Ionic liquids and ionic liquid acids with high temperature stability for fuel cell and other high temperature applications, method of making and cell employing same
Abstract
Disclosed are developments in high temperature fuel cells including ionic liquids with high temperature stability and the storage of inorganic acids as di-anion salts of low volatility. The formation of ionically conducting liquids of this type having conductivities of unprecedented magnitude for non-aqueous systems is described. The stability of the di-anion configuration is shown to play a role in the high performance of the non-corrosive proton-transfer ionic liquids as high temperature fuel cell electrolytes. Performance of simple H.sub.2(g) electrolyte/O.sub.2(g) fuel cells with the new electrolytes is described. Superior performance both at ambient temperature and temperatures up to and above 200.degree. C. are achieved. Both neutral proton transfer salts and the acid salts with HSO.sup.-.sub.4 anions, give good results, the bisulphate case being particularly good at low temperatures and very high temperatures. The performance of all electrolytes is improved by the addition of a small amount of involatile base of pK.sub.a value intermediate between those of the acid and base that make the bulk electrolyte. The preferred case is the imidazole-doped ethylammonium hydrogensulfate which yields behavior superior in all respects to that of the industry standard phosphoric acid electrolyte.
- Inventors:
-
- Mesa, AZ
- Broadview Heights, OH
- Chandler, AZ
- Tokyo, JP
- Issue Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1013669
- Patent Number(s):
- 7867658
- Application Number:
- 10/555,468
- Assignee:
- Arizona Board of Regents for and on behalf of Arizona State University (Scottsdale, AZ)
- Patent Classifications (CPCs):
-
H - ELECTRICITY H01 - BASIC ELECTRIC ELEMENTS H01M - PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
Y - NEW / CROSS SECTIONAL TECHNOLOGIES Y02 - TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE Y02E - REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- DOE Contract Number:
- W-7405-ENG-36
- Resource Type:
- Patent
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Angell, C Austen, Xu, Wu, Belieres, Jean-Philippe, and Yoshizawa, Masahiro. Ionic liquids and ionic liquid acids with high temperature stability for fuel cell and other high temperature applications, method of making and cell employing same. United States: N. p., 2011.
Web.
Angell, C Austen, Xu, Wu, Belieres, Jean-Philippe, & Yoshizawa, Masahiro. Ionic liquids and ionic liquid acids with high temperature stability for fuel cell and other high temperature applications, method of making and cell employing same. United States.
Angell, C Austen, Xu, Wu, Belieres, Jean-Philippe, and Yoshizawa, Masahiro. Tue .
"Ionic liquids and ionic liquid acids with high temperature stability for fuel cell and other high temperature applications, method of making and cell employing same". United States. https://www.osti.gov/servlets/purl/1013669.
@article{osti_1013669,
title = {Ionic liquids and ionic liquid acids with high temperature stability for fuel cell and other high temperature applications, method of making and cell employing same},
author = {Angell, C Austen and Xu, Wu and Belieres, Jean-Philippe and Yoshizawa, Masahiro},
abstractNote = {Disclosed are developments in high temperature fuel cells including ionic liquids with high temperature stability and the storage of inorganic acids as di-anion salts of low volatility. The formation of ionically conducting liquids of this type having conductivities of unprecedented magnitude for non-aqueous systems is described. The stability of the di-anion configuration is shown to play a role in the high performance of the non-corrosive proton-transfer ionic liquids as high temperature fuel cell electrolytes. Performance of simple H.sub.2(g) electrolyte/O.sub.2(g) fuel cells with the new electrolytes is described. Superior performance both at ambient temperature and temperatures up to and above 200.degree. C. are achieved. Both neutral proton transfer salts and the acid salts with HSO.sup.-.sub.4 anions, give good results, the bisulphate case being particularly good at low temperatures and very high temperatures. The performance of all electrolytes is improved by the addition of a small amount of involatile base of pK.sub.a value intermediate between those of the acid and base that make the bulk electrolyte. The preferred case is the imidazole-doped ethylammonium hydrogensulfate which yields behavior superior in all respects to that of the industry standard phosphoric acid electrolyte.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Tue Jan 11 00:00:00 EST 2011},
month = {Tue Jan 11 00:00:00 EST 2011}
}
Works referenced in this record:
The Room Temperature Ionic Liquid 1-Ethyl-3-methylimidazolium Tetrafluoroborate: Electrochemical Couples and Physical Properties
journal, January 1997
- Fuller, Joan
- Journal of The Electrochemical Society, Vol. 144, Issue 11
Preparation of Novel Room-Temperature Molten Salts by Neutralization of Amines
journal, January 2000
- Hirao, Michiko; Sugimoto, Hiromi; Ohno, Hiroyuki
- Journal of The Electrochemical Society, Vol. 147, Issue 11
Electrical Conductivity of Solid and Molten Lithium Sulfate
journal, February 1965
- Kvist, Arnold; Lundén, Arnold
- Zeitschrift für Naturforschung A, Vol. 20, Issue 2
Ionic Liquids by Proton Transfer: Vapor Pressure, Conductivity, and the Relevance of Δp K a from Aqueous Solutions
journal, December 2003
- Yoshizawa, Masahiro; Xu, Wu; Angell, C. Austen
- Journal of the American Chemical Society, Vol. 125, Issue 50
Formation of Glasses from Liquids and Biopolymers
journal, March 1995
- Angell, C. A.
