文献类型：期刊文献

英文题名：Trade-off between reversibility and fast Zn2+ kinetics: Toward ultra-stable low-temperature aqueous zinc-ion batteries

作者：Zhang, Junye[1];Wang, Linlin[2];Liao, Yuping[1];Huang, Chen[1];Zhu, Hangtian[1];Wang, Juan[1];Yuan, Linying[2];Shen, Tianchen[2];Lu, Shigang[2];Chen, Luyang[1]

机构：[1]East China Univ Sci & Technol, Sch Mat Sci & Engn, Key Lab Ultrafine Mat, Minist Educ, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]Shanghai Univ, Inst Sustainable Energy, Coll Sci, Shanghai 200444, Peoples R China

年份：2025

卷号：77

外文期刊名：ENERGY STORAGE MATERIALS

收录：;EI(收录号：20251418180684);WOS:【SCI-EXPANDED(收录号:WOS:001465900500001)】；

基金：National Overseas High-Level Talent Youth Program in China.r National Overseas High-Level Talent Youth Program in China.

语种：英文

外文关键词：Hydrated deep eutectic electrolytes; Ligand-oriented solvation shell; H-bonds intensity; Anti-freezing and inhibiting the dissolution; Zn2+ kinetics

摘要：Despite their environmental friendliness, security and high volumetric energy density of zinc anodes, aqueous Zinc-ion batteries (AZIBs) still face poor reversibility of Zn anodes, especially under high current density, originating from various parasitic reactions induced by high activity of water. The hydrated deep eutectic electrolyte (HDEE) effectively suppresses parasitic reactions, but the electrochemical performance still needs to be optimized. Here, our research emphasized the importance of balancing enhanced reversibility and fast Zn2+ transfer kinetics. A new green and low-cost HDEE (Zn(ClO4)(2)6H(2)O/Glycerol) is developed, and then an optimized solvation structure [Zn(H2O)(2.0)(Gl)(1.3)(ClO4)(2.7)](2)(+) can be formed by adding glycerol (Gl), which not only maintains a high Zn2+ diffusion coefficient (1.2 x 10(-7) cm(2) s(-1)), but also disrupts the bulk water network via strong H-bonding with ClO4- and water, significantly lowering the freezing point (-65 degrees C) and inhibiting the parasitic reactions/cathode dissolution. Furthermore, the evolution of the HDEEs solvation chemistry and its impact on the electrode/electrolyte interfacial stabilities can be understood through precise adjustments of the molar ratios of Zn(ClO4)(2)6H(2)O and Gl, molecular dynamics and COMSOL simulation. The Zn//Zn with the HDEE (Zn|HDEE|Zn cells) can cycle for similar to 5000 h without short-circuiting at 1 mA cm(-2), which is roughly 12.5 times more stable than ordinary aqueous electrolyte, indicating effective suppression of parasitic reactions. The Zn//NH4V4O10 with HDEE (Zn|HDEE|NH4V4O10 cells) can stably cycle 3500 cycles with 120 mAh g(-1) at 10 A g(-1) at room temperature and 1000 cycles with 95 mAh g(-1) at 5 A g(-1) at a low temperature of -20 degrees C. This study provides a path toward the development of HDEE electrolyte and a thorough comprehension of the influence of Zn2+ solvation structure on reversibility.