The DOI matches its Crossref record; 72 of the 72 references it cites were found in a registry or an index.
Dynamic Reoxidation/Reduction-Driven Atomic Interdiffusion for Highly Selective CO2 Reduction toward Methane
Abstract
Understanding the dynamic structural reconstruction/transformation of catalysts during electrochemical CO 2 reduction reaction (CO 2 RR) is highly desired for developing more efficient and selective catalysts, yet still lacks in-depth realization. Herein, we study a model system of copper nanowires with various degrees of silver modifications as electrocatalysts for CO 2 RR. Among them, the Cu 68 Ag 32 nanowire catalyst achieves the highest activity and selectivity toward methane with an extremely high faradaic efficiency of ∼60%, about 3 times higher than that of primitive Cu nanowires, and even surpasses the most efficient catalysts for producing methane. By using in situ grazing-angle X-ray scattering/diffraction, X-ray absorption spectroscopy, and Raman techniques, we found that the Cu 68 Ag 32 nanowires underwent an irreversible structural reconstruction and well-stabilized chemical state of Cu on the catalyst surface under the working CO 2 RR conditions, which greatly facilitates the CO 2 to methane conversion. Further analysis reveals that the restructuring phenomenon can be ascribed to a reoxidation/reduction-driven atomic interdiffusion between Cu and Ag. This work reveals the first empirical demonstration by deploying comprehensive in situ techniques to track the dynamic structural reconstruction/transformation in a model bimetallic system, which not only establishes a good understanding of the correlation between catalyst surface structure and catalytic selectivity but also provides deep insights into designing more developed electrocatalysts for CO 2 RR and beyond.
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Cites
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Cited by
Operando studies reveal active Cu nanograins for CO2 electroreduction
Yang, Y., Louisia, S., Yu, S., Jin, J., Roh, I., Chen, C., Fonseca Guzman, M. V., Feijóo, J., Chen, P.-C., Wang, H., et al. (2023) · Nature · doi:10.1038/s41586-022-05540-0 · Cited by 830
Atomic Metal–Support Interaction Enables Reconstruction-Free Dual-Site Electrocatalyst
Sun, H., Tung, C.-W., Qiu, Y., Zhang, W., Wang, Q., Li, Z., Tang, J., Chen, H.-C., Wang, C., & Chen, H. M. (2022) · Journal of the American Chemical Society · doi:10.1021/jacs.1c08890 · Cited by 369
Self-citationWang, J., Tan, H., Zhu, Y., Chu, H., & Chen, H. M. (2021) · Angewandte Chemie International Edition · doi:10.1002/anie.202017181 · Cited by 322
Self-citationZhu, Y., Kuo, T.-R., Li, Y.-H., Qi, M.-Y., Chen, G., Wang, J., Xu, Y.-J., & Chen, H. M. (2021) · Energy & Environmental Science · doi:10.1039/d0ee03903a · Cited by 308
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Metadata
- Authors
- Chang, C.-J., Lin, S.-C., Chen, H.-C., Wang, J., Zheng, K. J., Zhu, Y., & Chen, H. M.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2020-06-19
- Volume
- 142
- Issue
- 28
- Pages
- 12119-12132
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W3036499806
- Cited by
- 323
- References
- 72
- FWCI
- 9.15
- Type
- journal article
- Language
- en
- Open access
- closed
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- Chang, C.-J., Lin, S.-C., Chen, H.-C., Wang, J., Zheng, K. J., Zhu, Y., & Chen, H. M. (2020). Dynamic Reoxidation/Reduction-Driven Atomic Interdiffusion for Highly Selective CO2 Reduction toward Methane. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.0c01859
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