Selective oxidation of methane to methanol in oleum over Pd/C catalyst

摘要

The selective oxidation of methane to methanol over Pd/C catalysts generated from a PdCl2, precursor was investigated in oleum. Characterization of the catalysts was performed by X-ray diffraction, X-ray photo-electron spectroscopy, high-resolution transmission electron microscopy, and CO adsorption. The major product ill the oxidation reaction was methyl bisulfate, which was then hydrolyzed into methanol. Methane conversion of 23.6% with methanol selectivity of 69.5% and yield of 16.4% was achieved under the optimum conditions of 5% Pd/C, 30 mu mol Pd, reatction temperature 180 degrees C, methane pressure 4. 0 MPa, reaction time 4 h, and 50% sulfur trioxide concentration. After facile separation with the reactants and pretreatment, the catalyst could be reused several times with considerable stability. The selective oxidation of methane catalyzed by Pd/C catalysts in oleum possibly involved an electrophilic substitute mechanism. The catalystic performance was related to the Pd loading, dispersion, and particle size.