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Vol. 13 (2021)

Reversible Magnesium Metal Anode Enabled by Cooperative Solvation/Surface Engineering in Carbonate Electrolytes

https://doi.org/10.1007/s40820-021-00716-1
Caiyun Wang
School of Materials Science and Engineering, State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, Zhejiang, People’s Republic of China
Yao Huang
School of Materials Science and Engineering, State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, Zhejiang, People’s Republic of China
Yunhao Lu
School of Materials Science and Engineering, State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, Zhejiang, People’s Republic of China
Hongge Pan
School of Materials Science and Engineering, State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, Zhejiang, People’s Republic of China
Ben Bin Xu
Mechanical and Construction Engineering, Faculty of Engineering and Environment, Northumbria University, Newcastle upon Tyne NE1 8ST, UK
Wenping Sun
School of Materials Science and Engineering, State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, Zhejiang, People’s Republic of China
Mi Yan
School of Materials Science and Engineering, State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, Zhejiang, People’s Republic of China
Yinzhu Jiang
School of Materials Science and Engineering, State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, Zhejiang, People’s Republic of China

Corresponding Author: Yinzhu Jiang

yzjiang@zju.edu.cn

Nano-Micro Letters, Vol. 13 (2021), Article Number: 195

Abstract

Magnesium metal anode holds great potentials toward future high energy and safe rechargeable magnesium battery technology due to its divalent redox and dendrite-free nature. Electrolytes based on Lewis acid chemistry enable the reversible Mg plating/stripping, while they fail to match most cathode materials toward high-voltage magnesium batteries. Herein, reversible Mg plating/stripping is achieved in conventional carbonate electrolytes enabled by the cooperative solvation/surface engineering. Strongly electronegative Cl from the MgCl2 additive of electrolyte impairs the Mg…O = C interaction to reduce the Mg2+ desolvation barrier for accelerated redox kinetics, while the Mg2+-conducting polymer coating on the Mg surface ensures the facile Mg2+ migration and the effective isolation of electrolytes. As a result, reversible plating and stripping of Mg is demonstrated with a low overpotential of 0.7 V up to 2000 cycles. Moreover, benefitting from the wide electrochemical window of carbonate electrolytes, high-voltage (> 2.0 V) rechargeable magnesium batteries are achieved through assembling the electrode couple of Mg metal anode and Prussian blue-based cathodes. The present work provides a cooperative engineering strategy to promote the application of magnesium anode in carbonate electrolytes toward high energy rechargeable batteries.


Highlights:


1 A cooperative solvation/surface engineering approach is reported to achieve the reversible Mg plating/stripping in conventional carbonate electrolytes.
2 Benefitting from the strategy, Mg2+ can easily overcome the reduced desolvation barrier and penetrate the Mg2+-conducting polymer coating, deposited on the Mg metal anode successfully, promoting the application of magnesium anode in carbonate electrolytes toward high-energy rechargeable batteries.

Keywords

Rechargeable magnesium batteries Metal anode Solvation effect Passivation Carbonate electrolytes
Wang, Caiyun, Yao Huang, Yunhao Lu, Hongge Pan, Ben Bin Xu, Wenping Sun, Mi Yan, and Yinzhu Jiang. 2021. “Reversible Magnesium Metal Anode Enabled by Cooperative Solvation/Surface Engineering in Carbonate Electrolytes”. Nano-Micro Letters 13 (September):195. https://doi.org/10.1007/s40820-021-00716-1.
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