Recognizing the Universality of Copper Reconstruction Via Dissolution-Redeposition at the Onset of CO(2) Reduction

认识到在二氧化碳还原初期,铜通过溶解-再沉积过程进行重构的普遍性

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Abstract

The electrochemical CO(2) reduction (ECO(2)R) on copper (Cu) remains one of the most promising pathways to convert CO(2) into value-added products. However, it suffers from severe restructuring, resulting in the unknown structural identity of the ECO(2)R active catalyst. Here, we show that dissolution-redeposition is the universal early-stage restructuring mechanism in ECO(2)R, occurring across all the tested Cu morphologies, including foils, nanoparticles, oxide-derived films, and gas diffusion electrodes. Using identical location scanning electron microscopy, we directly visualize and confirm that this transformation begins at the reaction onset, reshaping catalyst morphology and complicating structure-activity interpretations. Our findings demonstrate that all the Cu catalysts act as precursors to their true, in situ-formed active phase, generated through the reduction of Cu oxides and electrolyte-driven dissolution-redeposition. Recognizing the universality of this transformation is essential for accurate mechanistic understanding and the rational design of future Cu-based ECO(2)R catalysts.

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