期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 21, 页码 8072-8077出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201915803
关键词
active sites; electrocatalysis; nickel iron oxyhydroxide; oxygen evolution reaction; Raman spectroscopy
资金
- European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie Grant [838367]
- ERC [681292]
- Marie Curie Actions (MSCA) [838367] Funding Source: Marie Curie Actions (MSCA)
- European Research Council (ERC) [681292] Funding Source: European Research Council (ERC)
Nickel iron oxyhydroxide is the benchmark catalyst for the oxygen evolution reaction (OER) in alkaline medium. Whereas the presence of Fe ions is essential to the high activity, the functions of Fe are currently under debate. Using oxygen isotope labeling and operando Raman spectroscopic experiments, we obtain turnover frequencies (TOFs) of both Ni and Fe sites for a series of Ni and NiFe layered double hydroxides (LDHs), which are structurally defined samples of the corresponding oxyhydroxides. The Fe sites have TOFs 20200 times higher than the Ni sites such that at an Fe content of 4.7% and above the Fe sites dominate the catalysis. Higher Fe contents lead to larger structural disorder of the NiOOH host. A volcano-type correlation was found between the TOFs of Fe sites and the structural disorder of NiOOH. Our work elucidates the origin of the Fe-dependent activity of NiFe LDH, and suggests structural ordering as a strategy to improve OER catalysts.
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