Communication: The electronic entropy of charged defect formation and its impact on thermochemical redox cycles

Lany, Stephan

doi:10.1063/1.5022176

Title: Communication: The electronic entropy of charged defect formation and its impact on thermochemical redox cycles

Journal Article · 21 February 2018 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/1.5022176 · OSTI ID:1424583

Lany, Stephan ^[1]

National Renewable Energy Lab. (NREL), Golden, CO (United States)

The ideal material for solar thermochemical water splitting, which has yet to be discovered, must satisfy stringent conditions for the free energy of reduction, including, in particular, a sufficiently large positive contribution from the solid-state entropy. By inverting the commonly used relationship between defect formation energy and defect concentration, it is shown here that charged defect formation causes a large electronic entropy contribution manifesting itself as the temperature dependence of the Fermi level. This result is a general feature of charged defect formation and motivates new materials design principles for solar thermochemical hydrogen production.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Next Generation of Materials by Design: Incorporating Metastability (CNGMD)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Hydrogen and Fuel Cell Technologies Program (EE-3F); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1424583

Alternate ID(s):: OSTI ID: 1421582

Report Number(s):: NREL/JA-5K00-70968; TRN: US1801926

Journal Information:: Journal of Chemical Physics, Vol. 148, Issue 7; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 19 works

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Defect phase diagram for doping of Ga ₂ O ₃ Lany, Stephan APL Materials, Vol. 6, Issue 4 https://doi.org/10.1063/1.5019938	journal	April 2018
Computational Fermi level engineering and doping-type conversion of Ga2O3 via three-step synthesis process Goyal, Anuj; Zakutayev, Andriy; Stevanović, Vladan arXiv https://doi.org/10.48550/arxiv.2103.16639	text	January 2021