Cai Guorui, Holoubek John, Li Mingqian, Gao Hongpeng, Yin Yijie, Yu Sicen, Liu Haodong, Pascal Tod A, Liu Ping, Chen Zheng
Department of NanoEngineering, University of California, San Diego, La Jolla, CA 92093.
Program of Chemical Engineering, University of California, San Diego, La Jolla, CA 92093.
Proc Natl Acad Sci U S A. 2022 Jul 12;119(28):e2200392119. doi: 10.1073/pnas.2200392119. Epub 2022 Jul 5.
All-climate temperature operation capability and increased energy density have been recognized as two crucial targets, but they are rarely achieved together in rechargeable lithium (Li) batteries. Herein, we demonstrate an electrolyte system by using monodentate dibutyl ether with both low melting and high boiling points as the sole solvent. Its weak solvation endows an aggregate solvation structure and low solubility toward polysulfide species in a relatively low electrolyte concentration (2 mol L). These features were found to be vital in avoiding dendrite growth and enabling Li metal Coulombic efficiencies of 99.0%, 98.2%, and 98.7% at 23 °C, -40 °C, and 50 °C, respectively. Pouch cells employing thin Li metal (50 μm) and high-loading sulfurized polyacrylonitrile (3.3 mAh cm) cathodes (negative-to-positive capacity ratio = 2) output 87.5% and 115.9% of their room temperature capacity at -40 °C and 50 °C, respectively. This work provides solvent-based design criteria for a wide temperature range Li-sulfur pouch cells.
全气候温度运行能力和提高的能量密度已被视为两个关键目标,但在可充电锂电池中很少能同时实现。在此,我们展示了一种电解质体系,其使用具有低熔点和高沸点的单齿二丁醚作为唯一溶剂。其弱溶剂化赋予了一种聚集溶剂化结构,并且在相对较低的电解质浓度(2 mol/L)下对多硫化物物种的溶解度较低。发现这些特性对于避免枝晶生长以及在23°C、-40°C和50°C时分别实现99.0%、98.2%和98.7%的锂金属库仑效率至关重要。采用薄锂金属(50μm)和高负载硫化聚丙烯腈(3.3 mAh/cm²)阴极(负正容量比 = 2)的软包电池在-40°C和50°C时分别输出其室温容量的87.5%和115.9%。这项工作为宽温度范围的锂硫软包电池提供了基于溶剂的设计标准。