Abstract
Oxidative desulfurization (ODS) is the promising new method for super deep desulfurization of fuel oil. The oxidative desulfurization performance of the metal-N4-chelates metallophthalocyanines (MPcs) is related to the chemical properties of conjugate structures and the central metal ions. Herein, a biomimetic catalytic system composed of metallophthalocyanines (MPcR4, M = Mn(II), Fe(II), Co(II), Ni(II), Cu(II), Zn(II); R = -H, -COOH, -NO2, -NH2) and molecular O2 was performed to study the influence of MN4-type coordination structure in metallophthalocyanines for the degradation of dibenzothiophene (DBT) in model oil containing n-octane. The results reveal that the conjugate structures and the center metal ions of metallophthalocyanines played key roles in oxidative desulfurization performance. The inductive effect of different R substituents strongly affected the electron cloud distribution of the conjugate structures and the catalytic performance. Moreover, the catalytic activity of MPcs, which is related to the d electronic configuration and ligand-field effects, does not sequentially increase with the increase in the d electron number of central metal ions.
Highlights
With the aggravation of environmental pollution problems, the removal of sulfur compounds in vehicle fuel has become an important research focus
A 100 mL three-neck flask was selected for the oxidative desulfurization experiment; the oxygen cylinder and reflux condenser were linked to the flask
The residue sulfur concentration and the oxidation products of dibenzothiophene(DBT) in model fuel were analyzed by gas chromatography (Flame Photometric Detector, Agilent 6890 (Shanghai, China)
Summary
With the aggravation of environmental pollution problems, the removal of sulfur compounds in vehicle fuel has become an important research focus. The catalytic activity of the metal-N4-chelate macrocycles is affected by the chemical properties of the ligand field and the central metal ion. Gation of substituent and phthalocyanine ring influences the electron cloud density distribution of the system and catalytic activity. GSilnetglsettatsetaotexyogxeyngemnomleocluecleusleosxoidxidzeizaenadnddedceocmompopsoeseorogrgananicicccoommppoouunnddss[[1199]]..TThheerreeffoorree,, molecular oxygen is an ideal oxidant for the catalytic oxidative desulfurization system of tthhee pphhtthhaallooccyyaanniinnee ccoommpplleexx..
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