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Title: Nonuniform Ionic and Electronic Transport of Ceramic and Polymer/Ceramic Hybrid Electrolyte by Nanometer-Scale Operando Imaging for Solid-State Battery

Journal Article · · Advanced Energy Materials

Replacing the liquid electrolyte in lithium batteries with solid-state ion conductor is promising for next-generation energy storage that is safe and has high energy density. In this work, nanometer-resolution ionic and electronic transport imaging of Li3PS4 (LPS), a solid-state electrolyte (SSE), is reported. This nm resolution is achieved by using a logarithm-scale current amplifier that enhances the current sensitivity to the fA range. Large fluctuations of ion current—one to two orders of magnitude on the LPS and on the LPS region of a polymer/LPS bulk hybrid SSE—that must be mitigated to eliminate Li dendrite formation and growth, are found. This ion current fluctuation is understood in terms of highly anisotropic transport kinetic barriers along the different crystalline axes due to different grain orientations in the polycrystalline and glass ceramic materials. The results on the bulk hybrid SSE show a sharp transition of ionic and electronic transport at the LPS/polymer boundary and decreases in average ionic current with decreasing polyimine particle size and with extensive cycling. The results elucidate the mechanism of polyimine extension into interparticles to prevent Li dendrite growth. This work opens up novel characterization of charge transport, which relates to Li plating and stripping for solid-state-batteries.

Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Laboratory Directed Research and Development (LDRD) Program; National Research Foundation of Korea (NRF)
Grant/Contract Number:
AC36-08GO28308; NRF-2018M1A2A2063340; AR0000781
OSTI ID:
1659845
Alternate ID(s):
OSTI ID: 1615416
Report Number(s):
NREL/JA-5K00-76038; MainId:6602; UUID:930b58da-7348-ea11-9c31-ac162d87dfe5; MainAdminID:13486
Journal Information:
Advanced Energy Materials, Vol. 10, Issue 21; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 19 works
Citation information provided by
Web of Science