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In situ synthesis of sub-nanometer metal particles on hierarchically porous metal–organic frameworks via interfacial control for highly efficient catalysis†
Chemical Science ( IF 7.6 ) Pub Date : 2017-12-14 00:00:00 , DOI: 10.1039/c7sc04269h
Pei Zhang 1, 2 , Chunjun Chen 1, 2 , Xinchen Kang 1, 2 , Lujun Zhang 1, 2 , Congyi Wu 1 , Jianling Zhang 1, 2 , Buxing Han 1, 2
Affiliation  

In this work, we developed a strategy to in situ synthesize sub-nanometer metal particle/hierarchically mesoporous metal–organic framework (MOF) composites in emulsion. In this route, water droplets in the emulsion acted as both a solvent of the metal precursors and a template for the hierarchical mesopores of MOFs, and the surfactant was an emulsifier and a reductant for generating metal particles. Au/Zn-MOFs (MOFs formed by Zn2+ and methylimidazole), Ru/Zn-MOFs, Pd/Zn-MOFs, and Au/Cu-MOFs (MOFs formed by Cu2+ and methylimidazole) were prepared using this method, in which ultrafine metal particles (e.g. 0.8 nm) were immobilized uniformly on hierarchically mesoporous MOFs. Au/Zn-MOFs and Au/Cu-MOFs showed outstanding catalytic performances for the selective aerobic oxidation of cyclohexene to 2-cyclohexen-1-one in the absence of an initiator, and Ru/Zn-MOFs were very active and selective for the hydrogenation of diphenyl sulfoxide to diphenyl sulfide. In addition, the catalysts were also very stable in the reactions.

中文翻译:


通过界面控制在分级多孔金属有机框架上原位合成亚纳米金属颗粒以实现高效催化†



在这项工作中,我们开发了一种在乳液中原位合成亚纳米金属颗粒/分层介孔金属有机骨架(MOF)复合材料的策略。在该路线中,乳液中的水滴既充当金属前驱体的溶剂,又充当MOF分级介孔的模板,表面活性剂充当乳化剂和生成金属颗粒的还原剂。使用该方法制备了Au/Zn-MOFs(由Zn 2+和甲基咪唑形成的MOFs)、Ru/Zn-MOFs、Pd/Zn-MOFs和Au/Cu-MOFs(由Cu 2+和甲基咪唑形成的MOFs),其中超细金属颗粒(例如0.8 nm)均匀地固定在分级介孔MOF上。 Au/Zn-MOFs 和 Au/Cu-MOFs 在没有引发剂的情况下对环己烯选择性有氧氧化生成 2-环己烯-1-酮表现出出色的催化性能,而 Ru/Zn-MOFs 对环己烯选择性有氧氧化具有非常高的活性和选择性。二苯亚砜加氢生成二苯硫醚。此外,催化剂在反应中也非常稳定。
更新日期:2017-12-14
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