期刊论文
Liu, Ying-Ya
Wang, AJ (reprint author), Dalian Univ Technol, State Key Lab Fine Chem, Dalian 116029, Peoples R China.
Leus, Karen,Sun, Zhichao,Li, Xiang,Depauw, Hannes,Wang, Anjie,Zhang, Jian,Van der Voort, Pascal
2019-03-15
MICROPOROUS AND MESOPOROUS MATERIALS
SCIE、EI
J
277
245-252
1387-1811
Molybdenum-bipyridine complex; Metal-organic framework; Oxidative desulfurization; Dibenzothiophene; Diesel
In this work, we report the catalytic performance of a MoO2Cl2 anchored metal-organic framework, Mo@COMOC-4, in the oxidative desulfurization (ODS) process on a continuous fixed-bed reactor. Mo@COMOC-4 was examined as a catalyst in the oxidation of model oils containing dibenzothiophene (DBT), benzothiophene (BT) or 4,6-dimethyldibenzothiophene (4,6-DMDBT). In a 50-h ODS reaction of DBT at 70 degrees C, with tert-butyl hydroperoxide (TBHP) as the oxidant, a constant high DBT conversion of nearly 80% was observed along with a high oxidant utility of over 85%, where DBT was converted rapidly into DBT sulfone. XRD and ICP analysis show that the structure of Mo@COMOC-4 was well preserved, with no significant leaching of Mo species. In addition, Mo@COMOC-4 can also oxidize a hydrogenated diesel oil, and 74% sulfur removal efficiency was achieved, with an extraction recovery of 92.5% after acetonitrile extraction. Spectroscopic characterization confirmed the formation of a molybdenum peroxide complex from MoO2Cl2 under TBHP treatment, a plausible catalytic process was proposed based on the experiment evidence as well as FT-IR and FT-FIR characterization results.