Selective electrochemical reduction of CO/CO to high-valuable C products is of great importance to alleviate the global warming and energy crisis problems, while the selective production of C is severely limited by the CC coupling pathway on the catalyst interface. Herein, by employing a Cu/Cu charge-ordered metal-organic framework (MOF) material (denoted to be Cu4BHT) as a CO electroreduction catalyst, a high acetate selectivity of 50.3% at 0.7 V versus reversible hydrogen electrode (RHE) has been achieved. An in-depth mechanism study reveals that the charge-ordered Cu/Cu pair on Cu4BHT interface favors the CO bond activation, CC coupling, and proton-coupled electron transfer dynamics, which results in the selective formation of C products. This work illustrates the critical role of employing charge-ordered Cu/Cu catalytic site pair for CC coupling, which paves the way for designing highly selective catalysts to promote the formation of the C products.

中文翻译：

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电荷有序 Cu+/Cu2+ 对调控一氧化碳高选择性电还原成乙酸盐

CO/CO选择性电化学还原为高价值的C产物对于缓解全球变暖和能源危机问题具有重要意义，而C的选择性生产却受到催化剂界面上CC偶联途径的严重限制。在此，通过采用Cu/Cu电荷有序金属有机骨架（MOF）材料（记为Cu4BHT）作为CO电还原催化剂，相对于可逆氢电极（RHE），在0.7 V电压下乙酸盐选择性高达50.3%实现了。深入的机理研究表明，Cu4BHT 界面上的电荷有序 Cu/Cu 对有利于 CO 键活化、CC 耦合和质子耦合电子转移动力学，从而导致 C 产物的选择性形成。这项工作说明了采用电荷有序的 Cu/Cu 催化位点对进行 CC 偶联的关键作用，这为设计高选择性催化剂以促进 C 产物的形成铺平了道路。