articleJournal of the American Chemical SocietyJan 20, 2026Closed access

Unraveling the Steric Effect of Trialkyl Phosphates on the Solvation Sheath and Solid Electrolyte Interphase in High-Efficiency Magnesium Electrolytes

Argonne National Laboratory · University of Waterloo · +5 more institutions

PubMed
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Abstract

Designing Mg-compatible and chloride-free electrolytes is important to achieving high-voltage and long-life Mg metal batteries. In electrolytes based on Mg(OTf)2/diglyme: triethyl phosphate that exhibit near 100% Coulombic efficiency for Mg plating/stripping at high current densities and capacities, the TXP (X = alkyl group) plays a key role. Herein, we unveil steric hindrance as the fundamental origin of this role in optimizing the Mg2+ solvation structure and forming electrolyte-derived solid electrolyte interphases. The steric hindrance was tuned by systematically changing the alkyl chain length of the phosphate (TXP) from one to five. Its impact on altering bulk electrolyte solvation and interfacial SEI…

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