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• W2270074747 abstract "Template-assisted synthesis routes were developed to obtain functional materials like carbon, silicon carbide, various metal oxides and metal nitrides with high surface area and large pore volume having defined pore and particle size distributions [1-3]. Fe-N-C non-noble metal catalysts have been prepared by a template-assisted synthesis route using FeCl3 or CoCl2, pyrrole and a mesoporous silica gel as the template [4]. The resulting materials were shown to exhibit good catalytic activity for the oxygen reduction reaction in acidic media. Here, RuSex/C catalysts, which consist of highly dispersed ruthenium-selenium clusters supported on porous carbon, were prepared by the direct impregnation of a hard template (silica gel) with an aqueous mixture of all the required reactants: sucrose (carbon source), RuCl3•xH2O and SeO2. The resulting RuSex/C catalysts have high surface areas, large pore volumes and show good catalytic activity for the oxygen reduction reaction. Sucrose was added to an aqueous solution of RuCl3•xH20 and SeO2 (0.1M or 0.3M; with a molar ratio of 1:1). This “one pot” process allows the complete infiltration of the reactant mixture into the template porosity. After the infiltration step, the composite material was heat-treated in argon at a final temperature of 900°C for 2 hours. After cooling to 300°C, the gas supply was switched to 5% hydrogen in argon and reductive annealing took place for 2 hours. The obtained composite was then treated with 40% hydrofluoric acid at room temperature to remove the silica template. Increasing the RuCl3•xH20 and SeO2 contents in the synthesis batch increased the Ruand Se-contents of the resulting RuSex/C catalysts. The nitrogen adsorption isotherms of catalyst samples prepared from 0.1M RuSe and 0.3M RuSe respectively are shown in Fig. 1. Two pronounced capillary condensation steps at relative pressures between 0.6 and 0.9 were observed for the RuSex/C catalysts indicating the existence of pore systems with different pore size. The results in Figures 1 are consistent with earlier work on Fe-N-C catalysts prepared by this template-assisted synthesis route [4]. Most of the porosity of these catalysts is created when the inorganic template is removed, and thus the pore size can be controlled by changing the original template. Calculated pore size distributions showed these materials to have pore sizes ranging from 1 nm to 50 nm. The catalytic activity of the RuSex/C catalysts towards the oxygen reduction reaction was tested in an oxygen-saturated solution of HClO4 (0.1M) at room temperature using the rotating-ring disk electrode method. The electrode was rotated at 900 rpm during measurement. Figure 2 shows the current density versus applied electrode potential and demonstrates that the samples prepared from 0.1M RuSe and 0.3M RuSe solutions are active oxygen reduction electrocatalysts. These catalysts exhibit onset potentials between 0.83 V and 0.88 V vs RHE and reach a high diffusion-limited current. Both the onset potential and the halfwave potential increase as the amount of Ru and Se in the catalyst sample increases suggesting that increasing the Ru and Se content increases the number of active sites. The hydrogen peroxide yield varied between 4 to 5% for both catalyst samples. We have presented a novel and very efficient onepot preparation method for the synthesis of highly dispersed ruthenium-selenium clusters supported on porous carbon. The amount of Ru and Se in the resulting RuSex/C catalysts could be easily controlled by changing the initial concentration of RuCl3•xH2O and SeO2 in the precursor mixture." @default.
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• W2270074747 date "2008-01-01" @default.
• W2270074747 modified "2023-10-14" @default.
• W2270074747 title "Templated RuSe-based Catalysts for Proton Exchange Membrane Fuel Cells" @default.
• W2270074747 doi "https://doi.org/10.1149/ma2008-02/11/772" @default.
• W2270074747 hasPublicationYear "2008" @default.
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