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Identification of Surface Reactivity Descriptor for Transition Metal Oxides in Oxygen Evolution Reaction
Abstract
A number of important reactions such as the oxygen evolution reaction (OER) are catalyzed by transition metal oxides (TMOs), the surface reactivity of which is rather elusive. Therefore, rationally tailoring adsorption energy of intermediates on TMOs to achieve desirable catalytic performance still remains a great challenge. Here we show the identification of a general and tunable surface structure, coordinatively unsaturated metal cation (MCUS), as a good surface reactivity descriptor for TMOs in OER. Surface reactivity of a given TMO increases monotonically with the density of MCUS, and thus the increase in MCUS improves the catalytic activity for weak-binding TMOs but impairs that for strong-binding ones. The electronic origin of the surface reactivity can be well explained by a new model proposed in this work, wherein the energy of the highest-occupied d-states relative to the Fermi level determines the intermediates' bonding strength by affecting the filling of the antibonding states. Our model for the first time well describes the reactivity trends among TMOs, and would initiate viable design principles for, but not limited to, OER catalysts.
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Cites
Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces
Man, I. C., Su, H., Calle‐Vallejo, F., Hansen, H. A., Martínez, J. I., Inoglu, N. G., Kitchin, J., Jaramillo, T. F., Nørskov, J. K., & Rossmeisl, J. (2011) · ChemCatChem · doi:10.1002/cctc.201000397 · Cited by 4,769
Trends in electrocatalysis on extended and nanoscale Pt-bimetallic alloy surfaces
Stamenkovic, V. R., Mun, B. S., Arenz, M., Mayrhofer, K. J. J., Lucas, C. A., Wang, G., Ross, P. N., & Markovic, N. M. (2007) · Nature Materials · doi:10.1038/nmat1840 · Cited by 3,252
Alloys of platinum and early transition metals as oxygen reduction electrocatalysts
Greeley, J., Stephens, I. E. L., Bondarenko, A. S., Johansson, T. P., Hansen, H. A., Jaramillo, T. F., Rossmeisl, J., Chorkendorff, I., & Nørskov, J. K. (2009) · Nature Chemistry · doi:10.1038/nchem.367 · Cited by 3,203
Toward the rational design of non-precious transition metal oxides for oxygen electrocatalysis
Hong, W. T., Risch, M., Stoerzinger, K. A., Grimaud, A., Suntivich, J., & Shao-Horn, Y. (2015) · Energy & Environmental Science · doi:10.1039/c4ee03869j · Cited by 2,089
Cited by
A review on fundamentals for designing oxygen evolution electrocatalysts
Song, J., Wei, C., Huang, Z.-F., Liu, C., Zeng, L., Wang, X., & Xu, Z. J. (2020) · Chemical Society Reviews · doi:10.1039/c9cs00607a · Cited by 2,936
Chatenet, M., Pollet, B. G., Dekel, D. R., Dionigi, F., Deseure, J., Millet, P., Braatz, R. D., Bazant, M. Z., Eikerling, M., Staffell, I., et al. (2022) · Chemical Society Reviews · doi:10.1039/d0cs01079k · Cited by 2,025
Xiao, Z., Huang, Y.-C., Dong, C.-L., Xie, C., Liu, Z., Du, S., Chen, W., Yan, D., Tao, L., Shu, Z., et al. (2020) · Journal of the American Chemical Society · doi:10.1021/jacs.0c00257 · Cited by 1,445
Recent Progress on Multimetal Oxide Catalysts for the Oxygen Evolution Reaction
Kim, J. S., Kim, B., Kim, H., & Kang, K. (2018) · Advanced Energy Materials · doi:10.1002/aenm.201702774 · Cited by 940
Li, P., Wang, M., Duan, X., Zheng, L., Cheng, X., Zhang, Y., Kuang, Y., Li, Y., Ma, Q., Feng, Z., et al. (2019) · Nature Communications · doi:10.1038/s41467-019-09666-0 · Cited by 717
Metadata
- Authors
- Tao, H. B., Fang, L., Chen, J., Yang, H. B., Gao, J., Miao, J., Chen, S., & Liu, B.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2016-08-01
- Volume
- 138
- Issue
- 31
- Pages
- 9978-9985
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2478937906
- Cited by
- 468
- References
- 4
- FWCI
- 7.60
- Type
- journal article
- Language
- en
- Open access
- closed
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- Tao, H. B., Fang, L., Chen, J., Yang, H. B., Gao, J., Miao, J., Chen, S., & Liu, B. (2016). Identification of Surface Reactivity Descriptor for Transition Metal Oxides in Oxygen Evolution Reaction. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.6b05398
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