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Direct oxidation of methane at low temperature using Pt/c,pd/c,Pt/c-ato and pd/c-ato electrocatalysts prepared by sodium borohydride reduction process

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燃料化学学报 2018年第9期46卷 1137-1145页

作者： J.Nandenha E.H.Fontes R.M.Piasentin F.c.Fonseca A.O.Neto Instituto de Pesquisas Energéticas e Nucleares IPEN/CNEN-SPAv.Prof.Lineu Prestes2242 Cidade UniversitáriaCEP 05508-000Sao PauloSPBrazil

The main objective of this paper was to characterize the voltammetric profiles of the Pt/c,Pt/c-ato,pd/c and pd/cato electrocatalysts and study their catalytic activities for methane oxidation in an acidic electrolyte at 25 ℃ and in a direct methane proton exchange membrane fuel cell at 80 ℃. The electrocatalysts prepared also were characterized by X-ray diffraction( XRD) and transmission electron microscopy( TEM). The diffractograms of the Pt/c and Pt/c-ato electrocatalysts show four peaks associated with Pt face-centered cubic( fcc) structure,and the diffractograms of pd/c and pd/c-ato show four peaks associated with pd face-centered cubic( fcc) structure. For Pt/c-ato and pd/c-ato,characteristic peaks of cassiterite( SnO_2) phase are observed,which are associated with Sb-doped SnO_2( ato) used as supports for electrocatalysts. cyclic voltammograms( cV) of all electrocatalysts after adsorption of methane show that there is a current increase during the anodic scan. However,this effect is more pronounced for Pt/c-ato and pd/c-ato. This process is related to the oxidation of the adsorbed species through the bifunctional mechanism,where ato provides oxygenated species for the oxidation of cO or HcO intermediates adsorbed in Pt or pd sites. From in situ ATR-FTIR( Attenuated Total Reflectance-Fourier Transform Infrared) experiments for all electrocatalysts prepared the formation of HcO or cO intermediates are observed,which indicates the production of carbon dioxide. Polarization curves at 80 ℃in a direct methane fuel cell( DMEFc) show that pd/c and Pt/c electroacatalysts have superior performance to pd/c-ato and Pt/c-ato in methane oxidation.

关键词： sodium borohydride reduction process Pt/c-ato and pd/c-ato electrocatalysts methane oxidation acidic electrolytes polarization curves

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