Deep Oxidative Desulfurization of Dibenzothiophene in Simulated Oil and Real Diesel Using Heteropolyanion-Substituted Hydrotalcite-Like Compounds as Catalysts

Molecules

Fengli Yu¹ 

[1] School of Environmental Science and Engineering, Shandong University, Jinan 250100, China; E-Mail:

关键词: oxidative desulfurization;    heteropolyanion;    hydrotalcite-like compounds;    hydrogen peroxide;   

DOI  :  10.3390/molecules181113691

来源: mdpi

【 摘 要 】

Three heteropolyanion substituted hydrotalcite-like compounds (HPA-HTLcs) including Mg₉Al₃(OH)₂₄[PW₁₂O₄₀](MgAl-PW₁₂), Mg₉Al₃(OH)₂₄[PMo₁₂O₄₀] (MgAl-PMo₁₂) and Mg₁₂Al₄(OH)₃₂[SiW₁₂O₄₀] (MgAl-SiW₁₂), were synthesized, characterized and used as catalysts for the oxidative desulfurization of simulated oil (dibenzothiophene, DBT, in n-octane). MgAl-PMo₁₂ was identified as an effective catalyst for the oxidative removal of DBT under very mild conditions of atmospheric pressure and 60 °C in a biphasic system using hydrogen peroxide as oxidant and acetonitrile as extractant. The conversion of DBT was nearly 100%. As a result, because of the influence of the electron density and the space steric hindrance, the oxidation reactivity of the different sulfur compounds in simulated oil followed the order DBT > 4,6-dimethyldibenzothiophene (4,6-DMDBT) > benzothiophene (BT) > thiophene (TH). When the reaction is finished, the catalysts can be recovered from the acetonitrile phase by filtration. The recovered MgAl-PMo₁₂ retains nearly the same catalytic activity as the fresh material. Moreover, MgAl-PMo₁₂ was found to exhibit an ideal catalytic activity in the oxidative desulfurization of real diesel resulting in a total remaining sulfur content of 9.12 ppm(w).

【 授权许可】

CC BY   
© 2013 by the authors; licensee MDPI, Basel, Switzerland.