期刊
NATURE CHEMISTRY
卷 9, 期 5, 页码 457-465出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.2695
关键词
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资金
- Skoltech-MIT Center for Electrochemical Energy
- SMART programme
- Department of Energy (DOE)
- National Energy Technology Laboratory (NETL), Solid State Energy Conversion Alliance (SECA) Core Technology Program [DEFE0009435]
- Netherlands Organization for Scientific Research (NWO) within the research programme of BioSolar Cells - Dutch Ministry of Economic Affairs, Agriculture and Innovation
- Office of Science of the US Department of Energy [DE-AC02-05CH11231]
Understanding how materials that catalyse the oxygen evolution reaction (OER) function is essential for the development of efficient energy-storage technologies. The traditional understanding of the OER mechanism on metal oxides involves four concerted proton-electron transfer steps on metal-ion centres at their surface and product oxygen molecules derived from water. Here, using in situ O-18 isotope labelling mass spectrometry, we provide direct experimental evidence that the O-2 generated during the OER on some highly active oxides can come from lattice oxygen. The oxides capable of lattice-oxygen oxidation also exhibit pH-dependent OER activity on the reversible hydrogen electrode scale, indicating non-concerted proton-electron transfers in the OER mechanism. Based on our experimental data and density functional theory calculations, we discuss mechanisms that are fundamentally different from the conventional scheme and show that increasing the covalency of metal-oxygen bonds is critical to trigger lattice-oxygen oxidation and enable non-concerted proton-electron transfers during OER.
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