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In overcoming the Li+ desolvation barrier for low‐temperature battery operation, a weakly‐solvated electrolyte based on carboxylate solvent has shown promises. In case of an organic‐anion‐enriched primary solvation sheath (PSS), we found that the electrolyte tends to form a highly swollen, unstable solid electrolyte interphase (SEI) that shows a high permeability to the electrolyte components, accounting...
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