Hierarchically microporous membranes for highly energy-efficient gas separations

Luo, Shuangjiang; Han, Tianliang; Wang, Can; Sun, Ying; ZHANG, Hongjun; Guo, Ruilan; Zhang, Suojiang

doi:10.1039/d2im00049k

Cited by 19 publications

(6 citation statements)

References 103 publications

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“…After thermal oxidative treatment, a bimodal micropore size distribution containing ultramicropores and submicropores is observed for TOC-PI-Trip-TB-450-30min. The hierarchical microporosity can be ascribed to the synergistic effect of oxidative cross-linking and degradation, which potentially leads to the enhancement of permeability due to the ultramicropores and selectivity due to submicropores . Similar results were also observed for the PI-Trip and PI-TB series membranes.…”

Section: Resultssupporting

confidence: 71%

“…In contrast, synthetic microporous polymer membranes with relatively low cost, good processability, and customizable gas transport properties are fabricated by dense polymer chain packing, and gas transport primarily follows the solution-diffusion mechanism . Conventional synthetic microporous polymer membranes are usually susceptible to a permeability–selectivity tradeoff, also identified as the upper bounds, − presumably due to the broad micropore size distribution induced by amorphous and random segmental packing. , …”

Section: Introductionmentioning

confidence: 99%

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Direct Thermal Oxidative Cross-Linking in Air toward Hierarchically Microporous Polymer Membranes for Advanced Molecular Sieving

Xie,

Zheng,

Chen

et al. 2023

Ind. Eng. Chem. Res.

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In situ thermal oxidative cross-linking provides an efficient strategy for manipulating microporosity in polymeric gas separation membranes. Herein, we report a rational macromolecular design combining microporous polymers with thermal oxidative cross-linking to fabricate highly permselective membranes for advanced energy-efficient gas separations. We demonstrate that direct thermal treatment in air induces both oxidative chain scission and thermal oxidative crosslinking, leading to a hierarchically microporous architecture enabling simultaneous enhancement of permeability and selectivity. Consequently, the TOC-PI-Trip-TB-450-30min membrane containing both the triptycene and Troger's base moieties upon thermal treatment at 450 °C for 30 min in air exhibits H 2 and CO 2 permeabilities of 1138 and 640 Barrer, respectively, and H 2 /N 2 , H 2 /CH 4 , and CO 2 /CH 4 selectivities of 76, 121, and 68, respectively, exceeding or approaching the state-of-the-art upper bounds. This study also confirmed that the microcavity characteristics and gas permeation performance of the thermal-oxidatively cross-linked membranes are highly tunable by regulating the polymer structure, oxidative temperature, and reaction time.

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Section: Resultssupporting

confidence: 71%

Section: Introductionmentioning

confidence: 99%

Direct Thermal Oxidative Cross-Linking in Air toward Hierarchically Microporous Polymer Membranes for Advanced Molecular Sieving

Xie,

Zheng,

Chen

et al. 2023

Ind. Eng. Chem. Res.

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“…The narrow necking (the first pore size distribution of 0.4−0.7 nm) had a molecule sieving effect, and the second one of 0.7− 1.0 nm was beneficial for rapid gas transport, rendering significantly improved gas separation property for various gas pairs compared to conventional polymer membranes with generally broad pore size distributions. 54 Among the three SACPs, SACP-PhMe shows the highest peak intensity, with SACP-Me being the lowest, consistent with WAXD and FFV results.…”

Section: Synthesis and Characterization Of Sacpssupporting

confidence: 82%

Finely Tuning the Microporosity and Gas Permeation Properties in Superacid-Catalyzed Polymers of Intrinsic Microporosity

Gong,

Cai,

Wang

et al. 2023

Ind. Eng. Chem. Res.

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Superacid-catalyzed polymers of intrinsic microporosity have attracted increasing attention in membrane-mediated gas separation due to their good processability, facile polymerization procedure, and tunable microporosity and gas separation performance. In this study, we synthesized a series of new superacid-catalyzed polymers with fully ladder backbones and welldefined micropores using a one-pot condensation polymerization. The incorporation of a contorted spirobisindane building block facilitated the formation of highly microporous structures in the resulting polymers, enhancing their intrinsic microporosity and gas separation properties. Among the three SACPs, SACP-PhMe exhibited the largest d-spacing value, specific surface area, and pore volume due to its bulkiest side group. The gas separation performance of the SACP membranes surpassed several benchmark polymer membranes, with the SACP-PhMe membrane demonstrating excellent performance in separating CO 2 /CH 4 , H 2 /CH 4 , O 2 /N 2 , and H 2 /N 2 . The SACP-Me membrane exhibited the lowest porosity, making it less susceptible to CO 2 absorption and showing superior plasticization resistance. The results highlight the promising gas separation properties of the SACPs and their potential for various gas separation applications, offering new opportunities for advanced polymer membrane design.

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“…Gas separation membranes have found widespread applications in fields including air separation, , hydrogen or organic gas recovery, − natural gas purification, , carbon dioxide separation, and so on. Compared with traditional gas separation methods, such as low-temperature distillation and pressure swing adsorption, a gas separation membrane has the advantages of a small footprint, high separation efficiency, low cost, and simple operation, leading to its rapid development. , …”

Section: Introductionmentioning

confidence: 99%

Effects of ortho Functional Groups on the Thermo-Oxidative Cross-Linking Process and Gas Separation Properties of Phenolphthalein-Based Polyimides

Cheng,

Chen,

Zhao

et al. 2024

Macromolecules

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Polyimides containing lactone rings can be thermo-oxidatively cross-linked to enhance gas separation properties and antiplasticization performance. Degradation of the lactone ring at high temperature is crucial to generate free radicals for cross-linking. Determining the thermal stability of the lactone ring is required to set an appropriate heating protocol for thermal cross-linking. To elucidate the relation between polymer structure and the thermal stability of the lactone ring, we prepared two phenolphthalein-based diamines, AMPB and AHPB. These diamines were reacted with 6FDA and DAM to form three copolyimides using azeotropic distillation and chemical imidization. This was used to design copolyimides containing lactone rings and different ortho functional groups including −OH, −OCH3, and −OOCCH3. By characterizing the physiochemical properties of these copolyimides and performing molecular simulations, we discovered that the stronger the electron-donating ability of the ortho groups, the higher the temperature at which the lactone ring began to degrade. Copolyimides with a relatively weak electron-donating groups, −OH and −OOCCH3, could be oxidatively cross-linked at 275 °C, while the copolyimide with a −OCH3 group could be only cross-linked at a temperature above 325 °C. Moreover, the gas separation property, mechanical properties, and plasticization resistance were improved after cross-linking.

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Hierarchically microporous membranes for highly energy-efficient gas separations

Abstract: The implementation of synthetic polymer membranes in gas separations ranging from natural gas sweetening, hydrogen recovery, helium extraction, carbon capture, and oxygen/nitrogen enrichment etc., has stimulated vigorous development of high-performance...

Cited by 19 publications

References 103 publications

Direct Thermal Oxidative Cross-Linking in Air toward Hierarchically Microporous Polymer Membranes for Advanced Molecular Sieving

Direct Thermal Oxidative Cross-Linking in Air toward Hierarchically Microporous Polymer Membranes for Advanced Molecular Sieving

Finely Tuning the Microporosity and Gas Permeation Properties in Superacid-Catalyzed Polymers of Intrinsic Microporosity

Effects of ortho Functional Groups on the Thermo-Oxidative Cross-Linking Process and Gas Separation Properties of Phenolphthalein-Based Polyimides

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