Unraveling the Selectivity of Acidic CO<sub>2</sub> Reduction in CuAg Tandem Electrocatalysts.
basic_science · Level V
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- Record sourced from PubMed, PMID 42247624.
- Also identified by DOI 10.1021/acs.nanolett.6c01920.
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Abstract
Acidic electrocatalytic CO<sub>2</sub> reduction (CO<sub>2</sub>R) 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 "CH<sub>4</sub>-C<sub>2+</sub>-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 CO<sub>2</sub>R electrocatalysis in acidic media, providing compositional design principles for selective multicarbon product generation.