Electrochemical conversion of small molecules such as carbon dioxide (CO₂) and carbon monoxide (CO) to high-value multi-carbon products (C₂₊) offers a chemical upgrade approach for fuels and chemical feedstock production using renewable energy, in the possible absence of the petrochemical industry under the new energy system such as hydrogen economy. Identifying robust and efficient electrocatalysts to selectively produce C₂₊ products remains a challenge. Herein, we report a synthetic strategy of atomically dispersing copper atoms on nitrogen-rich porous carbon (Cu–N–C) through pyrolysis of a supramolecular assembly. Benefitting from the unsaturated coordination structure, in KOH electrolyte, the Cu–N–C with a Cu content of 6.9 wt% exhibits a maximum acetate Faradaic efficiency (FE) of 30% with an acetate partial current density as high as 48 mA cm⁻² in electrochemical CO reduction. Different from the C–C coupling mechanism on metallic copper, we propose a CO insertion mechanism for the acetate production on the single site copper catalyst.

将二氧化碳（CO ₂）和一氧化碳（CO）等小分子电化学转化为高价值的多碳产物（C ₂₊），为使用可再生能源的燃料和化学原料生产提供了一种化学升级方法，在可能的情况下氢经济等新能源体系下石化行业的缺位。识别强大而有效的电催化剂以选择性产生C ₂₊产品仍然是一个挑战。在这里，我们报告了一种通过超分子组装的热解将铜原子原子分散在富氮多孔碳（Cu–N–C）上的合成策略。来自不饱和协调结构中受益，在KOH电解质中，Cu-N-C与6.9重量％的Cu含量％表现出30％的最大乙酸法拉第效率（FE）与乙酸盐的部分的电流密度高达48毫安厘米^{- 2}在电化学中CO的还原。与金属铜上的C–C偶联机理不同，我们提出了在单中心铜催化剂上生成乙酸盐的CO插入机理。