- Science, Vol. 267, Issue 5206
A highly conductive composite electrolyte consisting of polymer and room temperature molten fluorohydrogenates
journal, August 2002
- Tsuda, T.
- Solid State Ionics, Vol. 149, Issue 3-4
Polymer Solid Acid Composite Membranes for Fuel-Cell Applications
journal, January 2000
- Boysen, Dane A.; Chisholm, Calum R. I.; Haile, Sossina M.
- Journal of The Electrochemical Society, Vol. 147, Issue 10
Molecular relaxation properties studied by Rayleigh–Brillouin scattering from aqueous solutions of ammonium nitrate salts
journal, March 1990
- Lee, Y. T.; Schroeder, J.; Choi, C. S.
- The Journal of Chemical Physics, Vol. 92, Issue 6
Ionic Liquids as Alternatives to Traditional Organic and Inorganic Solvents
book, January 2003
- Pagni, Richard M.
- Green Industrial Applications of Ionic Liquids
Phase diagram, electrical conductivity, and cation diffusion of the system lithium sulphate - zinc sulphate
journal, December 1983
- Lunden, A.; Bengtzelius, A.; Kaber, R.
- Solid State Ionics, Vol. 9-10
Contrasting conductance/viscosity relations in liquid states of vitreous and polymer solid electrolytes
journal, April 1988
- McLin, M.; Angell, C. A.
- The Journal of Physical Chemistry, Vol. 92, Issue 8
Fast ion motion in glassy and amorphous materials
journal, December 1983
- Angell, C.
- Solid State Ionics, Vol. 9-10
The phase behaviour of 1-alkyl-3-methylimidazolium tetrafluoroborates; ionic liquids and ionic liquid crystals
journal, January 1999
- Holbrey, John D.; Seddon, Kenneth R.
- Journal of the Chemical Society, Dalton Transactions, Issue 13
The Performance and Stability of Ambient Temperature Molten Salts for Solar Cell Applications
journal, January 1996
- Papageorgiou, N.
- Journal of The Electrochemical Society, Vol. 143, Issue 10
Micelle formation in ethylammonium nitrate, a low-melting fused salt
journal, July 1982
- Evans, D. Fennell; Yamauchi, Akira; Roman, Ronald
- Journal of Colloid and Interface Science, Vol. 88, Issue 1
Electrolyte solutions for technology - new aspects and approaches
journal, September 1999
- Barthel, J. M. G.; Gores, H. J.; Neueder, R.
- Pure and Applied Chemistry, Vol. 71, Issue 9
Non-aqueous electrolyte solutions in chemistry and modern technology
book, January 1983
- Barthel, Josef; Gores, Heiner-J.; Schmeer, Georg
- Physical and Inorganic Chemistry
Preparation and characterization of matrices for phosphoric acid fuel cells
journal, January 1997
- Caires, M. I.; Buzzo, M. L.; Ticianelli, E. A.
- Journal of Applied Electrochemistry, Vol. 27, Issue 1, p. 19-24
A high-performance phosphoric acid fuel cell
journal, December 2001
- Neergat, M.; Shukla, A. K.
- Journal of Power Sources, Vol. 102, Issue 1-2
Origin and Control of Low-Melting Behavior in Salts, Polysalts, Salt Solvates, and Glassformers
book, January 2002
- Angell, C. A.
- Molten Salts: From Fundamentals to Applications
On the mechanism of the thermal transformations in solid ammonium nitrate
journal, March 1962
- Brown, R. N.; McLaren, A. C.
- Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences, Vol. 266, Issue 1326, p. 329-343
Self-diffusion of methylammonium cations in the high-temperature solid phase of CH3NH3NO3
journal, January 1985
- Ishida, Hiroyuki; Ikeda, Ryuichi; Nakamura, Daiyu
- Journal of the Chemical Society, Faraday Transactions 2, Vol. 81, Issue 6
Reorientational motion in superionic sulfates: A Raman linewidth study
journal, August 1985
- Börjesson, L.; Torell, L. M.
- Physical Review B, Vol. 32, Issue 4
Liquid-crystalline ionic liquids
journal, January 1996
- Bowlas, Christopher J.; Bruce, Duncan W.; Seddon, Kenneth R.
