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Electrocatalytic Nitrate and Nitrite Reduction toward Ammonia Using Cu2O Nanocubes: Active Species and Reaction Mechanisms
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High Resolution Image Download MS PowerPoint Slide The electrochemical reduction of nitrate (NO 3 – ) and nitrite (NO 2 – ) enables sustainable, carbon-neutral, and decentralized routes to produce ammonia (NH 3 ). Copper-based materials are promising electrocatalysts for NO x – conversion to NH 3 . However, the underlying reaction mechanisms and the role of different Cu species during the catalytic process are still poorly understood. Herein, by combining quasi in situ X-ray photoelectron spectroscopy (XPS) and operando X-ray absorption spectroscopy (XAS), we unveiled that Cu is mostly in metallic form during the highly selective reduction of NO 3 – /NO 2 – to NH 3 . On the contrary, Cu(I) species are predominant in a potential region where the two-electron reduction of NO 3 – to NO 2 – is the major reaction. Electrokinetic analysis and in situ Raman spectroscopy was also used to propose possible steps and intermediates leading to NO 2 – and NH 3, respectively. This work establishes a correlation between the catalytic performance and the dynamic changes of the chemical state of Cu, and provides crucial mechanistic insights into the pathways for NO 3 – /NO 2 – electrocatalytic reduction.
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Cited by
Phu, T. K. C., Hong, W. T., Han, H., Song, Y. I., Kim, J. H., Roh, S. H., Kim, M.-C., Koh, J. H., Oh, B.-K., Kim, J. Y., et al. (2024) · Materials Today · doi:10.1016/j.mattod.2024.05.007 · Cited by 22
Metadata
- Authors
- Bai, L., Franco, F., Timoshenko, J., Rettenmaier, C., Scholten, F., Jeon, H. S., Yoon, A., Rüscher, M., Herzog, A., Haase, F. T., Kühl, S., Chee, S. W., Bergmann, A., & Beatriz, R. C.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2024-04-01
- Volume
- 146
- Issue
- 14
- Pages
- 9665-9678
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W4393374969
- Cited by
- 473
- References
- 53
- FWCI
- 30.59
- Type
- journal article
- Language
- en
- Open access
- hybrid
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