Recognizing the Universality of Copper Reconstruction Via Dissolution–Redeposition at the Onset of CO <sub>2</sub> Reduction
The electrochemical CO<sub>2</sub> reduction (ECO<sub>2</sub>R) on copper (Cu) remains one of the most promising pathways to convert CO<sub>2</sub> into value-added products. However, it suffers from severe restructuring, resulting in the unknown structural identity of the ECO<sub>2</sub>R active catalyst. Here, we show that dissolution-redeposition is the universal early-stage restructuring mechanism in ECO<sub>2</sub>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, <i>in situ</i>-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<sub>2</sub>R catalysts.
Authors
- Yasmin Bastos Pissolitto (ORCID: https://orcid.org/0000-0002-6412-2088)
- Francisco Trivinho‐Strixino (ORCID: https://orcid.org/0000-0002-0990-0270)
- Ana Rebeka Kamšek (ORCID: https://orcid.org/0009-0008-6247-3256)
- Francisco Ruiz‐Zepeda (ORCID: https://orcid.org/0000-0002-2637-3433)
- Lidija D. Rafailović (ORCID: https://orcid.org/0000-0002-9643-9338)
- Mitja Kostelec
- Marjan Bele (ORCID: https://orcid.org/0000-0001-7746-5672)
- Luka Suhadolnik (ORCID: https://orcid.org/0000-0002-9103-6687)
- Nejc Hodnik (ORCID: https://orcid.org/0000-0002-7113-9769)
- Martin Šala (ORCID: https://orcid.org/0000-0001-7845-860X)
- Wojciech J. Stępniowski (ORCID: https://orcid.org/0000-0002-5251-6901)
- Stefan Popović (ORCID: https://orcid.org/0000-0001-6878-2991)
- Adam Elbataioui (ORCID: https://orcid.org/0009-0009-3882-6098)
- Blaž Tomc
- Mohammed Azeezulla Nazrulla
- Matic Plut
Institutions
- Austrian Academy of Sciences (AT)
- Universidade Federal de São Carlos (BR)
- University of Nova Gorica (SI)
- Military University of Technology in Warsaw (PL)
- Institute of Metals and Technology (SI)
- Erich Schmid Institute of Materials Science (AT)
- Photonic Science (United Kingdom) (GB)
- Division of Materials Science and Engineering (AU)
- Material Sciences (United States) (US)
- Department of Chemistry and Material Sciences (RU)
- National Institute of Chemistry (SI)
Publication Details
- Journal
- The Journal of Physical Chemistry Letters
- Published
- 2025-09-04
- DOI
- https://doi.org/10.1021/acs.jpclett.5c01974
- Citations
- 7
- Primary Topic
- CO2 Reduction Techniques and Catalysts
- Type
- article
- Field-Weighted Citation Impact
- 2.54
Funders
- Fundação de Amparo à Pesquisa do Estado de São Paulo
- Coordenação de Aperfeiçoamento de Pessoal de Nível Superior
- Narodowe Centrum Nauki
- Javna Agencija za Raziskovalno Dejavnost RS
- European Research Council
- H2020 Marie Skłodowska-Curie Actions