期刊
ACS APPLIED ENERGY MATERIALS
卷 5, 期 8, 页码 9429-9436出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsaem.2c00978
关键词
all-solid-state battery; lithium sulfur battery; active material; ionic conductivity; lithium sulfide
资金
- JST ALCA-SPRING [JPMJAL1301]
- JSPS KAKENHI [18H05255]
Lithium sulfur batteries are promising due to their high energy densities. This study investigates the charge-discharge mechanism of a Li2S-LiI solid solution in all-solid-state batteries, achieving high reversible capacity. The formation of an ionic conductive structure rich in LiI enables nearly fully solid phase S/Li2S reactions in all-solid-state batteries.
Lithium sulfur (Li/S) batteries are promising next-generation battery candidates owing to their high energy densities. In particular, the fast solid-state S/Li2S redox reactions are crucial to increase the energy density and extend the cycle life of such batteries. However, the poor electronic and ionic conductivities of S and Li2S result in a low reversible capacity. Therefore, an electrode design is required to achieve high-energy-density Li/S batteries. In this study, we investigated the charge-discharge mechanism of a solid solution of Li2S and LiI (Li2S-LiI) in all-solid-state batteries showing excellent electrochemical properties, including cycling performance. We found that a high reversible capacity was achieved despite the high conversion of Li2S into S because the ionic conductivity of the positive electrode was maintained during charging and discharging, and this was a result of the formation of an ionic conductive structure comprising LiI-rich domains. Crucially, essentially fully solid phase S/Li2S reactions in all-solid-state batteries were attained by fully eliminating the sulfide solid electrolyte from the positive electrode. These findings enable the design of S- and Li2S-based positive electrodes for solid phase redox reactions for use in high-energy-density Li/S batteries.
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