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Tailoring Coordination in Conventional Ether-Based Electrolytes for Reversible Magnesium-Metal Anodes
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PRE
AI
W
Z
张
Y
H
Y
Z
B
陈
X
杨
DOI：10.1002/anie.202205187.png)
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Abstract
En 中文
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.
Keywords:
Conventional Electrolytes
Mg-Metal Batteries
Organophosphorus Additives
Solid-Electrolyte Interphase
Solvation Sheath Rearrangement
Journal
IF:
16.9
Papers:
5.6W
Citations:
53.0W
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Cited Papers