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Issue 13, 2020
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Multiscale optimization of Li-ion diffusion in solid lithium metal batteries via ion conductive metal–organic frameworks

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Abstract

Optimization of solid electrolytes (SEs) is of great significance for lithium-based solid state batteries (SSBs). However, insufficient Li ion transport, deficient interfacial compatibility and formation of lithium dendrites lead to poor cycling performance. Based on Li+ conductive metal–organic frameworks (LCMOFs), herein a multiscale optimization strategy is put forward to facilitate Li+ transport within the MOFs (molecular scale), between the MOFs’ boundaries (nanoscale) and across the SE/electrode interface (microscale) in SSBs. LCMOFs are obtained by binding Li+ onto ionogenic chemical groups (–CO2H, –SO3H and –OH) in nanoscale dispersed MOFs. Both experimental results and DFT simulations confirm the key role of ionogenic groups for Li+ transport. Furthermore, benefiting from the optimized interfaces between LCMOF crystals, SEs with excellent electrochemical properties are obtained, including a high ionic conductivity of 1.06 × 10−3 S cm−1 at 25 °C, a wide electrochemical window from 2.0 to 4.5 V, low interfacial resistances and stable Li plating/stripping. The fabricated Li|SE|LiFePO4 SSB exhibits high and stable charge/discharge capacities under wide operation temperatures ranging from −20 to 60 °C.

Graphical abstract: Multiscale optimization of Li-ion diffusion in solid lithium metal batteries via ion conductive metal–organic frameworks

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Supplementary files

Article information


Submitted
06 Dec 2019
Accepted
03 Mar 2020
First published
04 Mar 2020

Nanoscale, 2020,12, 6976-6982
Article type
Communication

Multiscale optimization of Li-ion diffusion in solid lithium metal batteries via ion conductive metal–organic frameworks

Q. Zhang, D. Li, J. Wang, S. Guo, W. Zhang, D. Chen, Q. Li, X. Rui, L. Gan and S. Huang, Nanoscale, 2020, 12, 6976
DOI: 10.1039/C9NR10338D

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