First-Principles Prediction of the Electrochemical Stability and Reaction Mechanisms of Solid-State Electrolytes.

Autor:	Schwietert TK; Storage of Electrochemical Energy, Department of Radiation Science and Technology, Faculty of Applied Sciences, Delft University of Technology, Mekelweg 15, Delft 2929JB, The Netherlands., Vasileiadis A; Storage of Electrochemical Energy, Department of Radiation Science and Technology, Faculty of Applied Sciences, Delft University of Technology, Mekelweg 15, Delft 2929JB, The Netherlands., Wagemaker M; Storage of Electrochemical Energy, Department of Radiation Science and Technology, Faculty of Applied Sciences, Delft University of Technology, Mekelweg 15, Delft 2929JB, The Netherlands.
Jazyk:	angličtina
Zdroj:	JACS Au [JACS Au] 2021 Aug 16; Vol. 1 (9), pp. 1488-1496. Date of Electronic Publication: 2021 Aug 16 (Print Publication: 2021).
DOI:	10.1021/jacsau.1c00228
Abstrakt:	Solid-state batteries have significant advantages over conventional liquid batteries, providing improved safety, design freedom, and potentially reaching higher power and energy densities. The major obstacle in the commercial realization of solid-state batteries is the high resistance at the interfaces. To overcome this bottleneck, it is essential to achieve an in-depth fundamental understanding of the crucial electrochemical processes at the interface. Conventional electrochemical stability calculations for solid electrolytes, determining the formation energy toward the energetically favorable decomposition products, often underestimate the stability window because kinetics are not included. In this work, we introduce a computational scheme that takes the redox-activity of the solid electrolytes into account in calculating the electrochemical stability, and it in many cases appears to dictate the electrochemical stability. This methodology is applied to different chemical and structural classes of solid electrolytes, exhibiting excellent agreement with experimentally observed electrochemical stability. In contrast with current perception, the results suggest that the electrochemical stability of solid electrolytes is not always determined by the decomposition products but often originates from the intrinsic stability of the material itself. The processes occurring outside the stability window can lead toward phase separation or solid solution depending on the reaction mechanism of the material. These newly gained insights provide better predictions of the practical voltage ranges and structural stabilities of solid electrolytes, guiding solid-state batteries toward better interfaces and material design. Competing Interests: The authors declare no competing financial interest. (© 2021 The Authors. Published by American Chemical Society.)
Databáze:	MEDLINE
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