Revealing the High Salt Concentration Manipulated Evolution Mechanism on the Lithium Anode in Quasi‐Solid‐State Lithium‐Sulfur Batteries

• Published in: Angewandte Chemie International Edition Vol. 61; no. 52; pp. e202212744 - n/a
• Main Authors: Liu, Gui‐Xian, Tian, Jian‐Xin, Wan, Jing, Li, Yuan, Shen, Zhen‐Zhen, Chen, Wan‐Ping, Zhao, Yao, Wang, Fuyi, Liu, Bing, Xin, Sen, Guo, Yu‐Guo, Wen, Rui
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 23.12.2022
• Edition: International ed. in English
• Subjects: Anions; Anode Process; Anodes; Batteries; Electrochemical analysis; Electrochemistry; Electrolytes; Energy storage; High Salt Concentration; In-Situ AFM; Interfacial properties; Lithium; Lithium sulfur batteries; Molecular dynamics; Molten salt electrolytes; Quasi-Solid-State Lithium-Sulfur Battery; Reaction mechanisms; Salts; Solid Electrolyte Interphase; Solid electrolytes; Storage batteries; Sulfur; Sulphur; High Salt Concentration; In-Situ AFM; Solid Electrolyte Interphase; Anode Process; Quasi-Solid-State Lithium-Sulfur Battery
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202212744

Lithium‐sulfur batteries are promising candidates of energy storage devices. Both adjusting salt/solvent ratio and applying quasi‐solid‐state electrolytes are regarded as effective strategies to improve the lithium (Li) anode performance. However, reaction mechanisms and interfacial properties in quasi‐solid‐state lithium‐sulfur (QSSLS) batteries with high salt concentration are not clear. Here we utilize in‐situ characterizations and molecular dynamics simulations to unravel aforesaid mysteries, and construct relationships of electrolyte structure, interfacial behaviour and performance. The generation mechanism, formation process, and mechanical/chemical/electrochemical properties of the anion‐derived solid electrolyte interphase (SEI) are deeply explored. Li deposition uniformity and dissolution reversibility are further tuned by the sustainable SEI. These straightforward evidences and deepgoing studies would guide the electrolyte design and interfacial engineering of QSSLS batteries. The electrochemical processes at the Li anode/electrolyte interface are disclosed in quasi‐solid‐state lithium‐sulfur batteries with high salt concentration via in‐situ atomic force microscopy and optical microscopy. The 3D morphology, local mechanics, and ion conductivity of the on‐site formed solid electrolyte interphase are in‐situ measured and analyzed to reveal the regulation effect of high salt concentration on interfacial electrochemistry.