甲烷部分氧化反应的磷钨酸催化剂研究

Study on the Phosphotungsticacid Catalyst Used for Partial Oxidation of Methane

以磷钨酸为催化剂和氧化剂,进行了无氧条件下的甲烷气固相部分氧化的实验研究,考察了磷钨酸催化剂的制备条件、载体影响以及反应温度对甲烷部分氧化反应的影响等。磷钨酸催化剂可有效催化甲烷部分氧化反应,甲烷首先转化生成醋酸甲酯,醋酸甲酯水解生成甲醇。制备的催化剂以SiO2为载体,采用载体质量15%（wt）的磷钨酸水溶液回流浸渍4h、120℃干燥2h、300℃焙烧4h制得。甲烷部分氧化反应在0.10MPa、267-280℃进行,甲烷转化率为26.61%,目的产物收率25.82%。

Under the condition of without the existence of oxygen, the partial oxidation of methane over phosphotungstieaeid catalysts was studied. The effects of catalyst preparation conditions, catalyst supporters used and reaction temperature on the partial oxidation reaction of methane were investigated. It was found that the methane is transformed into methyl bisulfate at first, and then the latter is hydrolyzed into methanol. The most appropriate phosphotungsticacid catalyst preparation method found is taking SiO2 as catalyst supporter and dipping in phosphotungsticacid aqueous solution with reflux for 4 h, then drying at 120℃ for 2 h and calcinating at 300℃ for 4 h. Using the prepared phosphotungsticacid catalyst and under the operation temperature of 267-280℃ and pressure of 0.10 MPa, the methanol yield of 25.82% and the methane conversion rate of 26.61% can be obtained.