Direct conversion of methane to methyl acetate with nitrous oxide and carbon monoxide over heterogeneous catalysts containing both rhodium and iron phosphate | |
Qiang Yuan ; Qinghong Zhang ; Zhang QH(张庆红) ; Ye Wang ; Wang Y(王野) | |
2005-05 | |
关键词 | methane oxidative carbonylation methyl acetate nitrous oxide rhodium iron phosphates MCM-41 |
英文摘要 | The formation of methyl acetate during the conversion of CH4 with N2O and CO over heterogeneous catalysts containing both rhodium and iron phosphate was studied. For two series of Rh-doped FePO4 catalysts prepared by different methods, the optimum atomic ratios of Rh/Fe for methyl acetate formation are 1:600-1:400. The Rh-FePO4 catalyst prepared from a mixed aqueous solution exhibits a higher rate and turnover frequency for methyl acetate formation than the Rh/FePO4 prepared by the impregnation method. Characterizations with XRD, diffuse-reflectance UV-vis, TEM, and H-2-TPR suggest that Rh3+ ions are mainly incorporated into the lattice of FePO4 in the Rh-FePO4 prepared from the mixed aqueous solution, whereas Rh(III) species probably exist on the surface of FePO4 in the Rh/FePO4 prepared by impregnation. The support of Rh(III) species and FePO4 by MCM-41 by a co-impregnation method can drastically increase the rate and turnover frequency for methyl acetate formation, whereas a two-step impregnation method leads to catalysts without methyl acetate formation. The dual site containing Rh(III) species and FePO4 in close proximity is proposed to account for methyl acetate formation. A possible reaction mechanism has been proposed on the basis of kinetic investigations. (c) 2005 Elsevier Inc. All rights reserved. |
语种 | 英语 |
出版者 | ACADEMIC PRESS INC ELSEVIER SCIENCE |
内容类型 | 期刊论文 |
源URL | [http://dx.doi.org/doi:10.1016/j.jcat.2005.04.025] |
专题 | 化学化工-已发表论文 |
推荐引用方式 GB/T 7714 | Qiang Yuan,Qinghong Zhang,Zhang QH,et al. Direct conversion of methane to methyl acetate with nitrous oxide and carbon monoxide over heterogeneous catalysts containing both rhodium and iron phosphate[J],2005. |
APA | Qiang Yuan,Qinghong Zhang,张庆红,Ye Wang,&王野.(2005).Direct conversion of methane to methyl acetate with nitrous oxide and carbon monoxide over heterogeneous catalysts containing both rhodium and iron phosphate.. |
MLA | Qiang Yuan,et al."Direct conversion of methane to methyl acetate with nitrous oxide and carbon monoxide over heterogeneous catalysts containing both rhodium and iron phosphate".(2005). |
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