Zinc Titanium Nitride Semiconductor toward Durable Photoelectrochemical Applications.

Autor:	Greenaway AL; Materials Chemical and Computational Science Directorate, National Renewable Energy Laboratory, Golden, Colorado 80401, United States., Ke S; Materials and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.; Department of Materials Science and Engineering, University of California Berkeley, Berkeley, California 94720, United States., Culman T; Materials Chemical and Computational Science Directorate, National Renewable Energy Laboratory, Golden, Colorado 80401, United States., Talley KR; Materials Chemical and Computational Science Directorate, National Renewable Energy Laboratory, Golden, Colorado 80401, United States., Mangum JS; Materials Chemical and Computational Science Directorate, National Renewable Energy Laboratory, Golden, Colorado 80401, United States., Heinselman KN; Materials Chemical and Computational Science Directorate, National Renewable Energy Laboratory, Golden, Colorado 80401, United States., Kingsbury RS; Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States., Smaha RW; Materials Chemical and Computational Science Directorate, National Renewable Energy Laboratory, Golden, Colorado 80401, United States., Gish MK; Materials Chemical and Computational Science Directorate, National Renewable Energy Laboratory, Golden, Colorado 80401, United States., Miller EM; Materials Chemical and Computational Science Directorate, National Renewable Energy Laboratory, Golden, Colorado 80401, United States., Persson KA; Department of Materials Science and Engineering, University of California Berkeley, Berkeley, California 94720, United States.; Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States., Gregoire JM; Division of Engineering and Applied Science, California Institute of Technology, Pasadena, California 91125, United States., Bauers SR; Materials Chemical and Computational Science Directorate, National Renewable Energy Laboratory, Golden, Colorado 80401, United States., Neaton JB; Materials and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.; Department of Physics, University of California Berkeley, Berkeley, California 94720, United States.; Kavli Energy Nanosciences Institute at Berkeley, Berkeley, California 94720, United States., Tamboli AC; Materials Chemical and Computational Science Directorate, National Renewable Energy Laboratory, Golden, Colorado 80401, United States.; Department of Physics, Colorado School of Mines, Golden, Colorado 80401, United States., Zakutayev A; Materials Chemical and Computational Science Directorate, National Renewable Energy Laboratory, Golden, Colorado 80401, United States.
Jazyk:	angličtina
Zdroj:	Journal of the American Chemical Society [J Am Chem Soc] 2022 Aug 03; Vol. 144 (30), pp. 13673-13687. Date of Electronic Publication: 2022 Jul 20.
DOI:	10.1021/jacs.2c04241
Abstrakt:	Photoelectrochemical fuel generation is a promising route to sustainable liquid fuels produced from water and captured carbon dioxide with sunlight as the energy input. Development of these technologies requires photoelectrode materials that are both photocatalytically active and operationally stable in harsh oxidative and/or reductive electrochemical environments. Such photocatalysts can be discovered based on co-design principles, wherein design for stability is based on the propensity for the photocatalyst to self-passivate under operating conditions and design for photoactivity is based on the ability to integrate the photocatalyst with established semiconductor substrates. Here, we report on the synthesis and characterization of zinc titanium nitride (ZnTiN 2 ) that follows these design rules by having a wurtzite-derived crystal structure and showing self-passivating surface oxides created by electrochemical polarization. The sputtered ZnTiN 2 thin films have optical absorption onsets below 2 eV and n-type electrical conduction of 3 S/cm. The band gap of this material is reduced from the 3.36 eV theoretical value by cation-site disorder, and the impact of cation antisites on the band structure of ZnTiN 2 is explored using density functional theory. Under electrochemical polarization, the ZnTiN 2 surfaces have TiO 2 - or ZnO-like character, consistent with Materials Project Pourbaix calculations predicting the formation of stable solid phases under near-neutral pH. These results show that ZnTiN 2 is a promising candidate for photoelectrochemical liquid fuel generation and demonstrate a new materials design approach to other photoelectrodes with self-passivating native operational surface chemistry.
Databáze:	MEDLINE
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