Efficient Diesel Desulfurization by Novel Amphiphilic Polyoxometalate-Based Hybrid Catalyst at Room Temperature
Amphiphilic hybrid catalysts were prepared by modifying [SMo<sub>12</sub>O<sub>40</sub>]<sup>2−</sup> with tetrabutylammonium bromide (TBAB), 1-butyl-3-methylimidazole bromide (BMIMBr) and octadecyl trimethyl ammonium bromide (ODAB), respectively. The prepared cat...
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MDPI AG
2023-03-01
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| Series: | Molecules |
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| Online Access: | https://www.mdpi.com/1420-3049/28/6/2539 |
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| author | Jie Zhao Bingquan Wang Rui Wang Ivan V. Kozhevnikov Korchak Vladimir |
| author_facet | Jie Zhao Bingquan Wang Rui Wang Ivan V. Kozhevnikov Korchak Vladimir |
| author_sort | Jie Zhao |
| collection | DOAJ |
| description | Amphiphilic hybrid catalysts were prepared by modifying [SMo<sub>12</sub>O<sub>40</sub>]<sup>2−</sup> with tetrabutylammonium bromide (TBAB), 1-butyl-3-methylimidazole bromide (BMIMBr) and octadecyl trimethyl ammonium bromide (ODAB), respectively. The prepared catalysts were characterized by IR, XRD, SEM, TG and XPS. The desulfurization performance of the catalysts was investigated in model oil and actual diesel using hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) as an oxidant and acetonitrile as an extractant. All catalysts exhibited favorable activity for removing sulfur compounds at room temperature. Dibenzothiophene (DBT) can be nearly completely removed using SMo<sub>12</sub>O<sub>40</sub><sup>2−</sup>-organic catalysts within a short reaction time. For different sulfur compounds, the [TBA]<sub>2</sub>SMo<sub>12</sub>O<sub>40</sub> catalyst showed a better removal effect than the [BMIM]<sub>2</sub>SMo<sub>12</sub>O<sub>40</sub> and [ODA]<sub>2</sub>SMo<sub>12</sub>O<sub>40</sub> catalyst. The [TBA]<sub>2</sub>SMo<sub>12</sub>O<sub>40</sub> dissolved in extraction solvent could be reused up to five times in an oxidative desulfurization (ODS) cycle with no significant loss of activity. The [BMIM]<sub>2</sub>SMo<sub>12</sub>O<sub>40</sub> performed as a heterogeneous catalyst able to be recycled from the ODS system and maintained excellent catalytic activity. The catalysts showed a positive desulfurization effect in real diesel treatment. Finally, we described the ODS desulfurization mechanism of DBT using SMo<sub>12</sub>O<sub>40</sub><sup>2−</sup>-organic hybrid catalysts. The amphiphilic hybrid catalyst cation captures DBT, while SMo<sub>12</sub>O<sub>40</sub><sup>2−</sup> reacts with the oxidant H<sub>2</sub>O<sub>2</sub> to produce peroxy-active species. DBT can be oxidized to its sulfone by the action of peroxy-active species to achieve ODS desulfurization. |
| first_indexed | 2024-03-11T06:07:03Z |
| format | Article |
| id | doaj.art-1d73c6992d4d4df0a35ed809ee736f75 |
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| language | English |
| last_indexed | 2024-03-11T06:07:03Z |
| publishDate | 2023-03-01 |
