Transformation of CO<sub>2</sub> with Glycerol to Glycerol Carbonate over ETS-10 Zeolite-Based Catalyst
Catalytic conversion of CO<sub>2</sub> with the surplus glycerol (GL) produced from biodiesel manufacturing has attracted much academic and industrial attention, which proves the urgent requirement for developing high-performance catalysts to afford significant environmental benefits. He...
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| Format: | Article |
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MDPI AG
2023-02-01
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| Series: | Molecules |
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| Online Access: | https://www.mdpi.com/1420-3049/28/5/2272 |
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| author | Zhangxi Gao Mei Xiang Mingyang He Weiyou Zhou Jiayao Chen Jiamin Lu Zeying Wu Yaqiong Su |
| author_facet | Zhangxi Gao Mei Xiang Mingyang He Weiyou Zhou Jiayao Chen Jiamin Lu Zeying Wu Yaqiong Su |
| author_sort | Zhangxi Gao |
| collection | DOAJ |
| description | Catalytic conversion of CO<sub>2</sub> with the surplus glycerol (GL) produced from biodiesel manufacturing has attracted much academic and industrial attention, which proves the urgent requirement for developing high-performance catalysts to afford significant environmental benefits. Herein, titanosilicate ETS-10 zeolite-based catalysts with active metal species introduced by impregnation were employed for coupling CO<sub>2</sub> with GL to efficiently synthesize glycerol carbonate (GC). The catalytic GL conversion at 170 °C miraculously reached 35.0% and a 12.7% yield of GC was obtained on Co/ETS-10 with CH<sub>3</sub>CN as a dehydrating agent. For comparison, Zn/ETS- Cu/ETS-10, Ni/ETS-10, Zr/ETS-10, Ce/ETS-10, and Fe/ETS-10 were also prepared, which showed inferior coordination between GL conversion and GC selectivity. Comprehensive analysis revealed that the presence of moderate basic sites for CO<sub>2</sub> adsorption-activation played a crucial role in regulating catalytic activity. Moreover, the appropriate interaction between cobalt species and ETS-10 zeolite was also of great significance for improving the glycerol activation capacity. A plausible mechanism was proposed for the synthesis of GC from GL and CO<sub>2</sub> in the presence of CH<sub>3</sub>CN solvent over Co/ETS-10 catalyst. Moreover, the recyclability of Co/ETS-10 was also measured and it proved to be recycled at least eight times with less than 3% decline in GL conversion and GC yield after a simple regeneration process through calcination at 450 °C for 5 h in air. |
| first_indexed | 2024-03-11T07:16:08Z |
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| id | doaj.art-04d2edffa9204c099496e7e9c849b053 |
| institution | Directory Open Access Journal |
| issn | 1420-3049 |
| language | English |
| last_indexed | 2024-03-11T07:16:08Z |
| publishDate | 2023-02-01 |
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| record_format | Article |
| series | Molecules |
| spelling | doaj.art-04d2edffa9204c099496e7e9c849b0532023-11-17T08:14:19ZengMDPI AGMolecules1420-30492023-02-01285227210.3390/molecules28052272Transformation of CO<sub>2</sub> with Glycerol to Glycerol Carbonate over ETS-10 Zeolite-Based CatalystZhangxi Gao0Mei Xiang1Mingyang He2Weiyou Zhou3Jiayao Chen4Jiamin Lu5Zeying Wu6Yaqiong Su7Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, Changzhou 213164, ChinaResearch Center of Secondary Resources and Environment, School of Chemical Engineering and Materials, Changzhou Institute of Technology, Changzhou 213032, ChinaJiangsu Key Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, Changzhou 213164, ChinaJiangsu Key Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, Changzhou 213164, ChinaResearch Center of Secondary Resources and Environment, School of Chemical Engineering and Materials, Changzhou Institute of Technology, Changzhou 213032, ChinaResearch Center of Secondary Resources and Environment, School of Chemical Engineering and Materials, Changzhou Institute of Technology, Changzhou 213032, ChinaJiangsu Key Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, Changzhou 213164, ChinaXi’an Key Laboratory of Sustainable Energy Materials Chemistry, State Key Laboratory of Electrical Insulation and Power Equipment, School of Chemistry, Xi’an Jiaotong University, Xi’an 710049, ChinaCatalytic conversion of CO<sub>2</sub> with the surplus glycerol (GL) produced from biodiesel manufacturing has attracted much academic and industrial attention, which proves the urgent requirement for developing high-performance catalysts to afford significant environmental benefits. Herein, titanosilicate ETS-10 zeolite-based catalysts with active metal species introduced by impregnation were employed for coupling CO<sub>2</sub> with GL to efficiently synthesize glycerol carbonate (GC). The catalytic GL conversion at 170 °C miraculously reached 35.0% and a 12.7% yield of GC was obtained on Co/ETS-10 with CH<sub>3</sub>CN as a dehydrating agent. For comparison, Zn/ETS- Cu/ETS-10, Ni/ETS-10, Zr/ETS-10, Ce/ETS-10, and Fe/ETS-10 were also prepared, which showed inferior coordination between GL conversion and GC selectivity. Comprehensive analysis revealed that the presence of moderate basic sites for CO<sub>2</sub> adsorption-activation played a crucial role in regulating catalytic activity. Moreover, the appropriate interaction between cobalt species and ETS-10 zeolite was also of great significance for improving the glycerol activation capacity. A plausible mechanism was proposed for the synthesis of GC from GL and CO<sub>2</sub> in the presence of CH<sub>3</sub>CN solvent over Co/ETS-10 catalyst. Moreover, the recyclability of Co/ETS-10 was also measured and it proved to be recycled at least eight times with less than 3% decline in GL conversion and GC yield after a simple regeneration process through calcination at 450 °C for 5 h in air.https://www.mdpi.com/1420-3049/28/5/2272CO<sub>2</sub>glycerolglycerol carbonateETS-10 zeolitecobalt-based catalyst |
| spellingShingle | Zhangxi Gao Mei Xiang Mingyang He Weiyou Zhou Jiayao Chen Jiamin Lu Zeying Wu Yaqiong Su Transformation of CO<sub>2</sub> with Glycerol to Glycerol Carbonate over ETS-10 Zeolite-Based Catalyst Molecules CO<sub>2</sub> glycerol glycerol carbonate ETS-10 zeolite cobalt-based catalyst |
| title | Transformation of CO<sub>2</sub> with Glycerol to Glycerol Carbonate over ETS-10 Zeolite-Based Catalyst |
| title_full | Transformation of CO<sub>2</sub> with Glycerol to Glycerol Carbonate over ETS-10 Zeolite-Based Catalyst |
| title_fullStr | Transformation of CO<sub>2</sub> with Glycerol to Glycerol Carbonate over ETS-10 Zeolite-Based Catalyst |
| title_full_unstemmed | Transformation of CO<sub>2</sub> with Glycerol to Glycerol Carbonate over ETS-10 Zeolite-Based Catalyst |
| title_short | Transformation of CO<sub>2</sub> with Glycerol to Glycerol Carbonate over ETS-10 Zeolite-Based Catalyst |
| title_sort | transformation of co sub 2 sub with glycerol to glycerol carbonate over ets 10 zeolite based catalyst |
| topic | CO<sub>2</sub> glycerol glycerol carbonate ETS-10 zeolite cobalt-based catalyst |
| url | https://www.mdpi.com/1420-3049/28/5/2272 |
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