An Atomic Insight into the Chemical Origin and Variation of the Dielectric Constant in Liquid Electrolytes

被引:150
作者
Yao, Nan [1 ]
Chen, Xiang [1 ]
Shen, Xin [1 ]
Zhang, Rui [2 ]
Fu, Zhong-Heng [1 ]
Ma, Xia-Xia [1 ]
Zhang, Xue-Qiang [1 ]
Li, Bo-Quan [2 ]
Zhang, Qiang [1 ]
机构
[1] Tsinghua Univ, Dept Chem Engn, Beijing Key Lab Green Chem React Engn & Technol, Beijing 100084, Peoples R China
[2] Beijing Inst Technol, Adv Res Inst Multidisciplinary Sci, Beijing 100081, Peoples R China
基金
中国国家自然科学基金; 中国博士后科学基金;
关键词
dielectric constant; liquid electrolytes; molecular dynamics simulations; solvent mixtures; temperature; DIFFUSION-COEFFICIENTS; METAL BATTERIES; LI; TEMPERATURES; SOLVATION; TRANSPORT; DESIGN; MODELS; ANODES; IONS;
D O I
10.1002/anie.202107657
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The dielectric constant is a crucial physicochemical property of liquids in tuning solute-solvent interactions and solvation microstructures. Herein the dielectric constant variation of liquid electrolytes regarding to temperatures and electrolyte compositions is probed by molecular dynamics simulations. Dielectric constants of solvents reduce as temperatures increase due to accelerated mobility of molecules. For solvent mixtures with different mixing ratios, their dielectric constants either follow a linear superposition rule or satisfy a polynomial function, depending on weak or strong intermolecular interactions. Dielectric constants of electrolytes exhibit a volcano trend with increasing salt concentrations, which can be attributed to dielectric contributions from salts and formation of solvation structures. This work affords an atomic insight into the dielectric constant variation and its chemical origin, which can deepen the fundamental understanding of solution chemistry.
引用
收藏
页码:21473 / 21478
页数:6
相关论文
共 53 条
[1]  
[Anonymous], 2021, ANGEW CHEM, V133, P4136
[2]  
[Anonymous], 2018, ANGEW CHEM, V130, P5399
[3]   Design of electrolyte solutions for Li and Li-ion batteries: a review [J].
Aurbach, D ;
Talyosef, Y ;
Markovsky, B ;
Markevich, E ;
Zinigrad, E ;
Asraf, L ;
Gnanaraj, JS ;
Kim, HJ .
ELECTROCHIMICA ACTA, 2004, 50 (2-3) :247-254
[4]   Dielectric relaxation of aqueous NaCl solutions [J].
Buchner, R ;
Hefter, GT ;
May, PM .
JOURNAL OF PHYSICAL CHEMISTRY A, 1999, 103 (01) :1-9
[5]   Machine learning for molecular and materials science [J].
Butler, Keith T. ;
Davies, Daniel W. ;
Cartwright, Hugh ;
Isayev, Olexandr ;
Walsh, Aron .
NATURE, 2018, 559 (7715) :547-555
[6]   Electrolyte design for LiF-rich solid-electrolyte interfaces to enable high-performance microsized alloy anodes for batteries [J].
Chen, Ji ;
Fan, Xiulin ;
Li, Qin ;
Yang, Hongbin ;
Khoshi, M. Reza ;
Xu, Yaobin ;
Hwang, Sooyeon ;
Chen, Long ;
Ji, Xiao ;
Yang, Chongyin ;
He, Huixin ;
Wang, Chongmin ;
Garfunkel, Eric ;
Su, Dong ;
Borodin, Oleg ;
Wang, Chunsheng .
NATURE ENERGY, 2020, 5 (05) :386-397
[7]  
Chen L. F., 2004, Microwave Electronics: Measurement and Materials Characterization. Hoboken, NJ
[8]   High-Voltage Lithium-Metal Batteries Enabled by Localized High-Concentration Electrolytes [J].
Chen, Shuru ;
Zheng, Jianming ;
Mei, Donghai ;
Han, Kee Sung ;
Engelhard, Mark H. ;
Zhao, Wengao ;
Xu, Wu ;
Liu, Jun ;
Zhang, Ji-Guang .
ADVANCED MATERIALS, 2018, 30 (21)
[9]   Atomic Insights into the Fundamental Interactions in Lithium Battery Electrolytes [J].
Chen, Xiang ;
Zhang, Qiang .
ACCOUNTS OF CHEMICAL RESEARCH, 2020, 53 (09) :1992-2002
[10]  
Christian R., 2011, Solvents and Solvent Effects in Organic Chemistry