Aqueous zinc‐ion batteries (ZIBs) enjoy a good reputation for being safe, affordable to produce, and ecologically friendly due to the use of water‐based electrolytes. The main factors restricting the development of ZIBs, however, are the negative effects of dendrite deposition on the zinc anode and the dissolution of common cathodes such as Mn and V‐based cathodes. Various techniques have been used to address these issues, including regulating the electrolyte concentration or solvation structure, developing a coating or current collector to lessen anode dendrite growth, and improving the structural stability of the cathode. Recently, functionalized separator strategies have gained popularity as effective ways to improve ZIB performance. The use of a functionalized separator is also a practical technique to save costs and increase the volumetric energy density of the battery by substituting a functionalized separator for the usual thick and expensive glass fiber separator. The development of functionalized separators in ZIBs is the subject of ongoing research, and this work presents the most recent findings in a systematic manner, focusing on both the effects and the methods to prepare or modify them. Finally, a brief explanation of the constraints and future potential of current functionalized separator development is provided.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/aenm.202300403

Functionalized Separator Strategies toward Advanced Aqueous Zinc‐Ion Batteries

Ultrathin separators are indispensable to high‐energy‐density zinc‐ion batteries (ZIBs), but their easy failure caused by zinc dendrites poses a great challenge. Herein, 23 µm‐thick functional ultrathin separators (FUSs), realizing superb electrochemical stability of zinc anodes and outstanding long‐term durability of ultrathin separators, are reported. In the FUSs, an ultrathin but mechanically strong nanoporous membrane substrate benefits fast and flux‐homogenized Zn2+ transport, while a metal–organic framework (MOF)‐derived C/Cu nanocomposite decoration layer provides rich low‐barrier zinc nucleation sites, thereby synergistically stabilizing zinc anodes to inhibit zinc dendrites and dendrite‐caused separator failure. Investigation of the zinc affinity of the MOF‐derived C/Cu nanocomposites unravels the high zincophilicity of heteroatom‐containing C/Cu interfaces. Zinc anodes coupled with the FUSs present superior electrochemical stability, whose operation lifetime exceeds 2000 h at 1 mA cm−2 and 600 h at 10 mA cm−2, 40–50 times longer than that of the zinc anodes using glass‐fiber separators. The reliability of the FUSs in ZIBs and zinc‐ion hybrid supercapacitors is also validated. This work proposes a new strategy to stabilize zinc anodes and provides theoretical guidance in developing ultrathin separators for high‐energy‐density zinc‐based energy storage.

Functional Ultrathin Separators Proactively Stabilizing Zinc Anodes for Zinc‐Based Energy Storage

Rational design of ZnMn2O4 nanoparticles on carbon nanotubes for high-rate and durable aqueous zinc-ion batteries

Fe2VO4 nanoparticles on rGO as anode material for high-rate and durable lithium and sodium ion batteries

Carbon‐based nanomaterials, including graphene, fullerenes, and carbon nanotubes, are attracting significant attention as promising materials for next‐generation energy storage and conversion applications. They possess unique physicochemical properties, such as structural stability and flexibility, high porosity, and tunable physicochemical features, which render them well suited in these hot research fields. Technological advances at atomic and electronic levels are crucial for developing more efficient and durable devices. This comprehensive review provides a state‐of‐the‐art overview of these advanced carbon‐based nanomaterials for various energy storage and conversion applications, focusing on supercapacitors, lithium as well as sodium‐ion batteries, and hydrogen evolution reactions. Particular emphasis is placed on the strategies employed to enhance performance through nonmetallic elemental doping of N, B, S, and P in either individual doping or codoping, as well as structural modifications such as the creation of defect sites, edge functionalization, and inter‐layer distance manipulation, aiming to provide the general guidelines for designing these devices by the above approaches to achieve optimal performance. Furthermore, this review delves into the challenges and future prospects for the advancement of carbon‐based electrodes in energy storage and conversion.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/advs.202301045

Recent Advances in Carbon‐Based Electrodes for Energy Storage and Conversion

Zinc-based energy storage with functionalized carbon nanotube/polyaniline nanocomposite cathodes

Aerogel-structured MnO2 cathode assembled by defect-rich ultrathin nanosheets for zinc-ion batteries

Stable anode-free zinc-ion batteries enabled by alloy network-modulated zinc deposition interface

Mn‐based cathodes have been widely explored for aqueous zinc‐ion batteries (ZIBs), by virtue of their high theoretical capacity and low cost. However, Mn‐based cathodes suffer from poor rate capability and cycling performance. Researchers have presented various approaches to address these issues. Therefore, these endeavors scattered in various directions (e. g., designing electrode structures, defect engineering and optimizing electrolytes) are necessary to be connected through a systematic review. Hence, we comprehensively overview Mn‐based cathode materials for ZIBs from the aspects of phase compositions, electrochemical behaviors and energy storage mechanisms, and try to build internal relations between these factors. Modification strategies of Mn‐based cathodes are then introduced. Furthermore, this review also provides some new perspectives on future efforts toward high‐energy and long‐life Mn‐based cathodes for ZIBs.

Material Design and Energy Storage Mechanism of Mn‐Based Cathodes for Aqueous Zinc‐Ion Batteries

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