[20120314]

 

Catalytic oxidation of thiophene and its derivatives via dual activation for ultra-deep desulfurization of fuels

 

    

    A catalyst system composed of tungstate and Bronsted acidic ionic liquids (BAILs) was found to be highly active for the oxidative desulfurization (ODS) removal of thiophene, benzothiophene (BT) and their derivatives from model oil using 30 wt.% H2O2 as the oxidant. Five BAILs, [Hnmp]BF4, [Hmim]BF4, [Hnmp]HSO4, [Hmim]HSO4 and [Hnmp][CH3SO3] (nmp = N-methyl-pyrrolidonium, mim = N-methylimidazolium), and various commercial tungstate compounds were investigated. High activity was obtained for the combination of ammonium tungstate and BAILs [Hnmp]BF4. In this catalytic reaction, sulfur-content of model oil containing BT could be decreased from 700 ng/L to less than 1 ng/L. Turnover frequency (TOF) for BT oxidation is higher than 19410-3 s-1, and that of in non-BAILs [Bmim]BF4 is less than 1110-3 s-1. Noteworthily, the ODS of thiophene, which has been regarded as difficult task, can be also achieved up to 99% conversion with a TOF of 710-3 s-1. The FT-IR, 1H-NMR and electrochemical measurements evidences indicate that the strong hydrogen bonding between the sulfur-containing compounds and [Hnmp]BF4 and the oxidative function of the tungstate synergistically activate the reactants and result in the excellent catalytic performance.

 

    

Article
Catalytic oxidation of thiophene and its derivatives via dual activation for ultra-deep desulfurization of fuels
Boyu Zhang, Zongxuan Jiang, Jun Li, Yongna Zhang, Feng Lin, Yan Liu*, Can Li*
J. Catal, 2012, 287, 5-12 DOI: 10.1016/j.jcat.2011.11.003
http://www.sciencedirect.com/science/article/pii/S0021951711003642

 

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