期刊
NATURE CHEMISTRY
卷 10, 期 2, 页码 149-154出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.2886
关键词
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资金
- Ontario Research Fund Research Excellence Program, NSERC
- CIFAR Bio-Inspired Solar Energy programme
- China Scholarship Council (CSC) [20140625004]
- National Basic Research Program of China [2014CB931703]
- STCSM [16JC1400702, 14ZR14110200]
- NSFC [21503079]
- China Scholarship Council/University of Toronto Joint Funding Program [201406745001]
- 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
- Center for Functional Nanomaterials [DE-SC0012704]
- Office of Science of the US DOE [DE-AC02-05CH11231]
The efficiency with which renewable fuels and feedstocks are synthesized from electrical sources is limited at present by the sluggish oxygen evolution reaction (OER) in pH-neutral media. We took the view that generating transition-metal sites with high valence at low applied bias should improve the activity of neutral OER catalysts. Here, using density functional theory, we find that the formation energy of desired Ni4+ sites is systematically modulated by incorporating judicious combinations of Co, Fe and non-metal P. We therefore synthesized NiCoFeP oxyhydroxides and probed their oxidation kinetics with in situ soft X-ray absorption spectroscopy (sXAS). In situ sXAS studies of neutral-pH OER catalysts indicate ready promotion of Ni4+ under low overpotential conditions. The NiCoFeP catalyst outperforms IrO2 and retains its performance following 100 h of operation. We showcase NiCoFeP in a membrane-free CO2 electroreduction system that achieves a 1.99 V cell voltage at 10 mA cm(-2), reducing CO2 into CO and oxidizing H2O to O-2 with a 64% electricity-to-chemical-fuel efficiency.
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