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학술지 Effect of Lithium Substitution Ratio of Polymeric Binders on Interfacial Conduction within All-Solid-State Battery Anodes
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신동옥, 김형준, 최재철, 김주영, 강석훈, 박영삼, 조맹효, 이용민, 조경재, 이영기
ACS Applied Materials & Interfaces, v.15 no.10, pp.13131-13143
American Chemical Society (ACS)
22ZB1200, ICT 소재·부품·장비 자립기술 및 도전기술 개발, 황치선
Problematic issues with electrically inert binders have been less serious in the conventional lithium-ion batteries by virtue of permeable liquid electrolytes (LEs) for ionic connection and/or carbonaceous additives for electronic connection in the electrodes. Contrary to electron-conductive binders used to maximize an active loading level, the development of ion-conductive binders has been lacking owing to the LE-filled electrode configuration. Herein, we represent a tactical strategy for improving the interfacial Li+ conduction in all-solid-state electrolyte-free graphite (EFG) electrodes where the solid electrolytes are entirely excluded, using lithium-substitution-modulated (LSM) binders. Finely tuning a lithium substitution ratio, a conductive LSM-carboxymethyl cellulose (CMC) binder is prepared from a controlled direct Na+/Li+ exchange reaction without a hazardous acid involvement. The EFG electrode employing LSM with a maximum degree of substitution of lithium (DSLi) of ~68% in our study shows a considerably higher rate capability of 1.05 mA h cm-2 at 1 C and a capacity retention of ~61.9% after 200 cycles at 0.5 C than those using sodium-CMC (Na-CMC) (0.78 mA h cm-2, ~49.5%) and LSM with ~35% lithium substitution (0.93 mA h cm-2, ~55.4%). More importantly, the correlation between the phase transition near the bottom region of the EFG electrode and the state of charge (SOC) is systematically investigated, clarifying that the improvement of the interfacial conduction is proportional to the DSLi of the CMC binders. Theoretical calculations combined with experimental results further verify that creating the continuous interface through abundant pathways for mobile ions using the Li+-conductive binder is the enhancement mechanism of the interfacial conduction in the EFG electrode, mitigating serious charge transfer resistance.
KSP 제안 키워드
Active loading, Carboxymethyl cellulose, Degree of substitution(d.s.), Enhancement mechanism, Interfacial conduction, Ion batteries, Liquid electrolyte, Maximum degree, Na-CMC, Phase transition, Rate Capability