氨基化中空SiO_2杂多化合物复合型催化剂的合成、表征及催化燃油深度脱硫性能  

Synthesis,Characterization and Catalytic Fuel Ultra-deep Desulfurization of Hollow Amino-SiO_2 Supported Heteropoly Compound Catalyst

作　　者：刘日嘉[1] 王睿[1] 

机构地区：[1]山东大学环境科学与工程学院,济南250100

出　　处：《高等学校化学学报》2013年第12期2814-2820,共7页Chemical Journal of Chinese Universities

基　　金：国家自然科学基金(批准号:20976097;21076116;21211120165;21311120297);中国石油天然气集团公司石油科技创新基金(批准号:2010D-5006-0405);山东省自然科学基金(批准号:ZR2011BM023)资助

摘　　要：采用分散聚合法制得中空SiO2微粒,将其氨基化后负载磷钨酸(HPW),最终制得氨基化中空SiO2磷钨酸复合型催化剂(NH4PW-SiO2),并对催化剂进行了N2吸附-脱附、傅里叶变换红外光谱(FTIR)、X射线衍射(XRD)、扫描电子显微镜(SEM)和电感耦合等离子体原子发射光谱(ICP-OES)表征.考察了以NH4PWSiO2为催化剂,过氧化氢为氧化剂,乙腈为萃取剂的催化氧化萃取燃油深度脱硫性能.探讨了催化剂用量、氧硫比、催化剂与氧化剂预接触时间、反应温度和初始硫含量对脱硫效果的影响.结果表明,在催化剂用量为模拟油品质量的1.0%,氧硫摩尔比为15,催化剂与过氧化氢预接触4 min,反应温度为60℃,初始硫含量为350 mg/L的条件下,反应180 min时硫含量已降至2.45 mg/L,脱硫率达99.3%.催化氧化萃取时的脱硫率比单纯萃取时的脱硫率高45.1%.此外,催化剂用于真实汽油及柴油的催化氧化脱硫也得到了很好的脱硫效果,且催化剂重复使用5次后,脱硫效率未见明显降低.Hollow SiO2 was prepared by dispersion aggragation before uploading HPW. The prepared catalyst was characterized by N2 adsorption-desorption, FTIR, XRD and SEM. The method of catalytic extraction fuel ultra-deep desulfurization was developed using hydrogen peroxide as oxidant and MeCN as extractants. The effects of catalyst dosage, O/S molar ratio, pre-immersion time of the catalyst in H2 02 solution, reaction tem- perature and initial sulfur content were investigated. Under the favourable operating conditions recommended as follows： mass ratio of catalyst dosage and simulated diesel of 1.0%, O/S molar ratio of 15, pre-immersion time of the catalyst in H202 solution being 4 min, temperature of 60 ~C and initial sulfur content of 350 mg/L, the sulfur content of simulated diesel can be reduced from 350 mg/L to 2. 45 mg/L, with a desulfurization effi- ciency of 99.3% at 180 rain, The overal desulfurization efficiency reaches 99.3% , higher than that by mere extraction by 45.1%, efficiency significantly. Moreover, NHaPW-SiO2 for real gasoline and diesel catalytic oxidative desulfurization was obtained with good effect and the catalyst recovered demonstrates almost the same activity as the fresh after 5 recycles.

关 键 词：杂多化合物 中空SiO2 氧化脱硫 硫化物 过氧化氢 

分 类 号：O643.3[理学—物理化学]