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The Zn//V2O5 system not only faces the incontrollable growth of zinc (Zn) dendrites, but also withstands the cross‐talk effect of by‐products produced from the cathode side to the Zn anode, inducing interelectrode talk and aggravating battery failure. To tackle these issues, we construct a rapid Zn2+‐conducting hydrogel electrolyte (R‐ZSO) to achieve Zn deposition modulation and side reaction inhibition in Zn//V2O5 full cells. The polymer matrix and BN exhibit a robust anchoring effect on SO42−, accelerating Zn2+ migration and enabling dense Zn deposition behavior. Therefore, the Zn//Zn symmetric cells based on the R‐ZSO electrolyte can operate stably for more than 1500 h, which is six times higher than that of cells employing the blank electrolyte. More importantly, the R‐ZSO hydrogel electrolyte effectively decouples the cross‐talk effects, thus breaking the infinite loop of side reactions. As a result, the Zn//V2O5 cells using this modified hydrogel electrolyte demonstrate stable operation over 1,000 cycles, with a capacity loss rate of only 0.028 % per cycle. Our study provides a promising gel chemistry, which offers a valuable guide for the construction of high‐performance and multifunctional aqueous Zn‐ion batteries. [ABSTRACT FROM AUTHOR]

Heterostructures with interfacial effects have exhibited great potential for improving the electrochemical kinetics of electrode materials. However, the application of heterostructures is hampered by complicated synthesis parameters and numerous single components. Herein, a multiple‐templating synthesis strategy is proposed to improve the interfacial effect of heterojunction composites, mitigate volume variation upon lithiation/de‐lithiation, and increase interfacial compatibility with poly‐oxyethylene‐based (PEO‐based) electrolytes. Benefiting from the structural and compositional superiorities, the novel NiS/SnO2/MOF (NSM) electrode achieves superior electrochemical performance with exceptional specific capacity, outstanding rate capability and ultralong cyclability. As a result of the compatibility between organic components and the porous properties of metal organic frameworks (MOFs), the NSM electrode exhibits greater interfacial compatibility with PEO‐based solid‐state electrolytes. This work not only describes a meticulous protocol for heterostructured high‐performance electrode materials, but also provides a new insight to enhance the connectivity between the interfaces of solid‐state batteries. [ABSTRACT FROM AUTHOR]

Due to the excellent specific capacity and high working voltage, manganese oxide (MnO2) has attracted considerable attention for aqueous zinc‐ion batteries (AZIBs). However, the irreversible structural collapse and sluggish ionic diffusion lead to poor rate capability and inferior lifespan. Herein, we proposed a novel organic/inorganic hybrid cathode of carbon‐based poly(4,4′‐oxybisbenzenamine)/MnO2 (denoted as C@PODA/MnO2) for AZIBs. Various in/ex situ analyses and theoretical calculations prove that PODA chains with C=N groups can provide a more active surface/interface for ion/electron mobility and zinc ion storage in the hybrid cathode. More importantly, newly formed Mn−N interfacial bonds can effectively promote ion diffusion and prevent Mn atoms dissolution, enhancing redox kinetics and structural integrity of MnO2. Accordingly, C@PODA/MnO2 cathode exhibits high capacity (321 mAh g−1 or 1.7 mAh cm−2 at 0.1 A g−1), superior rate performance (88 mAh g−1 at 10 A g−1) and excellent cycling stability over 2000 cycles. Hence, rational interfacial designs shed light on the development of organic/inorganic cathodes for advanced AZIBs. [ABSTRACT FROM AUTHOR]

Dendrite growth and corrosion issues have significantly hindered the usability of Zn anodes, which further restricts the development of aqueous zinc-ion batteries (AZIBs). In this study, a zinc-philic and hydrophobic Zn (100) crystal plane end-capping reagent (ECR) is introduced into the electrolyte to address these challenges in AZIBs. Specifically, under the mediation of 100-ECR, the electroplated Zn configures oriented dense deposition of (100) crystal plane texture, which slows down the formation of dendrites. Furthermore, owing to the high corrosion resistance of the (100) crystal plane and the hydrophobic protective interface formed by the adsorbed ECR on the electrode surface, the Zn anode demonstrates enhanced reversibility and higher Coulombic efficiency in the modified electrolyte. Consequently, superior electrochemical performance is achieved through this novel crystal plane control strategy and interface protection technology. The Zn//VO 2 cells based on the modified electrolyte maintained a high-capacity retention of ≈80.6% after 1350 cycles, corresponding to a low-capacity loss rate of only 0.014% per cycle. This study underscores the importance of deposition uniformity and corrosion resistance of crystal planes over their type. And through crystal plane engineering, a high-quality (100) crystal plane is constructed, thereby expanding the range of options for viable Zn anodes., (© 2024 Wiley‐VCH GmbH.)

