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Synergistic Effects of Interfacial Chemistry and Ion-Solvent Interactions to Enable Reversible Magnesium Metal Anode in Chloride-Free Mg(TFSI)2 Electrolytes SCIE
期刊论文 | 2025 | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
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Abstract :

Passivation of magnesium (Mg) anode in the chloride-free magnesium bis(trifluoromethanesulfonyl)imide (Mg(TFSI)(2)) electrolyte is a key challenge for Mg metal batteries. Tailoring solvation structure and solid electrolyte interphase (SEI) has been considered an effective strategy. Herein, a series of imidazole co-solvents with different branched-chain structures (methyl, ethyl, and propyl) are introduced into the Mg(TFSI)(2)-ether electrolyte to address the passivation issue. The ion-solvent interaction, interfacial adsorption effect, and SEI formation are comprehensively studied by theoretical calculations and experimental characterizations. Through molecular structure analysis, the long-chain 1-propylimidazole (PrIm) exhibits a strong coordination ability to Mg2+ and a favorable parallel adsorption configuration on the Mg surface. As a result, PrIm co-solvent can not only restructure the solvation sheath of Mg2+, but also act as a dynamic protective shield to repel a part of TFSI- and 1,2-dimethoxyethane (DME) away from the Mg surface. Benefiting from the synergistic regulation effect of interfacial chemistry and ion-solvent interactions, the chloride-free Mg(TFSI)(2)-DME + PrIm electrolyte ensures minimal interface passivation and achieves highly reversible Mg plating/stripping. This work provides a guiding strategy for solvation structure regulation and interface engineering for rechargeable Mg metal batteries.

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Adsorption Adsorption Imidazole co-solvent Imidazole co-solvent Magnesium metal battery Magnesium metal battery Mg(TFSI)(2) electrolyte Mg(TFSI)(2) electrolyte Solvation structure Solvation structure

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GB/T 7714 Yang, Aoqi , Gao, Xiang , Pei, Maojun et al. Synergistic Effects of Interfacial Chemistry and Ion-Solvent Interactions to Enable Reversible Magnesium Metal Anode in Chloride-Free Mg(TFSI)2 Electrolytes [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 .
MLA Yang, Aoqi et al. "Synergistic Effects of Interfacial Chemistry and Ion-Solvent Interactions to Enable Reversible Magnesium Metal Anode in Chloride-Free Mg(TFSI)2 Electrolytes" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2025) .
APA Yang, Aoqi , Gao, Xiang , Pei, Maojun , Zhou, Jiacong , Wang, Honggang , Liao, Can et al. Synergistic Effects of Interfacial Chemistry and Ion-Solvent Interactions to Enable Reversible Magnesium Metal Anode in Chloride-Free Mg(TFSI)2 Electrolytes . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 .
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