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| spelling | doaj.art-1d73c6992d4d4df0a35ed809ee736f752023-11-17T12:51:44ZengMDPI AGMolecules1420-30492023-03-01286253910.3390/molecules28062539Efficient Diesel Desulfurization by Novel Amphiphilic Polyoxometalate-Based Hybrid Catalyst at Room TemperatureJie Zhao0Bingquan Wang1Rui Wang2Ivan V. Kozhevnikov3Korchak Vladimir4School of Environmental Science and Engineering, Shandong University, Qingdao 266237, ChinaSchool of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, ChinaSchool of Environmental Science and Engineering, Shandong University, Qingdao 266237, ChinaDepartment of Chemistry, University of Liverpool, Liverpool L69 7ZD, UKN. N. Semenov Federal Research Center of Chemical Physics, Russian Academy of Sciences, Moscow 119991, RussiaAmphiphilic hybrid catalysts were prepared by modifying [SMo<sub>12</sub>O<sub>40</sub>]<sup>2−</sup> with tetrabutylammonium bromide (TBAB), 1-butyl-3-methylimidazole bromide (BMIMBr) and octadecyl trimethyl ammonium bromide (ODAB), respectively. The prepared catalysts were characterized by IR, XRD, SEM, TG and XPS. The desulfurization performance of the catalysts was investigated in model oil and actual diesel using hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) as an oxidant and acetonitrile as an extractant. All catalysts exhibited favorable activity for removing sulfur compounds at room temperature. Dibenzothiophene (DBT) can be nearly completely removed using SMo<sub>12</sub>O<sub>40</sub><sup>2−</sup>-organic catalysts within a short reaction time. For different sulfur compounds, the [TBA]<sub>2</sub>SMo<sub>12</sub>O<sub>40</sub> catalyst showed a better removal effect than the [BMIM]<sub>2</sub>SMo<sub>12</sub>O<sub>40</sub> and [ODA]<sub>2</sub>SMo<sub>12</sub>O<sub>40</sub> catalyst. The [TBA]<sub>2</sub>SMo<sub>12</sub>O<sub>40</sub> dissolved in extraction solvent could be reused up to five times in an oxidative desulfurization (ODS) cycle with no significant loss of activity. The [BMIM]<sub>2</sub>SMo<sub>12</sub>O<sub>40</sub> performed as a heterogeneous catalyst able to be recycled from the ODS system and maintained excellent catalytic activity. The catalysts showed a positive desulfurization effect in real diesel treatment. Finally, we described the ODS desulfurization mechanism of DBT using SMo<sub>12</sub>O<sub>40</sub><sup>2−</sup>-organic hybrid catalysts. The amphiphilic hybrid catalyst cation captures DBT, while SMo<sub>12</sub>O<sub>40</sub><sup>2−</sup> reacts with the oxidant H<sub>2</sub>O<sub>2</sub> to produce peroxy-active species. DBT can be oxidized to its sulfone by the action of peroxy-active species to achieve ODS desulfurization.https://www.mdpi.com/1420-3049/28/6/2539desulfurizationdieselpolyoxometalateoxidation catalysis |
| spellingShingle | Jie Zhao Bingquan Wang Rui Wang Ivan V. Kozhevnikov Korchak Vladimir Efficient Diesel Desulfurization by Novel Amphiphilic Polyoxometalate-Based Hybrid Catalyst at Room Temperature Molecules desulfurization diesel polyoxometalate oxidation catalysis |
| title | Efficient Diesel Desulfurization by Novel Amphiphilic Polyoxometalate-Based Hybrid Catalyst at Room Temperature |
| title_full | Efficient Diesel Desulfurization by Novel Amphiphilic Polyoxometalate-Based Hybrid Catalyst at Room Temperature |
| title_fullStr | Efficient Diesel Desulfurization by Novel Amphiphilic Polyoxometalate-Based Hybrid Catalyst at Room Temperature |
| title_full_unstemmed | Efficient Diesel Desulfurization by Novel Amphiphilic Polyoxometalate-Based Hybrid Catalyst at Room Temperature |
| title_short | Efficient Diesel Desulfurization by Novel Amphiphilic Polyoxometalate-Based Hybrid Catalyst at Room Temperature |
| title_sort | efficient diesel desulfurization by novel amphiphilic polyoxometalate based hybrid catalyst at room temperature |
| topic | desulfurization diesel polyoxometalate oxidation catalysis |
| url | https://www.mdpi.com/1420-3049/28/6/2539 |
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