Tellurium with Reversible Six-Electron Transfer Chemistry for High-Performance Zinc Batteries.
Ze ChenShengnan WangZhiquan WeiYiqiao WangZhuoxi WuYue HouJiaxiong ZhuYanbo WangGuojin LiangZhaodong HuangAo ChenDonghong WangChunyi ZhiPublished in: Journal of the American Chemical Society (2023)
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 Te 2- /Te 0 redox with a low voltage plateau at ∼0.59 V (vs Zn 2+ /Zn) rather than the expected positive valence conversion of Te 0 to Te n + , inhibiting the development of Te-based batteries toward high output voltage and energy density. Herein, the desired reversible Te 2- /Te 0 /Te 2+ /Te 4+ 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 Te n + 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 kg Te -1 or 227 Wh L cathdoe+anode -1 ), 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.