Spatially resolved structural order in low-temperature liquid electrolyte

Author:

Xie Yujun123ORCID,Wang Jingyang34ORCID,Savitzky Benjamin H.2,Chen Zheng5,Wang Yu3ORCID,Betzler Sophia3,Bustillo Karen2ORCID,Persson Kristin67ORCID,Cui Yi4ORCID,Wang Lin-Wang3,Ophus Colin2ORCID,Ercius Peter23ORCID,Zheng Haimei37ORCID

Affiliation:

1. Department of Nuclear Engineering, University of California, Berkeley, Berkeley, CA 94720, USA.

2. National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.

3. Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.

4. Department of Materials Science and Engineering, Stanford University, Palo Alto, CA 94305, USA.

5. Department of Mechanical Engineering and Materials Science, Yale University, New Haven, CT 06511, USA.

6. Energy Technologies Area, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.

7. Department of Materials Science and Engineering, University of California, Berkeley, Berkeley, CA 94720, USA.

Abstract

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 (LiPF 6 ) 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 + -(PF 6 ) n ( n  > 2) local structural order induced by high LiPF 6 salt concentration.

Publisher

American Association for the Advancement of Science (AAAS)

Subject

Multidisciplinary

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