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深入了解阴离子-溶剂相互作用以促进纯SiO||LiNiMnCoO全电池中醚基电解质的稳定运行。

Insights into Anion-Solvent Interactions to Boost Stable Operation of Ether-Based Electrolytes in Pure-SiO ||LiNi Mn Co O Full Cells.

作者信息

Tian Yi-Fan, Tan Shuang-Jie, Lu Zhuo-Ya, Xu Di-Xin, Chen Han-Xian, Zhang Chao-Hui, Zhang Xu-Sheng, Li Ge, Zhao Yu-Ming, Chen Wan-Ping, Xu Quan, Wen Rui, Zhang Juan, Guo Yu-Guo

机构信息

CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences (CAS), 100190, Beijing, P. R. China.

School of Chemical Sciences, University of Chinese Academy of Sciences, 100049, Beijing, P. R. China.

出版信息

Angew Chem Int Ed Engl. 2023 Aug 14;62(33):e202305988. doi: 10.1002/anie.202305988. Epub 2023 Jul 7.

Abstract

Ether solvents with superior reductive stability promise excellent interphasial stability with high-capacity anodes while the limited oxidative resistance hinders their high-voltage operation. Extending the intrinsic electrochemical stability of ether-based electrolytes to construct stable-cycling high-energy-density lithium-ion batteries is challenging but rewarding. Herein, the anion-solvent interactions were concerned as the key point to optimize the anodic stability of the ether-based electrolytes and an optimized interphase was realized on both pure-SiO anodes and LiNi Mn Co O cathodes. Specifically, the small-anion-size LiNO and tetrahydrofuran with high dipole moment to dielectric constant ratio realized strengthened anion-solvent interactions, which enhance the oxidative stability of the electrolyte. The designed ether-based electrolyte enabled a stable cycling performance over 500 cycles in pure-SiO ||LiNi Mn Co O full cell, demonstrating its superior practical prospects. This work provides new insight into the design of new electrolytes for emerging high-energy density lithium-ion batteries through the regulation of interactions between species in electrolytes.

摘要

具有优异还原稳定性的醚类溶剂有望与高容量阳极实现出色的界面稳定性,但其有限的抗氧化性阻碍了它们在高电压下的运行。扩展醚基电解质的固有电化学稳定性以构建稳定循环的高能量密度锂离子电池具有挑战性但很有意义。在此,阴离子与溶剂的相互作用被视为优化醚基电解质阳极稳定性的关键要点,并在纯SiO阳极和LiNiMnCoO阴极上都实现了优化的界面。具体而言,小阴离子尺寸的LiNO和具有高偶极矩与介电常数比的四氢呋喃实现了增强的阴离子-溶剂相互作用,从而提高了电解质的氧化稳定性。所设计的醚基电解质在纯SiO||LiNiMnCoO全电池中实现了超过500次循环的稳定循环性能,展示了其优越的实际应用前景。这项工作通过调节电解质中各物种之间的相互作用为新兴的高能量密度锂离子电池新型电解质的设计提供了新的见解。

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