Abstract
Formic acid is an advantageous liquid organic hydrogen carrier. It is relatively nontoxic and can be synthesized by the reaction of CO2 with sustainable hydrogen or by biomass decomposition. As an alternative to more widely studied powdery catalysts, supported Pd-C catalytic thin films with controlled nanostructure and compositions were newly prepared in this work by magnetron sputtering on structured supports and tested for the formic acid decomposition reaction. A two-magnetron configuration (carbon and tailored Pd-C targets) was used to achieve a reduction in Pd consumption and high catalyst surface roughness and dispersion by increasing the carbon content. Activity and durability tests were carried out for the gas phase formic acid decomposition reaction on SiC foam monoliths coated with the Pd-C films and the effects of column width, surface roughness and thermal pre-reduction time were investigated. Activity of 5.04 molH2·gPd-1·h-1 and 92% selectivity to the dehydrogenation reaction were achieved at 300 °C for the catalyst with a lower column width and higher carbon content and surface roughness. It was also found that deactivation occurs when Pd is sintered due to the elimination of carbon and/or the segregation and agglomeration of Pd upon cycling. Magnetron sputtering deposition appears as a promising and scalable route for the one-step preparation of Pd-C catalytic films by overcoming the different deposition characteristics of Pd and C with an appropriate experimental design.