摘要
面向C1分子及低碳烷烃活化脱氢制备C2和C3烯烃等重要化工过程,设计高效、稳定的负载型金属催化剂,防止金属物种在苛刻的制备和反应条件下烧结成大尺寸纳米颗粒是一个关键的挑战.具有均匀亚纳米尺寸孔道和丰富三维晶体结构的多孔沸石分子筛,已被证明是将金属团簇封装在其孔道内以制备高效稳定金属催化剂的理想载体.更重要的是,亚纳米金属团簇和沸石骨架原子之间的相互作用可以调节其几何和电子结构.研发沸石孔道限域的亚纳米团簇型金属催化剂旨在利用这种联合的约束效应,诱导金属物种与具有活性位点的沸石骨架间的协同作用,进一步提升复合催化剂的催化性能,应用于多种催化反应过程.本文主要介绍了几种典型的方法制备沸石孔道限域的亚纳米团簇型金属催化剂,以及在CO_(2)和炔烃选择性加氢、甲酸分解产氢、氨硼烷水解产氢及丙烷脱氢制丙烯反应过程中的催化应用.
The design of efficient and stable supported metal catalysts to prevent metal species from sintering into large nanoparticles under harsh preparation and reaction conditions is key for various important processes,including the conversion of C1 resources and dehydrogenation of low carbon alkanes to C2 and C3 olefins.Zeolites with uniform subnano micropores and various three-dimensional crystalline structures have been proven as ideal supports for preparing highly efficient and stable metal catalysts via encapsulating subnanometric metal clusters within their pores,cages,and channels.Interactions between metal clusters and the zeolite skeleton can regulate their geometric and electronic structure.The development of zeolite-confined subnanometric cluster catalysts aims to take advantage of this joint confinement effect and induce synergy between guest metal species and active sites in host zeolite frameworks.This can further improve the catalytic activity of resultant composite catalysts,for applications in multiple catalytic reaction processes.In this review,typical preparation methods of zeoliteconfined subnanometric clusters and their catalytic applications in selective hydrogenation of CO_(2)and alkynes,hydrogen generation by formic acid decomposition and ammonia borane hydrolysis,and propane dehydrogenation to propene are discussed.
作者
马跃
徐浩
刘月明
张坤
吴鹏
何鸣元
MA Yue;XU Hao;LIU Yueming;ZHANG Kun;WU Peng;HE Mingyuan(Shanghai Key Laboratory of Green Chemistry and Chemical Processes,School of Chemistry and Molecular Engineering,East China Normal University,Shanghai 200062,China)
出处
《华东师范大学学报（自然科学版）》
CAS
CSCD
北大核心
2023年第1期82-94,共13页
Journal of East China Normal University(Natural Science)
基金
国家自然科学基金(21872052,21972044)
华东师范大学“幸福之花”先导研究基金(2020ST2203)。
关键词
沸石
团簇
约束效应
选择性加氢
丙烷脱氢
zeolite
clusters
confinement effect
selective hydrogenation
propane dehydrogenation
作者简介
第一作者:马跃,男,博士后,研究方向为沸石基催化材料.E-mail:yma@chem.ecnu.edu.cn;通信作者:吴鹏,男,教授,博士生导师,研究方向为多相催化与纳米多孔材料.E-mail:pwu@chem.ecnu.edu.cn。
