Journal
ADVANCED MATERIALS
Volume 31, Issue 41, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201902509
Keywords
metal-oxygen covalency; oxygen evolution reaction; spinel oxides; surface reconstruction; surface site density
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Funding
- Singapore Ministry of Education Tier 1Grant [RG3/18 (S)]
- Singapore Ministry of Education Tier 2 Grants [MOE2018-T2-2-027]
- National Research Foundation, Prime Minister's Office, Singapore under its Campus of Research Excellence and Technological Enterprise (CREATE) program
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The clean energy carrier, hydrogen, if efficiently produced by water electrolysis using renewable energy input, would revolutionize the energy landscape. It is the sluggish oxygen evolution reaction (OER) at the anode of water electrolyzer that limits the overall efficiency. The large spinel oxide family is widely studied due to their low cost and promising OER activity. As the distribution of transition metal (TM) cations in octahedral and tetrahedral site is an important variable controlling the electronic structure of spinel oxides, the TM geometric effect on OER is discussed. The dominant role of octahedral sites is found experimentally and explained by computational studies. The redox-active TM locating at octahedral site guarantees an effective interaction with the oxygen at OER conditions. In addition, the adjacent octahedral centers in spinel act cooperatively in promoting the fast OER kinetics. In remarkable contrast, the isolated tetrahedral TM centers in spinel prohibit the OER mediated by dual-metal sites. Furthermore, various spinel oxides preferentially expose octahedral-occupied cations on the surface, making the octahedral cations easily accessible to the reactants. The future perspectives and challenges in advancing fundamental understanding and developing robust spinel catalysts are discussed.
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