Valence state of transition metal center as an activity descriptor for CO2 reduction on single atom

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Carbon dioxide (CO2) catalytic reduction has been passionately pursued for a long period of time due to its special importance in alleviating the greenhouse effect as well as generating valuable fuels and chemicals [1].Among the various approaches for achieving CO2 conversion, considerable efforts have been devoted to electrochemical reduction of CO2 since this technology operates at ambient and mild environments and can potentially produce various useful products [2].By now, a variety of electrocatalysts based on transition metals, transition metal oxides, and transition metal dichalcogenides [3-5], have been proposed for electrochemical CO2 reduction reaction (CRR).Unfortunately, the current electrocatalysts are still confronted with two severe bottlenecks: Poor selectivity toward various products in CRR process, and the competition with hydrogen evolution reaction (HER) towards unwanted side-products [6].The former originates from associated multielectron transfer process of CRR [7], while the latter is mainly due to the fact that the equilibrium potentials for most products of the CRR are very close to HER [8].Thus, developing highly active and selective catalysts for electrochemical CRR remains one of the challenging issues in this field.
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