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Journal Article Electrolyte-free graphite electrode with enhanced interfacial conduction using Li+-conductive binder for high-performance all-solid-state batteries
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Authors
Dong Ok Shin, Hyungjun Kim, Seungwon Jung, Seoungwoo Byun, Jaecheol Choi, Min Pyeong Kim, Ju Young Kim, Seok Hun Kang, Young-Sam Park, Sung You Hong, Maenghyo Cho, Young-Gi Lee, Kyeongjae Cho, Yong Min Lee
Issue Date
2022-08
Citation
Energy Storage Materials, v.49, pp.481-492
ISSN
2405-8297
Publisher
Elsevier
Language
English
Type
Journal Article
DOI
https://dx.doi.org/10.1016/j.ensm.2022.04.029
Abstract
Electrodes supported by conductive binders are expected to outperform ones with inert binders that potentially disturb electronic/ionic contacts at interfaces. Unlike electron-conductive binders, the employment of Li+-conductive binders has attracted relatively little attention due to the liquid electrolyte (LE)-impregnated electrode configuration in the conventional lithium-ion batteries (LIBs). Herein, an all-solid-state electrolyte-free electrode where electrolyte components are completely excluded is introduced as a new tactical electrode construction to evaluate the effectiveness of the Li+-conductive binder on enhancing the interfacial conduction, ultimately leading to high-performance all-solid-state batteries (ASSBs). Conductive lithium carboxymethyl cellulose (Li-CMC) is prepared through an optimized two-step cation-exchange reaction without physical degradation. The electrolyte-free graphite electrode employing Li-CMC as the binder shows strikingly improved areal and volumetric capacity of 1.46 mAh cm?닋2 and 490 mAh cm?닋3 at a high current rate (1.91 mA cm?닋2) and 60 °C which are far superior to those (1.07 mAh cm?닋2 and 356.7 mAh cm?닋3) using Na-CMC. Moreover, systematic monitoring of the lithiation dynamics inside the electrolyte-free electrode clarifies that the interfacial Li+ conduction is greatly promoted in the Li-CMC electrode. Complementary analysis from in-depth electrochemical measurements and multiscale simulations verifies that serious internal resistance from impeded interparticle diffusion by inert binders can be substantially mitigated using Li-CMC.
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