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Doping strain induced bi-Ti3+ pairs for efficient N2 activation and electrocatalytic fixation
Open accessAbstract
The electrochemical N 2 fixation to produce ammonia is attractive but significantly challenging with low yield and poor selectivity. Herein, we first used density function theory calculations to reveal adjacent bi-Ti 3+ pairs formed on anatase TiO 2 as the most active electrocatalytic centers for efficient N 2 lying-down chemisorption and activation. Then, by doping of anatase TiO 2 with Zr 4+ that has similar d-electron configuration and oxide structure but relatively larger ionic size, the adjacent bi-Ti 3+ sites were induced and enriched via a strained effect, which in turn enhanced the formation of oxygen vacancies. The Zr 4+-doped anatase TiO 2 exhibited excellent electrocatalytic N 2 fixation performances, with an ammonia production rate (8.90 µg·h−1·cm−2) and a Faradaic efficiency of 17.3% at −0.45 V versus reversible hydrogen electrode under ambient aqueous conditions. Moreover, our work suggests a viewpoint to understand and apply the same-valance dopants in heterogeneous catalysis, which is generally useful but still poorly understood.
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Cites
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Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode
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Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces
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How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels
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Cited by
Guo, X., Gu, J., Lin, S., Zhang, S., Chen, Z., & Huang, S. (2020) · Journal of the American Chemical Society · doi:10.1021/jacs.9b13349 · Cited by 1,151
Self-citationRen, 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
Greatly Improving Electrochemical N 2 Reduction over TiO 2 Nanoparticles by Iron Doping
Wu, T., Zhu, X., Xing, Z., Mou, S., Li, C., Qiao, Y., Liu, Q., Luo, Y., Shi, X., Zhang, Y., et al. (2019) · Angewandte Chemie International Edition · doi:10.1002/anie.201911153 · Cited by 499
Density Functional Theory for Electrocatalysis
Liao, X., Lu, R., Xia, L., Liu, Q., Wang, H., Zhao, K., Wang, Z., & Zhao, Y. (2022) · ENERGY & ENVIRONMENTAL MATERIALS · doi:10.1002/eem2.12204 · Cited by 420
Metadata
- Authors
- Cao, N., Chen, Z., Zang, K., Xu, J., Zhong, J., Luo, J., Xu, X., & Zheng, G.
- Venue
- Nature Communications
- Published
- 2019-06-28
- Volume
- 10
- Issue
- 1
- Pages
- 2877-2877
- ISSN
- 2041-1723 (ISSN-L)
- OpenAlex
- W2953589763
- Cited by
- 374
- References
- 6
- FWCI
- 11.45
- Type
- journal article
- Language
- en
- Open access
- gold
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- Cao, N., Chen, Z., Zang, K., Xu, J., Zhong, J., Luo, J., Xu, X., & Zheng, G. (2019). Doping strain induced bi-Ti3+ pairs for efficient N2 activation and electrocatalytic fixation. Nature Communications. https://doi.org/10.1038/s41467-019-10888-5
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