Roles of Polymerized Anionic Clusters Stimulating for Hydrolysis Deterioration in Li7P3S11

Ji Su Kim, Wo Dum Jung, Sung Soo Shin, Sungeun Yang, Sangbaek Park, Jong Ho Lee, Byung Kook Kim, Jong Heun Lee, Hyoungchul Kim

Research output: Contribution to journalArticlepeer-review

Abstract

The atmospheric hydrolysis reaction in sulfide solid electrolytes (SEs) is destructive to their Li-ion conducting behavior, but a comprehensive understanding of their reaction steps is still lacking. Therefore, here, we studied the atmospheric deterioration of a well-known sulfide SE, Li7P3S11, based on the analogies between the hydrolysis and electrochemical reactions. Through analyzing the change in the S2pbinding energy, we found that the anionic structures of both air-exposed and delithiated sulfides were altered owing to Li-ion loss. Considering the high diffusivity and massive hydrate formation ability of Li ions, we found that the anionic structures of both air-exposed and delithiated sulfides were altered. We showed that the hydrolysis of sulfide SEs with anionic polymerization has a thermodynamically favorable final state energy of −3.85 eV because S ions offer high degrees of freedom in their charge states ranging from −0.89 to −0.31e.

Original languageEnglish
Pages (from-to)19509-19516
Number of pages8
JournalJournal of Physical Chemistry C
Volume125
Issue number35
DOIs
Publication statusPublished - 2021 Sep 9

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

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