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Title: Exploring the Use of Ionic Liquid Mixtures to Enhance the Performance of Dicationic Ionic Liquids

Abstract

Dicationic ionic liquids (DILs) of diverse structural architectures (including symmetrical and asymmetrical ammonium, phosphonium and heterodications and the bis(trifluoromethylsulfonyl)amide (NTf2-) anion) have been prepared and used as additives to N-methyl-N-ethoxyethylpyrrolidinium (P1EOE) NTf2, a relatively high-performing IL in terms of its transport properties (viscosity 53 mPa s). The three-ion, binary IL mixtures were characterized for their thermal and transport properties using differential scanning calorimetry, temperature dependent viscosity, conductivity and Pulsed Gradient Spin Echo (PGSE) NMR. Variable temperature 1H, 19F and 31P self-diffusion coefficients were determined at 25, 60 and 75°C. The order of the diffusion coefficients was D(P1EOE+) > D(anion) > D(dication), and the composition of the dication had a strong effect on the degree to which diffusion of all three species is more or less coupled. IL mixtures containing about 30 mol % of the dicationic NTf2 and 70 mol % of P1EOE NTf2 resulted in a significant decrease in glass transition temperatures and viscosities compared to the pure DIL. The mixtures extended the liquid range and potential for practical applications significantly. Finally, the data obtained here provides insight into the future design of dicationic salts tailored to exhibit lower viscosity and higher conductivities.

Authors:
 [1];  [2];  [3];  [3];  [3];  [4];  [5];  [6];  [6]
  1. Queensborough Community College, Bayside, NY (United States). Dept. of Chemistry
  2. Brooklyn College, Brooklyn, NY (United States). Physics Dept.
  3. Queensborough Community College of the City Univ. of New York, Bayside, NY (United States). Dept. of Chemistry
  4. Hunter College, New York, NY (United States). Dept. of Physics
  5. Univ. of Kelaniya (Sri Lanka). Dept. of Physics
  6. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Queensborough Community College, Bayside, NY (United States); Hunter College, New York, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS); National Science Foundation (NSF); National Inst. of Health (NIH) (United States); Staff Congress of the City Univ. of New York (PSC-CUNY) (United States)
Contributing Org.:
Brooklyn College, Brooklyn, NY (United States); Univ. of Kelaniya (Sri Lanka)
OSTI Identifier:
1358033
Report Number(s):
BNL-113883-2017-JA
Journal ID: ISSN 0013-4651; R&D Project: CO-004; KC0301010
Grant/Contract Number:  
SC0012704; 68132-00 46
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 164; Journal Issue: 8; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Asymmetrical; conductivity; Dicationic; Diffusion Coefficient; DSC; Ionic Liquids; Mixtures; NMR; PGSE

Citation Formats

Lall-Ramnarine, Sharon I., Suarez, Sophia N., Fernandez, Eddie D., Rodriguez, Chanele, Wei, Sujun, Gobet, Mallory, Jayakody, J. R. P., Dhiman, Surajdevprakash B., and Wishart, James F. Exploring the Use of Ionic Liquid Mixtures to Enhance the Performance of Dicationic Ionic Liquids. United States: N. p., 2017. Web. doi:10.1149/2.0271708jes.
Lall-Ramnarine, Sharon I., Suarez, Sophia N., Fernandez, Eddie D., Rodriguez, Chanele, Wei, Sujun, Gobet, Mallory, Jayakody, J. R. P., Dhiman, Surajdevprakash B., & Wishart, James F. Exploring the Use of Ionic Liquid Mixtures to Enhance the Performance of Dicationic Ionic Liquids. United States. https://doi.org/10.1149/2.0271708jes
Lall-Ramnarine, Sharon I., Suarez, Sophia N., Fernandez, Eddie D., Rodriguez, Chanele, Wei, Sujun, Gobet, Mallory, Jayakody, J. R. P., Dhiman, Surajdevprakash B., and Wishart, James F. 2017. "Exploring the Use of Ionic Liquid Mixtures to Enhance the Performance of Dicationic Ionic Liquids". United States. https://doi.org/10.1149/2.0271708jes. https://www.osti.gov/servlets/purl/1358033.
@article{osti_1358033,
title = {Exploring the Use of Ionic Liquid Mixtures to Enhance the Performance of Dicationic Ionic Liquids},
author = {Lall-Ramnarine, Sharon I. and Suarez, Sophia N. and Fernandez, Eddie D. and Rodriguez, Chanele and Wei, Sujun and Gobet, Mallory and Jayakody, J. R. P. and Dhiman, Surajdevprakash B. and Wishart, James F.},
abstractNote = {Dicationic ionic liquids (DILs) of diverse structural architectures (including symmetrical and asymmetrical ammonium, phosphonium and heterodications and the bis(trifluoromethylsulfonyl)amide (NTf2-) anion) have been prepared and used as additives to N-methyl-N-ethoxyethylpyrrolidinium (P1EOE) NTf2, a relatively high-performing IL in terms of its transport properties (viscosity 53 mPa s). The three-ion, binary IL mixtures were characterized for their thermal and transport properties using differential scanning calorimetry, temperature dependent viscosity, conductivity and Pulsed Gradient Spin Echo (PGSE) NMR. Variable temperature 1H, 19F and 31P self-diffusion coefficients were determined at 25, 60 and 75°C. The order of the diffusion coefficients was D(P1EOE+) > D(anion) > D(dication), and the composition of the dication had a strong effect on the degree to which diffusion of all three species is more or less coupled. IL mixtures containing about 30 mol % of the dicationic NTf2 and 70 mol % of P1EOE NTf2 resulted in a significant decrease in glass transition temperatures and viscosities compared to the pure DIL. The mixtures extended the liquid range and potential for practical applications significantly. Finally, the data obtained here provides insight into the future design of dicationic salts tailored to exhibit lower viscosity and higher conductivities.},
doi = {10.1149/2.0271708jes},
url = {https://www.osti.gov/biblio/1358033}, journal = {Journal of the Electrochemical Society},
issn = {0013-4651},
number = 8,
volume = 164,
place = {United States},
year = {Sat May 06 00:00:00 EDT 2017},
month = {Sat May 06 00:00:00 EDT 2017}
}

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Works referencing / citing this record:

Structure and properties of new dicationic ionic liquid DBTMEDA(BF4)2
journal, December 2018