模板法制备催化剂PW12@Fe-TiO2及其催化氧化脱硫性能

Preparation of PW12@Fe-TiO2 catalyst by template method and its catalytic oxidative desulfurization performances

采用模板法一步合成了一类多酸基PW12@Fe-TiO2材料,利用Raman、XRD、XPS和SEM表征手段对材料进行了结构表征。结果表明,磷钨酸(PW12)被包埋到Fe-TiO2中,形成球形结构。N2吸附-脱附测试显示,PW12@Fe-TiO2为介孔材料:孔径尺寸为4.1nm,比表面积为30.3m^2·g^-1。所合成材料作为催化剂,以H2O2为氧化剂,乙腈为溶剂,在模拟油的氧化脱硫反应体系中表现出较好的催化性能。当PW12@Fe-TiO2的加入量为40mg,反应底物为5.0mL,反应温度60℃,反应到40min时,DBT的去除率到达了99.9%。中断和循环实验结果表明,催化剂PW12@Fe-TiO2具有良好的稳定性,在相似的反应条件下,循环使用5次,催化剂的催化活性依然保持不变。

A polyoxometalate-based material has been synthesized by the one-step template,denoted as PW 12@Fe-TiO2.Multiple characterization methods namely Raman,XRD,XPS and SEM were used to characterize the resultant materials,and results indicated that phosphotungstic acid(PW12)is introduced into Fe-TiO2,forming spherical structure.N2 adsorption-desorption test showed that PW 12@Fe-TiO2 was mesoporous material with pore size of 4.1 nm and specific surface area of 30.3 m^2·g^-1.The resultant material was used as catalyst for the oxidative desulfurization of model oil,and exhibited good catalytic activity with H2O2 as oxidant and acetonitrile as solvent.The S-removal of DBT reached 99.9%after 40 min reaction at a temperature of 60℃ when dosage of catalyst PW12@Fe-TiO2 was 40 mg and reaction substrate was 5.0 mL.Leaching and recycling experiments revealed that catalyst PW12@Fe-TiO2 has excellent stability,and catalytic activities of the catalyst remain unchanged after five cycles under identical reaction conditions.