Li Qin, Yang Chongyin, Zhang Jiaxun, Ji Xiao, Xu Jijian, He Xinzi, Chen Long, Hou Singyuk, Uddin Jasim, Addison Dan, Sun Dalin, Wang Chunsheng, Wang Fei
Department of Materials Science, Fudan University, Shanghai, China.
Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD, USA.
Angew Chem Int Ed Engl. 2022 Dec 5;61(49):e202214126. doi: 10.1002/anie.202214126. Epub 2022 Nov 4.
Solid electrolyte interphase (SEI) formation and H O activity reduction in Water-in-Salt electrolytes (WiSE) with an enlarged stability window of 3.0 V have provided the feasibility of the high-energy-density aqueous Li-ion batteries. Here, we extend the cathodic potential of WiSE by rationally controlling intermolecular interaction and interphase chemistry with the introduction of trimethyl phosphate (TMP) into WiSE. The TMP not merely limits the H O activity via the strong interaction between TMP and H O but also contributes to the formation of reinforced SEI involving phosphate and LiF by manipulating the Li solvation structure. Thus, water-tolerance LiMn O (LMO)||Li Ti O (LTO) full cell with a P/N ratio of 1.14 can be assembled and achieve a long cycling life of 1000 times with high coulombic efficiency of >99.9 %. This work provides a promising insight into the cost-effective practical manufacture of LMO||LTO cells without rigorous moisture-free requirements.
具有3.0 V扩大稳定窗口的盐包水电解质（WiSE）中固体电解质界面（SEI）的形成和水活性的降低为高能量密度水系锂离子电池提供了可行性。在此，我们通过将磷酸三甲酯（TMP）引入WiSE中，合理控制分子间相互作用和界面化学，从而扩展了WiSE的阴极电位。TMP不仅通过TMP与水之间的强相互作用限制水活性，还通过操纵锂溶剂化结构，有助于形成包含磷酸盐和LiF的强化SEI。因此，可以组装P/N比为1.14的耐水LiMn₂O₄（LMO）||Li₂Ti₃O₇（LTO）全电池，并实现1000次的长循环寿命，库仑效率>99.9 %。这项工作为无需严格无水分要求的LMO||LTO电池的经济高效实际制造提供了有前景的见解。
