Breaking solvation dominance of ethylene carbonate via molecular charge engineering enables lower temperature battery

Low temperatures severely impair the performance of lithium-ion batteries, which demand powerful electrolytes with wide liquidity ranges, facilitated ion diffusion, and lower desolvation energy. The keys lie in establishing mild interactions between Li⁺ and solvent molecules internally, which are hard to achieve in commercial ethylene-carbonate based electrolytes. Herein, we tailor the solvation structure with low-ε solvent-dominated coordination, and unlock ethylene-carbonate via electronegativity regulation of carbonyl oxygen. The modified electrolyte exhibits high ion conductivity (1.46 mS cm⁻¹) at -90 °C, and remains liquid at -110 °C. Consequently, 4.5 V graphite-based pouch cells achieve ~98% capacity over 200 cycles at -10 °C without lithium dendrite. These cells also retain ~60% of their room-temperature discharge capacity at -70 °C, and miraculously retain discharge functionality even at ~-100 °C after being fully charged at 25 °C. This strategy of disrupting solvation dominance of ethylene-carbonate through molecular charge engineering, opens new avenues for advanced electrolyte design.

Yuqing Chen, Qiu He, Yun Zhao, Wang Zhou, Peitao Xiao, Peng Gao, Naser Tavajohi, Jian Tu, Baohua Li, Xiangming He, Lidan Xing, Xiulin Fan, Jilei Liu