Gel polymer electrolytes (GPEs) hold tremendous potential for advancing high-energy-density and safe rechargeable solid-state batteries, making them a transformative technology for advancing electric vehicles. GPEs offer high ionic conductivity and mechanical stability, enabling their use in quasi-solid-state batteries that combine solid-state interfaces with liquid-like behavior. Various GPEs based on different materials, including flame-retardant GPEs, dendrite-free polymer gel electrolytes, hybrid solid-state batteries, and 3D printable GPEs, have been developed. Significant efforts have also been directed toward improving the interface between GPEs and electrodes. The integration of gel-based electrolytes into solid-state electrochemical devices has the potential to revolutionize energy storage solutions by offering improved efficiency and reliability. These advancements find applications across diverse industries, particularly in electric vehicles and renewable energy. This review comprehensively discusses the potential of GPEs as solid-state electrolytes for diverse battery systems, such as lithium-ion batteries (LiBs), lithium metal batteries (LMBs), lithium–oxygen batteries, lithium–sulfur batteries, zinc-based batteries, sodium–ion batteries, and dual-ion batteries. This review highlights the materials being explored for GPE development, including polymers, inorganic compounds, and ionic liquids. Furthermore, it underscores the transformative impact of GPEs on solid-state batteries and their role in enhancing the performance and safety of energy storage devices. 

Gel Polymer Electrolytes: Advancing Solid-State Batteries for High-Performance Applications

Single-atom catalysts (SACs) have been demonstrated to show exceptional reactivity and selectivity in catalytic reactions by effectively utilizing metal species, making them a favorable choice among the different active materials for energy conversion. However, SACs are still in the early stage of energy conversion, and problems like agglomeration and low energy conversion efficiency are hampering their practical applications. Substantial researches focus on support modifications, which are vital for SAC reactivity and stability due to the intimate relationship between metal atoms and support. In this review, a category of supports and a variety of surface engineering strategies employed in SA systems are summarized, including surface site engineering (heteroatom doping, vacancy introducing, surface groups grafting, and coordination tunning) and surface structure engineering (size/morphology control, cocatalyst deposition, facet engineering, and crystallinity control). Also, the merits of support surface engineering in single-atom systems are systematically introduced. Highlights are the comprehensive summary and discussions on the utilization of surface engineered SACs in diversified energy conversion applications including photocatalysis, electrocatalysis, thermocatalysis, and energy conversion devices. At the end of this review, we have discussed the potential and obstacles of using surface engineered SACs in the field of energy conversion. This review aims to guide the rational design and manipulation of SACs for target-specific applications by capitalizing on the characteristic benefits of support surface engineering. This article is protected by copyright. All rights reserved.

Surface Engineered Single-atom Systems for Energy Conversion.

Flexible zinc-air batteries (FZABs) have experienced rapid development due to the advantages of high theoretical energy density, wearable and notable safety. Wide-temperature FZABs have been challenged by rapid dehydration of gel-polymer electrolytes (GPEs) at high temperatures and freezing at low temperatures, as well as increased growth of zinc dendrites. Therefore, some studies have focused on constructing wide-temperature working FZAB using high water retention electrolytes while inhibiting the production of zinc dendrites. In this review, we first systematically examine several evaluation indicators for GPEs. Then, the strategies for improving the wide-temperature performance of GPEs are summarized based on four common polymer monomers. Additionally, reasonable strategies for suppressing zinc dendrites are explored. Finally, the future development directions for GPEs in FZABs are proposed. We hope that this review will provide guidance for the construction of wide-temperature and dendrite-free FZABs. 

