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中文摘要：
以PdCl2为前驱体，采用浸渍法制备了Pd／C催化剂，并在发烟硫酸中考察了其催化甲烷选择氧化反应的性能，采用X射线粉末衍射、X射线光电子能谱、高分辨透射电镜和CO吸附等方法对催化剂进行了表征。甲烷选择氧化反应得到的主产物硫酸单甲酯经水解后得到甲醇，在5％Pd／C催化剂、Pd用量30μmol、反应温度180℃、反应压力4．0MPa、反应时间4h和发烟硫酸中SO3含量为50％的优化工艺条件下，甲烷转化率为23．6％，甲醇的选择性和收率分别为69．5％和16．4％，在一定程度上可实现催化剂的多次重复使用。Pd／C催化剂上的甲烷选择氧化反应可能遵循亲电取代机理，催化性能与Pd负载量、Pd粒子尺寸和分散度等有关。
英文摘要：
The selective oxidation of methane to methanol over Pd/C catalysts generated from a PdC12 precursor was investigated in oleum. Characterization of the catalysts was performed by X-ray diffraction, X-ray photoelectron spectroscopy, high-resolution transmission electron microscopy, and CO adsorption. The major product in 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, 30μmol Pd, reaction temperature 180 ℃, 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 catalytic performance was related to the Pd loading, dispersion, and particle size.
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