Regulating the coordination environment of Ru single-atom catalysts and unravelling the reaction path of acetylene hydrochlorination
作者机构：State Key Laboratory of Elemento-Organic ChemistryKey Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)College of ChemistryNankai UniversityNo.94 Weijin RoadTianjin300071China
出 版 物：《Green Energy & Environment》 (绿色能源与环境（英文版）)
年 卷 期：2023年第8卷第4期
页 面：1141-1153页
核心收录：
学科分类：081702[工学-化学工艺] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 0806[工学-冶金工程] 0703[理学-化学] 0702[理学-物理学]
基 金：supported by the National Natural Science Foundation of China (NSFC,22172082,21978137,22102074,and 21878162) Natural Science Foundation of Tianjin (20JCZDJC00770) Postdoctoral Research Foundation of China (2021M701776) NCC Fund (NCC2020FH05)。
主 题：Single-atom catalyst Coordination environment Ru-based catalyst DFT calculations Acetylene hydrochlorination
摘 要：In this work,DFT calculations were used firstly to simulate the nitrogen coordinated metal single-atom catalysts(M-N_(x)SACs,M=Hg,Cu,Au,and Ru) to predict their catalytic activities in acetylene hydrochlorination.The DFT results showed that Ru-N_(x)SACs had the best catalytic performance among the four catalysts,and Ru-N_(x)SACs could effectively inhibit the reduction of ruthenium cation.To verify the DFT results,Ru-N_(x)SACs were fabricated by pyrolyzing MOFs in-situ spatially confined metal precursors.The N coordination environment could be controlled by changing the pyrolysis temperature.Catalytic performance tests indicated that low N coordination number(Ru-N_(2),Ru-N_(3))exhibited excellent catalytic activity and stability compared to RuCl_(3)catalyst.DFT calculations further revealed that Ru-N_(2)and Ru-N_(3)had a tendency to activate HCl at the first step of reaction,whereas Ru-N4tended to activate C_(2)H_(2).These findings will serve as a reference for the design and control of metal active sites.
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