Oxidative desulfurization of diesel fuel catalyzed by polyoxometalate immobilized on phosphazene-functionalized silica

被引:151
作者
Craven, Michael [1 ]
Xiao, Dong [1 ,3 ]
Kunstmann-Olsen, Casper [1 ]
Kozhevnikova, Elena F. [1 ]
Blanc, Frederic [1 ,2 ]
Steiner, Alexander [1 ]
Kozhevnikov, Ivan, V [1 ]
机构
[1] Univ Liverpool, Dept Chem, Liverpool L69 7ZD, Merseyside, England
[2] Univ Liverpool, Stephenson Inst Renewable Energy, Liverpool L69 7ZD, Merseyside, England
[3] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
基金
英国工程与自然科学研究理事会; 欧洲研究理事会;
关键词
Oxidative desulfurization; Polyoxometalate; Phosphazene; Heterogeneous catalysis; SOLID-STATE NMR; HYDROGEN-PEROXIDE; DEEP DESULFURIZATION; BIPHASIC OXIDATIONS; HETEROPOLY ACIDS; IONIC LIQUIDS; EFFICIENT; OILS; DIBENZOTHIOPHENE; EPOXIDATION;
D O I
10.1016/j.apcatb.2018.03.005
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Keggin-type polyoxometalates (POM) immobilized on alkylaminophosphazene (RPN)-functionalized silica (POM/RPN-SiO2) are new effective single-site solid catalysts for oxidative desulfurization (ODS) of diesel fuel under mild conditions in a biphasic system composed of a benzothiophene-containing model diesel fuel (heptane) and aqueous 30% H2O2 . The catalytic activity of POM/RPN-SiO2 was found to be influenced by the choice of POM and the amine R group in RPN, decreasing in the order PMo > PW > SiW and Bz > iBu > iPr, respectively. The most effective catalyst, PMo/BzPN-SiO2 (PMo = PMo12O403-), exhibited 100% removal of dibenzothiophene from model diesel fuel at 60 degrees C and ambient pressure and could be reused without loss of activity. This catalyst outperforms other recently reported heterogeneous catalysts for ODS in similar systems. C-13, Si-29 and P-31 MAS NMR, FUR, SEM, BET and elemental analysis were used to characterize the structure of surface phosphazene and POM species in the new catalysts.
引用
收藏
页码:82 / 91
页数:10
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