Improving the Catalytic Performance of BaMn(0.7)Cu(0.3)O(3) Perovskite for CO Oxidation in Simulated Cars Exhaust Conditions by Partial Substitution of Ba

通过部分取代钡提高BaMn(0.7)Cu(0.3)O(3)钙钛矿在模拟汽车尾气条件下对CO氧化的催化性能

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Abstract

The sol-gel method, adapted to aqueous media, was used for the synthesis of BaMn(0.7)Cu(0.3)O(3) (BMC) and Ba(0.9)A(0.1)Mn(0.7)Cu(0.3)O(3) (BMC-A, A = Ce, La or Mg) perovskite-type mixed oxides. These samples were fully characterized by ICP-OES, XRD, XPS, H(2)-TPR, BET, and O(2)-TPD and, subsequently, they were evaluated as catalysts for CO oxidation under different conditions simulating that found in cars exhaust. The characterization results show that after the partial replacement of Ba by A metal in BMC perovskite: (i) a fraction of the polytype structure was converted to the hexagonal BaMnO(3) perovskite structure, (ii) A metal used as dopant was incorporated into the lattice of the perovskite, (iii) oxygen vacancies existed on the surface of samples, and iv) Mn(IV) and Mn(III) coexisted on the surface and in the bulk, with Mn(IV) being the main oxidation state on the surface. In the three reactant atmospheres used, all samples catalysed the CO to CO(2) oxidation reaction, showing better performances after the addition of A metal and for reactant mixtures with low CO/O(2) ratios. BMC-Ce was the most active catalyst because it combined the highest reducibility and oxygen mobility, the presence of copper and of oxygen vacancies on the surface, the contribution of the Ce(IV)/Ce(III) redox pair, and a high proportion of surface and bulk Mn(IV). At 200 °C and in the 0.1% CO + 10% O(2) reactant gas mixture, the CO conversion using BMC-Ce was very similar to the achieved with a 1% Pt/Al(2)O(3) (Pt-Al) reference catalyst.

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