Unraveling the Selectivity of Acidic CO2 Reduction in CuAg Tandem Electrocatalysts
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Updated: Jun 7, 2026

Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
Yi Chen1, Taiping Ye2, Zhizhong He2
1Department of Applied Physical Sciences, The University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27514, United States.
Abstract:
Acidic electrocatalytic CO2 reduction (CO2R) offers compelling advantages in carbon efficiency and long-term stability. However, mechanistic insights into tandem electrocatalysis in acidic media remain limited due to the difficulty of resolving the coupled dynamics of intermediates at reactive interfaces. Here, we unveil a "CH4-C2+-CO" selectivity evolution across composition-graded CuAg tandem catalysts as Ag fraction increases from single-atom alloy to subnanoclusters to nanoparticle clusters. The surface composition simultaneously governs *CO intermediate binding strength and reorients the interfacial water microenvironment to direct local reaction pathways. The product selectivity of CuAg tandem catalysts is dictated by the regulation of *CO spillover from Ag to adjacent Cu domains, favoring either C-C coupling or CO desorption. Our findings establish a unified *CO/*H-centric mechanistic framework for tandem CO2R electrocatalysis in acidic media, providing compositional design principles for selective multicarbon product generation.
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