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Tuning the Electron Localization of Gold Enables the Control of Nitrogen‐to‐Ammonia Fixation
Open accessAbstract
The (photo)electrochemical N 2 reduction reaction (NRR) provides a favorable avenue for the production of NH 3 using renewable energy in mild operating conditions. Understanding and building an efficient catalyst with high NH 3 selectivity represents an area of intense interest for the early stages of development for NRR. Herein, we introduce a CoOx layer to tune the local electronic structure of Au nanoparticles with positive valence sites for boosting conversion of N 2 to NH 3. The catalysts, possessing high average oxidation states (ca. 40 %), achieve a high NH 3 yield rate of 15.1 μg cm−2 h−1 and a good faradic efficiency of 19 % at −0.5 V versus reversible hydrogen electrode. Experimental results and simulations reveal that the ability to tune the oxidation state of Au enables the control of N 2 adsorption and the concomitant energy barrier of NRR. Altering the Au oxidation state provides a unique strategy for control of NRR in the production of valuable NH 3.
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Cites
Dopant-induced electron localization drives CO2 reduction to C2 hydrocarbons
Zhou, Y., Che, F., Liu, M., Zou, C., Liang, Z., De Luna, P., Yuan, H., Li, J., Wang, Z., Xie, H., et al. (2018) · Nature Chemistry · doi:10.1038/s41557-018-0092-x · Cited by 1,171
De Luna, P., Quintero-Bermudez, R., Dinh, C.-T., Ross, M. B., Bushuyev, O. S., Todorović, P., Regier, T., Kelley, S. O., Yang, P., & Sargent, E. H. (2018) · Nature Catalysis · doi:10.1038/s41929-017-0018-9 · Cited by 1,046
Cited by
Ren, Y., Yu, C., Tan, X., Huang, H., Wei, Q., & Qiu, J. (2021) · Energy & Environmental Science · doi:10.1039/d0ee03596c · Cited by 565
Comprehensive Understanding of the Thriving Ambient Electrochemical Nitrogen Reduction Reaction
Zhao, X., Hu, G., Chen, G., Zhang, H., Zhang, S., & Wang, H. (2021) · Advanced Materials · doi:10.1002/adma.202007650 · Cited by 503
Bo, Y., Wang, H., Lin, Y., Yang, T., Ye, R., Li, Y., Hu, C., Du, P., Hu, Y., Liu, Z., et al. (2021) · Angewandte Chemie International Edition · doi:10.1002/anie.202104001 · Cited by 355
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Metadata
- Authors
- Zheng, J., Lyu, Y., Qiao, M., Veder, J. P., Marco, R. D., Bradley, J., Wang, R., Li, Y., Huang, A., Jiang, S. P., & Wang, S.
- Venue
- Angewandte Chemie International Edition
- Publisher
- Wiley
- Published
- 2019-11-04
- Volume
- 58
- Issue
- 51
- Pages
- 18604-18609
- ISSN
- 1433-7851 (ISSN-L)
- 1521-3773
- OpenAlex
- W2974866817
- Cited by
- 183
- References
- 2
- FWCI
- 5.85
- Type
- journal article
- Language
- en
- Open access
- bronze
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- Zheng, J., Lyu, Y., Qiao, M., Veder, J. P., Marco, R. D., Bradley, J., Wang, R., Li, Y., Huang, A., Jiang, S. P., & Wang, S. (2019). Tuning the Electron Localization of Gold Enables the Control of Nitrogen‐to‐Ammonia Fixation. Angewandte Chemie International Edition. https://doi.org/10.1002/anie.201909477
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