Authors
Yu-Hui Zhu, Shuang-Jie Tan, Zhi-Wei Yuan, Ya-Hui Wang, Xu-Sheng Zhang, Yao Zhao, Shuang-Yan Lang, Ying Zhang, Rui Wen, Chunli Bai, Yu-Guo Guo, Sen Xin
Published in
Angewandte Chemie (International ed. in English). Pages e6024891. Aug 23, 2026. Epub Aug 23, 2026.
Abstract
Electrolytes with exceptional (electro)chemical and thermal stability are essential prerequisites for high-energy-density rechargeable lithium batteries. Conventional aprotic ether and ester solvents contain polarizable C─H bonds that trigger parasitic proton transfer reactions on the high-voltage cathode surface, driving exothermic electrolyte decomposition and impairing battery cycling stability and safety. Here, we show that deuterium substitution at polarizable C-H moieties introduces kinetic and thermodynamic isotope effects to retard proton transfer and lower solvent oxidation Gibbs free energy. Consequently, the deuterated electrolytes exhibit improved anodic stability and mitigated decomposition during high-voltage charge-discharge of layered oxide cathodes, forming a compact and robust cathode-electrolyte interphase with suppressed CO2 release. The deuterated solvents also have lower combustion enthalpies than their protiated analogs, which translates to substantially reduced heat generation as confirmed by calorimetric measurements. Using deuterated tetrahydrofuran and dimethyl carbonate as model solvents, we validate that such electrolytes enable reversible cathode electrochemistry, as well as markedly improved cycling performance and thermal safety of Li||LiNi0.8Co0.1Mn0.1O2 batteries. This subatomic modification strategy offers a rational electrolyte design framework toward high-performance batteries.
PMID:
42633663
Bibliographic data and abstract were imported from PubMed on 24 Aug 2026.
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