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Aqueous Zn2+ ion batteries (AZIBs) are considered promising candidates for large‐scale energy storage systems. However, the critical technical bottlenecks, including Zn dendrite, corrosion reactions, and poor low‐temperature performance, significantly impede their commercialization. Here, γ‐valerolactone (γ‐GVL), a bioactive polar biomass‐based green solvent derived from lignocellulose, is introduced into electrolyte as a co‐solvent to improve the electrochemical stability of Zn anode and enhance its low‐temperature cycling performance. The non‐toxic γ‐GVL, serving as a strong hydrogen‐bonding ligand, coordinates with H2O to reconstruct the electrolyte's hydrogen bond network, broadening the electrochemical stability window and enhancing the anti‐frost properties of aqueous electrolytes. Moreover, γ‐GVL facilitates in situ formation of a heterogeneous solid‐electrolyte interphase (SEI) composed of ZnF2 and ZnS inorganic components. The heterogeneous interphases maintain superior ionic conductivity for Zn2+ transportation and hydrophobicity for H2O repulsion, synergistically enabling highly stable and dendrite‐free Zn deposition. Consequently, Zn||Zn cells exhibit improved cycling performance across a wide temperature range, achieving an extended cycle life of 5060 h at 25 °C and 2300 h at −40 °C. Zn||VO2 full cells show enhanced low‐temperature cyclability, retaining 97.0% capacity after 300 cycles at −20 °C, demonstrating substantial potential for advancing the commercialization of low‐temperature aqueous electrolytes.
Aqueous Zn2+ ion batteries (AZIBs) are considered promising candidates for large‐scale energy storage systems. However, the critical technical bottlenecks, including Zn dendrite, corrosion reactions, and poor low‐temperature performance, significantly impede their commercialization. Here, γ‐valerolactone (γ‐GVL), a bioactive polar biomass‐based green solvent derived from lignocellulose, is introduced into electrolyte as a co‐solvent to improve the electrochemical stability of Zn anode and enhance its low‐temperature cycling performance. The non‐toxic γ‐GVL, serving as a strong hydrogen‐bonding ligand, coordinates with H2O to reconstruct the electrolyte's hydrogen bond network, broadening the electrochemical stability window and enhancing the anti‐frost properties of aqueous electrolytes. Moreover, γ‐GVL facilitates in situ formation of a heterogeneous solid‐electrolyte interphase (SEI) composed of ZnF2 and ZnS inorganic components. The heterogeneous interphases maintain superior ionic conductivity for Zn2+ transportation and hydrophobicity for H2O repulsion, synergistically enabling highly stable and dendrite‐free Zn deposition. Consequently, Zn||Zn cells exhibit improved cycling performance across a wide temperature range, achieving an extended cycle life of 5060 h at 25 °C and 2300 h at −40 °C. Zn||VO2 full cells show enhanced low‐temperature cyclability, retaining 97.0% capacity after 300 cycles at −20 °C, demonstrating substantial potential for advancing the commercialization of low‐temperature aqueous electrolytes.
Rechargeable aqueous zinc batteries (AZBs) utilizing water‐borne electrolytes are intrinsically safe electrochemical devices that are promising in next‐generation energy storage. Such application requires adaptivity to global climate, especially at grid‐scale, thus their stability of electrochemical performance at varying temperatures is critical. Many essential properties of AZBs, i.e., ion transfer, redox kinetics, etc., are largely governed by the aqueous electrolytes in the batteries because of the relatively limited stable phase temperature of water. This limitation is extremely vital in cold regions since charging and discharging become more difficult at the sub‐zero range due to water freezing. Despite the development of various electrolyte strategies in recent years, comprehensive reviews focusing on this topic remain limited. This research reviews the diverse reasons underneath the failure of AZBs at extreme temperatures and provides a thorough analysis of possible resolutions from an electrolyte perspective. It starts with the challenges faced by AZBs at both high and low temperatures concerning the electrolytes. Different strategies addressing these challenges are discussed, providing insights into aqueous batteries under extreme temperature conditions. Finally, the review concludes with a summary and outlook on the design and structure of electrolytes for all‐weather AZBs, integrating innovative strategies from both aqueous and non‐aqueous battery systems.
Aqueous zinc‐ion batteries (AZIBs) attract attention due to their safety and high specific capacity. However, their practical applications are constrained by Zn anode corrosion, dendritic growth, and poor temperature adaptability induced by a strong hydrogen‐bond network in aqueous electrolytes. Herein, a universal strategy to design strong solvating electrolytes is proposed, in which the hydrogen‐bond network and solvation structures are reconstructed by regulating the dipolar‐dipolar and ion‐dipolar interactions simultaneously. Consequently, the hydrogen‐bond network in free water is largely weakened, and the water content in the Zn2+ solvated sheath is reduced, while the hydrogen‐bond network between solvents is strengthened, which effectively broadens the operating temperature range and suppresses Zn dendrites and corrosion. As a result, Zn anodes exhibit excellent platting/stripping efficiency with an average Coulombic Efficiency up to 99.89% after 2000 cycles at 0.5 mA cm−2, impressive cycling stability (5000 h, 0.5 mA cm−2/0.5 mA h cm−2), and a wide operating temperature range of 140 °C (−50–90 °C). Moreover, the Zn//V2O3 full cells also display enhanced temperature‐resistance, implying that the designed strong solvation electrolyte has practical application potential in extreme environments. This study suggests a promising strategy to design ideal electrolytes for high‐performance AZIBs with safety, ultralong cycling life, and satisfying temperature‐resistance.
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