期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 142, 期 5, 页码 2497-2505出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b12233
关键词
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资金
- U.S. Department of Energy through the Advanced Battery Materials Research (BMR) Program (Battery500 Consortium) [DE-EE0007762]
- National Science Foundation [DMR-1808517, NSF/DMR-1644779]
- State of Florida
- TAFEL [UTA18-000175]
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 Li-7 relaxation time and Li-6 -> Li-7 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 x 10(-4) S cm(-1) at 30 degrees 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 degrees C.
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