电子转移
催化作用
羧酸盐
偏苯三甲酸
化学
质子耦合电子转移
电化学
氧化还原
质子
铜
金属
无机化学
材料科学
光化学
物理化学
分子
立体化学
电极
有机化学
物理
量子力学
作者
Wei Zhang,Chuqiang Huang,Jiexin Zhu,Qiancheng Zhou,Ruohan Yu,Yali Wang,Pengfei An,Jing Zhang,Ming Qiu,Liang Zhou,Liqiang Mai,Zhiguo Yi,Ying Yu
标识
DOI:10.1002/anie.202112116
摘要
The electrochemical reduction of CO2 to hydrocarbons involves a multistep proton-coupled electron transfer (PCET) reaction. Second coordination sphere engineering is reported to be effective in the PCET process; however, little is known about the actual catalytic active sites under realistic operating conditions. We have designed a defect-containing metal-organic framework, HKUST-1, through a facile "atomized trimesic acid" strategy, in which Cu atoms are modified by unsaturated carboxylate ligands, producing coordinatively unsaturated Cu paddle wheel (CU-CPW) clusters. We investigate the dynamic behavior of the CU-CPW during electrochemical reconstruction through the comprehensive analysis of in situ characterization results. It is demonstrated that Cu2 (HCOO)3 is maintained after electrochemical reconstruction and that is behaves as an active site. Mechanistic studies reveal that CU-CPW accelerates the proton-coupled multi-electron transfer (PCMET) reaction, resulting in a deep CO2 reduction reaction.
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