期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 29, 页码 15821-15826出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202104123
关键词
electrochemistry; electronic structure; heterogeneous catalysis; hydrogen; kinetics
资金
- Australian Renewable Energy Agency (ARENA) [2018/RND008]
- Australian Research Council (Centre of Excellence for Electromaterials Science) [CE140100012]
- Australian Research Council [FT200100317, FT200100939, DP190101864]
- Russell and Jenny Tait Postgraduate Research Scholarship
- Australian Research Council [FT200100939] Funding Source: Australian Research Council
The study demonstrates the stable operation of [Co-Fe-Pb]O-x in acidic solutions without the addition of Pb2+ and Fe3+, showcasing promising performance in water electrooxidation. Low concentrations of Co2+ are shown to stabilize the catalytically active Co(Fe) sites, allowing for steady water electrooxidation at specific conditions.
The instability and expense of anodes for water electrolyzers with acidic electrolytes can be overcome through the implementation of a cobalt-iron-lead oxide electrocatalyst, [Co-Fe-Pb]O-x, that is self-healing in the presence of dissolved metal precursors. However, the latter requirement is pernicious for the membrane and especially the cathode half-reaction since Pb2+ and Fe3+ precursors poison the state-of-the-art platinum H-2 evolving catalyst. To address this, we demonstrate the invariably stable operation of [Co-Fe-Pb]O-x in acidic solutions through a cobalt-selective self-healing mechanism without the addition of Pb2+ and Fe3+ and investigate the kinetics of the process. Soft X-ray absorption spectroscopy reveals that low concentrations of Co2+ in the solution stabilize the catalytically active Co(Fe) sites. The highly promising performance of this system is showcased by steady water electrooxidation at 80 +/- 1 degrees C and 10 mA cm(-2), using a flat electrode, at an overpotential of 0.56 +/- 0.01 V on a one-week timescale.
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