As one of the most appealing energy storage technologies, aqueous zinc‐iodine batteries still suffer severe problems such as low energy density, slow iodine conversion kinetics, and polyiodide shuttle. This review summarizes the recent development of Zn─I2 batteries with a focus on the electrochemistry of iodine conversion and the underlying working mechanism. Starting from the fundamentals of Zn─I2 batteries, the electrochemistry of iodine conversion and zinc anode, as well as the scientific problems existing in Zn─I2 batteries are introduced. The concrete strategies dealing with cathode, anode, electrolyte, and separator challenges confronting Zn─I2 batteries are elaborated as well. To deepen the understanding of the electrochemistry of Zn─I2 batteries, the recent important findings of the underlying working mechanism of different Zn─I2 batteries are summarized in detail. Finally, some guidelines and directions for Zn─I2 batteries are also provided. This review is expected to deepen the understanding of Zn─I2 battery electrochemistry and promote their practical applications in the future.

Aqueous Zinc‐Iodine Batteries: From Electrochemistry to Energy Storage Mechanism

Aqueous dual-ion batteries (ADIBs) based on the cooperative redox of cations and iodine anions at the anode and cathode respectively, are attracting increasing interest because of high capacity and safety. However, the full-cell performance is limited by the sluggish iodine redox kinetics between iodide and polyiodide involving multiple electron transfer steps, and the undesirable shuttling effect of polyiodides. Here we report a versatile conjugated microporous polymer functionalized with secondary amine groups as an organocatalytic cathode for ADIB, which can be positively charged and electrostatically adsorb iodide, and organocatalyze iodine redox reactions through the amine groups. Both theoretical calculations and controlled experiments confirm that the secondary amine groups confine (poly)iodide species via hydrogen bonding, which is essential for accelerating iodine redox kinetics and reducing the polyiodide shuttling effect. The ADIB achieves an ultra-high capacity of 730 mAh g-1 with an ultra-small overpotential of 47 mV at 1 A g-1 , which also exhibits excellent rate performance and long cycling stability with a capacity retention of 74% after 5000 cycles at a high current density of 5 A g-1 . This work demonstrates the promise of developing organocatalysts for accelerating electrochemical processes, which remains a virtually unexplored area in electrocatalyst design for clean energy applications. This article is protected by copyright. All rights reserved.

Secondary Amines Functionalized Organocatalytic Iodine Redox for High-Performance Aqueous Dual-Ion Batteries.

Recently, aqueous zinc-ion batteries with conversion mechanisms have received wide attention in energy storage systems on account of excellent specific capacity, high power density, and energy density. Unfortunately, some characteristics of cathode material, zinc anode, and electrolyte still limit the development of aqueous zinc-ion batteries possessing conversion mechanism. Consequently, this paper provides a detailed summary of the development for numerous aqueous zinc-based batteries: zinc-sulfur (Zn-S) batteries, zinc-selenium (Zn-Se) batteries, zinc-tellurium (Zn-Te) batteries, zinc-iodine (Zn-I2 ) batteries, and zinc-bromine (Zn-Br2 ) batteries. Meanwhile, the reaction conversion mechanism of zinc-based batteries with conversion mechanism and the research progress in the investigation of composite cathode, zinc anode materials, and selection of electrolytes are systematically introduced. Finally, this review comprehensively describes the prospects and outlook of aqueous zinc-ion batteries with conversion mechanism, aiming to promote the rapid development of aqueous zinc-based batteries.

Advances in Aqueous Zinc Ion Batteries based on Conversion Mechanism: Challenges, Strategies, and Prospects.

A new class of ternary hydrated eutectic electrolytes is designed that can enable 2I + /I 2 /2I − redox couple four-electron conversion and oriented dendrite-free Zn plating/stripping for Zn–I 2 batteries. 

Designing Ternary Hydrated Eutectic Electrolyte Capable of Four-Electron Conversion for Advanced Zn-I2 Full Batteries

Zinc‐ion batteries with chalcogen‐based (S, Se, Te) cathodes have emerged as a promising candidate for utility‐scale energy storage systems and portable electronics, which have attracted rapid attention and offer tremendous opportunities owing to their excellent energy density, on top of the advantages of aqueous Zn batteries including cost‐effectiveness, inherent safety, and eco‐friendliness. Here, a comprehensive overview on the basic mechanism of zinc–chalcogen batteries with their great advantages and intrinsic issues is provided. More detailed recent progress is summarized and the existing challenges with promising strategies are provided as well. First, four specific types of batteries are presented, including: zinc–sulfur, zinc–selenium, zinc–selenium sulfide, and zinc–tellurium batteries. Second, the remaining challenges within chalcogen‐based cathodes in the material preparation, physicochemical properties, and battery performance are summarized and discussed. Meanwhile, a series of constructive strategies are comprehensively put forward for optimizing electrochemical performance. Finally, the future research perspectives of zinc–chalcogen batteries are proposed for the exploration and innovation of next‐generation green zinc storage applications.

