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Modification of Proton Conducting Metal-Organic Frameworks for Improved Performance in Fuel Cell Applications

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Advisor
Shimizu, George Kisa Hayashi
Author
Dawson, Karl William
Accessioned
2013-04-25T15:21:37Z
Available
2013-06-10T07:00:44Z
Issued
2013-04-25
Submitted
2013
Other
Metal-Organic Framework
Fuel Cell
Proton Exchange Membrane
MOF
Proton Conduction
AC Impedance Spectroscopy
Isomorphous Ligand Replacement
Pore Loading
Mixed Matrix Membrane
Subject
Chemistry--Inorganic
Type
Thesis
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Abstract
The use of metal-organic frameworks (MOFs) as proton conductors for practical applications is challenging, owing to the difficulties in obtaining a MOF with the desired conductivity levels and stability, and the complications of incorporating a polycrystalline powder into a device. This thesis examines these challenges, and addresses methods that could be used to improve the suitability of MOFs for commercial applications. First, an overview of the difficulties in preparing, measuring, and interpreting the data obtained from alternating current electrochemical impedance spectroscopy of MOFs is presented. Next, an examination of three potential methods of improving the performance of a proton conducting MOF, trisodium 1,3,5-trihydroxy-2,4,6-benzene trisulfonate (Na3Pgs), will be discussed. First, ligand doping of the Na3Pgs system, with 1,3,5 benzenetriphosphonic acid, was performed via a novel isomorphous ligand replacement method. The conductivity increased by an order of magnitude to (2.1 ± 0.5) x 10^-2 S/cm, which is the highest conductivity reported for any MOF system. Secondly, loading heterocycle guests into Na3Pgs improves the conductivity, but controlled loading is a relatively unexplored area, and was examined using Na3Pgs loaded with 1,2,4-triazole (Tz). It was found that Tz is incorporated into the system as the triazolium cation (HTz), giving the general formula [Na(1-x)(HTz)x]3Pgs, and that this kinetically controlled loading is affected by many synthetic parameters, but precise control over such systems is achievable. Finally, as a proof-of-principle, Na3Pgs was mixed with Nafion®, to examine whether a MOF mixed-matrix membrane could be used in a fuel cell. Homogeneous membranes were formed, and conductivity is improved under anhydrous conditions above 150°C, but a more stable MOF is required before commercial applications can be considered.
Corporate
University of Calgary
Faculty
Graduate Studies
Doi
http://dx.doi.org/10.11575/PRISM/26972
Uri
http://hdl.handle.net/11023/620
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