Ultramicroporous carbon molecular sieve membrane derived from hypercrosslinked ionic polymers for efficient H_(2)/CO_(2)separation  

超交联离子聚合物前驱体制备的超微孔碳分子筛膜,用于高效H_(2)/CO_(2)分离

作　　者：Jiaao Yao Jingjie Bi Hongyu Zuo Yuren Peng Liwei Wu Zixuan Zhang Xuelong He Baokang Lyu Nanwen Li Yaozu Liao Weiyi Zhang 姚家傲;毕静婕;左宏瑜;彭玉仁;吴礼威;张子轩;何学龙;吕宝康;李南文;廖耀祖;张卫懿

机构地区：[1]State Key Laboratory for Modification of Chemical Fibers and Polymer Materials,College of Materials Science and Engineering,Donghua University,Shanghai 201620,China [2]State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China

出　　处：《Science China Materials》2025年第3期888-896,共9页中国科学(材料科学)(英文版)

基　　金：supported by the Fundamental Research Funds for the Central Universities(2232022A-03 and 2232024Y-01);the National Natural Science Foundation of China(22102021,22375037,52073046,52373172,and 52103106);the National Key Research and Development Program of China(2022YFB3807100,2022YFB3807102,and 2022YFB3807103);the Program of Shanghai Academic Research Leader(21XD1420200);the Natural Science Foundation of Shanghai(23ZR1401100 and 21ZR1402700).

摘　　要：Carbon molecular sieve membranes(CMSMs)are a class of porous membranes inherited with excellent thermal stability,high tolerance and superior mechanical strength.Owing to their nanoporous structures,CMSMs usually hold significant potential for gas separation applications.Specifically,hyper-crosslinked ionic polymer(HIP)membranes possess a highly crosslinked nitrogen-rich framework,high thermal stability together with exceptional mechanical strength,making them excellent precursors for the CMSMs fabrication.Upon pyrolysis of HIP membranes,the resulting CMSMs featured with nitrogen functional sites exhibit strong interactions with CO_(2),which significantly reduces the CO_(2)permeability while other gas molecules continue to flow through the nanoporous membrane.The resultant CMSMs exhibited excellent H_(2)/CO_(2)selectivity with values of 10.75 and 7.09,together with ultra-high H_(2)permeability of 3052 and 9181 barrer,respectively,surpassing the Robeson upper bound.The preparation route towards CMSMs with high nitrogen content from HIP can significantly enrich the rational design and synthesis strategies of high-performance gas separation CMSM materials.碳分子筛膜(CMSMs)是一类具有优异热稳定性、高耐受性和优异机械强度的多孔膜.由于其具有纳米级多孔结构,CMSMs在气体分离应用中具有显著潜力.具体而言,超交联离子聚合物(HIP)膜拥有高度交联的富氮框架,高热稳定性以及卓越的机械强度,使其成为制备CMSMs的优良前驱体.通过对HIP膜进行热解,所得到的CMSMs具有氮功能位点,这种功能位点展现出与CO_(2)的强相互作用,从而显著降低CO_(2)的渗透率,而其他气体分子则继续跨膜运输.所得CMSMs表现出优异的H_(2)/CO_(2)选择性,分别达到10.75和7.09,以及超高的渗透系数,分别为3052和9181 barrer,超过了Robeson上限.利用HIP制备高氮含量的CMSMs,可以显著丰富高性能气体分离CMSM材料的合理设计和合成策略.

关 键 词：carbon molecular sieving membrane hyper-crosslinked ionic polymer membrane nitrogen-rich framework gas separation 

分 类 号：O64[理学—物理化学]