Journal
CHEMICAL ENGINEERING JOURNAL
Volume 445, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.136802
Keywords
Wide-temperature range; Low concentration electrolytes; Theoretical calculations; Solvation structure; Lithium metal batteries
Categories
Funding
- National Natural Science Founda-tion of China [52072105, 21676067]
- Anhui Provincial Natural Science Foundation [2108085J23]
- Key R&D Program of Anhui Province [202104a05020044]
- Major Science and Technology Projects in Anhui Province [202003a05020014]
- Fundamental Research Funds for the Central Universities [PA2021KCPY0028, JZ2020YYPY0109]
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This work proposes a solution based on LiDFBOP multi-salt low concentration electrolytes, which demonstrate good performance in wide-temperature Li metal batteries. Molecular dynamics simulations reveal the weaker attractive interactions between solvent molecules, resulting in lower viscosity and freezing point. The thermally stable Li salts have a significant effect on stabilizing the Li metal anode.
Current knowledge and works on high-energy-density Li metal batteries (LMBs) mainly focus on their room temperature performances. However, the wide-temperature properties of LMBs manifesting greater significance in their large-scale applications are rarely explored. In this work, two LiDFBOP-based multi-salt low concentration electrolytes (LCEs) are proposed and further explored by experiments and theoretical calculations for wide-temperature LMBs. Molecular dynamics (MD) simulations reveal the weaker attractive interactions between solvent molecules in LCEs, thus resulting in the lower viscosity and freezing point. Specially, the Li+ in representative solvation structures of LCEs possesses accelerated desolvation behavior with low charge-transfer impedance in Li||Li symmetric cells. Furthermore, the thermally stable Li salts in LCEs manifest obvious effect in stabilizing Li metal anode, which contributes to forming a compact solid electrolyte interphase (SEI) layer with good mechanical properties and high ionic conductivity. Ultimately, the Li||LiNi0.7Co0.1Mn0.2O2 battery exhibits extraordinary electrochemical performances over a wide temperature range (-25 degrees C to 70 degrees C). This work provides a facile and practical design strategy for the wide-temperature LMBs.
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