General and simple salts-mediating approach enables superior magnesium plating/stripping properties

Rechargeable Mg-metal batteries represent attractive alternatives to Li-ion/Li-metal counterparts owing to resource sustainability, cost and safety superiorities. Grignard reagents-based electrolytes enable Mg plating/stripping reversibly, but properties are still not satisfactory. In this work, a g...

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Main Authors: Ning Yuan, Jing Liu, Wenhao Sun, Min Wang, Changming Mao, Kun Chao, Zhenfang Zhou, Xiaosong Guo, Zhonghua Zhang, Guicun Li
Format: Article
Language:English
Published: Elsevier 2025-04-01
Series:Next Energy
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Online Access:http://www.sciencedirect.com/science/article/pii/S2949821X25000109
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author Ning Yuan
Jing Liu
Wenhao Sun
Min Wang
Changming Mao
Kun Chao
Zhenfang Zhou
Xiaosong Guo
Zhonghua Zhang
Guicun Li
author_facet Ning Yuan
Jing Liu
Wenhao Sun
Min Wang
Changming Mao
Kun Chao
Zhenfang Zhou
Xiaosong Guo
Zhonghua Zhang
Guicun Li
author_sort Ning Yuan
collection DOAJ
description Rechargeable Mg-metal batteries represent attractive alternatives to Li-ion/Li-metal counterparts owing to resource sustainability, cost and safety superiorities. Grignard reagents-based electrolytes enable Mg plating/stripping reversibly, but properties are still not satisfactory. In this work, a general and simple salts-mediating approach is proposed to enrich electrochemically-active species in Grignard reagents-based electrolytes. This hybrid electrolyte exhibits high ionic conductivity of 19.47 mS cm−1 (vs. 5.65 mS cm−1 for pure electrolytes), desirable electrochemical window (2.75 V vs. 1.75 V for pure electrolytes), exceptional Mg plating/stripping properties (140 cycles vs. 40 cycles for pure electrolytes). After introducing magnesium bis(trifluoromethanesulfonimide)/diglyme (abbreviated as “Mg(TFSI)2/G2”), originally negatively-charged ion pair species, such as [MgCl3]− and [Mg2Cl5]−, that adversely contribute to ionic conductivity and charge transfer processes, transform to active cations of [Mg(G2)2]2+ and [MgCl]+ through Mg2+-assisted Mg-Cl bond dissociation. This greatly improves active ion accessibility for Mg-metal anode and is beneficial for uniform Mg electrodeposition. In addition, unique MgCl-rich and carbonyl organic compounds-containing interphases are unveiled, which is conducive to active Mg electrodeposition. This general and simple salts-mediating approach can be extended to design better electrolytes for next-generation multivalent-metal batteries.
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series Next Energy
spelling doaj-art-caa6d703c92643dabc3b5b5613a0fa862025-02-05T04:32:55ZengElsevierNext Energy2949-821X2025-04-017100247General and simple salts-mediating approach enables superior magnesium plating/stripping propertiesNing Yuan0Jing Liu1Wenhao Sun2Min Wang3Changming Mao4Kun Chao5Zhenfang Zhou6Xiaosong Guo7Zhonghua Zhang8Guicun Li9College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR ChinaDepartment of Pharmacy, Jining Medical University, Rizhao 276826, PR ChinaCollege of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR ChinaCollege of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR ChinaCollege of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR ChinaCollege of Electromechanical Engineering, Qingdao University of Science and Technology, Qingdao 266061, PR China; Corresponding authors.College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR ChinaCollege of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR ChinaCollege of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR China; Corresponding authors.College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR ChinaRechargeable Mg-metal batteries represent attractive alternatives to Li-ion/Li-metal counterparts owing to resource sustainability, cost and safety superiorities. Grignard reagents-based electrolytes enable Mg plating/stripping reversibly, but properties are still not satisfactory. In this work, a general and simple salts-mediating approach is proposed to enrich electrochemically-active species in Grignard reagents-based electrolytes. This hybrid electrolyte exhibits high ionic conductivity of 19.47 mS cm−1 (vs. 5.65 mS cm−1 for pure electrolytes), desirable electrochemical window (2.75 V vs. 1.75 V for pure electrolytes), exceptional Mg plating/stripping properties (140 cycles vs. 40 cycles for pure electrolytes). After introducing magnesium bis(trifluoromethanesulfonimide)/diglyme (abbreviated as “Mg(TFSI)2/G2”), originally negatively-charged ion pair species, such as [MgCl3]− and [Mg2Cl5]−, that adversely contribute to ionic conductivity and charge transfer processes, transform to active cations of [Mg(G2)2]2+ and [MgCl]+ through Mg2+-assisted Mg-Cl bond dissociation. This greatly improves active ion accessibility for Mg-metal anode and is beneficial for uniform Mg electrodeposition. In addition, unique MgCl-rich and carbonyl organic compounds-containing interphases are unveiled, which is conducive to active Mg electrodeposition. This general and simple salts-mediating approach can be extended to design better electrolytes for next-generation multivalent-metal batteries.http://www.sciencedirect.com/science/article/pii/S2949821X25000109Magnesium batteriesElectrolytesElectrodepositionsDissociation kineticsGrignard reagents
spellingShingle Ning Yuan
Jing Liu
Wenhao Sun
Min Wang
Changming Mao
Kun Chao
Zhenfang Zhou
Xiaosong Guo
Zhonghua Zhang
Guicun Li
General and simple salts-mediating approach enables superior magnesium plating/stripping properties
Next Energy
Magnesium batteries
Electrolytes
Electrodepositions
Dissociation kinetics
Grignard reagents
title General and simple salts-mediating approach enables superior magnesium plating/stripping properties
title_full General and simple salts-mediating approach enables superior magnesium plating/stripping properties
title_fullStr General and simple salts-mediating approach enables superior magnesium plating/stripping properties
title_full_unstemmed General and simple salts-mediating approach enables superior magnesium plating/stripping properties
title_short General and simple salts-mediating approach enables superior magnesium plating/stripping properties
title_sort general and simple salts mediating approach enables superior magnesium plating stripping properties
topic Magnesium batteries
Electrolytes
Electrodepositions
Dissociation kinetics
Grignard reagents
url http://www.sciencedirect.com/science/article/pii/S2949821X25000109
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