A versatile single-ion electrolyte with a Grotthuss-like Li conduction mechanism for dendrite-free Li metal batteries

Batteries with Li metal anodes have the desirable feature of high energy density; however, the notorious problem of Li dendrite formation has impeded their practical applications. Herein, we present a versatile single-ion electrolyte, which is achieved by a different strategy of coordinating the ani...

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Bibliographic Details
Published in:Energy & environmental science 2019-09, Vol.12 (9), p.2741-275
Main Authors: Yuan, Shouyi, Bao, Junwei Lucas, Wei, Jishi, Xia, Yongyao, Truhlar, Donald G, Wang, Yonggang
Format: Article
Language:English
Subjects:
Anions
Batteries
Conduction
Copper
Dendrites
Electrolytes
Electrolytic cells
Energy
Flux density
High temperature
Ion transport
Lithium manganese oxides
Metal-organic frameworks
Metals
Perchlorate
Perchloric acid
Quantum mechanics
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Summary:Batteries with Li metal anodes have the desirable feature of high energy density; however, the notorious problem of Li dendrite formation has impeded their practical applications. Herein, we present a versatile single-ion electrolyte, which is achieved by a different strategy of coordinating the anions in the electrolyte on the open metal sites of a metal organic framework. Further investigations of the activation energy and theoretical quantum mechanical calculations suggest that Li ion transport inside the pores of Cu-MOF-74 is via a Grotthuss-like mechanism where the charge is transported by coordinated hopping of Li ions between the perchlorate groups. This single-ion electrolyte is versatile and has wide applications. When the single-ion electrolyte is used for LiLi symmetric cells and LiLiFePO 4 full cells, Li dendrites are suppressed. As a result, an ultralong cycle life is achieved for both cells. In addition, when the single-ion electrolyte is assembled into LiLiMn 2 O 4 batteries, the dissolution of Mn 2+ into the electrolyte is suppressed even at elevated temperatures, and a long cycle life with improved capacity retention is achieved for LiLiMn 2 O 4 batteries. Finally, when the single-ion electrolyte is applied to LiO 2 batteries, an improved cycle life with reduced overpotential is also achieved. A new versatile single-ion electrolyte with a Grotthuss-like Li conduction mechanism is proposed to address the issue of Li metal batteries.
ISSN:1754-5692
1754-5706
DOI:10.1039/c9ee01473j