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Antipulverization Electrode Based on Low‐Carbon Triple‐Shelled Superstructures for Lithium‐Ion Batteries
Authors:Lianhai Zu  Qingmei Su  Feng Zhu  Bingjie Chen  Huanhuan Lu  Chengxin Peng  Ting He  Gaohui Du  Pengfei He  Kai Chen  Shihe Yang  Jinhu Yang  Huisheng Peng
Affiliation:1. School of Chemical Science and Engineering, Tongji University, Shanghai, China;2. Research Center for Translational Medicine and Key Laboratory of Arrhythmias of the Ministry of Education of China, East Hospital, Tongji University School of Medicine, Shanghai, P. R. China;3. Institute of Physical Chemistry, Zhejiang Normal University, Jinhua, P. R. China;4. School of Aerospace Engineering and Applied Mechanics, Tongji University, Shanghai, China;5. Center for Advancing Materials Performance from the Nanoscale (CAMP‐Nano), State Key Laboratory for Mechanical Behavior of Materials, Xi'an Jiaotong University, Xi'an, China;6. School of Materials Science and Engineering, Tongji University, Shanghai, China;7. Department of Chemistry, The Hong Kong University of Science and Technology, Kowloon, Hong Kong, China;8. State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science and Laboratory of Advanced Materials, Fudan University, Shanghai, China
Abstract:The realization of antipulverization electrode structures, especially using low‐carbon‐content anode materials, is crucial for developing high‐energy and long‐life lithium‐ion batteries (LIBs); however, this technology remains challenging. This study shows that SnO2 triple‐shelled hollow superstructures (TSHSs) with a low carbon content (4.83%) constructed by layer‐by‐layer assembly of various nanostructure units can withstand a huge volume expansion of ≈231.8% and deliver a high reversible capacity of 1099 mAh g?1 even after 1450 cycles. These values represent the best comprehensive performance in SnO2‐based anodes to date. Mechanics simulations and in situ transmission electron microscopy suggest that the TSHSs enable a self‐synergistic structure‐preservation behavior upon lithiation/delithiation, protecting the superstructures from collapse and guaranteeing the electrode structural integrity during long‐term cycling. Specifically, the outer shells during lithiation processes are fully lithiated, preventing the overlithiation and the collapse of the inner shells; in turn, in delithiation processes, the underlithiated inner shells work as robust cores to support the huge volume contraction of the outer shells; meanwhile, the middle shells with abundant pores offer sufficient space to accommodate the volume change from the outer shell during both lithiation and delithiation. This study opens a new avenue in the development of high‐performance LIBs for practical energy applications.
Keywords:antipulverization  carbon  lithium‐ion batteries  SnO2  triple‐shelled structure
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