UiO-66-NH_(2)合成及其在混合基质碳捕集膜中的应用  

Synthesis of UiO−66−NH_(2)nanoparticles and its application in preparation of mixed-matrix membranes for carbon capture

作　　者：陈羿戬 生梦龙 李庆华 王志[1,2,3,4,5] CHEN Yijian;SHENG Menglong;LI Qinghua;WANG Zhi(School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072,China;Chemical Engineering Research Center,School of Chemical Engineering and Technology,Tianjin University,Tianjin 300350,China;Tianjin Key Laboratory of Membrane Science and Desalination Technology,Tianjin 300350,China;State Key Laboratory of Chemical Engineering,Tianjin University,Tianjin 300350,China;Tianjin Collaborative Innovation Center of Chemical Science and Engineering,Tianjin 300350,China)

机构地区：[1]天津大学化工学院,天津300072 [2]天津大学化工学院化学工程研究所,天津300350 [3]天津市膜科学与海水淡化技术重点实验室,天津300350 [4]天津大学化学工程联合国家重点实验室,天津300350 [5]天津化学化工协同创新中心,天津300350

出　　处：《洁净煤技术》2024年第10期58-68,共11页Clean Coal Technology

基　　金：国家自然科学基金资助项目(21938007);国家重点研发计划资助项目(2021YFB3801200);化学工程联合国家重点实验室开放课题资助项目(SKL-ChE-23B03)。

摘　　要：UiO-66-NH_(2)是典型Zr基金属有机框架(Zr-MOFs),在CO_(2)吸附领域应用前景广阔,是与聚乙烯基胺(PVAm)结合制备混合基质膜(MMMs)的较好填料。但UiO-66-NH_(2)合成反应规模化效应明显,难放大到十克级以上。通过调节水–乙酸的比例,合成了一系列UiO-66-NH_(2),并通过扫描电子显微镜(SEM)、X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、比表面积测试与孔隙率分析(BET)对样品进行表征。通过分析表征结果,提出一种水–乙酸促进Zr-MOFs二级结构(SBU)形成的机理,以此为指导成功实现UiO-66-NH_(2)颗粒的百克级规模化合成。此外,将该材料与聚乙烯基胺(PVAm)结合制备了UiO-66-NH_(2)/PVAm混合基质膜,用模拟烟道气(CO_(2)、N_(2)体积分数分别为15%、85%)进行分离性能测试,相较纯PVAm膜,UiO-66-NH_(2)/PVAm混合基质膜分离性能提高,CO_(2)渗透率达1937 GPU,CO_(2)/N_(2)分离因子达85。根据成本估算结果,用混合基质膜可有效减少碳捕集成本,在实际燃煤烟道气碳捕集中有应用前景。UiO−66−NH_(2)is a typical Zr−based metal-organic frameworks(Zr−MOFs)with considerable application prospect in CO_(2)adsorption.It is a good filler combined with polyvinylamine(PVAm)to prepare mixed-matrix membranes(MMMs).However,the scaling effect of UiO−66−NH_(2)preparation is too obvious to scale it up to more than ten-gram-scale.A series of UiO−66−NH_(2)was synthesized by changing the ratio of water-acetic acid.Scanning Electron Microscope(SEM),X−ray Diffraction(XRD),Fourier Transform Infrared(FTIR)and BET test were used to characterize the samples.Through the analysis of characterization results,a mechanism for water-acetic acid promotion of Zr−MOFs secondary-building-unit(SBU)formation was proposed,which has guided the hundred-gram-scale synthesis of UiO−66−NH_(2)particles.Furthermore,these particles were combined with polyvinylamine(PVAm)to prepare UiO−66−NH_(2)/PVAm MMMs,whose separation performance were tested using simulated flus gas(volume fractions of CO_(2)and N_(2)are 15%and 85%,separately).Compared with PVAm membranes,the separation performance of MMMs increases.The CO_(2)permeance reaches 1937 GPU and the CO_(2)/N_(2)separation factor reaches 85.The result of the cost estimation shows that the use of MMMs can effectively reduce the cost of carbon capture and it also has application prospects in flus gas carbon capture.

关 键 词：UiO-66-NH_(2) 规模化制备 膜分离 CO_(2)捕集 水促进 

分 类 号：X701[环境科学与工程—环境工程] TQ051[化学工程]