沸石膜在分离烟气中CO_(2)的挑战:沸石与载体间结合力研究进展  

Challenge of zeolite membranes in separating CO_(2)from flue gas:Advances in research on binding forces between zeolite and carriers

作　　者：梁鼎成 杨录录 解强[1] 谢珠璨 邓青文 郭滨硕 LIANG Dingcheng;YANG Lulu;XIE Qiang;XIE Zhucan;DENG Qingwen;GUO Binshuo(School of Chemical and Environmental Engineering,China University of Mining and Technology-Beijing,Beijing 100083,China)

机构地区：[1]中国矿业大学(北京)化学与环境工程学院,北京100083

出　　处：《洁净煤技术》2024年第1期163-172,共10页Clean Coal Technology

基　　金：国家自然科学基金资助项目(22008255);国家重点研发计划资助项目(2022YFC3701900,2022YFD2200904);中央高校基本科研业务费资助项目(2022XJHH06,2023ZKPYHH02)。

摘　　要：发电厂烟气中CO_(2)是主要碳排放源之一,利用沸石膜孔径大小进行CO_(2)分离则是实现碳中和、降低碳排放的重要手段。然而,在高温高压气体环境下使用沸石膜分离烟气时,沸石与载体结合并不紧密,易导致膜层在分离烟气过程中破裂或与载体发生剥离,为沸石膜大规模分离CO_(2)提出挑战。综述了沸石与载体之间的结合方式以及结合力特性,并对定量表征结合力强弱的方法进行归纳、总结。结果表明,Decadodecasil 3R(DD3R)沸石具有全硅结构及介于CO_(2)/N_(2)分子大小的孔隙尺寸,可与经过酸处理的陶瓷载体形成相对稳固的共价键,从而形成结合紧密的沸石膜。即使在水蒸气影响下,该膜仍能有效实现烟气中CO_(2)/N_(2)分离;传统试验方法(如超声法、划痕法和压痕法)在研究载体、沸石和改性剂界面的结合力时无法提供详细数据,分子模拟能有效弥补这些不足,在原子尺度上模拟材料界面的结合情况并进行量化,从而为筛选最优的载体改性方法提供了坚实的理论基础。One of the primary sources of carbon emissions is CO_(2),which may be separated from flue gas in power plants using zeolite membranes with different pore sizes.This technique is crucial for achieving carbon neutralization and lowering carbon emissions.The connection between the zeolite and the carrier is not strong when zeolite membranes are used to segregate flue gas in high-temperature and high-pressure gas conditions.It can easily cause the membrane layer to rupture or peel off the carrier during the flue gas separation,making large-scale zeolite membrane separation difficult.The binding modes between zeolites and carriers and the characteristics of the binding force were reviewed,and the methods for quantitatively characterizing the binding force were summarized.The results show that the all-silica Decadodecasil 3R(DD3R)zeolite,which has pore diameters between CO_(2)/N_(2)molecules,may form strong covalent solid connections with the ceramic carrier that has been treated with acid,producing a zeolite membrane that is tightly attached.Even in the presence of steam,the membrane efficiently separates CO_(2)/N_(2)from flue gas.Traditional experimental methods(such as ultrasonication,scratching,and indentation)cannot provide detailed data when examining the bonding at the interface between the carrier,zeolite,and modifier.However,molecular simulation can compensate for these shortcomings by simulating and quantifying the bonding at the material′s interface at the atomic scale,offering a robust theoretical foundation for selecting the best carrier modification technique.

关 键 词：沸石膜 烟气 碳捕集 结合力 改性 

分 类 号：TQ028[化学工程]