Multiscale X-ray scattering elucidates activation and deactivation of oxide-derived copper electrocatalysts for CO2 reduction
Abstract Electrochemical reduction of carbon dioxide (CO2) into sustainable fuels and base chemicals requires precise control over and understanding of activity, selectivity and stability descriptors of the electrocatalyst under operation. Identification of the active phase under working conditions,...
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-55742-5 |
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| author | J. de Ruiter V. R. M. Benning S. Yang B. J. den Hartigh H. Wang P. T. Prins J. M. Dorresteijn J. C. L. Janssens G. Manna A. V. Petukhov B. M. Weckhuysen F. T. Rabouw W. van der Stam |
| author_facet | J. de Ruiter V. R. M. Benning S. Yang B. J. den Hartigh H. Wang P. T. Prins J. M. Dorresteijn J. C. L. Janssens G. Manna A. V. Petukhov B. M. Weckhuysen F. T. Rabouw W. van der Stam |
| author_sort | J. de Ruiter |
| collection | DOAJ |
| description | Abstract Electrochemical reduction of carbon dioxide (CO2) into sustainable fuels and base chemicals requires precise control over and understanding of activity, selectivity and stability descriptors of the electrocatalyst under operation. Identification of the active phase under working conditions, but also deactivation factors after prolonged operation, are of the utmost importance to further improve electrocatalysts for electrochemical CO2 conversion. Here, we present a multiscale in situ investigation of activation and deactivation pathways of oxide-derived copper electrocatalysts under CO2 reduction conditions. Using well-defined Cu2O octahedra and cubes, in situ X-ray scattering experiments track morphological changes at small scattering angles and phase transformations at wide angles, with millisecond to second time resolution and ensemble-scale statistics. We find that undercoordinated active sites promote CO2 reduction products directly after Cu2O to Cu activation, whereas less active planar surface sites evolve over time. These multiscale insights highlight the dynamic and intimate relationship between electrocatalyst structure, surface-adsorbed molecules, and catalytic performance, and our in situ X-ray scattering methodology serves as an additional tool to elucidate the factors that govern electrocatalyst (de)stabilization. |
| format | Article |
| id | doaj-art-e2dceaec67eb41d18fadbb3818718dc1 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-e2dceaec67eb41d18fadbb3818718dc12025-01-05T12:39:23ZengNature PortfolioNature Communications2041-17232025-01-0116111110.1038/s41467-024-55742-5Multiscale X-ray scattering elucidates activation and deactivation of oxide-derived copper electrocatalysts for CO2 reductionJ. de Ruiter0V. R. M. Benning1S. Yang2B. J. den Hartigh3H. Wang4P. T. Prins5J. M. Dorresteijn6J. C. L. Janssens7G. Manna8A. V. Petukhov9B. M. Weckhuysen10F. T. Rabouw11W. van der Stam12Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Faculty of Science, Utrecht UniversitySoft Condensed Matter, Debye Institute for Nanomaterials Science, Faculty of Science, Utrecht UniversityInorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Faculty of Science, Utrecht UniversityInorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Faculty of Science, Utrecht UniversityInorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Faculty of Science, Utrecht UniversityInorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Faculty of Science, Utrecht UniversityInorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Faculty of Science, Utrecht UniversityInorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Faculty of Science, Utrecht UniversityThe European Synchrotron (ESRF)Physical and Colloid Chemistry group, Debye Institute for Nanomaterials Science, Faculty of Science, Utrecht UniversityInorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Faculty of Science, Utrecht UniversityInorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Faculty of Science, Utrecht UniversityInorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science and Institute for Sustainable and Circular Chemistry, Faculty of Science, Utrecht UniversityAbstract Electrochemical reduction of carbon dioxide (CO2) into sustainable fuels and base chemicals requires precise control over and understanding of activity, selectivity and stability descriptors of the electrocatalyst under operation. Identification of the active phase under working conditions, but also deactivation factors after prolonged operation, are of the utmost importance to further improve electrocatalysts for electrochemical CO2 conversion. Here, we present a multiscale in situ investigation of activation and deactivation pathways of oxide-derived copper electrocatalysts under CO2 reduction conditions. Using well-defined Cu2O octahedra and cubes, in situ X-ray scattering experiments track morphological changes at small scattering angles and phase transformations at wide angles, with millisecond to second time resolution and ensemble-scale statistics. We find that undercoordinated active sites promote CO2 reduction products directly after Cu2O to Cu activation, whereas less active planar surface sites evolve over time. These multiscale insights highlight the dynamic and intimate relationship between electrocatalyst structure, surface-adsorbed molecules, and catalytic performance, and our in situ X-ray scattering methodology serves as an additional tool to elucidate the factors that govern electrocatalyst (de)stabilization.https://doi.org/10.1038/s41467-024-55742-5 |
| spellingShingle | J. de Ruiter V. R. M. Benning S. Yang B. J. den Hartigh H. Wang P. T. Prins J. M. Dorresteijn J. C. L. Janssens G. Manna A. V. Petukhov B. M. Weckhuysen F. T. Rabouw W. van der Stam Multiscale X-ray scattering elucidates activation and deactivation of oxide-derived copper electrocatalysts for CO2 reduction Nature Communications |
| title | Multiscale X-ray scattering elucidates activation and deactivation of oxide-derived copper electrocatalysts for CO2 reduction |
| title_full | Multiscale X-ray scattering elucidates activation and deactivation of oxide-derived copper electrocatalysts for CO2 reduction |
| title_fullStr | Multiscale X-ray scattering elucidates activation and deactivation of oxide-derived copper electrocatalysts for CO2 reduction |
| title_full_unstemmed | Multiscale X-ray scattering elucidates activation and deactivation of oxide-derived copper electrocatalysts for CO2 reduction |
| title_short | Multiscale X-ray scattering elucidates activation and deactivation of oxide-derived copper electrocatalysts for CO2 reduction |
| title_sort | multiscale x ray scattering elucidates activation and deactivation of oxide derived copper electrocatalysts for co2 reduction |
| url | https://doi.org/10.1038/s41467-024-55742-5 |
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