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Three-Electron Transfer-Based High-Capacity Organic Lithium-Iodine (Chlorine) Batteries
Authors:Xinliang Li  Yanlei Wang  Junfeng Lu  Shimei Li  Pei Li  Zhaodong Huang  Guojin Liang  Hongyan He  Chunyi Zhi
Institution:1. Key Laboratory of Material Physics, Ministry of Education, School of Physics and Microelectronics, Zhengzhou University, Zhengzhou, 450052 China

Department of Materials Science and Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong, 999077 China

These authors contributed equally to this work.;2. Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190 China

These authors contributed equally to this work.;3. Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190 China;4. Department of Materials Science and Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong, 999077 China

Hong Kong Center for Cerebro-Cardiovascular Health Engineering (COCHE), 999077 Shatin, NT, HKSAR, China;5. Department of Materials Science and Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong, 999077 China

Abstract:Conversion-type batteries apply the principle that more charge transfer is preferable. The underutilized electron transfer mode within two undermines the electrochemical performance of halogen batteries. Here, we realised a three-electron transfer lithium-halogen battery based on I/I+ and Cl/Cl0 couples by using a common commercial electrolyte saturated with Cl anions. The resulting Li||tetrabutylammonium triiodide (TBAI3) cell exhibits three distinct discharging plateaus at 2.97, 3.40, and 3.85 V. Moreover, it has a high capacity of 631 mAh g−1I (265 mAh g−1electrode, based on entire mass loading) and record-high energy density of up to 2013 Wh kg−1I (845 Wh kg−1electrode). To support these findings, experimental characterisations and density functional theory calculations were conducted to elucidate the redox chemistry involved in this novel interhalogen strategy. We believe our paradigm presented here has a foreseeable inspiring effect on other halogen batteries for high-energy-density pursuit.
Keywords:Chloride Redox  Electrochemistry  Halogen Battery  Interhalogens  Multi-Electron Conversion
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