Silicon oxide/Nafion composite membranes were studied for operation in hydrogen/oxygen proton-exchange membrane fuel cells ͑PEMFCs͒ from 80 to 140°C. The composite membranes were prepared either by an impregnation of Nafion 115 via sol-gel processing of tetraethoxysilane or by preparing a recast film, using solubilized Nafion 115 and a silicon oxide polymer/gel. Tetraethoxysilane, when reacted with water in an acidic medium, undergoes polymerization to form a mixture of SiO 2 and siloxane polymer with product hydroxide and ethoxide groups. This material is referred to as SiO s /-OH/-OEt. When Nafion is used as the acidic medium, the SiO 2 /siloxane polymer forms within the membrane. All composite membranes had a silicon oxide content of less than or equal to 10 wt %. The silicon oxide improved the water retention of the composite membranes, increasing proton conductivity at elevated temperatures. Attenuated total reflectance-Fourier transform infrared spectroscopy and scanning electron microscopy experiments indicated an evenly distributed siloxane polymer of SiO 2 /-OH/-OEt in the composite membranes. At a potential of 0.4 V, silicon oxide/Nafion 115 composite membranes delivered four times the current density obtained with unmodified Nafion 115 in a H 2 /O 2 PEMFC at 130°C and a pressure of 3 atm. Furthermore, silicon oxide-modified membranes were more robust than the control membranes ͑unmodified Nafion 115 and recast Nafion͒, which degraded after high operation temperature and thermal cycling.

Metal-oxide-recast Nafion composite membranes were studied for operation in hydrogen/oxygen protonexchange membrane fuel cells (PEMFC) from 80 to 130 °C and at relative humidities ranging from 75 to 100%. Membranes of nominal 125 µm thickness were prepared by suspending a variety of metal oxide particles (SiO 2 , TiO 2 , Al 2 O 3 , and ZrO 2 ) in solubilized Nafion. The composite membranes were characterized using electrochemical, X-ray scattering, spectroscopic, mechanical, and thermal analysis techniques. Membrane characteristics were compared to fuel cell performance. These studies indicated a specific chemical interaction between polymer sulfonate groups and the metal oxide surface for systems that provide a good elevated-temperature (i.e., fuel-cell operation above 120 °C) performance. Composite systems that incorporate either a TiO 2 or a SiO 2 phase produced superior elevated-temperature, lowhumidity behavior compared to that of a simple Nafion-based fuel cell. Improved temperature tolerance permits the introduction of at least 500 ppm CO contaminant in the H 2 fuel stream without cell failure, in contrast to standard Nafion-based cells, which fail below 50 ppm of carbon monoxide.

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