-inorganic composite materials with different polymers and inorganic particles.