The electrochemical reduction of carbon monoxide (COR) holds significant promise as an ecofriendly approach for producing valuable chemicals, such as acetate. However, the current unsatisfactory activity and selectivity of this process hinder its future implementation. In this study, we develop and study a catalyst composite comprising lanthanum fluoride (LaF₃) crystal support and copper (Cu) as the active phase. Under typical COR conditions, the LaF₃–Cu electrocatalyst demonstrates remarkable selectivity, exceeding 40% at −0.95 V vs. RHE, with a partial current density of over 280 mA cm^–2 for acetate production. In contrast, the pristine Cu catalyst achieves only 56 mA cm^–2 at −1.12 V vs. RHE with a low selectivity of <10%. Through detailed kinetic and computational studies, we attribute this remarkable enhancement in both selectivity and activity toward acetate formation to the stabilization of the ethenone intermediate at the LaF₃/Cu interface during COR. Inspired by this finding, we extended this substrate effect to a bimetallic copper–silver catalyst, which led to a notable increase in acetate selectivity (>66%) under the same conditions. Overall, our findings introduce a universal strategy based on substrate effects for the development of selective and active COR catalysts.

中文翻译：

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Cu/LaF3 界面促进电催化 CO 向乙酸的转化

一氧化碳 (COR) 的电化学还原作为一种生产醋酸盐等有价值化学品的环保方法具有重大前景。然而，目前该过程的活性和选择性不令人满意，阻碍了其未来的实施。在这项研究中，我们开发和研究了一种包含氟化镧（LaF ₃）晶体载体和铜（Cu）作为活性相的催化剂复合材料。在典型的COR条件下，LaF ₃ –Cu电催化剂表现出显着的选择性，在-0.95 V vs. RHE下超过40%，用于乙酸盐生产的部分电流密度超过280 mA cm ^–2。相比之下，原始 Cu 催化剂在 -1.12 V vs. RHE 下仅达到 56 mA cm ^–2，选择性较低，<10%。通过详细的动力学和计算研究，我们将乙酸盐形成的选择性和活性的显着增强归因于 COR 期间 LaF ₃ /Cu 界面处乙烯酮中间体的稳定性。受这一发现的启发，我们将这种底物效应扩展到双金属铜银催化剂，这导致在相同条件下乙酸盐选择性显着增加（> 66％）。总的来说，我们的研究结果介绍了一种基于底物效应的通用策略，用于开发选择性和活性 COR 催化剂。