Understanding Li-ion thermodynamic and kinetic behaviors in concentrated electrolyte for the development of aqueous lithium-ion batteries

被引:16
|
作者
Hu, Jiangtao [1 ]
Guo, Haodan [2 ]
Li, Yiwei [1 ]
Wang, Hongbin [1 ]
Wang, Ziqi [1 ]
Huang, Weiyuan [1 ]
Yang, Luyi [1 ]
Chen, Haibiao [3 ]
Lin, Yuan [2 ]
Pan, Feng [1 ]
机构
[1] Peking Univ, Sch Adv Mat, Shenzhen Grad Sch, Shenzhen 518055, Peoples R China
[2] Chinese Acad Sci, CAS Res Educ Ctr Excellence Mol Sci, Inst Chem, Beijing Natl Lab Mol Sci,Key Lab Photochem, Beijing 100190, Peoples R China
[3] Shenzhen Polytech, Inst Marine Biomed, Shenzhen 518055, Peoples R China
基金
中国国家自然科学基金;
关键词
Aqueous electrolyte; High-concentration; Li-ion; Thermodynamic and kinetic behaviors; ACTIVITY-COEFFICIENTS; DESOLVATION;
D O I
10.1016/j.nanoen.2021.106413
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
High-concentration aqueous electrolytes are attractive for deployments in future lithium-ion batteries due to high safety, environmental friendliness, and wide voltage window. It is of great significance to understand the Liion behaviors in high concentration conditions for both mechanistic studies and commercial applications. Herein, by analyzing cyclic voltammetry and voltage profiles using a customized single-particle model, we clarify the Li-ion thermodynamic and kinetic behaviors in aqueous electrolytes at various concentrations using LiFePO4 as the active electrode. With the increase of the electrolyte concentration, the equilibrium potentials of LiFePO4 shift to higher values, which is attributed to the increased Li-ion activity and activity coefficient induced by the formation of polymeric solution structure ((Li+(H2O)2)n) at high concentrations. To further quantify the interface reaction constants (k0) and the activation energy (Ea), theoretical simulations based upon experimental data are carried out, identifying that the sluggish Li-ion desolvation process is the main contributor to the slower interface kinetics in high concentration electrolytes. Other factors affecting the Li-ion interface process, including temperature, scan rate, and type of anion, are also evaluated here. These fundamental understandings are of great value to the development of high-concentration aqueous electrolyte, in a cost-effective, sustainable and efficient way.
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页数:7
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