Abstract
The emergence of synergistic effects in multicomponent catalysts can result in breakthrough advances in the electrochemical reduction of carbon dioxide. Copper-indium catalysts show high performance toward carbon monoxide production but also extensive structural and compositional changes under operation. The origin of the synergistic effect and the nature of the active phase are not well understood, thus hindering optimization efforts. Here we develop a platform that sheds light into these aspects, based on microfabricated model electrodes that are evaluated under conventional experimental conditions. The relationship among the electrode performance, geometry and composition associates the high carbon monoxide evolution activity of copper-indium catalysts to indium-poor bimetallic phases, which are formed upon exposure to reaction conditions in the vicinity of the interfaces between copper oxide and an indium source. The exploratory extension of this approach to the copper-tin system demonstrates its versatility and potential for the study of complex multicomponent electrocatalysts.
Highlights
The emergence of synergistic effects in multicomponent catalysts can result in breakthrough advances in the electrochemical reduction of carbon dioxide
A way to bridge this gap is to use micro- and nanostructuring processes, which have been valuable for studying other photoand electrochemical systems[23,24,25], to fabricate model electrodes that can be tested under eCO2RR conditions and whose catalytic performance can be directly related to their structure and composition, as recently demonstrated by epitaxially grown Cu electrodes[26], and by Au and Cu catalysts with a controlled grain-boundary density[27,28,29]
Based on our previous work on indium-modified electrocatalysts, we initially hypothesized that the synergistic effect observed in these systems was due to the existence of bifunctional sites with high CO evolution activity located at the interfaces between oxidic indium phases and metallic components[20,21,22]
Summary
The emergence of synergistic effects in multicomponent catalysts can result in breakthrough advances in the electrochemical reduction of carbon dioxide. The behaviour of these catalysts is marked by the occurrence of extensive structural and compositional changes upon exposure to reaction conditions[19,21] In this context, the synthesis and characterization of materials with a high degree of structural and compositional control are key to deconvoluting this complex picture and obtaining insights into the nature of the active sites in these multicomponent catalysts. The synthesis and characterization of materials with a high degree of structural and compositional control are key to deconvoluting this complex picture and obtaining insights into the nature of the active sites in these multicomponent catalysts In this direction, surface science studies have investigated the role of metal–oxide interfaces in the adsorption and activation of CO2 over Au/CeOx catalysts[22], but the applicability of ultra-high vacuum techniques in the eCO2RR is limited by their large gap with the actual environment of the electrochemical reaction. This study shows how its high-throughput capability combined with careful consideration of the geometry in the design can overcome such limitations to derive catalytically valuable insights
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