Iodine/Chlorine Multi‐Electron Conversion Realizes High Energy Density Zinc‐Iodine Batteries

Abstract Aqueous zinc‐iodine (Zn‐I2) batteries are promising energy storage devices; however, the conventional single‐electron reaction potential and energy density of iodine cathode are inadequate for practical applications. Activation of high‐valence iodine cathode reactions has evoked a compellin...

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Main Authors: Jiajin Zhao, Yan Chen, Mengyan Zhang, Ziqi An, Binbin Nian, Wenfeng Wang, Hao Wu, Shumin Han, Yuan Li, Lu Zhang
Format: Article
Language:English
Published: Wiley 2025-01-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202410988
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author Jiajin Zhao
Yan Chen
Mengyan Zhang
Ziqi An
Binbin Nian
Wenfeng Wang
Hao Wu
Shumin Han
Yuan Li
Lu Zhang
author_facet Jiajin Zhao
Yan Chen
Mengyan Zhang
Ziqi An
Binbin Nian
Wenfeng Wang
Hao Wu
Shumin Han
Yuan Li
Lu Zhang
author_sort Jiajin Zhao
collection DOAJ
description Abstract Aqueous zinc‐iodine (Zn‐I2) batteries are promising energy storage devices; however, the conventional single‐electron reaction potential and energy density of iodine cathode are inadequate for practical applications. Activation of high‐valence iodine cathode reactions has evoked a compelling direction to developing high‐voltage zinc‐iodine batteries. Herein, ethylene glycol (EG) is proposed as a co‐solvent in a water‐in‐deep eutectic solvent (WiDES) electrolyte, enabling significant utilization of two‐electron‐transfer I+/I0/I− reactions and facilitating an additional reversibility of Cl0/Cl− redox reaction. Spectroscopic characterizations and calculations analyses reveal that EG integrates into the Zn2+ solvation structure as a hydrogen‐bond donor, competitively binding O atoms in H2O, which triggers a transition from water‐rich to water‐poor clusters of Zn2+, effectively disrupting the H2O hydrogen‐bond network. Consequently, the aqueous Zn‐I2 cell achieves an exceptional capacity of 987 mAh gI2−1 with an energy density of 1278 Wh kgI2−1, marking an enhancement of ≈300 mAh g−1 compared to electrolyte devoid of EG, and enhancing the Coulombic efficiency (CE) from 68.2% to 98.7%. Moreover, the pouch cell exhibits 3.72 mAh cm−2 capacity with an energy density of 4.52 mWh cm−2, exhibiting robust cycling stability. Overall, this work contributes to the further development of high‐valence and high‐capacity aqueous Zn‐I2 batteries.
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spelling doaj-art-668ed59712774737ba1002b4d241162d2025-01-09T11:44:46ZengWileyAdvanced Science2198-38442025-01-01121n/an/a10.1002/advs.202410988Iodine/Chlorine Multi‐Electron Conversion Realizes High Energy Density Zinc‐Iodine BatteriesJiajin Zhao0Yan Chen1Mengyan Zhang2Ziqi An3Binbin Nian4Wenfeng Wang5Hao Wu6Shumin Han7Yuan Li8Lu Zhang9College of Environment and Chemical Engineering Hebei Key Laboratory of Applied Chemistry State Key Laboratory of Metastable Materials Science and Technology Yanshan University Qinhuangdao 066004 P. R. ChinaCollege of Environment and Chemical Engineering Hebei Key Laboratory of Applied Chemistry State Key Laboratory of Metastable Materials Science and Technology Yanshan University Qinhuangdao 066004 P. R. ChinaCollege of Environment and Chemical Engineering Hebei Key Laboratory of Applied Chemistry State Key Laboratory of Metastable Materials Science and Technology Yanshan University Qinhuangdao 066004 P. R. ChinaCollege of Environment and Chemical Engineering Hebei Key Laboratory of Applied Chemistry State Key Laboratory of Metastable Materials Science and Technology Yanshan University Qinhuangdao 066004 P. R. ChinaState Key Laboratory of Materials‐Oriented Chemical Engineering School of Pharmaceutical Sciences Nanjing Tech University Nanjing Jiangsu 210009 P. R. ChinaCollege of Environment and Chemical Engineering Hebei Key Laboratory