Promoted hydrogenation of CO_(2) to methanol over single-atom Cu sites with Na^(+)-decorated microenvironment  

作　　者：Li-Li Ling Xinyu Guan Xiaoshuo Liu Xiao-Mei Lei Zhongyuan Lin Hai-Long Jiang 

机构地区：[1]Hefei National Research Center for Physical Sciences at the Microscale,Department of Chemistry,University of Science and Technology of China,Hefei 230026,China [2]School of Energy and Power Engineering,North China Electric Power University,Baoding 071003,China [3]School of Energy and Environment,Southeast University,Nanjing 210096,China

出　　处：《National Science Review》2024年第6期257-265,共9页国家科学评论（英文版）

摘　　要：Although single-atom Cu sites exhibit high efficiency in CO_(2) hydrogenation to methanol, they are prone toforming Cu nanoparticles due to reduction and aggregation under reaction conditions, especially at hightemperatures. Herein, single-atom Cu sites stabilized by adjacent Na^(+) ions have been successfullyconstructed within a metal–organic framework (MOF)-based catalyst, namely MOF-808-NaCu. It is foundthat the electrostatic interaction between the Na^(+) and H^(δ−) species plays a pivotal role in upholding theatomic dispersion of Cu in MOF-808-NaCu during CO_(2) hydrogenation, even at temperatures of up to275℃. This exceptional stabilization effect endows the catalyst with excellent activity (306 g·kg_(cat)^(−1)·h^(−1)),high selectivity to methanol (93%) and long-term stability at elevated reaction temperatures, far surpassingthe counterpart in the absence of Na^(+) (denoted as MOF-808-Cu). This work develops an effective strategyfor the fabrication of stable single-atom sites for advanced catalysis by creating an alkali-decoratedmicroenvironment in close proximity.

关 键 词：single-atom sites metal-organic framework CO_(2)hydrogenation heterogeneous catalysis alkali-metal decoration 

分 类 号：O643.36[理学—物理化学] TQ264.1[理学—化学]