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Engineering Solid Electrolyte Interface at Nano-Scale for High-Performance Hard Carbon in Sodium-Ion Batteries
Authors:Mengying Ma  Haoran Cai  Chenlu Xu  Renzhi Huang  Shurong Wang  Huilin Pan  Yong-Sheng Hu
Affiliation:1. Department of Chemistry, Zhejiang University, Hangzhou, 310027 China

State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou, 310027 China;2. Department of Chemistry, Zhejiang University, Hangzhou, 310027 China;3. Beijing Advanced Innovation Center for Materials Genome Engineering, Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190 China

Abstract:Engineering the structure and chemistry of solid electrolyte interface (SEI) on electrode materials is crucial for rechargeable batteries. Using hard carbon (HC) as a platform material, a correlation between Na+ storage performance, and the properties of SEI is comprehensively explored. It is found that a “good” SEI layer on HC may not be directly associated with certain kinds of SEI components, such as NaF and Na2O. Whereas, arranging nano SEI components with refined structures constructs the foundation of “good” SEI that enables fast Na+ storage and interface stability of HC in Na-ion batteries. A layer-by-layer SEI on HC with inorganic-rich inner layer and tolerant organic-rich outer flexible layer can facilitate excellent rate and cycling life. Besides, SEI layer as the gate for Na+ from electrolyte to HC electrode can modulate interfacial crystallographic structures of HC with pillar-solvent that function as “pseudo-SEI” for fast and stable Na+ storage in optimal 1 m NaPF6-TEGDME electrolytes. Such a layer-by-layer SEI combined with a “pseudo-SEI” layer for HC enables an outstanding rate of 192 mAh g?1 at 2 C and stable cycling over 1100 cycles at 0.5 C. This study provides valuable guidance to improve the electrochemical performance of electrode materials through regulation of SEI in optimal electrolytes.
Keywords:hard carbon  pseudo-SEI  SEI chemistry  SEI structure  sodium ion batteries
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