Performance of V–Fe based catalysts on the oxidation of dibenzothiophenes
To obtain fossil fuels with ultra-low S levels at friendly conditions, different V oxides formulations on alumina modified with Fe were characterized and selected to oxidize dibenzothiophene (DBT), 4-methyl DBT and 4,6-dimethyl DBT prevailing in diesel fuel. V–Fe based catalysts (5 or 10 wt% of V) w...
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| Vydané v: | Chemosphere (Oxford) Ročník 362; s. 142791 |
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| Hlavní autori: | , , |
| Médium: | Journal Article |
| Jazyk: | English |
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England
Elsevier Ltd
01.08.2024
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| ISSN: | 0045-6535, 1879-1298, 1879-1298 |
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| Abstract | To obtain fossil fuels with ultra-low S levels at friendly conditions, different V oxides formulations on alumina modified with Fe were characterized and selected to oxidize dibenzothiophene (DBT), 4-methyl DBT and 4,6-dimethyl DBT prevailing in diesel fuel. V–Fe based catalysts (5 or 10 wt% of V) were obtained by impregnation of ammonium metavanadate solutions on Fe-modified alumina, obtained by impregnation of Mohr salt on pseudoboehmite (2 wt% of Fe). The catalysts were calcined in air atmosphere, and after were partially reduced with H2 flux to obtain a mix of several oxidation states of V and Fe species, to evaluate the interaction of Fe in VOx/Al2O3 catalysts and determine its effect on the oxidation processes. The structural and optical properties, as well as surface species, were determined by SEM-EDS, TPR, XRD, Raman, ATR-FTIR, photoluminescence, UV–Vis diffuse reflectance, and XPS spectroscopy. The catalytic performance was evaluated in oxidative desulfurization (ODS) and photocatalytic ODS (PODS) processes. The experimental results showed the addition of Fe promoted the catalytic activity of both ODS and PODS reactions. ODS activities of V–Fe catalysts increase up to 7.5 times with respect to V catalysts without Fe, and the most active catalyst (V5Fer) presents a characteristic oxidation time of 50 min for 4,6-DMDBT. The PODS activity of V10Fec was like ODS activity, showing it is possible to oxidize the dibenzothiophenes under friendly conditions to obtain lower S levels. The promoting effect of Fe was due to the interaction of Fe2+ and Fe3+ with the catalytic support, favoring the distribution of surface V3+ and V4+ species. Additionally, Fe improved the optical properties of the catalysts since the bandgap energy decrease and low recombination rate of the electron-hole pair were observed. Therefore, V–Fe based catalysts are photocatalytically actives to be used in PODS processes.
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•V–Fe based catalysts were synthetized and assessed in the PODS processes.•Fe promoted the V distribution as isolated and two-dimensional polymeric species.•Fe diminished the bandgap and the [e−/h+] recombination rate of the catalysts.•More exposed V species favored the catalytic and photocatalytic activity.•Oxidation activities of V–Fe catalysts increased 7.5 folds to catalysts without Fe. |
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| AbstractList | To obtain fossil fuels with ultra-low S levels at friendly conditions, different V oxides formulations on alumina modified with Fe were characterized and selected to oxidize dibenzothiophene (DBT), 4-methyl DBT and 4,6-dimethyl DBT prevailing in diesel fuel. V–Fe based catalysts (5 or 10 wt% of V) were obtained by impregnation of ammonium metavanadate solutions on Fe-modified alumina, obtained by impregnation of Mohr salt on pseudoboehmite (2 wt% of Fe). The catalysts were calcined in air atmosphere, and after were partially reduced with H2 flux to obtain a mix of several oxidation states of V and Fe species, to evaluate the interaction of Fe in VOx/Al2O3 catalysts and determine its effect on the oxidation processes. The structural and optical properties, as well as surface species, were determined by SEM-EDS, TPR, XRD, Raman, ATR-FTIR, photoluminescence, UV–Vis diffuse reflectance, and XPS spectroscopy. The catalytic performance was evaluated in oxidative desulfurization (ODS) and photocatalytic ODS (PODS) processes. The experimental results showed the addition of Fe promoted the catalytic activity of both ODS and PODS reactions. ODS activities of V–Fe catalysts increase up to 7.5 times with respect to V catalysts without Fe, and the most active catalyst (V5Fer) presents a characteristic oxidation time of 50 min for 4,6-DMDBT. The PODS activity of V10Fec was like ODS activity, showing it is possible to oxidize the dibenzothiophenes under friendly conditions to obtain lower S levels. The promoting effect of Fe was due to the interaction of Fe2+ and Fe3+ with the catalytic support, favoring the distribution of surface V3+ and V4+ species. Additionally, Fe improved the optical properties of the catalysts since the bandgap energy decrease and low recombination rate of the electron-hole pair were observed. Therefore, V–Fe based catalysts are photocatalytically actives to be used in PODS processes.
