摘要
以不同的过渡金属化合物作为催化剂,在发烟硫酸溶剂中进行了甲烷液相部分氧化反应的研究,考察了催化剂种类、催化剂用量、反应温度、反应时间、发烟硫酸浓度等工艺条件对目的产物收率的影响,同时对反应的催化机理进行了探讨.甲烷在部分氧化反应中首先转化为硫酸单甲酯,后者进一步水解得到甲醇.以V2O5作为甲烷液相部分氧化反应的催化剂时甲烷转化率可达54.5%,目的产物选择性为45.5%,相应的工艺条件为催化剂用量0.025 mol,反应温度180℃,发烟硫酸中SO3含量50%,反应时间2 h.V2O5催化的甲烷液相部分氧化反应遵循亲电取代机理,溶剂发烟硫酸是甲烷转化的关键因素之一.
The partial oxidation of methane over the V2O5 catalyst in oleum was studied. The effects of reaction temperature, V2O5 content and reaction time on the methane conversion and methanol yield were investigated. The reaction mechanism was also discussed. It was found that methane was first transformed into methyl bisulfate which was then hydrolyzed into methanol. The process of the partial oxidation of methane catalyzed by V20s involved in the electrophilic alternative mechanism, and the sulfur trioxide in oleum was necessary for the reaction system. Among the catalysts tested, V2O5 showed higher activity and selectivity. The maximum methanol yield of 45.596 and methane conversion of 54.596 were obtained under the conditions of n （V2O5） = 0. 024 5 mol, θ = 180℃ , p = 4.0 MPa and t = 2 h when the content of sulfur trioxide in oleum was about 50%.
出处
《催化学报》
SCIE
EI
CAS
CSCD
北大核心
2005年第11期1027-1030,共4页
基金
陕西省教育厅专项基金资助项目(01JK098)
关键词
甲烷
部分氧化
五氧化二钒
发烟硫酸
甲醇
反应机理
methane, partial oxidation, vanadium pentoxide, oleum, methanol, reaction mechanism
