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Title: Membrane-electrode structures for molecular catalysts for use in fuel cells and other electrochemical devices

Abstract

Water soluble catalysts, (M)meso-tetra(N-Methyl-4-Pyridyl)Porphinepentachloride (M=Fe, Co, Mn & Cu), have been incorporated into the polymer binder of oxygen reduction cathodes in membrane electrode assemblies used in PEM fuel cells and found to support encouragingly high current densities. The voltages achieved are low compared to commercial platinum catalysts but entirely consistent with the behavior observed in electroanalytical measurements of the homogeneous catalysts. A model of the dynamics of the electrode action has been developed and validated and this allows the MEA electrodes to be optimized for any chemistry that has been demonstrated in solution. It has been shown that improvements to the performance will come from modifications to the structure of the catalyst combined with optimization of the electrode structure and a well-founded pathway to practical non-platinum group metal catalysts exists.

Inventors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1326793
Patent Number(s):
9,455,451
Application Number:
14/052,576
Assignee:
The Regents of the University of California (Oakland, CA) LBNL
DOE Contract Number:
AC02-05CH11231
Resource Type:
Patent
Resource Relation:
Patent File Date: 2013 Oct 11
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 30 DIRECT ENERGY CONVERSION

Citation Formats

Kerr, John B., Zhu, Xiaobing, Hwang, Gi Suk, Martin, Zulima, He, Qinggang, Driscoll, Peter, Weber, Adam, and Clark, Kyle. Membrane-electrode structures for molecular catalysts for use in fuel cells and other electrochemical devices. United States: N. p., 2016. Web.
Kerr, John B., Zhu, Xiaobing, Hwang, Gi Suk, Martin, Zulima, He, Qinggang, Driscoll, Peter, Weber, Adam, & Clark, Kyle. Membrane-electrode structures for molecular catalysts for use in fuel cells and other electrochemical devices. United States.
Kerr, John B., Zhu, Xiaobing, Hwang, Gi Suk, Martin, Zulima, He, Qinggang, Driscoll, Peter, Weber, Adam, and Clark, Kyle. 2016. "Membrane-electrode structures for molecular catalysts for use in fuel cells and other electrochemical devices". United States. doi:. https://www.osti.gov/servlets/purl/1326793.
@article{osti_1326793,
title = {Membrane-electrode structures for molecular catalysts for use in fuel cells and other electrochemical devices},
author = {Kerr, John B. and Zhu, Xiaobing and Hwang, Gi Suk and Martin, Zulima and He, Qinggang and Driscoll, Peter and Weber, Adam and Clark, Kyle},
abstractNote = {Water soluble catalysts, (M)meso-tetra(N-Methyl-4-Pyridyl)Porphinepentachloride (M=Fe, Co, Mn & Cu), have been incorporated into the polymer binder of oxygen reduction cathodes in membrane electrode assemblies used in PEM fuel cells and found to support encouragingly high current densities. The voltages achieved are low compared to commercial platinum catalysts but entirely consistent with the behavior observed in electroanalytical measurements of the homogeneous catalysts. A model of the dynamics of the electrode action has been developed and validated and this allows the MEA electrodes to be optimized for any chemistry that has been demonstrated in solution. It has been shown that improvements to the performance will come from modifications to the structure of the catalyst combined with optimization of the electrode structure and a well-founded pathway to practical non-platinum group metal catalysts exists.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = 2016,
month = 9
}

Patent:

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  • An electrode supported electrolyte membrane includes an electrode layer 630 facing an electrolyte layer 620. The opposing side of the electrode layer 630 includes a backing layer 640 of a material with a thermal expansion coefficient approximately equal to the thermal expansion coefficient of the electrolyte layer 620. The backing layer 640 is in a two dimensional pattern that covers only a portion of the electrolyte layer 630. An electrochemical cell such as a SOFC is formed by providing a cathode layer 610 on an opposing side of the electrolyte layer 620.
  • A combination, unitary, membrane and electrode assembly with a solid polymer electrolyte membrane, and first and second electrodes at least partially embedded in opposed surfaces of the membrane. The electrodes each comprise a respective group of finely divided carbon particles, very finely divided catalytic particles supported on internal and external surfaces of the carbon particles and a proton conductive material intermingled with the catalytic and carbon particles. A first group of finely divided carbon particles forming the first electrode has greater water attraction and retention properties, and is more hydrophilic than a second group of carbon particles forming the secondmore » electrode. In a preferred method, the membrane electrode assembly of the invention is prepared by forming a slurry of proton conductive material and at least one group of the carbon and catalyst particles. The slurry is applied to the opposed surfaces of the membrane and heated while being pressed to the membrane for a time and at a temperature and compressive load sufficient to embed at least a portion of the particles into the membrane.« less
  • A method of making a combination, unitary, membrane and electrode assembly having a solid polymer electrolyte membrane, and first and second electrodes at least partially embedded in opposed surfaces of the membrane. The electrodes each comprise a respective group of finely divided carbon particles, very finely divided catalytic particles supported on internal and external surfaces of the carbon particles and a proton conductive material intermingled with the catalytic and carbon particles. A first group of finely divided carbon particles forming the first electrode has greater water attraction and retention properties, and is more hydrophilic than a second group of carbonmore » particles forming the second electrode. In a preferred method, the membrane electrode assembly of the invention is prepared by forming a slurry of proton conductive material and at least one group of the carbon and catalyst particles. The slurry is applied to the opposed surfaces of the membrane and heated while being pressed to the membrane for a time and at a temperature and compressive load sufficient to embed at least a portion of the particles into the membrane.« less
  • A method is described for making a combination, unitary, membrane and electrode assembly having a solid polymer electrolyte membrane, and first and second electrodes at least partially embedded in opposed surfaces of the membrane. The electrodes each comprise a respective group of finely divided carbon particles, very finely divided catalytic particles supported on internal and external surfaces of the carbon particles and a proton conductive material intermingled with the catalytic and carbon particles. A first group of finely divided carbon particles forming the first electrode has greater water attraction and retention properties, and is more hydrophilic than a second groupmore » of carbon particles forming the second electrode. In a preferred method, the membrane electrode assembly of the invention is prepared by forming a slurry of proton conductive material and at least one group of the carbon and catalyst particles. The slurry is applied to the opposed surfaces of the membrane and heated while being pressed to the membrane for a time and at a temperature and compressive load sufficient to embed at least a portion of the particles into the membrane. 10 figs.« less
  • In a sodium sulphur cell or other electrochemical cell or energy conversion device in which beta-alumina is used as a solid electrolyte in contact with liquid sodium, improved wetting of the electrolyte by the sodium is obtained by coating the electrolyte, on the surface in contact with the sodium, with a metal, such as lead or bismuth, which will form an alloy with sodium. Conveniently the electrolyte is coated with an aqueous solution of lead acetate, dried and the lead acetate decomposed by heating to leave a lead coating.