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Tuning the Catalytic Preference of Ruthenium Catalysts for Nitrogen Reduction by Atomic Dispersion
Abstract
Developing cost‐effective, high‐performance nitrogen reduction reaction (NRR) electrocatalysts is required for the production of green and low‐cost ammonia under ambient conditions. Here, a strategy is proposed to adjust the reaction preference of noble metals by tuning the size and local chemical environment of the active sites. This proof‐of‐concept model is realized by single ruthenium atoms distributed in a matrix of graphitic carbon nitride (Ru SAs/g‐C 3 N 4). This model is compared, in terms of the NRR activity, to bulk Ru. The as‐synthesized Ru SAs/g‐C 3 N 4 exhibits excellent catalytic activity and selectivity with an NH 3 yield rate of 23.0 µg mg cat−1 h−1 and a Faradaic efficiency as high as 8.3% at a low overpotential (0.05 V vs the reversible hydrogen electrode), which is far better than that of the bulk Ru counterpart. Moreover, the Ru SAs/g‐C 3 N 4 displays a high stability during five recycling tests and a 12 h potentiostatic test. Density functional theory calculations reveal that compared to bulk Ru surfaces, Ru SAs/g‐C 3 N 4 has more facile reaction thermodynamics, and the enhanced NRR performance of Ru SAs/g‐C 3 N 4 originates from a tuning of the d‐electron energies from that of the bulk to a single‐atom, causing an up‐shift of the d‐band center toward the Fermi level.
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Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode
Nørskov, J. K., Rossmeisl, J., Logadottir, A., Lindqvist, L., Kitchin, J. R., Bligaard, T., & Jónsson, H. (2004) · The Journal of Physical Chemistry B · doi:10.1021/jp047349j · Cited by 13,153
Metal-free efficient photocatalyst for stable visible water splitting via a two-electron pathway
Liu, J., Liu, Y., Liu, N., Han, Y., Zhang, X., Huang, H., Lifshitz, Y., Lee, S.-T., Zhong, J., & Kang, Z. (2015) · Science · doi:10.1126/science.aaa3145 · Cited by 4,468
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Single-Atom Catalysts across the Periodic Table
Kaiser, S. K., Chen, Z., Faust Akl, D., Mitchell, S., & Pérez-Ramírez, J. (2020) · Chemical Reviews · doi:10.1021/acs.chemrev.0c00576 · Cited by 1,367
Self-citationDescriptors 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
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
Synthesis Strategies, Catalytic Applications, and Performance Regulation of Single‐Atom Catalysts
Xi, J., Jung, H. S., Xu, Y., Xiao, F., Bae, J. W., & Wang, S. (2021) · Advanced Functional Materials · doi:10.1002/adfm.202008318 · Cited by 282
Metadata
- Authors
- Yu, B., Li, H., White, J., Donne, S., Yi, J., Xi, S., Fu, Y., Henkelman, G., Yu, H., Chen, Z., & Ma, T.
- Venue
- Advanced Functional Materials
- Publisher
- Wiley
- Published
- 2019-11-12
- Volume
- 30
- Issue
- 6
- ISSN
- 1616-301X (ISSN-L)
- 1616-3028
- OpenAlex
- W2985655614
- Cited by
- 232
- References
- 2
- FWCI
- 6.92
- Type
- journal article
- Language
- en
- Open access
- closed
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- Yu, B., Li, H., White, J., Donne, S., Yi, J., Xi, S., Fu, Y., Henkelman, G., Yu, H., Chen, Z., & Ma, T. (2020). Tuning the Catalytic Preference of Ruthenium Catalysts for Nitrogen Reduction by Atomic Dispersion. Advanced Functional Materials. https://doi.org/10.1002/adfm.201905665
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