of Applied Chemistry State Key Laboratory of Metastable Materials Science and Technology Yanshan University Qinhuangdao 066004 P. R. ChinaCollege of Environment and Chemical Engineering Hebei Key Laboratory of Applied Chemistry State Key Laboratory of Metastable Materials Science and Technology Yanshan University Qinhuangdao 066004 P. R. ChinaCollege of Environment and Chemical Engineering Hebei Key Laboratory of Applied Chemistry State Key Laboratory of Metastable Materials Science and Technology Yanshan University Qinhuangdao 066004 P. R. ChinaCollege of Environment and Chemical Engineering Hebei Key Laboratory of Applied Chemistry State Key Laboratory of Metastable Materials Science and Technology Yanshan University Qinhuangdao 066004 P. R. ChinaCollege of Environment and Chemical Engineering Hebei Key Laboratory of Applied Chemistry State Key Laboratory of Metastable Materials Science and Technology Yanshan University Qinhuangdao 066004 P. R. ChinaAbstract Aqueous zinc‐iodine (Zn‐I2) batteries are promising energy storage devices; however, the conventional single‐electron reaction potential and energy density of iodine cathode are inadequate for practical applications. Activation of high‐valence iodine cathode reactions has evoked a compelling direction to developing high‐voltage zinc‐iodine batteries. Herein, ethylene glycol (EG) is proposed as a co‐solvent in a water‐in‐deep eutectic solvent (WiDES) electrolyte, enabling significant utilization of two‐electron‐transfer I+/I0/I− reactions and facilitating an additional reversibility of Cl0/Cl− redox reaction. Spectroscopic characterizations and calculations analyses reveal that EG integrates into the Zn2+ solvation structure as a hydrogen‐bond donor, competitively binding O atoms in H2O, which triggers a transition from water‐rich to water‐poor clusters of Zn2+, effectively disrupting the H2O hydrogen‐bond network. Consequently, the aqueous Zn‐I2 cell achieves an exceptional capacity of 987 mAh gI2−1 with an energy density of 1278 Wh kgI2−1, marking an enhancement of ≈300 mAh g−1 compared to electrolyte devoid of EG, and enhancing the Coulombic efficiency (CE) from 68.2% to 98.7%. Moreover, the pouch cell exhibits 3.72 mAh cm−2 capacity with an energy density of 4.52 mWh cm−2, exhibiting robust cycling stability. Overall, this work contributes to the further development of high‐valence and high‐capacity aqueous Zn‐I2 batteries.https://doi.org/10.1002/advs.202410988deep eutectic solvent electrolyteethylene glycolhigh energy densityiodinezinc battery
spellingShingle Jiajin Zhao
Yan Chen
Mengyan Zhang
Ziqi An
Binbin Nian
Wenfeng Wang
Hao Wu
Shumin Han
Yuan Li
Lu Zhang
Iodine/Chlorine Multi‐Electron Conversion Realizes High Energy Density Zinc‐Iodine Batteries
Advanced Science
deep eutectic solvent electrolyte
ethylene glycol
high energy density
iodine
zinc battery
title Iodine/Chlorine Multi‐Electron Conversion Realizes High Energy Density Zinc‐Iodine Batteries
title_full Iodine/Chlorine Multi‐Electron Conversion Realizes High Energy Density Zinc‐Iodine Batteries
title_fullStr Iodine/Chlorine Multi‐Electron Conversion Realizes High Energy Density Zinc‐Iodine Batteries
title_full_unstemmed Iodine/Chlorine Multi‐Electron Conversion Realizes High Energy Density Zinc‐Iodine Batteries
title_short Iodine/Chlorine Multi‐Electron Conversion Realizes High Energy Density Zinc‐Iodine Batteries
title_sort iodine chlorine multi electron conversion realizes high energy density zinc iodine batteries
topic deep eutectic solvent electrolyte
ethylene glycol
high energy density
iodine
zinc battery
url https://doi.org/10.1002/advs.202410988
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AT ziqian iodinechlorinemultielectronconversionrealizeshighenergydensityzinciodinebatteries
AT binbinnian iodinechlorinemultielectronconversionrealizeshighenergydensityzinciodinebatteries
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