Powered by renewable electricity, electrochemical CO2 reduction (CO2R) offers a sustainable route for the production of fuels and chemicals that are traditionally produced from fossil fuels. However, designing and developing an efficient electrocatalyst for CO2-to-C2+ product conversion remains challenging. Here, a gold-copper tandem catalyst electrode design is introduced that leverages the structural effects of a wrinkled morphology to improve the CO2R selectivity and activity in a three-electrode electrochemical cell. The wrinkled electrode structure significantly increases the electrochemical active surface area, resulting in enhanced CO2R current density for both the singular wrinkled gold and wrinkled copper electrodes. Specifically, there is a 130 % increase in partial current density towards CO for a wrinkled gold electrode versus planar gold electrode at −0.7 V versus the reversible hydrogen electrode (VRHE), and a 50 % increase in partial current density for C2+ products for a wrinkled copper electrode at −1.05 VRHE compared to a planar copper electrode. A wrinkled gold-copper tandem electrode further enhances the partial current density of C2+ products by an additional 60 % beyond that of the wrinkled copper electrode (at −1.05 VRHE), illustrating the synergistic effect of the three-dimensional wrinkled morphology combined with tandem catalysis. Tafel plot analysis revealed effective mass transport for C2+ product generation on the optimized wrinkled gold-copper tandem electrode, attributed to the local *CO production by the tandem catalyst, facilitating enhanced C-C coupling on the copper catalyst compared to a purely copper based electrode. Experimental results show that the design and manipulation of the morphology of the tandem catalyst electrode achieved via step-by-step optimization can significantly enhance the selectivity and activity of the catalyst in converting CO2 to desired fuels and chemicals.

中文翻译：

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通过起皱进行串联金/铜催化和形态调整，以促进 CO2 电还原成 C2+ 产物


电化学 CO2 还原 （CO2R） 由可再生电力提供动力，为生产传统上由化石燃料生产的燃料和化学品提供了一条可持续的途径。然而，设计和开发一种用于 CO2 到 C2+ 产品转化的高效电催化剂仍然具有挑战性。本文介绍了一种金铜串联催化剂电极设计，该设计利用褶皱形态的结构效应来提高三电极电化学电池中 CO2R 的选择性和活性。褶皱电极结构显著增加了电化学活性表面积，从而提高了单一褶皱金和褶皱铜电极的 CO2R 电流密度。具体来说，与可逆氢电极 （VRHE） 相比，−0.7 V 时起皱金电极的 CO 部分电流密度增加了 130%，−1.05 VRHE 时起皱铜电极的 C2+ 产物的部分电流密度增加了 50%。褶皱金铜串联电极进一步将 C2+ 产物的部分电流密度提高了 60%，比褶皱铜电极（在 -1.05 VRHE 时）高出 60%，说明了三维褶皱形态与串联催化相结合的协同效应。塔菲尔图分析显示，在优化的褶皱金铜串联电极上，C2+ 产物生成具有有效的质量传递，这归因于串联催化剂的局部 *CO 产生，与纯铜基电极相比，有助于增强铜催化剂上的 C-C 偶联。 实验结果表明，通过逐步优化实现的串联催化剂电极形态的设计和操纵可以显著提高催化剂将 CO2 转化为所需燃料和化学品的选择性和活性。