Abstract

New heterogeneous catalyst was synthesized via covalent anchoring of oxovanadium(IV) complex of 5,5?-dibromobis(salicyledene)diethylenetriamine (VO[5-Br(Saldien)]) on the surface of chloro-modified graphene oxide (GO@CTS). The structure of the catalyst was investigated using different characterization techniques such as XRD, SEM, EDX, FT-IR, TG, DTA and ICP-AES analyses. The synthesized heterogeneous oxovanadium(IV) was an efficient catalyst for high yield and selective oxidation desulfurization (ODS) of dibenzothiophene (DBT) as a model oil using H2O2 as oxidant and formic acid as a promoter. The effects of the catalyst mass, reaction temperature and time, formic acid/H2O2 ratio and molar ratio of H2O2 to the total amount of sulfur (O/S) on oxidation desulfurization activity were investigated. Moreover, the prepared catalyst can be easily separated from the reaction mixture and reused six times without a significant loss of catalytic activity and selectivity.

Highlights

  • Growing energy demand will be accompanied by growing greenhouse gas (GHG) emissions e.g. CO2 with an impact on climate change and non-GHG emissions e.g. NOx, SO2, volatile organic compounds and particulate materials with an impact on local air quality.[1]

  • The results clearly demonstrated the presence of vanadium in the synthesized heterogeneous catalyst, Graphene oxide (GO)@5-Br(Saldien)VO

  • The results indicated that of GO@5-Br(Saldien)VO was quite reliable for oxidation desulfurization (ODS) in comparison with other catalysts

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Summary

Introduction

Growing energy demand will be accompanied by growing greenhouse gas (GHG) emissions e.g. CO2 with an impact on climate change and non-GHG emissions e.g. NOx, SO2, volatile organic compounds and particulate materials with an impact on local air quality.[1]. Results showed that the immobilization of homogeneous complexes onto the polystyrene support enhances their stability and catalytic reactions are heterogeneous in nature.[26] Ogunlaja and coworkers reported a continuous flow system for oxidative desulfurization of refractory organosulfur compounds by two oxovanadium(IV) polymer supported catalysts.[23] Graphene oxide (GO) has attracted considerable attention as one of the most promising supports to immobilize homogeneous vanadium complexes.[27] Mungse et al reported the covalent anchoring of an oxovanadium Schiff base complex onto GO nanosheets for the oxidation of various alcohols, diols, and α-hydroxyketones to carbonyl compounds using tert-butylhydroperoxide (TBHP) as an oxidant.[28] Verma et al reported that oxovanadium Schiff base supported graphene oxide exhibited a higher catalytic efficiency than the homogeneous vanadyl acetylacetonate for epoxidation of fatty acids and esters.[29] Hajjar and coworkers reported the application of nano-graphene sheet supported Co and Mo species in the HDS process. The prepared catalyst was successfully reused for six runs without a significant loss in catalytic activity

Experimental
Results and Discussion
2. Evaluation of Catalytic Activity
Conclusions
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