1,8‐Diazabicyclo[5.4.0]undec‐7‐ene as Cyclic Ether Electrolyte Polymerization Inhibition for Wide‐Temperature‐Range High‐Rate Lithium‐ion Batteries
Abstract 1,3‐Dioxolane (DOL), with its broad liquid phase temperature window and low Li+‐solvent binding energy, stands out as an ideal solvent candidate for the wide‐temperature and high‐rate electrolytes. Unfortunately, DOL is susceptible to undergo ring‐opening polymerization under common lithium...
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Wiley
2025-01-01
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| Online Access: | https://doi.org/10.1002/advs.202409259 |
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| author | Hui Tian Zixin Hong Zhenhan Fang Yufeng Luo Hengcai Wu Fei Zhao Qunqing Li Shoushan Fan Jiaping Wang |
| author_facet | Hui Tian Zixin Hong Zhenhan Fang Yufeng Luo Hengcai Wu Fei Zhao Qunqing Li Shoushan Fan Jiaping Wang |
| author_sort | Hui Tian |
| collection | DOAJ |
| description | Abstract 1,3‐Dioxolane (DOL), with its broad liquid phase temperature window and low Li+‐solvent binding energy, stands out as an ideal solvent candidate for the wide‐temperature and high‐rate electrolytes. Unfortunately, DOL is susceptible to undergo ring‐opening polymerization under common lithium salts, which markedly retards the reaction kinetics. This work introduces the organic basic additive 1,8‐Diazabicyclo[5.4.0]undec‐7‐ene (DBU) to effectively suppress the polymerization, thus achieving compatibility between LiFSI, LiDFOB lithium salts, and DOL. Furthermore, density functional theory (DFT) calculations are utilized to elucidate the underlying mechanisms of DOL polymerization and to clarify how DBU inhibits its polymerization. The resulting electrolyte, devoid of polymer chain formation, forms a weak solvation structure rich in anions, which demonstrates rapid ion transport kinetics in the bulk electrolyte and excellent electrochemical stability at the electrolyte–electrode interfaces (EEIs) simultaneously. When applied to the LiFePO4||graphite full cell, it exhibits exceptional wide‐temperature and high‐rate performance, with specific capacities reaching 101.2 mAh g −1 at room temperature (20 C), 36.9 mAh g−1 at −40 °C (0.5 C), and 118.0 mAh g−1 at 60 °C (20 C). This study significantly guides the development of wide‐temperature, high‐rate electrolytes. |
| format | Article |
| id | doaj-art-89bc1305db194a82b3c4f5c86844657f |
| institution | Kabale University |
| issn | 2198-3844 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Wiley |
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| series | Advanced Science |
| spelling | doaj-art-89bc1305db194a82b3c4f5c86844657f2025-01-13T15:29:43ZengWileyAdvanced Science2198-38442025-01-01122n/an/a10.1002/advs.2024092591,8‐Diazabicyclo[5.4.0]undec‐7‐ene as Cyclic Ether Electrolyte Polymerization Inhibition for Wide‐Temperature‐Range High‐Rate Lithium‐ion BatteriesHui Tian0Zixin Hong1Zhenhan Fang2Yufeng Luo3Hengcai Wu4Fei Zhao5Qunqing Li6Shoushan Fan7Jiaping Wang8Department of Physics and Tsinghua‐Foxconn Nanotechnology Research Center Tsinghua University Beijing 100084 ChinaDepartment of Physics and Tsinghua‐Foxconn Nanotechnology Research Center Tsinghua University Beijing 100084 ChinaDepartment of Physics and Tsinghua‐Foxconn Nanotechnology Research Center Tsinghua University Beijing 100084 ChinaInstitute of Textiles and Clothing Hong Kong Polytechnic University Hong Kong SAR 99077 ChinaDepartment of Physics and Tsinghua‐Foxconn Nanotechnology Research Center Tsinghua University Beijing 100084 ChinaDepartment