Bulk Versus Surface Modification of Alumina with Mn and Ce Based Oxides for CH(4) Catalytic Combustion

利用锰和铈基氧化物对氧化铝进行体相与表面改性以用于CH(4)催化燃烧

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Abstract

This study presents the synthesis and characterization of lanthanum-modified alumina supported cerium-manganese mixed oxides, which were prepared by three different methods (coprecipitation, impregnation and citrate-based sol-gel method) followed by calcination at 500 °C. The physicochemical properties of the synthesized materials were investigated by various characterization techniques, namely: nitrogen adsorption-desorption isotherms, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) and H(2)-temperature programmed reduction (TPR). This experimental study demonstrated that the role of the catalytic surface is much more important than the bulk one. Indeed, the incipient impregnation of CeO(2)-MnO(x) catalyst, supported on an optimized amount of 4 wt.% La(2)O(3)-Al(2)O(3,) provided the best results of the catalytic combustion of methane on our catalytic micro-convertors. This is mainly due to: (i) the highest pore size dimensions according to the Brunauer-Emmett-Teller (BET) investigations, (ii) the highest amount of Mn(4+) or/and Ce(4+) on the surface as revealed by XPS, (iii) the presence of a mixed phase (Ce(2)MnO(6)) as shown by X-ray diffraction; and (iv) a higher reducibility of Mn(4+) or/and Ce(4+) species as displayed by H(2)-TPR and therefore more reactive oxygen species.

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