Precursor-chemistry engineering toward ultrapermeable carbon molecular sieve membrane for CO_(2)capture  

作　　者：Mengjie Hou Lin Li Ruisong Xu Yunhua Lu Jing Song Zhongyi Jiang Tonghua Wang Xigao Jian 

机构地区：[1]State Key Laboratory of Fine Chemicals,Dalian Key Laboratory of Membrane Materials and Membrane Processes,Laboratory of Carbon Membranes and Porous Materials,School of Chemical Engineering,Dalian University of Technology,Dalian 116024,Liaoning,China [2]School of Chemical Engineering,University of Science and Technology Liaoning,Anshan 114051,Liaoning,China [3]Key Laboratory for Green Chemical Technology of Ministry of Education,School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072,China

出　　处：《Journal of Energy Chemistry》2025年第3期421-430,共10页能源化学(英文版)

基　　金：financial support from the National Key R&D Program of China(2021YFB3801200);the National Natural Science Foundation of China(22278051,22178044,22308043);CNPC Innovation Found(2022DQ02-0608)。

摘　　要：Carbon capture is an important strategy and is implemented to achieve the goals of CO_(2)reduction and carbon neutrality.As a high energy-efficient technology,membrane-based separation plays a crucial role in CO_(2)capture.It is urgently needed for membrane-based CO_(2)capture to develop the high-performance membrane materials with high permeability,selectivity,and stability.Herein,ultrapermeable carbon molecular sieve(CMS)membranes are fabricated by py roly zing a finely-engineered benzoxazole-containing copolyimide precursor for efficient CO_(2)capture.The microstructure of CMS membrane has been optimized by initially engineering the precursor-chemistry and subsequently tuning the pyrolysis process.Deep insights into the structure-property relationship of CMSs are provided in detail by a combination of experimental characterization and molecular simulations.We demonstrate that the intrinsically high free volume environment of the precursor,coupled with the steric hindrance of thermostable contorted fragments,promotes the formation of loosely packed and ultramicroporous carbon structures within the resultant CMS membrane,thereby enabling efficient CO_(2)discrimination via size sieving and affinity.The membrane achieves an ultrahigh CO_(2)permeability,good selectivity,and excellent stability.After one month of long-term operation,the CO_(2)permeability in the mixed gas is maintained at 11,800 Barrer,with a CO_(2)/N_(2)selectivity exceeding 60.This study provides insights into the relationship between precursor-chemistry and CMS performance,and our ultrapermeable CMS membrane,which is scalable using thin film manufacturing,holds great potential for industrial CO_(2)capture.

关 键 词：CO_(2)capture Gas separation Carbon molecular sieve membrane precursor-chemistry 

分 类 号：TQ028.8[化学工程]