The Zn metal anode suffers from uncontrollable dendrite formation and intricate parasitic reactions that dramatically impede the commercialization of aqueous Zn metal batteries (AZMBs). This st proposes synergistic strategies for facilitating Zn2+ migration kinetics and regulating surface energy to achieve dendrite‐free Zn deposition and suppressing self‐corrosion by covering Zn anode with multifunctional covalent organic frameworks possessing sulfonate‐rich (SO3H) covalently‐tethered nanochannels (SCOFs). Benefiting from the vital interplay between SO3H and Zn2+, the SCOFs coatings form ample Zn2+ accelerated transport channels to extract Zn2+ from the electrolyte quickly, thereby promoting rapid desolvation of hydrated Zn2+, enhancing ion replenishment capability, and guaranteeing a steady stream of Zn2+ flux for endowing uniform and compact nucleation. Additionally, the zincophilic SCOFs significantly reduce the surface energy of the Zn (002) crystal plane, inducing preferentially crystallographic (002) orientation electroplating growth. Consequently, the SCOFs‐coated Zn anodes (SCOFs@Zn) demonstrate an excellent lifespan up to 4000 h at 5 mA cm−2, 1 mAh cm−2, and 3000 h at 5 mA cm−2, 2 mAh cm−2. Meanwhile, the full cell paired with the MnO2 cathode sustains remarkable reversibility within 1000 cycles. The synergistic approach to manipulating ion migration and surface energy provides new insights into developing highly stable AZMBs.

Highly Reversible Zn Metal Anodes Realized by Synergistically Enhancing Ion Migration Kinetics and Regulating Surface Energy

Aqueous rechargeable energy storage (ARES) has received tremendous attention in recent years due to its intrinsic merits of low cost, high safety, and environmental friendliness. However, the relatively higher freezing point of conventional aqueous electrolytes results in sluggish kinetics and inferior ion transport efficiency under low temperature, severely restricting their further development and practical applications. In order to deal with the existing issues, the design principles to develop low‐temperature ARES with excellent performance are discussed in‐depth and precisely classified, primarily with respect to electrode modification and electrolyte regulation. In addition, the related studies about low‐temperature ARES are systematically and comprehensively summarized. Finally, the critical bottlenecks, some suggestions, and future perspectives are also provided, which will help to address the current challenges of low‐temperature ARES. This review is expected to deepen the fundamental understanding of low‐temperature ARES and offer guiding suggestions to boost their future applications.

Design Strategies and Recent Advancements for Low‐Temperature Aqueous Rechargeable Energy Storage

This review details past attempts, breakthroughs, and computational/characterization methods in developing metal–iodine batteries along with their key innovations, deficiencies, and possible solutions. 

pdf/metal-iodine-batteries-achievements-challenges-and-future-dbd6gq3hp3.pdf

Metal–iodine batteries: achievements, challenges, and future

Aqueous zinc-ion batteries (ZIBs) with metal zinc as the anode possess the features of safety, environmental friendliness, and high specific capacity, which have attracted a great deal of attention in the past few years. The accompanying zinc dendrites are an important problem that endangers the battery performance. Therefore, the extensive research on the suppression strategies of Zn dendrites reflects a positive effect on improving the performance of ZIBs. In particular, the electrolyte additives (EAs) approach is considered a simple, reliable, and low-cost strategy to address the zinc dendritic issues and can inhibit or alleviate the growth of zinc dendrites while facilitating the amelioration of adverse reactions. In this review, the principles and processes of zinc dendrites, corrosion passivation, and hydrogen evolution side reactions on zinc anodes of ZIBs are firstly categorized. Then, the mitigation and inhibition of zinc dendrites and side reactions via different kinds of EAs are elaborated according to the regulation strategies of EAs, which provides an overview of the research on EAs conducted in recent years and proposed strategies to solve zinc dendrites and other problems. Finally, a reasonable outlook on the future improvement and development of EAs for ZIBs is described, which could provide some guidance for the evolution and design of EAs in the future.

