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Non-Flammable Electrolyte Mediated by Solvation Chemistry toward High-Voltage Lithium-Ion Batteries

Haoran ChengSchool of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, ChinaZheng MaState Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, ChinaPushpendra KumarSchool of Physical Sciences, Jawaharlal Nehru University, New Delhi 110067, IndiaHonghong LiangSchool of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, ChinaZhen CaoKAUST Catalysis Center, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi ArabiaHongliang XieState Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, ChinaLuigi CavalloKAUST Catalysis Center, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi ArabiaQian LiState Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, ChinaJun MingChangchun Institute of Applied Chemistry
2024en
ABI

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The development of nonflammable electrolytes can boost energy density and battery safety, especially for layered metal oxide cathodes operating at high voltage. However, most nonflammable electrolytes are designed in a high concentration for compatibility with graphite electrodes and/or less decomposition. Herein, we introduced a solvation structure-mediated model to develop a nonflammable electrolyte based on trimethyl phosphate (TMP) solvent at a normal concentration. This advancement allows the graphite || lithium cobalt oxide full cell to operate at 4.5 V, delivering high energy density and also exhibiting a nonflammable feature. This achievement is realized using previously unreported components, including carbonate solvent, ethylene sulfate (DTD) additives, and conventional LiPF6 salt. We analyzed the molecular behaviors of each electrolyte composition and also uncovered the unreported impact of DTD, highlighting its prerequisite conditions for effectively weakening the Li+-TMP interactions. This bottom-up design strategy offers a fresh perspective on regulating solvation structures and electrolyte formulations.

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