Tellurium with Reversible Six-Electron Transfer Chemistry for High-Performance Zinc Batteries

作者：Chen, Ze; Wang, Shengnan; Wei, Zhiquan; Wang, Yiqiao; Wu, Zhuoxi; Hou, Yue; Zhu, Jiaxiong; Wang, Yanbo; Liang, Guojin; Huang, Zhaodong; Chen, Ao; Wang, Donghong^*; Zhi, Chunyi^*

来源：Journal of the American Chemical Society, 2023, 145(37): 20521-20529.

DOI：10.1021/jacs.3c06488

• CATHODE MATERIAL
• ION BATTERY
• ELECTROLYTES

Chalcogens, especially tellurium (Te), as conversion-type cathodes possess promising prospects for zinc batteries (ZBs) with potential rich valence supply and high energy density. However, the conversion reaction of Te is normally restricted to the Te2-/Te-0 redox with a low voltage plateau at similar to 0.59 V (vs Zn2+/Zn) rather than the expected positive valence conversion of Te-0 to Ten+, inhibiting the development of Te-based batteries toward high output voltage and energy density. Herein, the desired reversible Te2-/Te-0/Te2+/Te4+ redox behavior with up to six-electron transfer was successfully activated by employing a highly concentrated Cl--containing electrolyte (Cl- as strong nucleophile) for the first time. Three flat discharge plateaus located at 1.24, 0.77, and 0.51 V, respectively, are attained with a total capacity of 802.7 mAh g(-1). Furthermore, to improve the stability of Ten+ products and enhance the cycling stability, a modified ionic liquid (IL)-based electrolyte was fabricated, leading to a high-performance Zn.Te battery with high areal capacity (7.13 mAh cm(-2)), high energy density (542 Wh kgTe(-1) or 227 Wh Lcathdoe+ (-1)(anode)), excellent cycling performance, and a low self-discharge rate based on 400 mAh-level pouch cell. The results enhance the understanding of tellurium chemistry in batteries, substantially promising a remarkable route for advanced ZBs.