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Published July 20, 2022 | Published + Supplemental Material
Journal Article Open

Addressing solar photochemistry durability with an amorphous nickel antimonate photoanode

Abstract

Renewable generation of fuels using solar energy is a promising technology whose deployment hinges on the discovery of materials with a combination of durability and solar-to-chemical conversion efficiency that has yet to be demonstrated. Stable operation of photoanodes has been demonstrated with wide-gap semiconductors, as well as protected visible gap semiconductors. Visible photoresponse from electrochemically stable materials is quite rare. In this paper, we report the high-throughput discovery of an amorphous Ni-Sb (1:1) oxide photoanode that meets the requirements of operational stability, visible photoresponse, and appreciable photovoltage. X-ray absorption characterization of Ni and Sb establishes a structural connection to rutile NiSb₂O₆, guiding electronic structure characterization via X-ray photoelectron experiments and density functional theory. This amorphous photoanode opens avenues for photoelectrode development due to the lack of crystal anisotropy combined with its operational stability, which mitigates the formation of an interphase that disrupts the semiconductor-electrolyte junction.

Additional Information

© 2022 The Author(s). Under a Creative Commons license - Attribution 4.0 International (CC BY 4.0). Received 23 March 2022, Revised 27 May 2022, Accepted 8 June 2022, Available online 27 June 2022. This material is based on work performed by the Liquid Sunlight Alliance, which is supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Fuels from Sunlight Hub under award DE-SC0021266. This research used computing resources from the Lawrencium computational cluster resource provided by the IT Division at the Lawrence Berkeley National Laboratory, supported by the Director, Office of Science, Office of Basic Energy Sciences, of the US Department of Energy under contract no. DE-AC02-05CH11231. Use of the Stanford Synchrotron Radiation Lightsource (beamlines 7-3 and 9-3), SLAC National Accelerator Laboratory, is supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under contract no. DE-AC02-76SF00515. National Renewable Energy Laboratory is operated by the Alliance for Sustainable Energy, LLC, for the US Department of Energy (DOE) under contract no. DE-AC36-08GO28308. The Resnick Sustainability Institute at Caltech is also acknowledged for its support of enabling infrastructure and facilities. The views expressed in this article do not necessarily represent the views of the DOE or the US Government. Author contributions. L.Z. conducted synthesis and diffraction experiments with support from K.K. Electronic structure calculations were conducted by E.A.P. and J.B.N. The grand potential and Pourbaix phase diagrams were created by K.K.R. and M.B. Photoelectrochemistry experiments were conducted by Y.L. and Y.W. Optical spectroscopy measurements were conducted by P.F.N. X-ray absorption measurements were conducted by X.L. and analyzed by Y.L. under guidance from J.Y. Electronic structure experiments were conducted by M.H.R. Hall measurements were conducted by S.R.B. J.M.G. supervised the work, designed experiments, and coordinated manuscript writing along with L.Z. using contributions from all authors. Data and code availability. Computational and experimental data are available at https://data.caltech.edu/records/20057 (10.22002/D1.20057). The code for processing experimental data is available at https://github.com/johnmgregoire/JCAPDataProcess. The authors declare no competing interests.

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Supplemental Material - 1-s2.0-S2666386422002405-mmc1.pdf

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Additional details

Created:
August 22, 2023
Modified:
October 23, 2023