High Energy Density Aqueous Zinc–Chalcogen (S, Se, Te) Batteries: Recent Progress, Challenges, and Perspective

Iodine has great potential in energy storage, but high solubility of I3- has seriously delayed its promotion. Benefited from abundant active sites and the open channel, two-dimensional coordination supramolecular networks (2D CSNs) is considered to be a candidate for energy storage. Herein, a 2D porphyrin-CSN cathode named Zn-TCPP for aqueous iodine dual-ion battery (DIB) shows an excellent specific capacity of 278 mAh g-1, and a high energy density of 340 Wh kg-1 at 5 A g-1, as well as a durable cycle performance of 5000 cycles and a high Coulombic efficiency of 98%. Molecular orbital theory, UV-vis, Raman spectroscopy and density functional theory (DFT) calculations reveal charge-transfer interaction between the donor of porphyrin nitrogen and the acceptor of I3-, and computational fluid dynamics (CFD) simulations demonstrate the contribution of 2D layered network structure of Zn-TCPP to the penetration of I3-.

A Two-Dimensional Porphyrin Coordination Supramolecular Network Cathode for High-performance Aqueous Dual-Ion Battery.

Iodine is considered to have broad application prospects in the field of electrochemical energy storage. However, the high solubility of I3- severely hampers its practical application, and the lack of research on the anchoring mechanism of I3- has seriously hindered the development of advanced cathode materials for iodine batteries. Herein, based on the molecular orbital theory, we studied the charge-transfer interaction between the acceptor of I3- with a σ* empty antibonding orbital and the donor of pyrimidine nitrogen with lone-pair electrons, which is proved by the results of UV-vis absorption spectroscopy, Raman spectroscopy, and density functional theory (DFT) calculations. The prepared dual-ion battery (DIB) exhibits a high voltage platform of 1.2 V, a remarkable discharge-specific capacity of up to 207 mAh g-1, and an energy density of 233 Wh kg-1 at a current density of 5 A g-1, as well as outstanding cycle stability (operating stably for 5000 cycles) with a high Coulombic efficiency of 97%, demonstrating excellent electrochemical performance and a promising prospect in stationary energy storage.

Anchoring I3- via Charge-Transfer Interaction by a Coordination Supramolecular Network Cathode for a High-Performance Aqueous Dual-Ion Battery.

Aqueous zinc metal batteries (ZMBs) are a promising sustainable technology for large-scale energy storage applications. However, the water is often associated with problematic parasitic reactions on both anode and cathode, leading to the low durability and reliability of ZMBs. Here, a multifunctional separator for the Zn-V2 O5 batteries by growing the coordination supramolecular network (CSN:Zn-MBA, MBA = 2-mercaptobenzoic acid) on the conventional non-woven fabrics (NWF) is developed. CSN tends to form a stronger coordination bond as a softer cation, enabling a thermodynamically preferred Zn2+ to VO2 + substitution in the network, leading to the formation of VO2 -MBA interface, that strongly obstructs the VO2 (OH)2 - penetration but simultaneously allows Zn2+ transfer. Moreover, Zn-MBA molecules can adsorb the OTF- and distribute the interfacial Zn2+ homogeneous, which facilitate a dendrite-free Zn deposition. The Zn-V2 O5 cells with Zn-MBA@NWF separator realize high capacity of 567 mAh g-1 at 0.2 A g-1 , and excellent cyclability over 2000 cycles with capacity retention of 82.2% at 5 A g-1 . This work combines the original advantages of the template and new function of metals via cation metathesis within a CSN, provides a new strategy for inhibiting vanadium oxide dissolution.

Suppression of Vanadium Oxide Dissolution via Cation Metathesis within a Coordination Supramolecular Network for Durable Aqueous Zn-V2 O5 Batteries.

Prussian blue analogs (PBAs) have been considered as a kind of promising cathode materials, but its poor cycle performance severely hinders their industrialization. Herein, by combining a zinc ferrocyanide (ZnHCF) cathode with aqueous ZnSO4/LiTFSI electrolyte and zinc metal anode, we achieved a stable anion insertion-type aqueous dual-ion battery (DIB) which displays a discharge specific capacity of 75.9 mAh g–1, an energy density of 124 Wh kg–1, and a discharge plateau of 1.8 V at 5 A g–1. Its specific capacity can still reach 57.4 mAh g–1 after 1200 cycles with a Coulombic efficiency of 97%. A reversible anion insertion mechanism of ZnHCF cathode based on the changes of the valency of iron and the insertion of TFSI– ion on crystal surface caused by electrostatic interaction is proposed and confirmed with a series of characterizations and density functional theory calculations (DFT). This work proposes the study of anion energy storage mechanism of PBAs and brings more opportunities for their large-scale applications in the future. 

Anion electrostatic insertion boosts efficient zinc ferrocyanide cathode for aqueous dual-ion battery

Dendrite-Free and Long-Standing Aqueous Zinc Metal Battery Achieved by In-Situ Grown Hydrophilic Coordination Supramolecular Networks

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