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Electrolyte-free graphite electrode with enhanced interfacial conduction using Li+-conductive binder for high-performance all-solid-state batteries

Title
Electrolyte-free graphite electrode with enhanced interfacial conduction using Li+-conductive binder for high-performance all-solid-state batteries
Author(s)
Shin, Dong OkKim, HyungjunChoi, JaecheolKim, Min PyeongKim, Ju YoungKang, Seok HunPark, Young-SamHong, Sung YouCho, MaenghyoLee, Young-GiCho, KyeongjaeLee, Yong Min
Issued Date
2022-08
Citation
Energy Storage Materials, v.49, pp.481 - 492
Type
Article
Author Keywords
interfacial conductionall-solid-state battery electrodecarboxymethyl celluloseLi+-conductive binder
Keywords
LITHIATIONVISCOSITYTOTAL-ENERGY CALCULATIONSCARBOXYMETHYL CELLULOSEAB-INITIOPOLYMERIC BINDERSSILICON ANODESLITHIUM
ISSN
2405-8297
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(-2) and 490 mAh cm(-3) at a high current rate (1.91 mA cm(-2)) and 60 C which are far superior to those (1.07 mAh cm(-2) and 356.7 mAh cm(-3)) 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.
URI
http://hdl.handle.net/20.500.11750/16965
DOI
10.1016/j.ensm.2022.04.029
Publisher
Elsevier BV
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Department of Energy Science and Engineering Battery Materials & Systems LAB 1. Journal Articles

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