期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 138, 期 31, 页码 9978-9985出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b05398
关键词
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资金
- Nanyang Technological University [M4080977.120]
- Singapore Ministry of Education Academic Research Fund (AcRF) [RG111/15]
- Agency for Science, Technology and Research of Singapore (A*Star) [M4070232.120]
- National Research Foundation (NRF), Prime Minister's Office, Singapore under its Campus for Research Excellence and Technological Enterprise (CREATE) program
- Ministry of Science and Technology of China under the National Basic Research Program [2012CB932800]
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 (M-CUS), as a good surface reactivity descriptor for TMOs in OER. Surface reactivity of a given TMO increases monotonically with the density of M-CUS, and thus the increase in M-CUS 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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