Preparation, characterization, and catalytic performances of cobalt catalysts supported on KIT-6 silicas in oxidative desulfurization of dibenzothiophene

•Catalysts of cobalt supported on modified KIT-6 silica were prepared and applied to oxidative desulfurization (ODS).•A novel Co/KIT-6 catalysis system was developed and evaluated with better DBT removal.•Response surface methodology was used to optimized the main variables for Co/KIT-6 catalytic OD...

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Veröffentlicht in:Fuel (Guildford) 2017-07, Vol.200, p.11-21
Hauptverfasser: Wei, Sainan, He, Huijun, Cheng, Yan, Yang, Chunping, Zeng, Guangming, Kang, Li, Qian, Hui, Zhu, Canyao
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container_issue
container_start_page 11
container_title Fuel (Guildford)
container_volume 200
creator Wei, Sainan
He, Huijun
Cheng, Yan
Yang, Chunping
Zeng, Guangming
Kang, Li
Qian, Hui
Zhu, Canyao
description •Catalysts of cobalt supported on modified KIT-6 silica were prepared and applied to oxidative desulfurization (ODS).•A novel Co/KIT-6 catalysis system was developed and evaluated with better DBT removal.•Response surface methodology was used to optimized the main variables for Co/KIT-6 catalytic ODS system.•Kinetics of ODS correlated well with the pseudo-first-order equation. Sulfur-containing compounds in oils are harmful to the ecosystem whose cost-effective removal is still a challenge. In this study, novel heterogeneous catalysts of cobalt supported on KIT-6 mesoporous silicas were prepared and evaluated for oxidative desulfurization (ODS) under ambient conditions using cyclohexanone peroxide (CYHPO) as the oxidant. The model oil was obtained via dissolving DBT in the n-octane. The conventional wet impregnation method was applied for the preparation of the catalysts, and cobalt nitrate was used as the precursor. The catalysts were characterized by XRD, N2-physisorption, FT-IR, TGA, SEM/TEM and XPS. Then their catalytic activities in total oxidation of dibenzothiophene (DBT) were evaluated at various conditions. DBT conversion by this heterogeneous ODS system reached 98.68%. Co/KIT-6 catalysts showed high ODS activity due to Ia3d mesoporous structure resulting in better cobalt dispersion, higher activity of Co, and faster diffusion of reactant and products. The Box-Behnken design showed that the optimum values for the conversion of DBT were 93°C (oxidation temperature), 1.6×10−1g (catalyst amount) and 5.7 (O/S molar ratio), respectively. The inhibitory effect of quinoline on ODS was higher than carbazole and indole, adding quinoline into model oil under same conditions led to a decrease of the conversion of DBT from 98.68% to 65.67% when the concentration of quinoline increased from 160ppm to 4845ppm. Kinetics data correlated well with the pseudo-first-order equation. These data showed that this novel Co/KIT-6 catalysis system has the potential to be applied in ODS from oils.
doi_str_mv 10.1016/j.fuel.2017.03.052
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Sulfur-containing compounds in oils are harmful to the ecosystem whose cost-effective removal is still a challenge. In this study, novel heterogeneous catalysts of cobalt supported on KIT-6 mesoporous silicas were prepared and evaluated for oxidative desulfurization (ODS) under ambient conditions using cyclohexanone peroxide (CYHPO) as the oxidant. The model oil was obtained via dissolving DBT in the n-octane. The conventional wet impregnation method was applied for the preparation of the catalysts, and cobalt nitrate was used as the precursor. The catalysts were characterized by XRD, N2-physisorption, FT-IR, TGA, SEM/TEM and XPS. Then their catalytic activities in total oxidation of dibenzothiophene (DBT) were evaluated at various conditions. DBT conversion by this heterogeneous ODS system reached 98.68%. Co/KIT-6 catalysts showed high ODS activity due to Ia3d mesoporous structure resulting in better cobalt dispersion, higher activity of Co, and faster diffusion of reactant and products. The Box-Behnken design showed that the optimum values for the conversion of DBT were 93°C (oxidation temperature), 1.6×10−1g (catalyst amount) and 5.7 (O/S molar ratio), respectively. The inhibitory effect of quinoline on ODS was higher than carbazole and indole, adding quinoline into model oil under same conditions led to a decrease of the conversion of DBT from 98.68% to 65.67% when the concentration of quinoline increased from 160ppm to 4845ppm. Kinetics data correlated well with the pseudo-first-order equation. 