of Physics and Tsinghua‐Foxconn Nanotechnology Research Center Tsinghua University Beijing 100084 ChinaDepartment of Physics and Tsinghua‐Foxconn Nanotechnology Research Center Tsinghua University Beijing 100084 ChinaDepartment of Physics and Tsinghua‐Foxconn Nanotechnology Research Center Tsinghua University Beijing 100084 ChinaDepartment of Physics and Tsinghua‐Foxconn Nanotechnology Research Center Tsinghua University Beijing 100084 ChinaAbstract 1,3‐Dioxolane (DOL), with its broad liquid phase temperature window and low Li+‐solvent binding energy, stands out as an ideal solvent candidate for the wide‐temperature and high‐rate electrolytes. Unfortunately, DOL is susceptible to undergo ring‐opening polymerization under common lithium salts, which markedly retards the reaction kinetics. This work introduces the organic basic additive 1,8‐Diazabicyclo[5.4.0]undec‐7‐ene (DBU) to effectively suppress the polymerization, thus achieving compatibility between LiFSI, LiDFOB lithium salts, and DOL. Furthermore, density functional theory (DFT) calculations are utilized to elucidate the underlying mechanisms of DOL polymerization and to clarify how DBU inhibits its polymerization. The resulting electrolyte, devoid of polymer chain formation, forms a weak solvation structure rich in anions, which demonstrates rapid ion transport kinetics in the bulk electrolyte and excellent electrochemical stability at the electrolyte–electrode interfaces (EEIs) simultaneously. When applied to the LiFePO4||graphite full cell, it exhibits exceptional wide‐temperature and high‐rate performance, with specific capacities reaching 101.2 mAh g −1 at room temperature (20 C), 36.9 mAh g−1 at −40 °C (0.5 C), and 118.0 mAh g−1 at 60 °C (20 C). This study significantly guides the development of wide‐temperature, high‐rate electrolytes.https://doi.org/10.1002/advs.202409259cyclic ether‐based electrolyteshigh rateslithium‐ion batteriespolymerization inhibitionswide temperatures |
| spellingShingle | Hui Tian Zixin Hong Zhenhan Fang Yufeng Luo Hengcai Wu Fei Zhao Qunqing Li Shoushan Fan Jiaping Wang 1,8‐Diazabicyclo[5.4.0]undec‐7‐ene as Cyclic Ether Electrolyte Polymerization Inhibition for Wide‐Temperature‐Range High‐Rate Lithium‐ion Batteries Advanced Science cyclic ether‐based electrolytes high rates lithium‐ion batteries polymerization inhibitions wide temperatures |
| title | 1,8‐Diazabicyclo[5.4.0]undec‐7‐ene as Cyclic Ether Electrolyte Polymerization Inhibition for Wide‐Temperature‐Range High‐Rate Lithium‐ion Batteries |
| title_full | 1,8‐Diazabicyclo[5.4.0]undec‐7‐ene as Cyclic Ether Electrolyte Polymerization Inhibition for Wide‐Temperature‐Range High‐Rate Lithium‐ion Batteries |
| title_fullStr | 1,8‐Diazabicyclo[5.4.0]undec‐7‐ene as Cyclic Ether Electrolyte Polymerization Inhibition for Wide‐Temperature‐Range High‐Rate Lithium‐ion Batteries |
| title_full_unstemmed | 1,8‐Diazabicyclo[5.4.0]undec‐7‐ene as Cyclic Ether Electrolyte Polymerization Inhibition for Wide‐Temperature‐Range High‐Rate Lithium‐ion Batteries |
| title_short | 1,8‐Diazabicyclo[5.4.0]undec‐7‐ene as Cyclic Ether Electrolyte Polymerization Inhibition for Wide‐Temperature‐Range High‐Rate Lithium‐ion Batteries |
| title_sort | 1 8 diazabicyclo 5 4 0 undec 7 ene as cyclic ether electrolyte polymerization inhibition for wide temperature range high rate lithium ion batteries |
| topic | cyclic ether‐based electrolytes high rates lithium‐ion batteries polymerization inhibitions wide temperatures |
| url | https://doi.org/10.1002/advs.202409259 |
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