Weakening ionic coordination for high ionic conductivity composite solid electrolytes
Author(s)
Type
Journal Article
Abstract
The special chemistry of N,N-dimethylformamide (DMF)-solvated Li+ [Li(DMF)x]+ migration results in polyvinylidene fluoride (PVDF)-based solid polymer electrolytes exhibiting high ionic conductivities. Incorporating ceramic fillers into PVDF electrolytes can further enhance the ionic conductivities. However, there is limited understanding of the desolvation process of Li+ during its transport through the ceramic fillers. Herein, we reveal that this desolvation process exhibits a large energy barrier that hinders the Li+ transport. The introduction of poly(methylhydrosiloxane) (PMHS) can weaken the ion–solvent coordination, forming loosely complexed [Li(DMF)x]+ and reducing their desolvation energy. This promotes rapid ceramic-involved Li+ pathways, enabling the electrolyte with a high ambient ionic conductivity of 7.5 × 10–4 S cm–1. Moreover, the facile desolvation process can enhance the kinetics and reduce side reactions at the electrode/electrolyte interfaces. Therefore, solid-state Li–Li symmetric cells can operate for a record 11 800 h, and LiNi0.8Co0.1Mn0.1O2|Li solid-state batteries also demonstrated exceptional cycling stability for more than 2200 cycles at 2C.
Date Issued
2024-05-10
Date Acceptance
2024-04-09
Citation
ACS Energy Letters, 2024, 9 (5), pp.2109-2115
ISSN
2380-8195
Publisher
American Chemical Society
Start Page
2109
End Page
2115
Journal / Book Title
ACS Energy Letters
Volume
9
Issue
5
Copyright Statement
© 2024 The Authors. Published by American Chemical Society. This publication is licensed under
CC-BY 4.0.
CC-BY 4.0.
License URL
Identifier
https://staging.pubs.acs.org/doi/10.1021/acsenergylett.4c00636
Publication Status
Published
Date Publish Online
2024-04-11