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author：

Yang, A. (Yang, A..) [1] | Gao, X. (Gao, X..) [2] | Pei, M. (Pei, M..) [3] | Zhou, J. (Zhou, J..) [4] | Wang, H. (Wang, H..) [5] | Liao, C. (Liao, C..) [6] | Xiao, J. (Xiao, J..) [7] | Liu, Y. (Liu, Y..) [8] | Yan, W. (Yan, W..) [9] | Zhang, J. (Zhang, J..) [10]

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Scopus

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.　©　2025　Wiley-VCH　GmbH.

Keyword：

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

Community：

  • [ 1 ] [Yang A.]Institute for New Energy Materials and Engineering, College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China
  • [ 2 ] [Yang A.]Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fujian, Fuzhou City, 350108, China
  • [ 3 ] [Gao X.]Institute for New Energy Materials and Engineering, College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China
  • [ 4 ] [Gao X.]Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fujian, Fuzhou City, 350108, China
  • [ 5 ] [Pei M.]Institute for New Energy Materials and Engineering, College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China
  • [ 6 ] [Pei M.]Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fujian, Fuzhou City, 350108, China
  • [ 7 ] [Zhou J.]Institute for New Energy Materials and Engineering, College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China
  • [ 8 ] [Zhou J.]Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fujian, Fuzhou City, 350108, China
  • [ 9 ] [Wang H.]Institute for New Energy Materials and Engineering, College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China
  • [ 10 ] [Wang H.]Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fujian, Fuzhou City, 350108, China
  • [ 11 ] [Liao C.]Institute for New Energy Materials and Engineering, College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China
  • [ 12 ] [Liao C.]Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fujian, Fuzhou City, 350108, China
  • [ 13 ] [Xiao J.]Institute for New Energy Materials and Engineering, College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China
  • [ 14 ] [Xiao J.]Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fujian, Fuzhou City, 350108, China
  • [ 15 ] [Liu Y.]Institute for New Energy Materials and Engineering, College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China
  • [ 16 ] [Liu Y.]Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fujian, Fuzhou City, 350108, China
  • [ 17 ] [Yan W.]Institute for New Energy Materials and Engineering, College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China
  • [ 18 ] [Yan W.]Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fujian, Fuzhou City, 350108, China
  • [ 19 ] [Zhang J.]Institute for New Energy Materials and Engineering, College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China
  • [ 20 ] [Zhang J.]Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fujian, Fuzhou City, 350108, China

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Source ：

Angewandte Chemie - International Edition

ISSN： 1433-7851

Year： 2025

Issue： 23

Volume： 64

1 6 . 1 0 0

JCR@2023

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ESI Highly Cited Papers on the List： 0 Unfold All

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30 Days PV： 2

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