期刊
CHEMSUSCHEM
卷 10, 期 22, 页码 4479-4490出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201701582
关键词
manganese oxide; reaction mechanisms; solar fuels; water oxidation; water splitting
资金
- Deutsche Forschungsgemeinschaft (DFG) [CRC 1073]
- Natural Sciences and Engineering Research Council of Canada
- National Research Council Canada
- Canadian Institutes of Health Research
- Province of Saskatchewan, Western Economic Diversification Canada
- University of Saskatchewan
Targeted improvement of the low efficiency of water oxidation during the oxygen evolution reaction (OER) is severely hindered by insufficient knowledge of the electrocatalytic mechanism on heterogeneous surfaces. We chose LiMn2O4 as a model system for mechanistic investigations as it shares the cubane structure with the active site of photosystem II and the valence of Mn3.5+ with the dark-stable S1 state in the mechanism of natural photosynthesis. The investigated LiMn2O4 nanoparticles are electrochemically stable in NaOH electrolytes and show respectable activity in any of the main metrics. At low overpotential, the key mechanistic parameters of Tafel slope, Nernst slope, and reaction order have constant values on the RHE scale of 62(1) mVdec(-1), 1(1) mVpH(-1), -0.04(2), respectively. These values are interpreted in the context of the well-studied mechanism of natural photosynthesis. The uncovered difference in the reaction sequence is important for the design of efficient bio-inspired electrocatalysts.
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