4.8 Article

Homogeneously dispersed multimetal oxygen-evolving catalysts

期刊

SCIENCE
卷 352, 期 6283, 页码 333-337

出版社

AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.aaf1525

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资金

  1. Ontario Research Fund-Research Excellence Program
  2. Natural Sciences and Engineering Research Council of Canada
  3. Canadian Insititute for Advanced Research Bio-Inspired Solar Energy program
  4. China Scholarship Council/University of Toronto [201406745001]
  5. Shanghai Municipal Natural Science Foundation [14ZR1410200]
  6. National Natural Science Foundation of China [21503079]
  7. China Scholarship Council (CSC) [20140625004]
  8. U.S. Department of Energy (DOE), Office of Basic Energy Science
  9. Laboratory-Directed Research and Development program through the SLAC National Accelerator Laboratory
  10. Agency for Administration of University and Research Grants of Catalonia (AGAUR) [2013 BP-A 00464]
  11. Center for Functional Nanomaterials, DOE Office of Science Facility, at Brookhaven National Laboratory [DE-SC0012704]
  12. Fundacao de Amparo a Pesquisa do Estado de Sao Paulo-Bolsa Estagio de Pesquisa no Exterior fellowship [2014/18327-9]
  13. Connaught Global Challenge program of the University of Toronto

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Earth-abundant first-row (3d) transition metal-based catalysts have been developed for the oxygen-evolution reaction (OER); however, they operate at overpotentials substantially above thermodynamic requirements. Density functional theory suggested that non-3d high-valency metals such as tungsten can modulate 3d metal oxides, providing nearoptimal adsorption energies for OER intermediates. We developed a room-temperature synthesis to produce gelled oxyhydroxides materials with an atomically homogeneous metal distribution. These gelled FeCoW oxyhydroxides exhibit the lowest overpotential (191 millivolts) reported at 10 milliamperes per square centimeter in alkaline electrolyte. The catalyst shows no evidence of degradation after more than 500 hours of operation. X-ray absorption and computational studies reveal a synergistic interplay between tungsten, iron, and cobalt in producing a favorable local coordination environment and electronic structure that enhance the energetics for OER.

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