The electrocatalytic reaction pathway is highly dependent on the intrinsic structure of the catalyst. CO₂/CO electroreduction has recently emerged as a potential approach for obtaining C₂₊ products, but it is challenging to achieve high selectivity for a single C₂₊ product. Herein, we develop a Cu atomic ensemble that satisfies the appropriate site distance and coordination environment required for electrocatalytic CO-to-acetate conversion, which shows outstanding overall performance with an acetate Faradaic efficiency of 70.2% with a partial current density of 225 mA cm^–2 and a formation rate of 2.1 mmol h^–1 cm^–2. Moreover, a single-pass CO conversion rate of 91% and remarkable stability can be also obtained. Detailed experimental and theoretical investigations confirm the significant advantages of the Cu atomic ensembles in optimizing C–C coupling, stabilizing key ketene intermediate (*CCO), and inhibiting the *HOCCOH intermediate, which can switch the CO reduction pathway from the ethanol/ethylene on the conventional metallic Cu site to the acetate on the Cu atomic ensembles.

中文翻译：

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在 Cu 原子系综上切换 CO 到乙酸盐电还原


电催化反应途径高度依赖于催化剂的本征结构。CO₂/CO 电还原最近已成为获得 C₂₊ 产物的一种潜在方法，但要实现单个 C₂₊ 产物的高选择性具有挑战性。在此，我们开发了一种 Cu 原子系综，它满足电催化 CO 到乙酸盐转化所需的适当位距和配位环境，它显示出出色的整体性能，乙酸盐法拉第效率为 70.2%，部分电流密度为 225 mA cm^–2，形成速率为 2.1 mmol h^–1 cm^–2.此外，还可以获得 91% 的单程 CO 转化率和显着的稳定性。详细的实验和理论研究证实了 Cu 原子系合体在优化 C-C 偶联、稳定关键乙烯酮中间体 （*CCO） 和抑制 *HOCCOH 中间体方面的显着优势，它可以将 CO 还原途径从常规金属 Cu 位点上的乙醇/乙烯切换到 Cu 原子系综上的乙酸盐。