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介孔二氧化硅负载磷钼酸催化剂的制备及其催化氧化脱硫
Preparation of Phosphomolybdic Acid Loaded on Mesoporous Silica and its Catalytic Oxidative Desulfurization
【Author】 Jianghua Qiu;Yuqin Zhang;Guanghui Wang;Danlin Zeng;Yang Chen;College of Chemical Engineering and Technology, Wuhan University of Science and Technology;
【机构】 武汉科技大学化学工程与技术学院;
【摘要】 以正硅酸乙酯为硅源,以季铵盐为模板剂,采用沉淀法制备了介孔二氧化硅负载磷钼酸(HPMo/SiO2)催化剂,考察了磷钼酸负载量、模板剂种类和煅烧温度等因素对催化剂结构和催化氧化脱硫性能的影响。结果表明,当磷钼酸负载量为20%时,比表面积和孔容分别达到最大值1211.36 m2/g和0.7879 mL/g;使用十六烷基三甲基氯化铵作模板剂时催化剂具有较大的平均孔径和较小的比表面积,而使用十八烷基三甲基氯化铵作模板剂时催化剂具有较大的比表面积和较小的平均孔径;适当的煅烧温度可以去除模板剂从而造孔,而过高的煅烧温度会造成催化剂孔隙结构坍塌,比表面积急剧下降。比表面积和孔径大小是影响脱硫效率的关键因素,当平均孔径变化不大的情况下,催化剂的比表面积越大时所对应的脱硫效率也就越高。催化剂用量、H2O2用量、反应温度和反应时间等因素对模型油的氧化脱硫均有影响。二苯并噻吩和苯并噻吩催化氧化反应都符合表观一级动力学规律,两者的表观活化能分别为33.03 KJ/moL和40.46 KJ/moL。
【Abstract】 The phosphomolybdic acid loaded on mesoporous silica was prepared by precipitation method using TEOS as the silica source and quaternary ammonium salts as the template. The influence of the factors as phosphomolybdic acid amount loaded, template type and calcination temperature on the structure and the catalytic oxidative desulfurization activity of the catalyst has been investigated. The results show that the specific surface area and the pore size are the key factors that affect the efficiency of desulfurization, and the desulfurization efficiency will be higher with larger specific surface in the case of little change in the average pore diameter. The catalyst’s specific surface area can reach 1211.36 m2/g with pore volume 0.7879 mL/g and pore size 2.60 nm. Kinetic analysis shows that dibenzothiophene and benzothiophene oxidation reaction accord with the apparent first-order kinetics law, and the activation energies are 33.03 KJ/mol and 40.46 KJ/mol respectively.
- 【会议录名称】 中国化学会第29届学术年会摘要集——第27分会:多孔功能材料
- 【会议名称】中国化学会第29届学术年会
- 【会议时间】2014-08-04
- 【会议地点】中国北京
- 【分类号】O643.36
- 【主办单位】中国化学会