期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 117, 期 28, 页码 16187-16192出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.2001529117
关键词
water-splitting catalysis; renewable energy; solar to fuels; electrocatalysis; acid-stable templating
资金
- Solar Photochemistry Program of the Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences of the US Department of Energy [DE-SC0017619]
- Graduate Research Fellowship from the NSF
- Enrico Fermi Fellowship at Argonne National Laboratory (ANL)
- Herchel Smith Graduate Fellowship in the Sciences
- Joseph J. Katz Fellowship at ANL
- Chemical, Biological and Geological Sciences, Basic Energy Sciences, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- NSF [ECS-0335765]
- US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
Earth-abundant oxygen evolution catalysts (OECs) with extended stability in acid can be constructed by embedding active sites within an acid-stable metal-oxide framework. Here, we report sta-ble NiPbOx films that are able to perform oxygen evolution reac-tion (OER) catalysis for extended periods of operation (>20 h) in acidic solutions of pH 2.5; conversely, native NiOx catalyst films dissolve immediately. In situ X-ray absorption spectroscopy and ex situ X-ray photoelectron spectroscopy reveal that PbO2 is un-perturbed after addition of Ni and/or Fe into the lattice, which serves as an acid-stable, conductive framework for embedded OER active centers. The ability to perform OER in acid allows the mechanism of Fe doping on Ni catalysts to be further probed. Catalyst activity with Fe doping of oxidic Ni OEC under acid con-ditions, as compared to neutral or basic conditions, supports the contention that role of Fe3+ in enhancing catalytic activity in Ni oxide catalysts arises from its Lewis acid properties.
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