The Zn//V 2 O 5 system not only faces the incontrollable growth of zinc (Zn) dendrites, but also withstands the cross-talk effect of by-products produced from the cathode side to the Zn anode, inducing interelectrode talk and aggravating battery failure. To tackle these issues, we construct a rapid Zn 2+ -conducting hydrogel electrolyte (R-ZSO) to achieve Zn deposition modulation and side reaction inhibition in Zn//V 2 O 5 full cells. The polymer matrix and BN exhibit a robust anchoring effect on SO 4 2- , accelerating Zn 2+ migration and enabling dense Zn deposition behavior. Therefore, the Zn//Zn symmetric cells based on the R-ZSO electrolyte can operate stably for more than 1500 h, which is six times higher than that of cells employing the blank electrolyte. More importantly, the R-ZSO hydrogel electrolyte effectively decouples the cross-talk effects, thus breaking the infinite loop of side reactions. As a result, the Zn//V 2 O 5 cells using this modified hydrogel electrolyte demonstrate stable operation over 1,000 cycles, with a capacity loss rate of only 0.028 % per cycle. Our study provides a promising gel chemistry, which offers a valuable guide for the construction of high-performance and multifunctional aqueous Zn-ion batteries., (© 2024 Wiley-VCH GmbH.)

Lithium-oxygen batteries (LOBs) are well known for their high energy density. However, their reversibility and rate performance are challenged due to the sluggish oxygen reduction/evolution reactions (ORR/OER) kinetics, serious side reactions and uncontrollable Li dendrite growth. The electrolyte plays a key role in transport of Li + and reactive oxygen species in LOBs. Here, we tailored a dilute electrolyte by screening suitable crown ether additives to promote lithium salt dissociation and Li + solvation through electrostatic interaction. The electrolyte containing 100 mM 18-crown-6 ether (100-18C6) exhibits enhanced electrochemical stability and triggers a solution-mediated Li 2 O 2 growth pathway in LOBs, showing high discharge capacity of 10 828.8 mAh g carbon -1 . Moreover, optimized electrode/electrolyte interfaces promote ORR/OER kinetics on cathode and achieve dendrite-free Li anode, which enhances the cycle life. This work casts new lights on the design of low-cost dilute electrolytes for high performance LOBs., (© 2023 Wiley-VCH GmbH.)

Due to the excellent specific capacity and high working voltage, manganese oxide (MnO 2 ) has attracted considerable attention for aqueous zinc-ion batteries (AZIBs). However, the irreversible structural collapse and sluggish ionic diffusion lead to poor rate capability and inferior lifespan. Herein, we proposed a novel organic/inorganic hybrid cathode of carbon-based poly(4,4'-oxybisbenzenamine)/MnO 2 (denoted as C@PODA/MnO 2 ) for AZIBs. Various in/ex situ analyses and theoretical calculations prove that PODA chains with C=N groups can provide a more active surface/interface for ion/electron mobility and zinc ion storage in the hybrid cathode. More importantly, newly formed Mn-N interfacial bonds can effectively promote ion diffusion and prevent Mn atoms dissolution, enhancing redox kinetics and structural integrity of MnO 2 . Accordingly, C@PODA/MnO 2 cathode exhibits high capacity (321 mAh g -1 or 1.7 mAh cm -2 at 0.1 A g -1 ), superior rate performance (88 mAh g -1 at 10 A g -1 ) and excellent cycling stability over 2000 cycles. Hence, rational interfacial designs shed light on the development of organic/inorganic cathodes for advanced AZIBs., (© 2022 Wiley-VCH GmbH.)