/pdf/electrolyte-additive-strategies-for-suppression-of-zinc-18ymw6ld.pdf

Electrolyte Additive Strategies for Suppression of Zinc Dendrites in Aqueous Zinc-Ion Batteries

Aqueous zinc–iodine batteries (Zn–I2) demonstrate great promise in large scale energy storage systems. However, their practical application faces significant challenges including dendrite formation, corrosion caused by polyiodine ions, and other side reactions at the zinc anode side. Herein, a facile and efficient pretreatment method for zinc anodes through the substitution reaction of Zn and SnF2 to create a dense and durable multifunctional surface layer (MSL). The MSL comprise tin (Sn) and ZnF2 phases on the zinc metal, in which Sn possesses good zinc affinity and a high hydrogen evolution overpotential, while ZnF2 provides pathways for radial ion transport. Importantly, both have a low binding energy with polyiodine ions, preventing the failure of the interface layer. Therefore, this interface layer can effectively mitigate zinc metal electrode dendrite formation, corrosion from polyiodine ions, and other side reactions induced by water, simultaneously. As a result, the Zn–I2 batteries performance is greatly improved and exhibited a stable cycling to 20 000 times with 80% capacity retention at a current density of 2 A g−1. Even the I2 loading is increased to 8 mg cm−2, it can still cycle stably for 5000 cycles with a capacity retention of 94%.

In situ Construction of Multifunctional Surface Coatings on Zinc Metal for Advanced Aqueous Zinc–Iodine Batteries

Although zinc-ion batteries are regarded as important alternatives for Li-ion batteries, the dendrite issues and side reactions are major obstacles for their development. Here, inspired by the idea of electrolyte modification, a simple and low-cost approach, that methanol is used as additive into Zn2+-containing electrolyte for long-life Zn ion batteries, was developed. Methanol can mix with water in any ratio through the formation of hydrogen bonds, which participates in the solvation shell of Zn2+ ion in a manner of forming the [Zn(OH2)x(CH3OH)y]2+ cations. The interaction between Zn2+, methanol and water can effectively suppress the side reactions. As a result, Zn/Zn symmetric cell shows a long-term stability for over 480 h at 1 mA cm−2 with 1 mAh cm−2. In addition, full battery based on the MnO2 cathode exhibits an improved capacity retention after 100 cycles at 0.1 A g−1 and an excellent electrochemical performance at low temperature. 

Electrolyte Modification for Long‐Life Zn Ion Batteries: Achieved by Methanol Additive

Zinc-iodine batteries (ZIBs) have attracted widespread attention because of their efficient capacity for ion transport and safety. However, the shuttle effect and physical properties of iodine species tremendously hinder their practical applications. Herein, we report a nitrogen-doped biomass litchi-shell derived porous carbon (marked as N-LPC) as the iodine host for ZIBs. The porous-rich structure of N-LPC is favorable for iodine loading and electron/ion transfers. Furthermore, the doping of heteroatomic nitrogen provides abundant anchoring sites to achieve strong interaction with iodine, thus the self-discharge can be suppressed effectively. Accordingly, the N-LPC/I2 composite cathode exhibits a specific capacity of 127 mAh/g at 100 mA g−1, as well as excellent rate capability and cycle stability. This study provides a strategy for discovering the cost-effective carbonaceous iodine host material. 

Nitrogen-doped litchi-shell derived porous carbon as an efficient iodine host for zinc-iodine batteries

Zn-modified zeolites host for dendrite-free zinc metal anodes

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Electrolyte Modification for Long‐Life Zn Ion Batteries: Achieved by Methanol Additive

Nitrogen-doped litchi-shell derived porous carbon as an efficient iodine host for zinc-iodine batteries

Zn-modified zeolites host for dendrite-free zinc metal anodes