Alkoxy-functionalized ionic liquid electrolytes: understanding ionic coordination of calcium ion speciation for the rational design of calcium electrolytes

被引:43
|
作者
Gao, Xinpei [1 ,2 ]
Liu, Xu [1 ,2 ]
Mariani, Alessandro [1 ,2 ]
Elia, Giuseppe Antonio [1 ,2 ]
Lechner, Manuel [3 ]
Streb, Carsten [3 ]
Passerini, Stefano [1 ,2 ]
机构
[1] Helmholtz Inst Ulm HIU, Helmholtzstr 11, D-89081 Ulm, Germany
[2] Karlsruhe Inst Technol KIT, POB 3640, D-76021 Karlsruhe, Germany
[3] Ulm Univ, Inst Inorgan Chem 1, Albert Einstein Allee 11, D-89081 Ulm, Germany
基金
欧盟地平线“2020”;
关键词
ELECTROCHEMICAL-BEHAVIOR; MG2+; BIS(TRIFLUOROMETHANESULFONYL)IMIDE; CONVERSION; SYSTEMS;
D O I
10.1039/d0ee00831a
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
There is growing interest in the rational design of electrolytes for multivalent-ion batteries by tuning the molecular-level interactions of solvate species present in the electrolytes. Herein, we report our effort to control Ca-ion speciation in ionic liquid (IL) based electrolytes through the design of alkoxy-functionalized cations. Quantitative analysis reveals that the alkoxy-functionalized ammonium cation (N-07(+)), bearing seven ether oxygen atoms, can effectively displace the bis(trifluoromethanesulfonyl)imide anion (TFSI-) from the Ca2+ ion coordination sphere, facilitating the reversible Ca deposition/stripping process. More importantly, post-analysis of Ca deposits surface chemistry and density functional theory calculations of Ca-ion speciation indicate the formation of an organic-rich, but inorganic-poor solid electrolyte interphase layer, which enables Ca2+ ion diffusion rather than passivating the Ca metal electrode. Finally, as a proof-of-concept, a prototype Ca/V2O5 cell using the optimized IL-based electrolyte ([Ca(BH4)(2)](0.05)[N07TFSI](0.95)) is demonstrated for the first time, exhibiting a remarkable initial discharge capacity of 332 mA h g(-1) and reversible capacity of 244 mA h g(-1).
引用
收藏
页码:2559 / 2569
页数:11
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