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Interfacial Evolution of Lithium Dendrites and Their Solid Electrolyte Interphase Shells of Quasi-Solid-State Lithium-Metal Batteries
Authors:Yang Shi  Jing Wan  Gui-Xian Liu  Tong-Tong Zuo  Yue-Xian Song  Prof Dr Bing Liu  Prof Dr Yu-Guo Guo  Prof Dr Rui Wen  Prof Dr Li-Jun Wan
Institution:1. Key Laboratory of Molecular Nanostructure and Nanotechnology, Beijing National Laboratory for Molecular Sciences, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China

University of the Chinese Academy of Sciences (China), Beijing, 100049 P. R. China

These authors contributed equally to this work.;2. Key Laboratory of Molecular Nanostructure and Nanotechnology, Beijing National Laboratory for Molecular Sciences, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China

University of the Chinese Academy of Sciences (China), Beijing, 100049 P. R. China;3. State Key Laboratory of Polymer Physics and Chemistry, Beijing National Laboratory for Molecular Sciences, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 China

University of the Chinese Academy of Sciences (China), Beijing, 100049 P. R. China;4. Key Laboratory of Molecular Nanostructure and Nanotechnology, Beijing National Laboratory for Molecular Sciences, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China

Abstract:Unstable electrode/solid-state electrolyte interfaces and internal lithium dendrite penetration hamper the applications of solid-state lithium-metal batteries (SSLMBs), and the underlying mechanisms are not well understood. Herein, in situ optical microscopy provides insights into the lithium plating/stripping processes in a gel polymer electrolyte and reveals its dynamic evolution. Spherical lithium deposits evolve into moss-like and branch-shaped lithium dendrites with increasing current densities. Remarkably, the on-site-formed solid electrolyte interphase (SEI) shell on the lithium dendrite is distinctly captured after lithium stripping. Inducing an on-site-formed SEI shell with an enhanced modulus to wrap the lithium precipitation densely and uniformly can regulate dendrite-free behaviors. An in-depth understanding of lithium dendrite evolution and its functional SEI shell will aid in the optimization of SSLMBs.
Keywords:batteries  dendrites  electrolytes  gel polymers  lithium
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