Facile synthesis of a mixed-conductive Li2S composites for all-solid-state lithium-sulfur batteries

Jiang, Huize; Han, Yu; Wang, Hui; Zhu, Yan; Guo, Qingpeng; Jiang, Haolong; Zheng, Chunman; Xie, Kai

doi:10.1007/s11581-020-03591-9

Cited by 11 publications

(9 citation statements)

References 41 publications

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“…99.5Li 2 SÁ 0.5AlI 3 ) demonstrated the best cell performance among the prepared cathode materials even though the ionic and electronic conductivity of Li 2 S-AlI 3 increased with increasing AlI 3 The capacities of all cells increased during the first 10 cycles, which has been well reported so far but the reason is not yet evident. 6,18,[34][35][36] One reason for the increase of capacity during the starting cycles may be the decomposition reactions of the solid electrolyte. 37 It is believed that the solid electrolyte in the cathode composite is activated by the high-energy ball milling employed to prepare the positive electrode composite in our study.…”

Section: Resultsmentioning

confidence: 99%

Synthesis of an AlI₃-doped Li₂S positive electrode with superior performance in all-solid-state batteries

et al. 2022

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Section: Resultsmentioning

confidence: 99%

Synthesis of an AlI₃-doped Li₂S positive electrode with superior performance in all-solid-state batteries

et al. 2022

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“…Nevertheless, high-resolution transmission electron microscopy (HR-TEM) observations have revealed the local structure of nanocomposite S/Li 2 S–carbon–sulfide SE electrodes prepared by ball milling before and after charge–discharge cycling. − It has been shown that triple-phase contacts, which are the contact points of electronic and ionic conductors and electrode active materials, are required for the electrochemical reaction of sulfur. Nanocomposites allow nanoscale electron and ion conduction pathways in the positive electrodes and can therefore enable high reversible capacities despite a high active material content. − One way to form a suitable composite is to mix sulfide SEs with conductive carbon additives. The electrochemical decomposition products of the SEs can then act as active materials. − However, only a few studies have attempted to determine the precise mechanism by which the ionic conduction path of SE affects the reversible capacity of S/Li 2 S. , We recently developed a Li 2 S–LiI solid solution with an antifluorite-type structure that exhibits a higher ionic conductivity than that of Li 2 S .…”

Section: Introductionmentioning

confidence: 99%

Li₂S–LiI Solid Solutions with Ionic Conductive Domains for Enhanced All-Solid-State Li/S Batteries

Fujita

Hakari

Sakuda

et al. 2022

ACS Appl. Energy Mater.

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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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“…To improve the electric transport properties in cathode composites, several research groups have developed cathode composites mixed with highly conductive electron additives and SEs . For instance, electron additives, such as mesoporous carbon, carbon nanotubes, − and reduced graphene oxide were blended into cathode composites. Similarly, sulfide-based SEs such as Li 10 GeP 2 S 12 , − Li 7 P 3 S 11 , Li 7 P 2 S 8 I, and Li 6 PS 5 Cl, − are used in cathode composites.…”

Section: Introductionmentioning

confidence: 99%

Understanding Decomposition of Electrolytes in All-Solid-State Lithium–Sulfur Batteries

2022

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The decomposition behavior of electrolytes affects the cycle stability and electrochemical redox activity in all-solid-state lithium−sulfur batteries (ASSLSBs). However, there is a sparse understanding of the electrochemistry of ASSLSBs involving the oxidative decomposition of sulfide solid electrolytes (SEs) due to the lack of fundamental studies. Herein, we unveil the redox chemistry related to Li 2 S/S conversion reaction, electrolyte decomposition, and redox reaction of the decomposition product, based on differential capacity curves. The oxidation reaction of Li 2 S proceeds simultaneously with a continuous oxidative decomposition of sulfide SEs. Raman spectroscopy of the cell after cycling shows that SEs in the cathode convert the thiophosphates with a S−S thiol bond via the decomposition behavior of the electrolytes. The implication of this reaction chemistry is expanded toward understanding the Li 2 S activation process in ASSLSBs. Additionally, we demonstrate that Li 2 S/SE interface modification by different rotation speeds of ball milling in SE mixing allows us to control the decomposition kinetics of electrolytes. The severe decomposition of electrolytes causes cycle fading instead of increasing the electrochemical redox activity in the early period. The findings of this work highlight the need for interface engineering to avoid severe degradation of electrolytes in the cathode and enhance the ability of SEs as a redox mediator.

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Facile synthesis of a mixed-conductive Li2S composites for all-solid-state lithium-sulfur batteries

Cited by 11 publications

References 41 publications

Synthesis of an AlI₃-doped Li₂S positive electrode with superior performance in all-solid-state batteries

Synthesis of an AlI₃-doped Li₂S positive electrode with superior performance in all-solid-state batteries

Li₂S–LiI Solid Solutions with Ionic Conductive Domains for Enhanced All-Solid-State Li/S Batteries

Understanding Decomposition of Electrolytes in All-Solid-State Lithium–Sulfur Batteries

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Facile synthesis of a mixed-conductive Li2S composites for all-solid-state lithium-sulfur batteries

Cited by 11 publications

References 41 publications

Synthesis of an AlI3-doped Li2S positive electrode with superior performance in all-solid-state batteries

Synthesis of an AlI3-doped Li2S positive electrode with superior performance in all-solid-state batteries

Li2S–LiI Solid Solutions with Ionic Conductive Domains for Enhanced All-Solid-State Li/S Batteries

Understanding Decomposition of Electrolytes in All-Solid-State Lithium–Sulfur Batteries

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Synthesis of an AlI₃-doped Li₂S positive electrode with superior performance in all-solid-state batteries

Synthesis of an AlI₃-doped Li₂S positive electrode with superior performance in all-solid-state batteries

Li₂S–LiI Solid Solutions with Ionic Conductive Domains for Enhanced All-Solid-State Li/S Batteries