Journal article

Authors list: McAlpine, J; Bloemendal, A; Dahl, JE; Carlson, RMK; Guzei, IA; Clewett, CFM; Tkachenko, BO; Schreiner, PR; Gebbie, MA

Publication year: 2023

Pages: 3545-3554

Journal: Chemistry of Materials

Volume number: 35

Issue number: 9

ISSN: 0897-4756

eISSN: 1520-5002

DOI Link: https://doi.org/10.1021/acs.chemmater.3c00141

Publisher: American Chemical Society

Abstract: 
As large-scale lithium-ion battery deployment accelerates, continued use of flammable organic electrolytes exacerbates issues associated with battery fires during operation and disposal. While ionic liquid-derived electrolytes promise safe, nonflammable alternatives to carbonate electrolytes, the use of ionic liquids in batteries is hindered by poor lithium transport due to the 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 the 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.

Harvard Citation style: McAlpine, J., Bloemendal, A., Dahl, J., Carlson, R., Guzei, I., Clewett, C., et al. (2023) Modulating Entropic Driving Forces to Promote High Lithium Mobility in Solid Organic Electrolytes, Chemistry of Materials, 35(9), pp. 3545-3554. https://doi.org/10.1021/acs.chemmater.3c00141

APA Citation style: McAlpine, J., Bloemendal, A., Dahl, J., Carlson, R., Guzei, I., Clewett, C., Tkachenko, B., Schreiner, P., & Gebbie, M. (2023). Modulating Entropic Driving Forces to Promote High Lithium Mobility in Solid Organic Electrolytes. Chemistry of Materials. 35(9), 3545-3554. https://doi.org/10.1021/acs.chemmater.3c00141