Fast Li+ Conduction Mechanism and Interfacial Chemistry of a NASICON/Polymer Composite Electrolyte

Nan Wu, Po Hsiu Chien, Yutao Li*, Andrei Dolocan, Henghui Xu, Biyi Xu, Nicholas S. Grundish, Haibo Jin, Yan Yan Hu, John B. Goodenough

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

234 Citations (Scopus)

Abstract

The unclear Li+ local environment and Li+ conduction mechanism in solid polymer electrolytes, especially in a ceramic/polymer composite electrolyte, hinder the design and development of a new composite electrolyte. Moreover, both the low room-temperature Li+ conductivity and large interfacial resistance with a metallic lithium anode of a polymer membrane limit its application below a relatively high temperature. Here we have identified the Li+ distribution and Li+ transport mechanism in a composite polymer electrolyte by investigating a new solid poly(ethylene oxide) (PEO)-based NASICON-LiZr2(PO4)3 composite with 7Li relaxation time and 6Li → 7Li trace-exchange NMR measurements. The Li+ population of the two local environments in the composite electrolytes depends on the Li-salt concentration and the amount of ceramic filler. A composite electrolyte with a [EO]/[Li+] ratio n = 10 and 25 wt % LZP filler has a high Li+ conductivity of 1.2 × 10-4 S cm-1 at 30 °C and a low activation energy owing to the additional Li+ in the mobile A2 environment. Moreover, an in situ formed solid electrolyte interphase layer from the reaction between LiZr2(PO4)3 and a metallic lithium anode stabilized the Li/composite-electrolyte interface and reduced the interfacial resistance, which provided a symmetric Li/Li cell and all-solid-state Li/LiFePO4 and Li/LiNi0.8Co0.1Mn0.1O2 cells a good cycling performance at 40 °C.

Original languageEnglish
Pages (from-to)2497-2505
Number of pages9
JournalJournal of the American Chemical Society
Volume142
Issue number5
DOIs
Publication statusPublished - 5 Feb 2020

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