- Chemical Communications, Issue 14
Competitive Interactions and Glassy State Extension in Lithium Salt Solutions
journal, May 1999
- Sivaraman, Alwarappa; Senapati, Hema; Angell, C. Austen
- The Journal of Physical Chemistry B, Vol. 103, Issue 20
Brønsted acid–base ionic liquids and their use as new materials for anhydrous proton conductors
journal, January 2003
- Susan, Md. A. B. H.; Noda, Akihiro; Mitsushima, Shigenori
- Chemical Communications, Issue 8
Weakly Coordinating Anions, and the Exceptional Conductivity of Their Nonaqueous Solutions
journal, January 2001
- Xu, Wu; Angell, C. Austen
- Electrochemical and Solid-State Letters, Vol. 4, Issue 1
Versatile organic iodide melts and glasses with high mole fractions of LiI: Glass transition temperatures and electrical conductivities
journal, December 1983
- Cooper, E.; Angell, C.
- Solid State Ionics, Vol. 9-10
Room-Temperature Molten Salts Based on the Quaternary Ammonium Ion
journal, October 1998
- Sun, J.; Forsyth, M.; MacFarlane, D. R.
- The Journal of Physical Chemistry B, Vol. 102, Issue 44
A Theory of Water and Ionic Solution, with Particular Reference to Hydrogen and Hydroxyl Ions
journal, August 1933
- Bernal, J. D.; Fowler, R. H.
- The Journal of Chemical Physics, Vol. 1, Issue 8
Brønsted Acid−Base Ionic Liquids as Proton-Conducting Nonaqueous Electrolytes
journal, May 2003
- Noda, Akihiro; Susan, Md. Abu Bin Hasan; Kudo, Kenji
- The Journal of Physical Chemistry B, Vol. 107, Issue 17
On the Kinetic Theory of Dense Fluids. XVI. The Ideal Ionic Melt
journal, March 1964
- Berne, Bruce; Rice, Stuart A.
- The Journal of Chemical Physics, Vol. 40, Issue 5
Use of Ionic Liquids for pi -Conjugated Polymer Electrochemical Devices
journal, July 2002
- Lu, W.
- Science, Vol. 297, Issue 5583
NMR study of proton transfer interactions in the system pyridine +HCl (0%–95%)
journal, October 1977
- Shuppert, J. W.; Angell, C. A.
- The Journal of Chemical Physics, Vol. 67, Issue 7
Working Salts: Syntheses and Uses of Ionic Liquids Containing Functionalized Ions
book, July 2002
- Davis, Jr., James H.
- ACS Symposium Series
Glass transitions in molecular liquids. I. Influence of proton transfer processes in hydrazine-based solutions
journal, June 1971
- Angell, C. A.; Sutter, E. J.
- The Journal of Physical Chemistry, Vol. 75, Issue 12
Room-Temperature Ionic Liquids. Solvents for Synthesis and Catalysis
journal, August 1999
- Welton, Thomas
- Chemical Reviews, Vol. 99, Issue 8, p. 2071-2084
Solvent-Free Electrolytes with Aqueous Solution-Like Conductivities
journal, October 2003
- Xu, W.
- Science, Vol. 302, Issue 5644
Rapid, clean, and mild O-acetylation of alcohols and carbohydrates in an ionic liquid
journal, March 2002
- Forsyth, Stewart A.; MacFarlane, Douglas R.; Thomson, Robin J.
- Chemical Communications, Issue 7
The Application of Room Temperature Molten Salt with Low Viscosity to the Electrolyte for Dye-Sensitized Solar Cell
journal, January 2001
- Matsumoto, Hajime; Matsuda, Toshihiko; Tsuda, Tetsuya
- Chemistry Letters, Vol. 30, Issue 1
A Highly Conductive Room Temperature Molten Fluoride: EMIF⋅2.3HF
journal, January 2002
- Hagiwara, Rika; Hirashige, Takayuki; Tsuda, Tetsuya
- Journal of The Electrochemical Society, Vol. 149, Issue 1
Ionic Liquids: Ion Mobilities, Glass Temperatures, and Fragilities
journal, June 2003
- Xu, Wu; Cooper, Emanuel I.; Angell, C. Austen
- The Journal of Physical Chemistry B, Vol. 107, Issue 25
Glass‐Forming Composition Regions and Glass Transition Temperatures for Aqueous Electrolyte Solutions
journal, February 1970
- Angell, C. A.; Sare, E. J.
- The Journal of Chemical Physics, Vol. 52, Issue 3
Design of New Ionic Liquids by Neutralization of Imidazole Derivatives with Imide-Type Acids
journal, January 2001
- Yoshizawa, Masahiro; Ogihara, Wataru; Ohno, Hiroyuki
- Electrochemical and Solid-State Letters, Vol. 4, Issue 6