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ZIF‐Induced d‐Band Modification in a Bimetallic Nanocatalyst: Achieving Over 44 % Efficiency in the Ambient Nitrogen Reduction Reaction
Abstract
The electrochemical nitrogen reduction reaction (NRR) offers a sustainable solution towards ammonia production but suffers poor reaction performance owing to preferential catalyst–H formation and the consequential hydrogen evolution reaction (HER). Now, the Pt/Au electrocatalyst d‐band structure is electronically modified using zeolitic imidazole framework (ZIF) to achieve a Faradaic efficiency (FE) of >44 % with high ammonia yield rate of >161 μg mg cat−1 h−1 under ambient conditions. The strategy lowers electrocatalyst d‐band position to weaken H adsorption and concurrently creates electron‐deficient sites to kinetically drive NRR by promoting catalyst–N 2 interaction. The ZIF coating on the electrocatalyst doubles as a hydrophobic layer to suppress HER, further improving FE by >44‐fold compared to without ZIF (ca. 1 %). The Pt/Au‐N ZIF interaction is key to enable strong N 2 adsorption over H atom.
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Heteroatom-doped transition metal electrocatalysts for hydrogen evolution reaction
Jin, H., Liu, X., Chen, S., Vasileff, A., Li, L., Jiao, Y., Song, L., Zheng, Y., & Qiao, S.-Z. (2019) · ACS Energy Letters · doi:10.1021/acsenergylett.9b00348 · Cited by 469
Cited by
Descriptors for the Evaluation of Electrocatalytic Reactions: d‐Band Theory and Beyond
Jiao, S., Fu, X., & Huang, H. (2022) · Advanced Functional Materials · doi:10.1002/adfm.202107651 · Cited by 719
Ren, Y., Yu, C., Tan, X., Huang, H., Wei, Q., & Qiu, J. (2021) · Energy & Environmental Science · doi:10.1039/d0ee03596c · Cited by 565
Bioinspired Framework Catalysts: From Enzyme Immobilization to Biomimetic Catalysis
Wang, K.-Y., Zhang, J., Hsu, Y.-C., Lin, H., Han, Z., Pang, J., Yang, Z., Liang, R.-R., Shi, W., & Zhou, H.-C. (2023) · Chemical Reviews · doi:10.1021/acs.chemrev.2c00879 · Cited by 490
Self-citationDong, K., Liang, J., Wang, Y., Xu, Z., Liu, Q., Luo, Y., Li, T., Li, L., Shi, X., Asiri, A. M., et al. (2021) · Angewandte Chemie International Edition · doi:10.1002/anie.202101880 · Cited by 339
Wang, J., Yuan, L., Zhang, P., Mao, J., Fan, J., & Zhang, X. L. (2024) · Nanoscale · doi:10.1039/d3nr06411e · Cited by 21
Metadata
- Authors
- Sim, H. Y. F., Chen, J. R. T., Koh, C. S. L., Lee, H. K., Han, X., Phan‐Quang, G. C., Pang, J. Y., Lay, C. L., Pedireddy, S., Phang, I. Y., Yeow, E. K. L., & Ling, X. Y.
- Venue
- Angewandte Chemie International Edition
- Publisher
- Wiley
- Published
- 2020-07-27
- Volume
- 59
- Issue
- 39
- Pages
- 16997-17003
- ISSN
- 1433-7851 (ISSN-L)
- 1521-3773
- OpenAlex
- W3029551610
- Cited by
- 182
- References
- 1
- FWCI
- 5.57
- Type
- journal article
- Language
- en
- Open access
- closed
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- Sim, H. Y. F., Chen, J. R. T., Koh, C. S. L., Lee, H. K., Han, X., Phan‐Quang, G. C., Pang, J. Y., Lay, C. L., Pedireddy, S., Phang, I. Y., Yeow, E. K. L., & Ling, X. Y. (2020). ZIF‐Induced d‐Band Modification in a Bimetallic Nanocatalyst: Achieving Over 44 % Efficiency in the Ambient Nitrogen Reduction Reaction. Angewandte Chemie International Edition. https://doi.org/10.1002/anie.202006071
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