Anion-Regulated Solvation Structure and Electrode Interface toward Rechargeable Magnesium Batteries.
basic_science · Level V
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- Record sourced from PubMed, PMID 40079399.
- Also identified by DOI 10.1021/acs.nanolett.4c06433.
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Abstract
Developing chlorine-free electrolytes enabling fast Mg<sup>2+</sup> transport through a solid/cathode-electrolyte interphase (SEI/CEI) remains critical for rechargeable magnesium batteries (RMBs). However, single-anion electrolytes often lack the necessary redox properties for this requirement. Here, we propose a dual-anion electrolyte combining magnesium bis(trifluoromethanesulfonyl)imide and 1-butyl-1-methylpiperidinium trifluoromethylsulfonate (PP<sub>14</sub>CF<sub>3</sub>SO<sub>3</sub>) in diglyme and 2-methoxyethylamine (MOEA) solvent, achieving efficient Mg plating/stripping, cathode compatibility, and high anodic stability. The electrostatic interactions between MOEA and Mg<sup>2+</sup>/CF<sub>3</sub>SO<sub>3</sub><sup>-</sup> stabilize the Mg-anode SEI while fostering C<sub><i>x</i></sub>N<sub><i>y</i></sub>-rich CEI formation. This leads to a significantly improved performance in Mg∥Mg and stainless steel (SS)∥Mg cells, with an extended lifespan over 2500 h and average Coulombic efficiency of 98.1%, respectively. Mo<sub>6</sub>S<sub>8</sub>∥Mg full cells exhibit excellent rate performance, while poly(6,6',6″-(benzene-1,3,5-triyl)tris(9,10-anthracenedione)) (PBAQ)∥Mg cells operate at 2.8 V (1 A g<sup>-1</sup>) with ∼70% capacity retention after 200 cycles. The work highlights anion-mediated solvation regulation, providing insights into advanced electrolyte engineering in high-performance RMBs.