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X-ray Photoelectron Spectroscopy and Resonant X-ray Spectroscopy Investigations of Interactions between Thin Metal Catalyst Films and Amorphous Titanium Dioxide Photoelectrode Protection Layers

Richter, Matthias H. and Cheng, Wen-Hui and Crumlin, Ethan J. and Drisdell, Walter S. and Atwater, Harry A. and Schmeißer, Dieter and Lewis, Nathan S. and Brunschwig, Bruce S. (2021) X-ray Photoelectron Spectroscopy and Resonant X-ray Spectroscopy Investigations of Interactions between Thin Metal Catalyst Films and Amorphous Titanium Dioxide Photoelectrode Protection Layers. Chemistry of Materials, 33 (4). pp. 1265-1275. ISSN 0897-4756. https://resolver.caltech.edu/CaltechAUTHORS:20210216-100602720

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Abstract

The use of electrochemistry, X-ray photoelectron spectroscopy, and resonant X-ray spectroscopy has unlocked the paradox of interfacial hole conduction through amorphous TiO₂ (a-TiO₂) to deposited Ni, Ir, and Au metal catalysts. Although electrocatalysts for the oxygen-evolution reaction derived from metallic Ir and Ni have mutually similar overpotentials in alkaline media, Si/a-TiO₂/Ir interfaces exhibit higher overpotentials than Si/a-TiO₂/Ni interfaces. The data allow formulation of full band energy diagrams for n-Si/a-TiO₂/metal interfaces for M = Ni, Ir, or Au. Although both Ni and Ir produce band bending in a-TiO₂ favoring hole conduction, only Ni creates multiple states within the a-TiO₂ band gap at the a-TiO₂/Ni interface, which produces a quasi-metallic interface at the a-TiO₂/Ni junction. Au, however, produces a flat-band interface that limits hole conduction without any new band gap states.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acs.chemmater.0c04043DOIArticle
ORCID:
AuthorORCID
Richter, Matthias H.0000-0003-0091-2045
Cheng, Wen-Hui0000-0003-3233-4606
Crumlin, Ethan J.0000-0003-3132-190X
Drisdell, Walter S.0000-0002-8693-4562
Atwater, Harry A.0000-0001-9435-0201
Schmeißer, Dieter0000-0002-7560-2634
Lewis, Nathan S.0000-0001-5245-0538
Brunschwig, Bruce S.0000-0002-6135-6727
Additional Information:© 2021 American Chemical Society. Received: October 15, 2020; Revised: January 25, 2021; Published: February 11, 2021. This work was supported through the Office of Science of the U.S. Department of Energy (DOE) under award no. DE SC0004993 to the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub. Research was in part carried out at the Molecular Materials Research Center of the Beckman Institute of the California Institute of Technology. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE AC02 05CH11231. E.J.C. was partially supported by an Early Career Award in the Condensed Phase and Interfacial Molecular Science Program in the Chemical Sciences, Geosciences, and Biosciences Division of the Office of Basic Energy Sciences of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. M.H.R. and W.H.C. carried out the investigation; E.J.C., W.S.D., H.A.A., and D.S. provided support for synchrotron studies and general discussion. M.H.R., W.H.C., N.S.L., and B.S.B. wrote the manuscript; and N.S.L. and B.S.B supervised the study. Author Contributions: M.H.R. and W.H.C. contributed equally to this work. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Department of Energy (DOE)DE-AC02-05CH11231
Subject Keywords:Oxides, Interfaces, Transition metals, Metals, Gold
Issue or Number:4
Record Number:CaltechAUTHORS:20210216-100602720
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20210216-100602720
Official Citation:X-ray Photoelectron Spectroscopy and Resonant X-ray Spectroscopy Investigations of Interactions between Thin Metal Catalyst Films and Amorphous Titanium Dioxide Photoelectrode Protection Layers. Matthias H. Richter, Wen-Hui Cheng, Ethan J. Crumlin, Walter S. Drisdell, Harry A. Atwater, Dieter Schmeißer, Nathan S. Lewis, and Bruce S. Brunschwig. Chemistry of Materials 2021 33 (4), 1265-1275; DOI: 10.1021/acs.chemmater.0c04043
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:108060
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:16 Feb 2021 18:17
Last Modified:24 Feb 2021 18:56

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