Rational Electrolyte Design for Elevated-Temperature and Thermally Stable Lithium-Ion Batteries with Nickel-Rich CathodesClick to copy article linkArticle link copied!
- Hao JiaHao JiaEnergy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Hao Jia
- Benjamin BroekhuisBenjamin BroekhuisEnergy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMcKetta Department of Chemical Engineering, The University of Texas at Austin, Austin, Texas 78712, United StatesMore by Benjamin Broekhuis
- Yaobin XuYaobin XuEnvironmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Yaobin Xu
- Zhijie YangZhijie YangDepartment of Chemistry, Virginia Tech, Blacksburg, Virginia 24061, United StatesMore by Zhijie Yang
- David KautzDavid KautzEnergy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by David Kautz
- Lirong ZhongLirong ZhongEnergy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Lirong Zhong
- Mark H. EngelhardMark H. EngelhardEnergy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Mark H. Engelhard
- Qian ZhaoQian ZhaoEnvironmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Qian Zhao
- Mark E. BowdenMark E. BowdenPhysical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Mark E. Bowden
- Bethany E. MatthewsBethany E. MatthewsEnergy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Bethany E. Matthews
- Callum ConnorCallum ConnorDepartment of Chemistry, Virginia Tech, Blacksburg, Virginia 24061, United StatesMore by Callum Connor
- Feng LinFeng LinDepartment of Chemistry, Virginia Tech, Blacksburg, Virginia 24061, United StatesMore by Feng Lin
- Chongmin WangChongmin WangEnvironmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Chongmin Wang
- Wu Xu*Wu Xu*E-mail: [email protected]Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United StatesMore by Wu Xu
Abstract

As the energy density of lithium-ion batteries (LIBs) increases, the shortened cycle life and the increased safety hazards of LIBs are drawing increasing concerns. To address such challenges, a series of localized high-concentration electrolytes (LHCEs) based on a solvating-solvent mixture of tetramethylene sulfone and trimethyl phosphate and a high flash-point diluent 1H,1H,5H-octafluoropentyl 1,1,2,2-tetrafluoroethyl ether were designed. The LHCEs exhibited nonflammability and greatly suppressed heat release at elevated temperatures, which would potentially improve the safety performance of the LIBs. Moreover, the optimal LHCE achieved capacity retentions of 87.1% and 81.7% in graphite||LiNi0.8Mn0.1Co0.1O2 cells after 500 cycles at 25 and 45 °C, respectively, which were significantly higher than the conventional electrolyte, whose capacity retentions were only 75.2% and 38.5% under the same conditions. Mechanistic studies revealed that the LHCE not only formed a more robust solid electrolyte interphase but also exhibited improved anodic stability, compared with the conventional electrolyte. This work sheds light on rational electrolyte design for high-energy density LIBs with high battery performance and low safety concerns.
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