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Surveying Metal Antimonate Photoanodes for Solar Fuel Generation

Zhou, Lan and Wang, Yu and Kan, Kevin and Lucana, Daphne M. and Guevarra, Dan and Lai, Yungchieh and Gregoire, John M. (2022) Surveying Metal Antimonate Photoanodes for Solar Fuel Generation. ACS Sustainable Chemistry & Engineering, 10 (48). pp. 15898-15908. ISSN 2168-0485. doi:10.1021/acssuschemeng.2c05239.

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Ternary antimonate (X-Sb-O) materials are surveyed as photoanodes aimed at solar-driven evolution of dioxygen from water to enable solar generation of fuels and chemicals. Exploring this class of materials is motivated by their recent proliferation as operationally stable electrochemical materials as well as the prior demonstration of X-Sb-O photocatalysts. The survey was conducted via combinatorial materials science methods with a high throughput workflow including parallel synthesis via cosputter deposition and annealing, combinatorial characterization via X-ray diffraction and fluorescence, and automated photoelectrochemistry using a scanning droplet cell. The resulting 5608 measurements of external quantum efficiency span X-Sb-O composition systems with 14 different elements (X = Mg, Al, Cr, Fe, Co, Ni, Cu, Zn, Y, Ag, In, La, Pb, Bi) as well as a variation in annealing temperature, electrolyte pH, and illumination sources ranging from 2.1 to 3.2 eV. Automated analysis of the resulting wealth of data enabled the discovery of 19 photoanode phases, including 9 with broad spectral response. The discoveries include transition metal antimonates, metal oxides comprising only main group elements, and amorphous photoanodes. The general Pourbaix stability of the ternary antimonates creates opportunities for continued development of operationally stable photoanodes, and the lack of open d-orbital character at the band edges of the main group oxides makes them particularly compelling for future study.

Item Type:Article
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URLURL TypeDescription
Zhou, Lan0000-0002-7052-266X
Wang, Yu0000-0003-3589-9274
Kan, Kevin0000-0002-5840-8928
Guevarra, Dan0000-0002-9592-3195
Lai, Yungchieh0000-0001-9392-1447
Gregoire, John M.0000-0002-2863-5265
Additional Information:This material is based on work performed by the Liquid Sunlight Alliance, which is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Fuels from Sunlight Hub under Award DE-SC0021266. D.L. acknowledges support as a Liquid Sunlight Alliance (LiSA) WAVE Fellow. The authors thank Nicholas B. Watkins for assistance with scanning electron microscope imaginig. Data supporting the figures, XRD patterns, and raw PEC data are available under a CC0 license at (doi: 10.22002/42gwd-8wg77).
Group:Liquid Sunlight Alliance
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0021266
Issue or Number:48
Record Number:CaltechAUTHORS:20221212-796684400.33
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:118319
Deposited By: Research Services Depository
Deposited On:18 Jan 2023 18:15
Last Modified:18 Jan 2023 18:15

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