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Strong solvent coordination effect inducing gradient solid-electrolyte-interphase formation for highly efficient Mg plating/stripping
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DOI：10.1016/j.ensm.2023.102939.png)
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Abstract
En 中文
Developing simple Mg-salt electrolytes without chlorine-containing additives is vital for the technical viability of rechargeable magnesium batteries (RMBs). However, the formation of an ion-blocking passivation layer on Mg anode in these electrolytes severely hinders the reversible Mg plating/stripping. Here we successfully designed a highly efficient and chlorine-free Mg(SO3CF3)2/ether electrolyte by introducing 2-methoxyethylamine (MOEA) with a strongly nucleophilic amidogen (-NH2) donor for competing solvation coordination. The preferred decomposition of MOEA in MOEA-coordinated Mg-ion complex generates organic N-containing species on sur-face of Mg anode. Accompanied by the SO3CF3- decomposition, the gradient organic-inorganic solid-electrolyte-interphase (SEI) could be formed. This gradient SEI enables a fast interfacial Mg2+ migration and uniform Mg plating/stripping at 5 mA cm-2 with 5 mAh cm- 2. The Mg(SO3CF3)2/ether/MOEA electrolyte exhibits high oxidation stability (3.5 V vs. Mg/Mg2+), high average Coulombic efficiency (99.3%, 1000 cycles), excellent rate performance (low overpotentials of 75, 270 and 570 mV at 0.5, 3.0 and 7.5 mA cm- 2, respectively) and realizes a stable cycle life of Mg||Mo6S8 coin cell (300 cycles at 1 C), when using 50 & mu;m Mg anode. Importantly, the re-lationships between solvation configuration, SEI chemistry and battery performance were successfully built to guide the design of simple Mg-salt electrolytes in RMBs.
Keywords:
Magnesium battery electrolytes
Solvation regulation
Gradient solid-electrolyte-interphase
Magnesium plating/stripping
High rate
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20.2
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5.6K
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6.3W
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