Статья

Origin of dendrite-free lithium deposition in concentrated electrolytes

Yawei ChenHefei National Laboratory for Physical Science at Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, ChinaMenghao LiDepartment of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055, ChinaYue LiuInstitute of Functional Nano and Soft Materials (FUNSOM), Soochow University, Suzhou, 215123, ChinaYulin JieHefei National Laboratory for Physical Science at Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, ChinaWanxia LiHefei National Laboratory for Physical Science at Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, ChinaFanyang HuangHefei National Laboratory for Physical Science at Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, ChinaXinpeng LiHefei National Laboratory for Physical Science at Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, ChinaZixu HeHefei National Laboratory for Physical Science at Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, ChinaXiaodi RenHefei National Laboratory for Physical Science at Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, ChinaYunhua ChenHefei National Laboratory for Physical Science at Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, ChinaXianhui MengNIO Incorporation, Shanghai, 201800, ChinaTao ChengInstitute of Functional Nano and Soft Materials (FUNSOM), Soochow University, Suzhou, 215123, China. [email protected]Meng GuDepartment of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055, China. [email protected]Shuhong JiaoHefei National Center for Physical Sciences at NanoscaleRuiguo CaoHefei National Laboratory for Physical Science at Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China. [email protected]

2023en

ABI

Аннотация

Abstract The electrolyte solvation structure and the solid-electrolyte interphase (SEI) formation are critical to dictate the morphology of lithium deposition in organic electrolytes. However, the link between the electrolyte solvation structure and SEI composition and its implications on lithium morphology evolution are poorly understood. Herein, we use a single-salt and single-solvent model electrolyte system to systematically study the correlation between the electrolyte solvation structure, SEI formation process and lithium deposition morphology. The mechanism of lithium deposition is thoroughly investigated using cryo-electron microscopy characterizations and computational simulations. It is observed that, in the high concentration electrolytes, concentrated Li + and anion-dominated solvation structure initiate the uniform Li nucleation kinetically and favor the decomposition of anions rather than solvents, resulting in inorganic-rich amorphous SEI with high interface energy, which thermodynamically facilitates the formation of granular Li. On the contrary, solvent-dominated solvation structure in the low concentration electrolytes tends to exacerbate the solvolysis process, forming organic-rich mosaic SEI with low interface energy, which leads to aggregated whisker-like nucleation and growth. These results are helpful to tackle the long-standing question on the origin of lithium dendrite formation and guide the rational design of high-performance electrolytes for advanced lithium metal batteries.

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Идентификаторы

DOI: 10.1038/s41467-023-38387-8

Цитирования и источники

Цитирований: 3Использованных источников: 0

Показатели — AkademScholar