Modulating entropic driving forces to promote high lithium mobility in solid organic electrolytes

24 January 2023, Version 1
This content is a preprint and has not undergone peer review at the time of posting.


As large-scale lithium-ion battery deployment accelerates, continued use of flammable organic electrolytes exacerbate issues associated with battery fires during operation and disposal. While ionic liquid-derived electrolytes promise safe, nonflammable alternatives to carbonate electrolytes, use of ionic liquids in batteries is hindered by poor lithium transport due to formation of long-lived lithium-anion complexes. We report the design and characterization of novel ionic liquid-inspired organic electrolytes that leverage unique self-assembly properties of molecular diamond templates, called “diamondoids.” Combining thermodynamic characterization, vibrational and magnetic spectroscopy, and single-crystal X-ray analysis, we determine that diamondoid-functionalized cations can facilitate formation of molecularly porous phases that resist restructuring upon dissolution of lithium salts. These electrolytes can suppress lithium-anion coordination, manifesting in substantially enhanced lithium-ion mobility in the organic ion matrix. Our results provide a new paradigm for enhancing lithium mobility in solid electrolytes by tuning entropic self-assembly to enhance organic cation-anion interactions, suppress lithium-anion coordination, and increase lithium mobility in solid electrolytes.


Ionic Liquids
Ion coordination
Lithium mobility

Supplementary materials

Supplemental Information
Supplemental information for the submitted work. Includes extra phase behavior data, Raman spectroscopy, and NMR characterization of chemicals tested. Also contains all crystallographic information required to analyze the crystal structure that is not included in the main text.


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