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In Science advances

Determining the degree and the spatial extent of structural order in liquids is a grand challenge. Here, we are able to resolve the structural order in a model organic electrolyte of 1 M lithium hexafluorophosphate (LiPF6) dissolved in 1:1 (v/v) ethylene carbonate:diethylcarbonate by developing an integrated method of liquid-phase transmission electron microscopy (TEM), cryo-TEM operated at -30°C, four-dimensional scanning TEM, and data analysis based on deep learning. This study reveals the presence of short-range order (SRO) in the high-salt concentration domains of the liquid electrolyte from liquid phase separation at the low temperature. Molecular dynamics simulations suggest the SRO originates from the Li+-(PF6-)n (n > 2) local structural order induced by high LiPF6 salt concentration.

Xie Yujun, Wang Jingyang, Savitzky Benjamin H, Chen Zheng, Wang Yu, Betzler Sophia, Bustillo Karen, Persson Kristin, Cui Yi, Wang Lin-Wang, Ophus Colin, Ercius Peter, Zheng Haimei

2023-Jan-13