Metal Oxide/(oxy)hydroxide Overlayers as Hole Collectors and Oxygen-Evolution Catalysts on Water-Splitting Photoanodes

Laskowski, Forrest A.  L.; Nellist, Michael R.; Qiu, Jingjing; Boettcher, Shannon W.

doi:10.1021/jacs.8b09449

Title: Metal Oxide/(oxy)hydroxide Overlayers as Hole Collectors and Oxygen-Evolution Catalysts on Water-Splitting Photoanodes

Journal Article · Tue Dec 11 00:00:00 EST 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.8b09449· OSTI ID:1599406

Laskowski, Forrest A. L. ^[1]; Nellist, Michael R. ^[1];

^[1];

^[1]

Univ. of Oregon, Eugene, OR (United States)

Solar water splitting provides a mechanism to convert and store solar energy in the form of stable chemical bonds. Water-splitting systems often include semiconductor photoanodes, such as n-Fe₂O₃ and n-BiVO₄, which use photogenerated holes to oxidize water. These photoanodes often exhibit improved performance when coated with metal-oxide/(oxy)hydroxide overlayers that are catalytic for the water-oxidation reaction. The mechanism for this improvement, however, remains a controversial topic. This is, in part, due to a lack of experimental techniques that are able to directly track the flow of photogenerated holes in such multicomponent systems. In this Perspective, we illustrate how this issue can be addressed by using a second working electrode to make direct current/voltage measurements on the catalytic overlayer during operation in a photoelectrochemical cell. Further, we discuss examples where the second working electrode is a thin metallic film deposited on the catalyst layer, as well as where it is the tip of a conducting atomic-force-microscopy probe. In applying these techniques to multiple semiconductors (Fe₂O₃, BiVO₄, Si) paired with various metal-(oxy)hydroxide overlayers (e.g., Ni(Fe)OxHy and CoOxHy), we found in all cases investigated that the overlayers collect photogenerated holes from the semiconductor, charging to potentials sufficient to drive water oxidation. The overlayers studied thus form charge-separating heterojunctions with the semiconductor as well as serve as water-oxidation catalysts.

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Research Organization:: Univ. of Oregon, Eugene OR (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Sloan Foundation; Dreyfus Foundation; M. J. Murdock Charitable Trust; W. M. Keck Foundation; ONAMI

DOE Contract Number:: SC0014279; 1309047

OSTI ID:: 1599406

Journal Information:: Journal of the American Chemical Society, Vol. 141, Issue 4; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

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Title: Metal Oxide/(oxy)hydroxide Overlayers as Hole Collectors and Oxygen-Evolution Catalysts on Water-Splitting Photoanodes

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