Tailoring Coordination in Conventional Ether‐Based Electrolytes for Reversible Magnesium‐Metal Anodes

Rechargeable magnesium (Mg) batteries based on conventional electrolytes are seriously plagued by the formation of the ion‐blocking passivation layer on the Mg metal anode. By tracking the Mg2+ solvation sheath, this work links the passivation components to the Mg2+‐solvents (1,2‐dimethoxyethane, DM...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2022-07, Vol.61 (30), p.e202205187-n/a
Main Authors: Zhao, Wanyu, Pan, Zhenghui, Zhang, Yijie, Liu, Yuan, Dou, Huanglin, Shi, Yayun, Zuo, Zhijun, Zhang, Bowen, Chen, Jianping, Zhao, Xiaoli, Yang, Xiaowei
Format: Article
Language:English
Subjects:
Anodes
Conventional Electrolytes
Coordination
Electrical resistivity
Electrode polarization
Electrolytes
Electrolytic cells
Magnesium
Mg-Metal Batteries
Organophosphorus Additives
Oxygen
Oxygen atoms
Passivity
Phosphorus
Rechargeable batteries
Sheaths
Solid-Electrolyte Interphase
Solvation
Solvation Sheath Rearrangement
Solvents
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Summary:Rechargeable magnesium (Mg) batteries based on conventional electrolytes are seriously plagued by the formation of the ion‐blocking passivation layer on the Mg metal anode. By tracking the Mg2+ solvation sheath, this work links the passivation components to the Mg2+‐solvents (1,2‐dimethoxyethane, DME) coordination and the consequent thermodynamically unstable DME molecules. On this basis, we propose a methodology to tailor solvation coordination by introducing the additive solvent with extreme electron richness. Oxygen atoms in phosphorus‐oxygen groups compete with that in carbon‐oxygen groups of DME for the coordination with Mg2+, thus softening the solvation sheath deformation. Meanwhile, the organophosphorus molecules in the rearranged solvation sheath decompose on the Mg surface, increasing the Mg2+ transport and electrical resistance by three and one orders of magnitude, respectively. Consequently, the symmetric cells exhibit superior cycling performance of over 600 cycles with low polarization. Solvation sheath rearrangement by tuning the Mg2+‐solvents coordination is effectively applied in the magnesium conventional electrolyte. The passivation problem due to solvent decomposition caused by the strong coordination is solved.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202205187