Three-Electron Transfer-Based High-Capacity Organic Lithium-Iodine (Chlorine) Batteries

作者：Li, Xinliang; Wang, Yanlei; Lu, Junfeng; Li, Shimei; Li, Pei; Huang, Zhaodong; Liang, Guojin; He, Hongyan^*; Zhi, Chunyi^*

来源：Angewandte Chemie - International Edition, 2023, 62(42).

DOI：10.1002/anie.202310168

• Chloride Redox
• Electrochemistry
• Halogen Battery
• Interhalogens
• Multi-Electron Conversion

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. @@@ The static organic lithium-iodine (chlorine) batteries fueled by brand-new three-electron redox chemistry (redox couples: I-/I+ and Cl-/Cl0) with electrochemically active tetrabutylammonium triiodide cathode exhibit the excellent specific energy density, representing a significant advancement in the field of halogen battery.+image

• 单位
  郑州大学; 中国科学院