TY - JOUR
T1 - Discovery of High-Capacity Asymmetric Three-Stage Redox Reactions of Iodine for Aqueous Batteries
AU - Xie, Zehui
AU - Liu, Zaichun
AU - Hong, Hu
AU - Du, Kai
AU - Luo, Ruihao
AU - Sajid, Muhammad
AU - Zhu, Zhengxin
AU - Jiang, Taoli
AU - Wang, Mingming
AU - Meng, Yahan
AU - Wang, Weiping
AU - Xu, Jingwen
AU - Hu, Yuxiang
AU - Chen, Wei
N1 - Publisher Copyright:
© 2025 American Chemical Society.
PY - 2025
Y1 - 2025
N2 - Iodine-based batteries have emerged prominently in grid energy storage due to their cost-effectiveness and versatility. However, traditional iodine cathodes featuring I-/I0 mechanisms struggle to meet the current demands for high-energy-density batteries, considering their limited specific capacity and voltage. Here, we discover a unique eight-electron-transfer asymmetric three-stage conversion of iodine facilitated by the formation of interhalogens. This mechanism involves a three-stage sequential charging from I-/I0, to I0/ICl2-, and finally ICl2-/ICl4-, with the prolonged third charging plateau significantly enhancing the specific capacity to 809.2 mAh g-1 of I2. During discharge, the cathode undergoes highly reversible but asymmetric conversions, with ICl3- as the intermediate. The mechanism is achieved by a regulated “chloride-in-acid” electrolyte with interlocking H-bond structures, which effectively reduces the free water content and stabilizes the interhalogen species. The iodine-hydrogen gas battery demonstrates stable cycling performance with an average Coulombic efficiency exceeding 98.2% for over 1000 cycles and an increased voltage from 0.47 to 0.75 V compared with the I-/I0 mechanism, which can be further enhanced to 1.43 V by utilizing zinc anode. This study broadens the application of interhalogen chemistry into conversion reactions, presenting great prospects for high-energy-density aqueous batteries.
AB - Iodine-based batteries have emerged prominently in grid energy storage due to their cost-effectiveness and versatility. However, traditional iodine cathodes featuring I-/I0 mechanisms struggle to meet the current demands for high-energy-density batteries, considering their limited specific capacity and voltage. Here, we discover a unique eight-electron-transfer asymmetric three-stage conversion of iodine facilitated by the formation of interhalogens. This mechanism involves a three-stage sequential charging from I-/I0, to I0/ICl2-, and finally ICl2-/ICl4-, with the prolonged third charging plateau significantly enhancing the specific capacity to 809.2 mAh g-1 of I2. During discharge, the cathode undergoes highly reversible but asymmetric conversions, with ICl3- as the intermediate. The mechanism is achieved by a regulated “chloride-in-acid” electrolyte with interlocking H-bond structures, which effectively reduces the free water content and stabilizes the interhalogen species. The iodine-hydrogen gas battery demonstrates stable cycling performance with an average Coulombic efficiency exceeding 98.2% for over 1000 cycles and an increased voltage from 0.47 to 0.75 V compared with the I-/I0 mechanism, which can be further enhanced to 1.43 V by utilizing zinc anode. This study broadens the application of interhalogen chemistry into conversion reactions, presenting great prospects for high-energy-density aqueous batteries.
UR - http://www.scopus.com/inward/record.url?scp=105008274778&partnerID=8YFLogxK
U2 - 10.1021/jacs.5c03581
DO - 10.1021/jacs.5c03581
M3 - 文章
AN - SCOPUS:105008274778
SN - 0002-7863
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
ER -