Issue 33, 2024

Decoupling Li+ conductivity and mechanical stability in a thermally reversible concentrated sulfone-based gel electrolyte for lithium metal batteries

Abstract

Increasing the liquid content has been recognized as an effective strategy to enhance the Li+ conductivity and electrode compatibility of gel electrolytes for lithium-metal batteries (LMBs). However, a low gelator content reduces the mechanical strength of gels. Herein, a mechanically stable gel electrolyte comprising 7 wt% methylcellulose (MC), 3 wt% 12-hydroxyoctadecanoic acid (12-HOA), and 90 wt% concentrated sulfone electrolyte (CSE) was developed. Because of its high electrolyte uptake, the MC/12-HOA gel electrolyte exhibits an ionic conductivity of 0.25 mS cm−1, which is similar to that of the neat CSE, and a Li+ transference number of 0.57, which is even higher than that of the CSE. Abundant ether groups on MC and hydroxyl groups on 12-HOA can strongly immobilize TFSIvia a hydrogen bond, endowing the MC/12-HOA gel with an elastic modulus of 10 MPa enough to form an 80 μm – thick self-supporting film and suppress Li dendrite growth. Additionally, a reversible gel–sol transition occurs in the MC/12-HOA gel at 329–331 K, which can be utilized to promote electrode wetting and seal the damages of electrolytes. As a result, the MC/12-HOA gel electrolyte displays reliable safety, practical flexibility, and suitable electrochemical performance in both the Li‖LiFePO4 and Li‖LiNi0.8Co0.1Mn0.1O2 cells, suggesting the great promise of the MC/12-HOA scaffold in gel electrolytes with different solvents for a wide range of applications in flexible devices.

Graphical abstract: Decoupling Li+ conductivity and mechanical stability in a thermally reversible concentrated sulfone-based gel electrolyte for lithium metal batteries

Supplementary files

Article information

Article type
Paper
Submitted
13 Apr 2024
Accepted
09 Jul 2024
First published
18 Jul 2024

J. Mater. Chem. A, 2024,12, 21912-21922

Decoupling Li+ conductivity and mechanical stability in a thermally reversible concentrated sulfone-based gel electrolyte for lithium metal batteries

X. Jiang, J. Chen, J. Zeng, W. Liu, X. Wu, Y. Lv, F. Liu, C. Zhang, Z. Li, X. Wang and S. Zhang, J. Mater. Chem. A, 2024, 12, 21912 DOI: 10.1039/D4TA02561J

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