journal article·2021-06-10

Solid-Like Nano-Anion Cluster Constructs a Free Lithium-Ion-Conducting Superfluid Framework in a Water-in-Salt Electrolyte

Pan Tan, Jinming Yue, Yuanxi Yu, Binghang Liu, Tao Liu, Lirong Zheng, Lunhua He, Xiaohua Zhang, Liumin Suo, Liang Hong

The Journal of Physical Chemistry C· Volume 125· Issue 22
Publisher page

Abstract

The ion transportation mechanism in a high-concentration solution remains unclear due to the complexity of the strong ion–ion/ion–solvent interaction, resulting in the invalidation of most ionic conducting theories based on diluted solutions. Here, a superconcentrated electrolyte (water-in-salt) is investigated by multiple experimental techniques, including advanced tools (NMR, synchrotron X-ray diffraction, and spallation neutron scattering), combined with molecular dynamics (MD) simulation to draw out its unique microstructure and uncover its intrinsic relationship with the ionic transportation. Based on the results, we firstly proposed the ionic transport model for the water-in-salt electrolyte, where the solid-like nano-anion clusters construct a superfluid framework and the lithium ion is able to move freely like in an ionic atmosphere. Our model gives a unified explanation to the unique phenomena previously discovered in water-in-salt electrolytes, including the decoupling of conductivity–viscosity and the nanophase separation between the anion and water. Our findings on the microstructure of the super-high-concentrated electrolyte and the involved unique Li-conducting mechanism can fill in the gap between a solid-state conductor and a dilute liquid electrolytic solution.
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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Advanced battery technologies research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

School of Physics and Astronomy, Shanghai Jiao Tong University, Shanghai 200240, China

Institute of Natural Sciences, Shanghai Jiao Tong University, Shanghai 200240, China

Beijing Advanced Innovation Center for Materials Genome Engineering, Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

Spallation Neutron Source Science Center, Dongguan 523803, China

Songshan Lake Materials Laboratory, Dongguan 523808, China

Center for Soft Condensed Matter Physics and Interdisciplinary Research & School of Physical Science and Technology and Jiangsu Key Laboratory of Thin Films, Soochow University, Suzhou 215006, China

Yangtze River Delta Physics Research Center Co. Ltd., Liyang 213300, China

Funding

Shanghai Municipal Education Commission · National Natural Science Foundation of China

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