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Title: Non-Faradaic Li + Migration and Chemical Coordination across Solid-State Battery Interfaces

Abstract

Efficient and reversible charge transfer is essential to realizing high-performance solid-state batteries. Efforts to enhance charge transfer at critical electrode–electrolyte interfaces have proven successful, yet interfacial chemistry and its impact on cell function remains poorly understood. Using X-ray photoelectron spectroscopy combined with electrochemical techniques, we elucidate chemical coordination near the LiCoO 2–LIPON interface, providing experimental validation of space-charge separation. Space-charge layers, defined by local enrichment and depletion of charges, have previously been theorized and modeled, but the unique chemistry of solid-state battery interfaces is now revealed. Here we highlight the non-Faradaic migration of Li+ ions from the electrode to the electrolyte, which reduces reversible cathodic capacity by ~15%. Inserting a thin, ion-conducting LiNbO 3 interlayer between the electrode and electrolyte, however, can reduce space-charge separation, mitigate the loss of Li+ from LiCoO 2, and return cathodic capacity to its theoretical value. This work illustrates the importance of interfacial chemistry in understanding and improving solid-state batteries.

Authors:
ORCiD logo [1];  [1]
  1. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1429829
Report Number(s):
SAND-2017-8864J
Journal ID: ISSN 1530-6984; 656354
DOE Contract Number:
AC04-94AL85000
Resource Type:
Journal Article
Resource Relation:
Journal Name: Nano Letters; Journal Volume: 17; Journal Issue: 11
Country of Publication:
United States
Language:
English

Citation Formats

Gittleson, Forrest S., and El Gabaly, Farid. Non-Faradaic Li + Migration and Chemical Coordination across Solid-State Battery Interfaces. United States: N. p., 2017. Web. doi:10.1021/acs.nanolett.7b03498.
Gittleson, Forrest S., & El Gabaly, Farid. Non-Faradaic Li + Migration and Chemical Coordination across Solid-State Battery Interfaces. United States. doi:10.1021/acs.nanolett.7b03498.
Gittleson, Forrest S., and El Gabaly, Farid. Tue . "Non-Faradaic Li + Migration and Chemical Coordination across Solid-State Battery Interfaces". United States. doi:10.1021/acs.nanolett.7b03498.
@article{osti_1429829,
title = {Non-Faradaic Li + Migration and Chemical Coordination across Solid-State Battery Interfaces},
author = {Gittleson, Forrest S. and El Gabaly, Farid},
abstractNote = {Efficient and reversible charge transfer is essential to realizing high-performance solid-state batteries. Efforts to enhance charge transfer at critical electrode–electrolyte interfaces have proven successful, yet interfacial chemistry and its impact on cell function remains poorly understood. Using X-ray photoelectron spectroscopy combined with electrochemical techniques, we elucidate chemical coordination near the LiCoO2–LIPON interface, providing experimental validation of space-charge separation. Space-charge layers, defined by local enrichment and depletion of charges, have previously been theorized and modeled, but the unique chemistry of solid-state battery interfaces is now revealed. Here we highlight the non-Faradaic migration of Li+ ions from the electrode to the electrolyte, which reduces reversible cathodic capacity by ~15%. Inserting a thin, ion-conducting LiNbO3 interlayer between the electrode and electrolyte, however, can reduce space-charge separation, mitigate the loss of Li+ from LiCoO2, and return cathodic capacity to its theoretical value. This work illustrates the importance of interfacial chemistry in understanding and improving solid-state batteries.},
doi = {10.1021/acs.nanolett.7b03498},
journal = {Nano Letters},
number = 11,
volume = 17,
place = {United States},
year = {Tue Oct 17 00:00:00 EDT 2017},
month = {Tue Oct 17 00:00:00 EDT 2017}
}