Selective oxidation of methane to formaldehyde by oxygen over silica-supported iron catalysts (Special column of methane transformation, Article) |
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Authors: | Jieli He Yang Li Dongli An Qinghong Zhang Ye Wang |
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Affiliation: | bState Key Laboratory of Physical Chemistry of Solid Surfaces, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China |
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Abstract: | FeOx-SiO2 catalysts prepared by a sol-gel method were studied for the selective oxidation of methane by oxygen. A single-pass formaldehyde yield of 2.0% was obtained over the FeOx-SiO2 with an iron content of 0.5 wt% at 898 K. This 0.5 wt% FeOx-SiO2 catalyst demonstrated significantly higher catalytic performances than the 0.5 wt% FeOx/SiO2 prepared by an impregnation method. The correlation between the catalytic performances and the characterizations with UV-Vis and H2-TPR suggested that the higher dispersion of iron species in the catalyst prepared by the sol-gel method was responsible for its higher catalytic activity for formaldehyde formation. The modification of the FeOx-SiO2 by phosphorus enhanced the formaldehyde selectivity, and a single-pass formaldehyde yield of 2.4% could be attained over a P-FeOx-SiO2 catalyst (P/Fe = 0.5) at 898 K. Raman spectroscopic measurements indicated the formation of FePO4 nanoclusters in this catalyst, which were more selective toward formaldehyde formation. |
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Keywords: | selective oxidation methane formaldehyde iron catalyst sol-gel method |
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