Song Jiahan, Si Yubing, Guo Wei, Wang Donghai, Fu Yongzhu
College of Chemistry, Zhengzhou University, Zhengzhou, 450001, P. R. China.
Department of Mechanical and Nuclear Engineering, The Pennsylvania State University, University Park, PA, 16802, USA.
Angew Chem Int Ed Engl. 2021 Apr 26;60(18):9881-9885. doi: 10.1002/anie.202016875. Epub 2021 Mar 23.
Deep eutectic electrolytes (DEEs) are a new class of electrolytes with unique properties. However, the intermolecular interactions of DEEs are mostly dominated by Li⋅⋅⋅O interactions, limiting the diversity of chemical space and material constituents. Herein, we report a new class of DEEs induced by Li⋅⋅⋅N interactions between 2,2'-dipyridyl disulfide (DpyDS) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). The strong ion-dipole interaction triggers the deep eutectic phenomenon, thus liberating the Li from LiTFSI and endowing the DEEs with promising ionic conductivity. These DEEs show admirable intrinsic safety, which cannot be ignited by flame. The DEE at the molar ratio of DpyDS:LiTFSI=4:1 (abbreviated as DEE-4:1) is electrochemically stable between 2.1 and 4.0 V vs. Li/Li , and exhibits an ionic conductivity of 1.5×10 S cm at 50 °C. The Li/LiFePO half cell with DEE-4:1 can provide a reversible capacity of 130 mAh g and Coulombic efficiency above 98 % at 50 °C.
深共熔电解质(DEEs)是一类具有独特性质的新型电解质。然而,DEEs的分子间相互作用大多由Li⋅⋅⋅O相互作用主导,限制了化学空间和材料成分的多样性。在此,我们报道了一类由2,2'-二吡啶二硫化物(DpyDS)与双(三氟甲磺酰)亚胺锂(LiTFSI)之间的Li⋅⋅⋅N相互作用诱导形成的新型DEEs。强烈的离子 - 偶极相互作用引发了深共熔现象,从而使Li从LiTFSI中释放出来,并赋予DEEs有前景的离子电导率。这些DEEs表现出令人钦佩的本质安全性,不会被火焰点燃。DpyDS与LiTFSI摩尔比为4:1的DEE(简称为DEE - 4:1)在相对于Li/Li 的2.1至4.0 V之间具有电化学稳定性,并且在50 °C时表现出1.5×10 S cm的离子电导率。具有DEE - 4:1的Li/LiFePO半电池在50 °C时可提供130 mAh g的可逆容量和高于98 %的库仑效率。