Blaž Tomc*, Marjan Bele*, Matic Plut, Mitja Kostelec, Stefan Popović, Mohammed Azeezulla Nazrulla, Francisco Ruiz-Zepeda, Ana Rebeka Kamšek, Martin Šala, Adam Elbataioui, Lidija D. Rafailović, Yasmin Bastos Pissolitto, Francisco Trivinho-Strixino, Wojciech Jerzy Stępniowski, Luka Suhadolnik and Nejc Hodnik*,
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Recognizing the Universality of Copper Reconstruction Via Dissolution–Redeposition at the Onset of CO2 Reduction
The electrochemical CO2 reduction (ECO2R) on copper (Cu) remains one of the most promising pathways to convert CO2 into value-added products. However, it suffers from severe restructuring, resulting in the unknown structural identity of the ECO2R active catalyst. Here, we show that dissolution–redeposition is the universal early-stage restructuring mechanism in ECO2R, 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 ECO2R catalysts.
期刊介绍:
The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.