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

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...

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Main Authors: Caiyun Wang, Yao Huang, Yunhao Lu, Hongge Pan, Ben Bin Xu, Wenping Sun, Mi Yan, Yinzhu Jiang
Format: Article
Language:English
Published: SpringerOpen 2021-09-01
Series:Nano-Micro Letters
Subjects:
Online Access:https://doi.org/10.1007/s40820-021-00716-1
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author Caiyun Wang
Yao Huang
Yunhao Lu
Hongge Pan
Ben Bin Xu
Wenping Sun
Mi Yan
Yinzhu Jiang
author_facet Caiyun Wang
Yao Huang
Yunhao Lu
Hongge Pan
Ben Bin Xu
Wenping Sun
Mi Yan
Yinzhu Jiang
author_sort Caiyun Wang
collection DOAJ
description 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.
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spelling doaj.art-f2c510273b18444095e6edf10fb414f02022-12-21T22:12:58ZengSpringerOpenNano-Micro Letters2311-67062150-55512021-09-0113111110.1007/s40820-021-00716-1Reversible Magnesium Metal Anode Enabled by Cooperative Solvation/Surface Engineering in Carbonate ElectrolytesCaiyun Wang0Yao Huang1Yunhao Lu2Hongge Pan3Ben Bin Xu4Wenping Sun5Mi Yan6Yinzhu Jiang7School of Materials Science and Engineering, State Key Laboratory of Clean Energy Utilization, Zhejiang UniversitySchool of Materials Science and Engineering, State Key Laboratory of Clean Energy Utilization, Zhejiang UniversitySchool of Materials Science and Engineering, State Key Laboratory of Clean Energy Utilization, Zhejiang UniversitySchool of Materials Science and Engineering, State Key Laboratory of Clean Energy Utilization, Zhejiang UniversityMechanical and Construction Engineering, Faculty of Engineering and Environment, Northumbria UniversitySchool of Materials Science and Engineering, State Key Laboratory of Clean Energy Utilization, Zhejiang UniversitySchool of Materials Science and Engineering, State Key Laboratory of Clean Energy Utilization, Zhejiang UniversitySchool of Materials Science and Engineering, State Key Laboratory of Clean Energy Utilization, Zhejiang UniversityAbstract 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.https://doi.org/10.1007/s40820-021-00716-1Rechargeable magnesium batteriesMetal anodeSolvation effectPassivationCarbonate electrolytes
spellingShingle Caiyun Wang
Yao Huang
Yunhao Lu
Hongge Pan
Ben Bin Xu
Wenping Sun
Mi Yan
Yinzhu Jiang
Reversible Magnesium Metal Anode Enabled by Cooperative Solvation/Surface Engineering in Carbonate Electrolytes
Nano-Micro Letters
Rechargeable magnesium batteries
Metal anode
Solvation effect
Passivation
Carbonate electrolytes
title Reversible Magnesium Metal Anode Enabled by Cooperative Solvation/Surface Engineering in Carbonate Electrolytes
title_full Reversible Magnesium Metal Anode Enabled by Cooperative Solvation/Surface Engineering in Carbonate Electrolytes
title_fullStr Reversible Magnesium Metal Anode Enabled by Cooperative Solvation/Surface Engineering in Carbonate Electrolytes
title_full_unstemmed Reversible Magnesium Metal Anode Enabled by Cooperative Solvation/Surface Engineering in Carbonate Electrolytes
title_short Reversible Magnesium Metal Anode Enabled by Cooperative Solvation/Surface Engineering in Carbonate Electrolytes
title_sort reversible magnesium metal anode enabled by cooperative solvation surface engineering in carbonate electrolytes
topic Rechargeable magnesium batteries
Metal anode
Solvation effect
Passivation
Carbonate electrolytes
url https://doi.org/10.1007/s40820-021-00716-1
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