Research progress in wide-temperature flexible zinc-air batteries

The development of high‐performance catalysts plays a crucial role in facilitating chemical production and reducing environmental contamination. Single‐atom catalysts (SACs), a class of catalysts that bridge the gap between homogeneous and heterogeneous catalysis, have garnered increasing attention because of their unique activity, selectivity, and stability in many pivotal reactions. Meanwhile, the scarcity of precious metal SACs calls for the arrival of cost‐effective SACs. Cobalt, as a common non‐noble metal, possesses tremendous potential in the field of single‐atom catalysis. Despite their potential, reviews about single‐atom Co catalysts (Co‐SACs) are lacking. Accordingly, this review thoroughly summarized various preparation methodologies of Co‐SACs, particularly pyrolysis; its application in the specific domain of organic synthesis and environmental remediation is discussed as well. The structure–activity relationship and potential catalytic mechanism of Co‐SACs are elucidated through some representative reactions. The imminent challenges and development prospects of Co‐SACs are discussed in detail. The findings and insights provided herein can guide further exploration and development in this charming area of catalyst design, leading to the realization of efficient and sustainable catalytic processes.

Preparation and Application of Single-Atom Cobalt Catalysts in Organic Synthesis and Environmental Remediation.

Microstructure and bionic engineering of triphase reaction interface for zinc-air batteries

Metal single atoms show outstanding electrocatalytic activity owing to the abundant atomic reactive sites and superior stability. However, the preparation of single atoms suffers from inexorable metal aggregation which is harmful to electrocatalytic activity. Here, ionic covalent organic frameworks (iCOFs) are employed as the sacrificial precursor to mitigate the metal aggregation and subsequent formation of bulky particles. Molecular dynamics simulation shows that iCOFs can trap and confine more Co ions as compared to neutral COFs, resulting in the formation of a catalyst composed of Co single atoms and uniformly distributed Co nanoparticles (CoSA&CoNP‐10). However, the neutral COFs derive a catalyst composed of Co atomic clusters and large Co nanoparticles (CoAC&CoNP‐25). The CoSA&CoNP‐10 catalyst exhibits higher oxygen bifunctional electrocatalytic activities than CoAC&CoNP‐25, coinciding with the density functional theory results. Taking the CoSA&CoNP‐10 as the air cathode in Zn–air batteries (ZABs), the aqueous ZAB presents a high power density of 181 mW cm−2, a specific capacity of 811 mAh g−1 as well as a long cycle life of 407 h at a current density of 10 mA cm−2, while the quasi‐solid state ZAB displays a power density of 179 mW cm−2 and the cycle life of 30 h.

Ionic Covalent Organic Frameworks‐Derived Cobalt Single Atoms and Nanoparticles for Efficient Oxygen Electrocatalysis

Gel polymer electrolyte (GPE) in quasi-solid state Zn-air battery (QSZAB) will release alkali during cycling, resulting in gradual dehydration of GPE, corrosion of Zn electrode, Zn dendrites growth, and therefore inferior performance. Here, hollow Sn microspheres are prepared on Zn substrate by the technique of colloidal self-assembly. The inner surfaces of hollow Sn microspheres are modified by 2-hydroxypropyl-β-cyclodextrin (hollow Sn-inner HPβCD) to regulate the released alkali at GPE|anode interface. The hollow Sn-inner HPβCD can lessen the leakage of released alkali, make stored alkali diffuse back to GPE during the charging process, and mitigate the loss of soluble Zn(OH)4 2- to suppress Zn dendrites growth. Resultantly, GPE in QSZAB with hollow Sn-inner HPβCD exhibits a high retention capacity for alkaline solution. The cell also exhibits a long cyclic lifespan of 127 h due to the effective regulation of released alkali, which outperforms QSZAB without hollow Sn-inner HPβCD by 7.94 times. This work rivets the regulation of released alkali at GPE|anode interface, providing new insight to improve QSZABs' performance.

Regulation of Released Alkali from Gel Polymer Electrolyte in Quasi-Solid State Zn-Air Battery.

Solvent-Free and in Situ Synthesis of Three-Dimensional Covalent Organic Frameworks Thin Films on Zn Anodes for Zn–Air Batteries

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Ionic Covalent Organic Frameworks‐Derived Cobalt Single Atoms and Nanoparticles for Efficient Oxygen Electrocatalysis

Regulation of Released Alkali from Gel Polymer Electrolyte in Quasi-Solid State Zn-Air Battery.

Solvent-Free and in Situ Synthesis of Three-Dimensional Covalent Organic Frameworks Thin Films on Zn Anodes for Zn–Air Batteries