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Space-Confined Atomic Clusters Catalyze Superassembly of Silicon Nanodots within Carbon Frameworks for Use in Lithium-Ion Batteries
Authors:Bingjie Chen  Dr. Lianhai Zu  Dr. Yao Liu  Dr. Ruijing Meng  Yutong Feng  Prof. Chengxin Peng  Feng Zhu  Tianzi Hao  Jiajia Ru  Prof. Yonggang Wang  Prof. Jinhu Yang
Affiliation:1. School of Chemical Science and Engineering, Tongji University, Shanghai, 200092 P. R. China

Research Center for Translational Medicine & Key Laboratory of Arrhythmias of the Ministry of Education of China, East Hospital, Tongji University School of Medicine, No. 150 Jimo Road, Shanghai, 200120 P. R. China;2. School of Chemical Science and Engineering, Tongji University, Shanghai, 200092 P. R. China

Department of Chemical Engineering, Monash University, Clayton, Australia;3. Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Institute of New Energy, Fudan University, Shanghai, 200433 China;4. School of Chemical Science and Engineering, Tongji University, Shanghai, 200092 P. R. China;5. School of Materials Science and Engineering, University of Shanghai for Science and Technology, Shanghai, 200093 China;6. School of Aerospace Engineering and Applied Mechanics, Tongji University, Shanghai, 200433 China

Abstract:Incorporating nanoscale Si into a carbon matrix with high dispersity is desirable for the preparation of lithium-ion batteries (LIBs) but remains challenging. A space-confined catalytic strategy is proposed for direct superassembly of Si nanodots within a carbon (Si NDs⊂C) framework by copyrolysis of triphenyltin hydride (TPT) and diphenylsilane (DPS), where Sn atomic clusters created from TPT pyrolysis serve as the catalyst for DPS pyrolysis and Si catalytic growth. The use of Sn atomic cluster catalysts alters the reaction pathway to avoid SiC generation and enable formation of Si NDs with reduced dimensions. A typical Si NDs⊂C framework demonstrates a remarkable comprehensive performance comparable to other Si-based high-performance half LIBs, and higher energy densities compared to commercial full LIBs, as a consequence of the high dispersity of Si NDs with low lithiation stress. Supported by mechanic simulations, this study paves the way for construction of Si/C composites suitable for applications in future energy technologies.
Keywords:Atomare Cluster  Kohlenstoffmatrizen  Pyrolyse-Strategien  Silicium  Strukturelle Stabilität
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