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Sulfur-containing compounds in oils are harmful to the ecosystem whose cost-effective removal is still a challenge. In this study, novel heterogeneous catalysts of cobalt supported on KIT-6 mesoporous silicas were prepared and evaluated for oxidative desulfurization (ODS) under ambient conditions using cyclohexanone peroxide (CYHPO) as the oxidant. The model oil was obtained via dissolving DBT in the n-octane. The conventional wet impregnation method was applied for the preparation of the catalysts, and cobalt nitrate was used as the precursor. The catalysts were characterized by XRD, N2-physisorption, FT-IR, TGA, SEM/TEM and XPS. Then their catalytic activities in total oxidation of dibenzothiophene (DBT) were evaluated at various conditions. DBT conversion by this heterogeneous ODS system reached 98.68%. Co/KIT-6 catalysts showed high ODS activity due to Ia3d mesoporous structure resulting in better cobalt dispersion, higher activity of Co, and faster diffusion of reactant and products. The Box-Behnken design showed that the optimum values for the conversion of DBT were 93°C (oxidation temperature), 1.6×10−1g (catalyst amount) and 5.7 (O/S molar ratio), respectively. The inhibitory effect of quinoline on ODS was higher than carbazole and indole, adding quinoline into model oil under same conditions led to a decrease of the conversion of DBT from 98.68% to 65.67% when the concentration of quinoline increased from 160ppm to 4845ppm. Kinetics data correlated well with the pseudo-first-order equation. 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Sulfur-containing compounds in oils are harmful to the ecosystem whose cost-effective removal is still a challenge. In this study, novel heterogeneous catalysts of cobalt supported on KIT-6 mesoporous silicas were prepared and evaluated for oxidative desulfurization (ODS) under ambient conditions using cyclohexanone peroxide (CYHPO) as the oxidant. The model oil was obtained via dissolving DBT in the n-octane. The conventional wet impregnation method was applied for the preparation of the catalysts, and cobalt nitrate was used as the precursor. The catalysts were characterized by XRD, N2-physisorption, FT-IR, TGA, SEM/TEM and XPS. Then their catalytic activities in total oxidation of dibenzothiophene (DBT) were evaluated at various conditions. DBT conversion by this heterogeneous ODS system reached 98.68%. Co/KIT-6 catalysts showed high ODS activity due to Ia3d mesoporous structure resulting in better cobalt dispersion, higher activity of Co, and faster diffusion of reactant and products. The Box-Behnken design showed that the optimum values for the conversion of DBT were 93°C (oxidation temperature), 1.6×10−1g (catalyst amount) and 5.7 (O/S molar ratio), respectively. The inhibitory effect of quinoline on ODS was higher than carbazole and indole, adding quinoline into model oil under same conditions led to a decrease of the conversion of DBT from 98.68% to 65.67% when the concentration of quinoline increased from 160ppm to 4845ppm. Kinetics data correlated well with the pseudo-first-order equation. These data showed that this novel Co/KIT-6 catalysis system has the potential to be applied in ODS from oils.</abstract><cop>Kidlington</cop><pub>Elsevier Ltd</pub><doi>10.1016/j.fuel.2017.03.052</doi><tpages>11</tpages><orcidid>https://orcid.org/0000-0003-3987-2722</orcidid></addata></record>
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source ScienceDirect Journals (5 years ago - present)
subjects Carbazole
Catalysis
Catalyst
Catalysts
Cobalt
Conversion
Cyclohexanone
Desulfurization
Desulfurizing
Dibenzothiophene
Diffusion rate
Ecosystem assessment
Indoles
Kinetics
Mesoporous silica
Oils & fats
Oxidation
Oxidative desulfurization
Peroxide
Quinoline
Reaction kinetics
Sulfur
X ray photoelectron spectroscopy
title Preparation, characterization, and catalytic performances of cobalt catalysts supported on KIT-6 silicas in oxidative desulfurization of dibenzothiophene
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