Sassenburg Mark, Iglesias van Montfort H P, Kolobov Nikita, Smith Wilson A, Burdyny Thomas
Department of Chemical Engineering, Delft University of Technology, 2629HZ, Delft, The Netherlands.
Department of Chemical and Biological Engineering and Renewable and Sustainable Energy Institute (RASEI), University of Colorado Boulder, Boulder, Colorado, 80303, United States.
ChemSusChem. 2025 Apr 14;18(8):e202401769. doi: 10.1002/cssc.202401769. Epub 2024 Dec 3.
The electrochemical reduction of carbon dioxide (CO) presents an opportunity to close the carbon cycle and obtain sustainably sourced carbon compounds. In recent years, copper has received widespread attention as the only catalyst capable of meaningfully producing multi-carbon (C) species. Notably carbon monoxide (CO) can also be reduced to C compounds on copper, motivating tandem systems that combine copper and CO-producing species, like silver, to enhance overall C selectivities. In this work, we examine the impact of layered-combinations of bulk Cu and Ag by varying the location and proportion of the CO-producing Ag layer. We report an effective increase in the C oxygenate selectivity from 23 % with a 100 nm Cu to 38 % for a 100 : 15 nm Cu : Ag layer. Notably, however, for all co-catalyst cases there is an overproduction of CO vs Cu alone, even for 5 nm Ag layers. Lastly, due to restructuring and interlayer mobility of the copper layer it is clear that the stability of copper limits the locational advantages of such tandem solutions.
二氧化碳（CO₂）的电化学还原为闭合碳循环和获得可持续来源的碳化合物提供了契机。近年来，铜作为唯一能够有效生成多碳（C₂+）物种的催化剂受到了广泛关注。值得注意的是，一氧化碳（CO）在铜上也能被还原为碳化合物，这促使人们开发出将铜与产CO物种（如银）相结合的串联体系，以提高整体碳选择性。在这项工作中，我们通过改变产CO的银层的位置和比例，研究了块状铜和银的层状组合的影响。我们报告称，C₂+含氧化合物的选择性从100 nm铜时的23%有效提高到100:15 nm铜:银层时的38%。然而，值得注意的是，对于所有共催化剂情况，与单独使用铜相比，CO的产量都会过量，即使是5 nm的银层也是如此。最后，由于铜层的重构和层间迁移，很明显铜的稳定性限制了这种串联体系的位置优势。
