W.C. acknowledges the startup funds from University of Science and Technology of China (KY2060000150) and the support from USTC Center for Micro and Nanoscale Research and Fabrication. H.N.A. and Y.C. would like to acknowledge the support of King Abdullah University of Science and Technology (KAUST) for their fund under grant # OSR-CRG2018-3735.

Opportunities of Aqueous Manganese‐Based Batteries with Deposition and Stripping Chemistry

Aqueous zinc-ion batteries (AZIBs) are an appealing battery system due to their low cost, intrinsic safety and environmental friendliness, while their application is plagued by the obstacles from the cathode, electrolyte and zinc anode. Summarizing the design principles and strategies towards the optimization of cathode, electrolyte and zinc anode is crucial for the development of AZIBs. Herein, we present a comprehensive analysis of the design principles and promising strategies towards the improvement of AZIBs. Firstly, the various reaction mechanisms are summarized and the existing issues associated with the cathode, electrolyte, and zinc anode are discussed to guide the rational design of AZIBs. Subsequently, we provide an in-depth and comprehensive discussion on the design principles and strategies for the electrodes/electrolyte/separator optimization, and analyze the advantages and disadvantages of various strategies. Importantly, the design principles and strategies of the newly appeared conversion-type AZIBs, such as Zn-S battery, Zn-Se battery are also discussed and analyzed. The effect of design strategies on the electrochemical performance and the relationship between the current issues and strategies are also unveiled in detail. Finally, some research trends and perspectives are provided for designing better AZIBs. 

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/eem2.12265

Designing Advanced Aqueous Zinc‐Ion Batteries: Principles, Strategies, and Perspectives

Aqueous zinc-ion batteries (AZIBs) are regarded as promising electrochemical energy storage devices owing to its low cost, intrinsic safety, abundant zinc reserves, and ideal specific capacity. Compared with other cathode materials, manganese dioxide with high voltage, environmental protection, and high theoretical specific capacity receives considerable attention. However, the problems of structural instability, manganese dissolution, and poor electrical conductivity make the exploration of high-performance manganese dioxide still a great challenge and impede its practical applications. Besides, zinc storage mechanisms involved are complex and somewhat controversial. To address these issues, tremendous efforts, such as surface engineering, heteroatoms doping, defect engineering, electrolyte modification, and some advanced characterization technologies, have been devoted to improving its electrochemical performance and illustrating zinc storage mechanism. In this review, we particularly focus on the classification of manganese dioxide based on crystal structures, zinc ions storage mechanisms, the existing challenges, and corresponding optimization strategies as well as structure–performance relationship. In the final section, the application perspectives of manganese oxide cathode materials in AZIBs are prospected. 

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/eem2.12575

Recent advances on challenges and strategies of manganese dioxide cathodes for aqueous zinc‐ion batteries

Guest-species-incorporation in manganese/vanadium-based oxides: Towards high performance aqueous zinc-ion batteries

Aqueous zinc-ion batteries have attracted extensive attention ascribing to affordability, intrinsic safety, and environmental benignity, which have revealed ideal alternative to lithium-ion batteries for large-scale energy storage systems. Nevertheless, the design of aqueous zinc-ion batteries is plagued by obstacles, such as dissolution of cathode materials, dendrites and side reactions of anode, and electrolyte consumption as compared to commercial lithium-ion batteries. In this regard, from the perspective of predominant issues encountered with aqueous zinc-ion batteries, this comprehensive review aims to systematically summarize the design principles and optimization strategies associated with the cathode, anode, electrolyte, and separator. Meanwhile, the impact of design strategies on electrochemistry, and the relationship between issues and strategies are revealed for guiding the rational design of advanced aqueous zinc-ion batteries. Eventually, a series of critical challenges, constructive solutions, and future trends toward cathode, anode, electrolyte and separator are dedicatedly proposed. We envisage that this review would endow researchers a readily accessible means to rapidly acquaint with optimization strategies and design principles for advanced aqueous zinc-ion batteries. 

Optimization Strategies Toward Advanced Aqueous Zinc-ion Batteries: From Facing Key Issues to Viable Solutions

Aqueous zinc-ion batteries, especially Zn-MnO2 battery, have attracted intensive attention owing to their unique features of high capacity, environmental friendliness, and safety. However, the problem of Mn dissolution hinders the development of zinc-ion batteries with long-term usage and high-rate performance. In this work, a novel preparation method for the polyaniline (PANI)-coated composite aerogel of MnO2 and rGO (MnO2/rGO/PANI) electrode is reported. The obtained composite possesses high electrical conductivity, and also effectively suppresses the dissolution of Mn. The fabricated MnO2/rGO/PANI//Zn battery exhibits a high capacity of 241.1 mAh·g−1 at 0.1 A·g−1, and an excellent capacity retention of 82.7% after 600 charge/discharge cycles. In addition, the rapid diffusion coefficient of the MnO2/rGO/PANI electrode was further examined by galvanostatic intermittent titration technique. This work provides new insights into the development of high-performance Zn-MnO2 battery with a better understanding of its diffusion kinetics.

Preparation of Polyaniline-coated Composite Aerogel of MnO2 and Reduced Graphene Oxide for High-performance Zinc-ion Battery

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Preparation of Polyaniline-coated Composite Aerogel of MnO2 and Reduced Graphene Oxide for High-performance Zinc-ion Battery