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Published May 23, 2017 | Supplemental Material
Journal Article Open

Quantum Mechanics Reactive Dynamics Study of Solid Li-Electrode/Li_6PS_5Cl-Electrolyte Interface

Abstract

We have performed a theoretical study of the Li/Li_6PS_5Cl interface and showed the ability of the applied computational methods to properly describe the chemical processes that occurs at the interface. After a 500 ps ab initio molecular dynamics simulation, we find that the Li/Li_6PS_5Cl interface decomposes with formation of multiple phases and the main decomposition products are Li_2S, Li_3P, LiCl, and possibly LiP. These findings are in good agreement with reported experimental data. The observed quick decomposition is attributed to the weak bonding between P and S. Basing on this and earlier obtained experimental results, we conclude that the chemical instability may be an intrinsic problem of PS based solid electrolytes when they are in contact with Li-metal. Our results validate effectivity of the available computational tools to reach a deeper insight into the evolution of interfacial structures and properties prior to experiment.

Additional Information

© 2017 American Chemical Society. Received 13 April 2017. Published online 23 May 2017. This work was supported by Bosch Energy Research Network Grant No. 13.01.CC11. We thank our Bosch colleague Dr. Boris Kozinsky for fruitful discussions and critical feedback on this work. The authors declare no competing financial interest.

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