Do Ionic Liquids Slow Down in Stages?

Borah, Bichitra; Acharya, Gobin Raj; Grajeda, Diana; Emerson, Matthew S.; Harris, Matthew A.; Abeykoon, AM Milinda; Sangoro, Joshua; Baker, Gary A.; Nieuwkoop, Andrew J.; Margulis, Claudio J.

doi:10.1021/jacs.3c08639

Title: Do Ionic Liquids Slow Down in Stages?

Journal Article · 14 November 2023 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.3c08639 · OSTI ID:2246888

^[1]; Acharya, Gobin Raj ^[2]; Grajeda, Diana ^[2];

^[1];

^[3]; Abeykoon, AM Milinda ^[4];

^[5];

^[6];

^[2];

^[1]

University of Iowa, Iowa City, IA (United States)
Rutgers University, Piscataway, NJ (United States)
University of Tennessee, Knoxville, TN (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
University of Tennessee, Knoxville, TN (United States); Ohio State University, Columbus, OH (United States)
University of Missouri, Columbia, MO (United States)

High impact recent articles have reported on the existence of a liquid–liquid (L–L) phase transition as a function of both pressure and temperature in ionic liquids (ILs) containing the popular trihexyltetradecylphosphonium cation (P_666,14⁺), sometimes referred to as the “universal liquifier”. The work presented here reports on the structural-dynamic pathway from liquid to glass of the most well-studied IL comprising the P_666,14⁺ cation. We present experimental and computational evidence that, on cooling, the path from the room-temperature liquid to the glass state is one of separate structural-dynamic changes. The first stage involves the slowdown of the charge network, while the apolar subcomponent is fully mobile. A second, separate stage entails the slowdown of the apolar domain. Whereas it is possible that these processes may be related to the liquid–liquid and glass transitions, more research is needed to establish this conclusively.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; CHE-1954358; CHE-1954373; CHE-1753282

OSTI ID:: 2246888

Report Number(s):: BNL-225092-2023-JAAM

Journal Information:: Journal of the American Chemical Society, Vol. 145, Issue 47; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Do Ionic Liquids Slow Down in Stages?

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