[Display omitted]
•V–Fe based catalysts were synthetized and assessed in the PODS processes.•Fe promoted the V distribution as isolated and two-dimensional polymeric species.•Fe diminished the bandgap and the [e−/h+] recombination rate of the catalysts.•More exposed V species favored the catalytic and photocatalytic activity.•Oxidation activities of V–Fe catalysts increased 7.5 folds to catalysts without Fe. To obtain fossil fuels with ultra-low S levels at friendly conditions, different V oxides formulations on alumina modified with Fe were characterized and selected to oxidize dibenzothiophene (DBT), 4-methyl DBT and 4,6-dimethyl DBT prevailing in diesel fuel. V-Fe based catalysts (5 or 10 wt% of V) were obtained by impregnation of ammonium metavanadate solutions on Fe-modified alumina, obtained by impregnation of Mohr salt on pseudoboehmite (2 wt% of Fe). The catalysts were calcined in air atmosphere, and after were partially reduced with H2 flux to obtain a mix of several oxidation states of V and Fe species, to evaluate the interaction of Fe in VOx/Al2O3 catalysts and determine its effect on the oxidation processes. The structural and optical properties, as well as surface species, were determined by SEM-EDS, TPR, XRD, Raman, ATR-FTIR, photoluminescence, UV-Vis diffuse reflectance, and XPS spectroscopy. The catalytic performance was evaluated in oxidative desulfurization (ODS) and photocatalytic ODS (PODS) processes. The experimental results showed the addition of Fe promoted the catalytic activity of both ODS and PODS reactions. ODS activities of V-Fe catalysts increase up to 7.5 times with respect to V catalysts without Fe, and the most active catalyst (V5Fer) presents a characteristic oxidation time of 50 min for 4,6-DMDBT. The PODS activity of V10Fec was like ODS activity, showing it is possible to oxidize the dibenzothiophenes under friendly conditions to obtain lower S levels. The promoting effect of Fe was due to the interaction of Fe2+ and Fe3+ with the catalytic support, favoring the distribution of surface V3+ and V4+ species. Additionally, Fe improved the optical properties of the catalysts since the bandgap energy decrease and low recombination rate of the electron-hole pair were observed. Therefore, V-Fe based catalysts are photocatalytically actives to be used in PODS processes.To obtain fossil fuels with ultra-low S levels at friendly conditions, different V oxides formulations on alumina modified with Fe were characterized and selected to oxidize dibenzothiophene (DBT), 4-methyl DBT and 4,6-dimethyl DBT prevailing in diesel fuel. V-Fe based catalysts (5 or 10 wt% of V) were obtained by impregnation of ammonium metavanadate solutions on Fe-modified alumina, obtained by impregnation of Mohr salt on pseudoboehmite (2 wt% of Fe). The catalysts were calcined in air atmosphere, and after were partially reduced with H2 flux to obtain a mix of several oxidation states of V and Fe species, to evaluate the interaction of Fe in VOx/Al2O3 catalysts and determine its effect on the oxidation processes. The structural and optical properties, as well as surface species, were determined by SEM-EDS, TPR, XRD, Raman, ATR-FTIR, photoluminescence, UV-Vis diffuse reflectance, and XPS spectroscopy. The catalytic performance was evaluated in oxidative desulfurization (ODS) and photocatalytic ODS (PODS) processes. The experimental results showed the addition of Fe promoted the catalytic activity of both ODS and PODS reactions. ODS activities of V-Fe catalysts increase up to 7.5 times with respect to V catalysts without Fe, and the most active catalyst (V5Fer) presents a characteristic oxidation time of 50 min for 4,6-DMDBT. The PODS activity of V10Fec was like ODS activity, showing it is possible to oxidize the dibenzothiophenes under friendly conditions to obtain lower S levels. The promoting effect of Fe was due to the interaction of Fe2+ and Fe3+ with the catalytic support, favoring the distribution of surface V3+ and V4+ species. Additionally, Fe improved the optical properties of the catalysts since the bandgap energy decrease and low recombination rate of the electron-hole pair were observed. Therefore, V-Fe based catalysts are photocatalytically actives to be used in PODS processes. To obtain fossil fuels with ultra-low S levels at friendly conditions, different V oxides formulations on alumina modified with Fe were characterized and selected to oxidize dibenzothiophene (DBT), 4-methyl DBT and 4,6-dimethyl DBT prevailing in diesel fuel. V-Fe based catalysts (5 or 10 wt% of V) were obtained by impregnation of ammonium metavanadate solutions on Fe-modified alumina, obtained by impregnation of Mohr salt on pseudoboehmite (2 wt% of Fe). The catalysts were calcined in air atmosphere, and after were partially reduced with H flux to obtain a mix of several oxidation states of V and Fe species, to evaluate the interaction of Fe in VO /Al O catalysts and determine its effect on the oxidation processes. The structural and optical properties, as well as surface species, were determined by SEM-EDS, TPR, XRD, Raman, ATR-FTIR, photoluminescence, UV-Vis diffuse reflectance, and XPS spectroscopy. The catalytic performance was evaluated in oxidative desulfurization (ODS) and photocatalytic ODS (PODS) processes. The experimental results showed the addition of Fe promoted the catalytic activity of both ODS and PODS reactions. ODS activities of V-Fe catalysts increase up to 7.5 times with respect to V catalysts without Fe, and the most active catalyst (V5Fer) presents a characteristic oxidation time of 50 min for 4,6-DMDBT. The PODS activity of V10Fec was like ODS activity, showing it is possible to oxidize the dibenzothiophenes under friendly conditions to obtain lower S levels. The promoting effect of Fe was due to the interaction of Fe and Fe with the catalytic support, favoring the distribution of surface V and V species. Additionally, Fe improved the optical properties of the catalysts since the bandgap energy decrease and low recombination rate of the electron-hole pair were observed. Therefore, V-Fe based catalysts are photocatalytically actives to be used in PODS processes. |
| ArticleNumber | 142791 |
| Author | Alvarez-Amparán, Marco A. Cedeño-Caero, Luis Chacon-Argaez, Uriel |
| Author_xml | – sequence: 1 givenname: Uriel surname: Chacon-Argaez fullname: Chacon-Argaez, Uriel – sequence: 2 givenname: Marco A. surname: Alvarez-Amparán fullname: Alvarez-Amparán, Marco A. – sequence: 3 givenname: Luis orcidid: 0000-0002-9873-0866 surname: Cedeño-Caero fullname: Cedeño-Caero, Luis email: caero@unam.mx |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/38972456$$D View this record in MEDLINE/PubMed |
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| CitedBy_id | crossref_primary_10_1016_j_cattod_2025_115377 crossref_primary_10_1007_s11244_025_02097_w crossref_primary_10_1016_j_jpcs_2025_113168 |
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| SubjectTerms | Catalysis Iron - chemistry Oxidation-Reduction Thiophenes - chemistry Vanadium - chemistry |
| Title | Performance of V–Fe based catalysts on the oxidation of dibenzothiophenes |
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