化工进展 ›› 2016, Vol. 35 ›› Issue (12): 3934-3941.DOI: 10.16085/j.issn.1000-6613.2016.12.029

• 工业催化 • 上一篇    下一篇

MoO2/g-C3N4催化剂的制备及其氧化脱除模拟油中的硫化物

邢鹏飞1, 李秀萍2, 贾宝军3, 赵荣祥1   

  1. 1 辽宁石油化工大学化学化工与环境学部石油化工学院, 辽宁 抚顺 113001;
    2 辽宁石油化工大学化学化工与环境学部化学与材料科学学院, 辽宁 抚顺 113001;
    3 抚顺石化公司石油三厂, 辽宁 抚顺 113001
  • 收稿日期:2016-03-24 修回日期:2016-05-30 出版日期:2016-12-05 发布日期:2016-12-05
  • 通讯作者: 赵荣祥,副教授,硕士生导师。E-mail:zylhzrx@126.com。
  • 作者简介:邢鹏飞(1989-),男,硕士研究生。

Preparation of MoO2/g-C3N4 catalyst and its application in the oxidation desulfurization of model oil

XING Pengfei1, LI Xiuping2, JIA Baojun3, ZHAO Rongxiang1   

  1. 1 College of Petrochemical Engineering, Liaoning University of Petroleum & Chemical Technology, Fushun 113001, Liaoning, China;
    2 College of Chemistry & Material Science Engineering, Liaoning University of Petroleum & Chemical Technology, Fushun 113001, Liaoning, China;
    3 Fushun Petrochemical Company No.3 Petrochemical Factory, Fushun 113001, Liaoning, China
  • Received:2016-03-24 Revised:2016-05-30 Online:2016-12-05 Published:2016-12-05

摘要: 采用高温煅烧MoO2和g-C3N4混合物制备了不同MoO2含量的MoO2/g-C3N4催化剂。采用X射线粉末衍射(XRD)、傅里叶红外光谱(FTIR)、扫描电镜(SEM)和N2吸附脱附对催化剂的结构和性能进行了表征。以MoO2/g-C3N4作为催化剂,H2O2为氧化剂,离子液体为萃取剂研究了反应体系的氧化脱硫性能。这项研究中考察了不同煅烧温度下制得的催化剂、负载量、氧化剂使用量、催化剂加入量、反应温度、萃取剂使用量、反应时间、硫化物类型等不同反应参数对脱硫率的影响。结果表明,在H2O2的使用量为0.2mL,MoO2/g-C3N4加入量为0.03g,1-乙基-3-甲基咪唑硫酸乙酯离子液体1.0mL,反应温度为70℃,反应时间60min的最佳工艺条件下,24%-MoO2/g-C3N4催化剂脱硫率可以达到94.8%,催化剂循环使用5次后活性没有明显下降。此外,研究了MoO2/g-C3N4在离子液体中的催化氧化反应机理。

关键词: 催化剂, 环境, 氧化, 氧化钼, 氮化碳, 二苯并噻吩

Abstract: MoO2/g-C3N4 catalysts with different MoO2 content were prepared by direct calcination of mixtures of g-C3N4 and MoO2. The structure and properties of the catalysts were characterized by XRD,FTIR,SEM,N2 adsorption-desorption. The desulfurization performance of the reaction system was investigated by using MoO2/g-C3N4 as the catalyst,H2O2 as oxidant,and ionic liquid as extractant. The effects of calcination temperature,content of MoO2,amount of hydrogen peroxide,dosage of catalyst,reaction temperature,amount of ionic liquid and the type of sulfur-containing compounds in oil,on the desulfurization efficiency were investigated. The result showed that under the optimal reaction conditions of V(H2O2)=0.2mL,m(catalyst)=0.03g,V(ILs)=1.0mL,reaction temperature 70℃ and reaction time 60min,the desulfurization efficiency of 24%-MoO2/g-C3N4 catalyst was 94.8% and the catalyst could be recycled 5 times without significant loss of activity. Furthermore,the catalytic oxidation reaction mechanism of MoO2/g-C3N4 in ionic liquid was studied in detail.

Key words: catalyst, environment, oxidation, molybdenum trioxide, carbon nitride, dibenzothiophene

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