Activating iodine redox by enabling single-atom coordination to dormant nitrogen sites to realize durable zinc–iodine batteries

Lee, Jisung; Lee, Wooseok; Back, Seungho; Yi, Seung Yeop; Lee, Seonggyu; Kim, Seongseop; Moon, Joonhee; Koh, Dong-Yeun; Kim, Kyeounghak; Back, Seoin; Lee, Jinwoo

doi:10.1039/d3ey00228d

EES. Catal.

2024

DOI: 10.1039/d3ey00228d

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Activating iodine redox by enabling single-atom coordination to dormant nitrogen sites to realize durable zinc–iodine batteries

Jisung Lee,

Wooseok Lee,

Seungho Back

et al.

Abstract: The introduction of a single Ni atom into an inactive N-doped carbon matrix, through its role as an electrocatalyst, awakens the dormant N sites, significantly suppressing the polyiodide shuttle effect and enhancing iodine redox kinetics.

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Cited by 4 publications

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Confining Iodine into Metal‐Organic Framework Derived Metal‐Nitrogen‐Carbon for Long‐Life Aqueous Zinc‐Iodine Batteries

Guo,

Xu,

Tang

et al. 2024

Advanced Materials

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Aqueous zinc–iodine batteries (AZIBs) are highly appealing for energy requirements owing to their safety, cost‐effectiveness, and scalability. However, the inadequate redox kinetics and severe shuttling effect of polyiodide ions impede their commercial viability. Herein, several Zn‐MOF‐derived porous carbon materials are designed, and the further preparation of iron–doped porous carbon (Fe–N–C, M9) with varied Fe doping contents is optimized based on a facile self‐assembly/carbonization approach. M9, with atomic Fe coordinated to nitrogen atoms, is employed as an efficient cathode host for AZIBs. Functional modifications of porous carbon hosts involving the doping species and levels are investigated. The adsorption tests, in situ Raman spectroscopy, and in situ UV–vis results demonstrate the adsorption capability and charge‐discharge mechanism for the iodine species. Furthermore, experimental findings and theoretical analyses have proven that the redox conversion of iodine is enhanced through a physicochemical confinement effect. This study offers basic principles for the strategic design of single‐atom dispersed carbon as an iodine host for high‐performance AZIBs. Flexible soft–pack battery and wearable microbattery applications also have implications for future long‐life aqueous battery designs.

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Confining Iodine into Metal‐Organic Framework Derived Metal‐Nitrogen‐Carbon for Long‐Life Aqueous Zinc‐Iodine Batteries

Guo,

Xu,

Tang

et al. 2024

Advanced Materials

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A Versatile Redox‐Active Electrolyte for Solid Fixation of Polyiodide and Dendrite‐Free Operation in Sustainable Aqueous Zinc‐Iodine Batteries

Back,

Xu,

Moon

et al. 2024

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Practical utilization of zinc‐iodine (Zn‐I2) batteries is hindered by significant challenges, primarily stemming from the polyiodide shuttle effect on the cathode and dendrite growth on the anode. Herein, a feasible redox‐active electrolyte has been introduced with tetraethylammonium iodide as an additive that simultaneously addresses the above mentioned challenges via polyiodide solidification on the cathode and the electrostatic shielding effect on the anode. The tetraethylammonium (TEA+) captures water‐soluble polyiodide intermediates (I3−, I5−), forming a solid complex at the cathode, thereby suppressing capacity loss during charge/discharge. Furthermore, the TEA+ mitigates dendrite growth on the Zn anode via the electrostatic shielding effect, promoting uniform and compact Zn deposition at the anode. Consequently, the Zn||Zn symmetric cell demonstrates superior cycling stability during Zn plating/stripping over 4,200 h at 1 mA cm−2 and 1 mAh cm−2. The Zn||NiNC full‐cell exhibits a stable capacity retention of 98.4% after 20 000 cycles (>5 months) with near‐unity Coulombic efficiency at 1 A g−1. The study provides novel insights for establishing a new direction for low‐cost, sustainable, and long‐lifespan Zn‐I2 batteries.

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Insights into the synergy effect in dual single-atom catalysts on defective CeO2 under CO2 hydrogenation

Park,

Hong,

Han

et al. 2025

Applied Catalysis B: Environment and Energy

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Activating iodine redox by enabling single-atom coordination to dormant nitrogen sites to realize durable zinc–iodine batteries

Abstract: The introduction of a single Ni atom into an inactive N-doped carbon matrix, through its role as an electrocatalyst, awakens the dormant N sites, significantly suppressing the polyiodide shuttle effect and enhancing iodine redox kinetics.

Cited by 4 publications

References 55 publications

Confining Iodine into Metal‐Organic Framework Derived Metal‐Nitrogen‐Carbon for Long‐Life Aqueous Zinc‐Iodine Batteries

Confining Iodine into Metal‐Organic Framework Derived Metal‐Nitrogen‐Carbon for Long‐Life Aqueous Zinc‐Iodine Batteries

A Versatile Redox‐Active Electrolyte for Solid Fixation of Polyiodide and Dendrite‐Free Operation in Sustainable Aqueous Zinc‐Iodine Batteries

Insights into the synergy effect in dual single-atom catalysts on defective CeO2 under CO2 hydrogenation

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