Yuyang Xiao, Xingfeng Lei*, Zixiang Zhang, Siyu Chen, Guo Xiong, Xiaohua Ma and Qiuyu Zhang*,
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引用次数: 0
Abstract
Cross-linked polymers for gas separation have significant advantages in increasing gas selectivity and separation stability. However, the cross-linking strategies unavoidably form permanent interchain covalent bonds and alter the polymer packing state, which largely decrease polymer solubility, static toughness, and reprocessability. Herein, a secondary-amine-containing diamine (HCBDA) derived from carbazole is synthesized and polymerized with 6FDA to furnish a gas-permeable polyimide (HCB-PI) with a pseudo-cross-linked hydrogen-bonding network and a strengthened charge-transfer complex (CTC) effect. Compared with the hydrogen-bonding free sample (CB-PI), HCB-PI displays a more homogeneous micropore distribution and denser chain packing, as is proven by positron annihilation lifetime spectroscopy, which results in enhanced selectivity for O2/N2 and CO2/CH4 gas pairs and antiplasticization property. Owing to the stronger interaction between the HCB-PI skeleton and molecular oxygen and thus the competitive adsorption mechanism, HCB-PI exhibits more enhanced O2/N2 selectivity in mixed-gas measurements (7.54) than in pure-gas measurements (6.58), with the overall separation property approaching the 2008 Robeson upper bound. Additionally, HCB-PI is heat-resistant and mechanically robust, exhibiting static toughness up to 108 MJ·m–3. Our designing concept for HCB-PI has been demonstrated to be efficacious for oxygen enrichment from air.
期刊介绍：
Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.
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