Promoted hydrogenation of CO2 to methanol over single-atom Cu sites with Na+-decorated microenvironment

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外文摘要：Although single-atom Cu sites exhibit high efficiency in CO2 hydrogenation to methanol,they are prone to forming Cu nanoparticles due to reduction and aggregation under reaction conditions,especially at high temperatures.Herein,single-atom Cu sites stabilized by adjacent Na+ions have been successfully constructed within a metal-organic framework(MOF)-based catalyst,namely MOF-808-NaCu.It is found that the electrostatic interaction between the Na+and Hδ-species plays a pivotal role in upholding the atomic dispersion of Cu in MOF-808-NaCu during CO2 hydrogenation,even at temperatures of up to 275℃.This exceptional stabilization effect endows the catalyst with excellent activity(306 g.kgcat-1-h-1),high selectivity to methanol(93％)and long-term stability at elevated reaction temperatures,far surpassing the counterpart in the absence of Na+(denoted as MOF-808-Cu).This work develops an effective strategy for the fabrication of stable single-atom sites for advanced catalysis by creating an alkali-decorated microenvironment in close proximity.

外文关键词：

single-atom sitesmetal-organic frameworkCO2 hydrogenationheterogeneous catalysisalkali-metal decoration

作者：

Li-Li Ling、Xinyu Guan、Xiaoshuo Liu、Xiao-Mei Lei、Zhongyuan Lin、Hai-Long Jiang

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作者单位：

Hefei National Research Center for Physical Sciences at the Microscale,Department of Chemistry,University of Science and Technology of China,Hefei 230026,China

School of Energy and Power Engineering,North China Electric Power University,Baoding 071003,China

School of Energy and Environment,Southeast University,Nanjing 210096,China

基金：

National Key Research and Development Program of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaStrategic Priority Research Program of the Chinese Academy of SciencesStrategic Priority Research Program of the Chinese Academy of SciencesChina Postdoctoral Science FoundationInternational Partnership Program of CASFundamental Research Funds for the Central Universities

项目编号：

2021YFA150040222331009U22A204012220522422301186XDB0450302XDB05400002021M703064123GJHZ2022028MIWK2060000041

出版年：

2024

DOI：

10.1093/nsr/nwae114

国家科学评论(英文版)

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ISSN：

年,卷(期)：2024.11(6)