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

Yuqing ChenCollege of Materials Science and Engineering, Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy, Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology, Hunan University, Changsha, 410082, People's Republic of ChinaQiu HeCollege of Materials Science and Engineering, Sichuan University, Chengdu, 610065, P. R. ChinaYun ZhaoInstitute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, ChinaWang ZhouCollege of Materials Science and Engineering, Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy, Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology, Hunan University, Changsha, 410082, People's Republic of ChinaPeitao XiaoCollege of Aerospace Science and Engineering, National University of Defense Technology, Changsha, 410073, ChinaPeng GaoCollege of Materials Science and Engineering, Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy, Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology, Hunan University, Changsha, 410082, People's Republic of ChinaNaser TavajohiDepartment of Chemistry, Umeå University, Umeå, 90187, SwedenJian TuBaohua LiInstitute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, ChinaXiangming HeInstitute of Nuclear and New Energy Technology, Tsinghua University, Beijing, 100084, ChinaLidan XingEngineering Research Center of MTEES (Ministry of Education), Research Center of BMET (Guangdong Province), Engineering Lab. of OFMHEB (Guangdong Province), Key Lab. of ETESPG (GHEI), And Innovative Platform for ITBMD (Guangzhou Municipality), School of Chemistry, South China Normal University, Guangzhou, 510006, ChinaXiulin FanState Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, ChinaJilei LiuCollege of Materials Science and Engineering, Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy, Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology, Hunan University, Changsha, 410082, People's Republic of China. [email protected]
2023en
ABI

Аннотация

Abstract 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.

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