Local Electric Field Microenvironment-Induced Dynamic Spatial Confinement to Stabilize I+ Toward High-Mass-Loading and Stable Zinc-Iodine Batteries

Liting Chen; Song Huang; Zhenfeng Feng; Zhenxin Lin; Haolong Huang; Minghui Ye; Yufei Zhang; Zhipeng Wen; Yongchao Tang; Xiaoqing Liu; Cheng Chao Li

doi:10.1002/anie.202510737

Local Electric Field Microenvironment-Induced Dynamic Spatial Confinement to Stabilize I⁺ Toward High-Mass-Loading and Stable Zinc-Iodine Batteries

Angew Chem Int Ed Engl. 2025 Jul 2:e202510737. doi: 10.1002/anie.202510737. Online ahead of print.

Authors

Liting Chen^#^{1

2}, Song Huang^#^{1

2}, Zhenfeng Feng^#^{1

2}, Zhenxin Lin^{1

2}, Haolong Huang^{1

2}, Minghui Ye^{1

2}, Yufei Zhang^{1

2}, Zhipeng Wen^{1

2}, Yongchao Tang^{1

2}, Xiaoqing Liu^{1

2}, Cheng Chao Li^{1

2}

Affiliations

¹ School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou, 510006, P.R. China.
² Guangdong Provincial Laboratory of Chemistry and Fine, Chemical Engineering Jieyang Center, Jieyang, 515200, P.R. China.

^# Contributed equally.

PMID: 40600661
DOI: 10.1002/anie.202510737

Abstract

Four-electron iodine conversion chemistry (I^-/I₂/I⁺) endows zinc-iodine batteries with competitive energy density. The stability of I⁺ conversion relies on its interaction with sufficient nucleophilic species (e.g., Cl^-, Br^-). However, under high iodine loading, nucleophilic species fail to afford sufficient coordination strength and number within thick iodine cathode to stabilize I⁺, thus compromising the high-voltage plateau and capacity. Here, we effectively spatially confine nucleophilic species (Cl^-) on the cathode by ─C─N⁺-induced localized electric field (LEF) microenvironment in polyquaternary ammonium iodide (PDDA-I). Spatial confinement maximizes Cl^- concentration on the cathode ensuring highly reversible I⁰/I⁺ conversion, even in the low-concentrated ZnCl₂ addition and high iodine loading. Importantly, the dynamically regulated Cl^- maintains a balance with iodine species at the ─C─N⁺ sites during cycling, effectively limiting the shuttling effect of polyiodides. Consequently, even adopting a high iodine loading of 16.03 mg cm^-2, the PDDA-I still maintains a distinct four-electron-conversion dual voltage plateau with a remarkable capacity of 4.97 mAh cm^-2. An impressive lifespan of 10 000 cycles is achieved at 12.6 mg cm^-2 with a capacity decay of 0.0012% per cycle, exceeding conventional iodine cathodes by 20-fold. This work provides an important reference for high-performance four-electron conversion zinc-iodine batteries at high iodine loading.

Keywords: High iodine mass loading; Local electric field microenvironment; Polyquaternary ammonium salt; Spatial confinement; Zn–I2 battery.

Abstract

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