Journal
MACROMOLECULES
Volume 46, Issue 3, Pages 867-873Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ma301999a
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Funding
- Office of Science of the U.S. Department of Energy [DE-SC0004993]
- Assistant Secretary for Energy Efficiency and Renewable Energy, Fuel Cell Technologies Program, of the U.S. Department of Energy [DE-AC02-05CH11231]
- U.S. Department of Energy, the Office of Energy Efficiency and Renewable Energy
- Fuel Cells Technology Program from General Motors Corporation [DE-EE0000470]
- Natural Sciences and Engineering Research Council of Canada (NSERC)
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
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Ion-conducting polymers are important materials for a variety of electrochemical applications. Perfluorinated ionomers, such as Nafion, are the benchmark materials for proton conduction and are widely used in fuel cells and other electrochemical devices including solar-fuel generators, chlor-alkali cells, and redox flow batteries. While the behavior of Nafion in bulk membranes (10 to 100s mu m thick) has been studied extensively, understanding its properties under thin-film confinement is limited. Elucidating the behavior of thin Nafion films is particularly important for the optimization of fuel-cell catalyst layers or vapor-operated solar-fuel generators, where a thin film of ionomer is responsible for the transport of ions to and from the active electrocatalytic centers. Using a combination of transport-property measurements and structural characterization, this work demonstrates that confinement of Nafion in thin films induced thickness-dependent proton conductivity and ionic-domain structure. Confining Nafion films to thicknesses below 50 nm on a silicon substrate results in a loss of microphase separation of the hydrophilic and hydrophobic domains, which drastically increases the material's water uptake while in turn decreasing its ionic conductivity.
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