电解质
乙腈
溶解
钒
水溶液
电化学
阴极
化学工程
材料科学
无机化学
插层(化学)
化学
电极
物理化学
有机化学
工程类
作者
Xiaolu Qin,Xu Zhao,Guobin Zhang,Zhiquan Wei,Linyuan Li,Xiaoke Wang,Zhi Chen,Hongfei Li,Cuiping Han,Baohua Li
出处
期刊:ACS Nano
[American Chemical Society]
日期:2023-06-20
卷期号:17 (13): 12040-12051
被引量:5
标识
DOI:10.1021/acsnano.2c07061
摘要
Currently, the development of calcium-ion batteries (CIBs) is still in its infancy and greatly plagued by the absence of satisfactory cathode materials and compatible electrolytes. Herein, an acetonitrile-water hybrid electrolyte is first developed in CIB chemistry, in which, the strong lubricating and shielding effect of water solvent significantly boosts the swift transport of bulky Ca2+, thus contributing to large capacity storage of Ca2+ in layered vanadium oxides (Ca0.25V2O5·nH2O, CVO). Meanwhile, the acetonitrile component noticeably suppresses the dissolution of vanadium species during repeated Ca2+-ion uptake/release, endowing the CVO cathode with a robust cycle life. More importantly, spectral characterization and molecular dynamics simulation confirm that the water molecules are well stabilized by the mutual hydrogen bonding with acetonitrile molecules (O-H···N), endowing the aqueous hybrid electrolyte with high electrochemical stability. By using this aqueous hybrid electrolyte, the CVO electrode shows a high specific discharge capacity of 158.2 mAh g-1 at 0.2 A g-1, an appealing capacity of 104.6 mAh g-1 at a high rate of 5 A g-1, and a capacity retention of 95% after 2000 cycles at 1.0 A g-1, which is a record-high performance for CIBs reported so far. A mechanistic study exemplifies the reversible extraction of Ca2+ from the gap of VO polyhedral layers, which are accompanied by the reversible V-O and V-V skeleton change as well as reversible variation of layer spacing. This work constitutes a major advance in developing high-performance Ca-ion batteries.
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