化工学报 ›› 2015, Vol. 66 ›› Issue (12): 4858-4864.DOI: 10.11949/j.issn.0438-1157.20150961

• 分离工程 • 上一篇    下一篇

Ti-Si-O双功能催化吸附材料的汽油光催化-吸附耦合脱硫性能

叶飞燕, 梅亮, 肖静, 夏启斌, 李忠   

  1. 华南理工大学化学与化工学院, 广东 广州 510640
  • 收稿日期:2015-06-23 修回日期:2015-09-03 出版日期:2015-12-05 发布日期:2015-12-05
  • 通讯作者: 肖静
  • 基金资助:

    国家自然科学基金项目(21306054);中石油创新基金项目。

UV photocatalysis-assisted adsorptive desulfurization of gasoline using bi-functional Ti-Si-O material

YE Feiyan, MEI Liang, XIAO Jing, XIA Qibin, LI Zhong   

  1. School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, Guangdong, China
  • Received:2015-06-23 Revised:2015-09-03 Online:2015-12-05 Published:2015-12-05
  • Supported by:

    supported by the National Natural Science Foundation of China(21306054) and the China Petroleum Foundation of Innovation.

摘要:

研究新型双功能Ti-Si-O吸附催化材料在紫外光照射下对汽油的光催化-吸附耦合脱硫性能。采用溶胶-凝胶法制备了Ti-Si-O双功能催化吸附材料,并用N2吸附法、XRD等对Ti-Si-O进行了结构表征;有机硫化物的含量和种类采用液相色谱、库仑仪、GC-MS和GC-SCD检测。实验结果表明:当钛硅摩尔比为3:7时,所制得的Ti-Si-O材料的光催化-吸附耦合脱硫性能最好,脱硫率达96%,优于单一的TiO2和SiO2材料;Ti0.3Si0.7O2对汽油中的3种有机硫化物的光催化-吸附耦合脱硫速率大小顺序为T > MT > BT;GC-MS产物检测表明汽油中的有机硫在Ti0.3Si0.7O2双功能催化吸附材料表面转化成极性较强的砜类物质,而后选择性地吸附在Ti0.3Si0.7O2表面;Ti0.3Si0.7O2可经过丙酮洗涤和热空气氧化法再生,5次循环使用后的脱硫性能基本维持不变;在光催化-吸附耦合工艺下,Ti0.3Si0.7O2材料可将真实汽油的硫含量降低至10 mg·g-1以下。

关键词: 汽油脱硫, 双功能, 光催化, 选择性, 制备, 再生

Abstract:

UV photocatalysis-assisted adsorptive desulfurization of bi-functional Ti-Si-O materials was investigated for clean gasoline. The Ti-Si-O materials were prepared by the sol-gel method and then characterized by N2 adsorption, X-ray diffraction, etc. Desulfurization performances of the Ti-Si-O materials were examined. Sulfur species in gasoline were measured by HPLC, coulomb instrument, GC-MS and GC-SCD. The results showed that at the Ti/Si mole ratio of 3:7, the desulfurization efficiency of the Ti-Si-O material reached the maximum [96%, 11.52 mg S·(g sorb)-1], which was more superior than those of the pure TiO2 and SiO2 materials. The photocatalysis-assisted adsorptive desulfurization (PADS) rates of Ti0.3Si0.7O2 for the three organosulfur compounds followed the order of T > MT > BT. On the basis of GC-MS analysis for desulfurized products, it could be judged that the organosulfur compounds in gasoline were firstly photocatalytically oxidized to polar sulfone over Ti0.3Si0.7O2, and then selectively adsorbed on Ti0.3Si0.7O2. Ti0.3Si0.7O2 can be efficiently regenerated by acetone washing and then hot air oxidation. The regenerated Ti0.3Si0.7O2 exhibited very good activity of oxidation and adsorption after five cycles of oxidation/adsorption and regeneration, and with this PADS technology, the real gasoline can be desulfurized to < 10 mm·g-1 by using Ti0.3Si0.7O2.

Key words: gasoline desulfurization, bi-function, photocatalysis, selectivity, preparation, regeneration

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