期刊
ENERGY & FUELS
卷 35, 期 3, 页码 2110-2120出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.energyfuels.0c03673
关键词
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资金
- National Nature Science Foundation of China [U1707603, 21625101, 21521005, U1507102]
- National Key Research and Development Program of China [2017YFB0307303]
- Beijing Natural Science Foundation [2182047]
- Fundamental Research Funds for the Central Universities [XK1802-6, XK1803-05, XK1902, 12060093063]
This study improved the catalytic materials for oxidative desulfurization reaction, with Al2O3-P2W15-Cn showing high efficiency in removing sulfur content within 9 minutes at 60 degrees Celsius. The catalyst exhibited excellent structural stability during the catalytic reaction, successfully removing 4,6-DMDBT and BT, with the outstanding performance of Al2O3-P2W15-C-18 confirmed by sulfur removal from an actual diesel sample.
Deep desulfurization of fuels has long been and remains to be a highly challenging issue. In this work, a trilacunary polyoxometalate of Na-12[alpha-P2W15O56]center dot 24H(2)O (P2W15)was covalently tethered onto the gamma-Al2O3 sphere, to which different alkyl chains (C-n, n = 8, 12, or 18) were grafted, leading to the formation of the Al2O3-P2W15-C-n. When the Al2O3-P2W15-Cn were applied to catalyze oxidative desulfurization reaction of dibenzothiophene (DBT) in the presence of H2O2, it displayed high efficiency for removal of sulfur content in 9 min under optimized conditions at 60 degrees C. In addition, the Al2O3-P2W15-C-n exhibited excellent structural stability during the catalytic reaction and can be used to remove 4,6-dimethyldibenzothiophene (4,6-DMDBT) and benzothiophene (BT) from fuel oils. The excellent performance of Al2O3-P2W15-C-18 was verified by sulfur removal for an actual diesel sample. Molecular dynamics simulations indicated that DBT showed strong tendency to be adsorbed on active sites, while DBTO2 (dibenzothiophene sulfone) can be desorbed much easier. This work opens up a new avenue for further study on oxidative desulfurization catalytic materials and the influence of catalyst structure on mass transfer.
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