Selective C–C Bond Cleavage in Diols and Lignin Models: High-Throughput Screening of Metal Oxide-Anchored Vanadium in Mesoporous Silica
The development of selective and robust heterogeneous oxidation catalysts is an enabling technology for conversion of biomass-derived platform chemicals. Vanadium active sites were incorporated into the structure of mesoporous silica via an ultra-fast, one-pot synthesis method based on microwave-ass...
| Main Authors: | , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
MDPI AG
2021-07-01
|
| Series: | Catalysts |
| Subjects: | |
| Online Access: | https://www.mdpi.com/2073-4344/11/8/901 |
| _version_ | 1797524396106055680 |
|---|---|
| author | Xinnan Lu Roxanne Clément Yong Lu Belén Albela R. Tom Baker Laurent Bonneviot |
| author_facet | Xinnan Lu Roxanne Clément Yong Lu Belén Albela R. Tom Baker Laurent Bonneviot |
| author_sort | Xinnan Lu |
| collection | DOAJ |
| description | The development of selective and robust heterogeneous oxidation catalysts is an enabling technology for conversion of biomass-derived platform chemicals. Vanadium active sites were incorporated into the structure of mesoporous silica via an ultra-fast, one-pot synthesis method based on microwave-assisted heating. In addition, Al/Ti/Zr/Ce anchoring ions were introduced in order to minimize vanadium leaching and better control its dispersion. The supported V-(Al/Ti/Zr/Ce)-MCM-41 composite materials were assessed as catalysts for aerobic C–C bond cleavage of simple models for lignin (1,2-diphenyl-2-methoxyethanol) and sugar-derived polyalcohols (<i>meso</i>-hydrobenzoin). The <i>Ti<sup>IV</sup></i> ions proved to be the best anchors to prevent V leaching, while <i>Al<sup>III</sup></i> and <i>Zr<sup>IV</sup></i> ions were the best to improve selective conversion of the substrates. The active sites in these catalysts are shown to be 2D VO<sub>x</sub> layers stabilized on the anchors. In a screen of twelve solvents, weakly polar solvents like toluene were found to be most suitable for this reaction, as was environmentally friendly ethyl acetate. The above properties, together with the high selectivity for C–C bond cleavage, advocate for a heterogeneous catalytic pathway, intrinsically different from that reported previously for molecular oxovanadium (V) catalysts. |
| first_indexed | 2024-03-10T08:56:46Z |
| format | Article |
| id | doaj.art-aee42d61244a409b86f765f7f8637ddb |
| institution | Directory Open Access Journal |
| issn | 2073-4344 |
| language | English |
| last_indexed | 2024-03-10T08:56:46Z |
| publishDate | 2021-07-01 |
| publisher | MDPI AG |
| record_format | Article |
| series | Catalysts |
| spelling | doaj.art-aee42d61244a409b86f765f7f8637ddb2023-11-22T07:06:27ZengMDPI AGCatalysts2073-43442021-07-0111890110.3390/catal11080901Selective C–C Bond Cleavage in Diols and Lignin Models: High-Throughput Screening of Metal Oxide-Anchored Vanadium in Mesoporous SilicaXinnan Lu0Roxanne Clément1Yong Lu2Belén Albela3R. Tom Baker4Laurent Bonneviot5Laboratoire de Chimie, Ecole Normale Supérieure de Lyon, Université de Lyon, 46 Allée d’Italie, CEDEX 07, 69364 Lyon, FranceDepartment of Chemistry and Biomolecular Sciences and Centre for Catalysis Research and Innovation, University of Ottawa, Ottawa, ON K1N 6N5, CanadaSchool of Chemistry and Molecular Engineering, East China Normal University, No. 3663 North Zhongshan Road, Shanghai 200062, ChinaLaboratoire de Chimie, Ecole Normale Supérieure de Lyon, Université de Lyon, 46 Allée d’Italie, CEDEX 07, 69364 Lyon, FranceDepartment of Chemistry and Biomolecular Sciences and Centre for Catalysis Research and Innovation, University of Ottawa, Ottawa, ON K1N 6N5, CanadaLaboratoire de Chimie, Ecole Normale Supérieure de Lyon, Université de Lyon, 46 Allée d’Italie, CEDEX 07, 69364 Lyon, FranceThe development of selective and robust heterogeneous oxidation catalysts is an enabling technology for conversion of biomass-derived platform chemicals. Vanadium active sites were incorporated into the structure of mesoporous silica via an ultra-fast, one-pot synthesis method based on microwave-assisted heating. In addition, Al/Ti/Zr/Ce anchoring ions were introduced in order to minimize vanadium leaching and better control its dispersion. The supported V-(Al/Ti/Zr/Ce)-MCM-41 composite materials were assessed as catalysts for aerobic C–C bond cleavage of simple models for lignin (1,2-diphenyl-2-methoxyethanol) and sugar-derived polyalcohols (<i>meso</i>-hydrobenzoin). The <i>Ti<sup>IV</sup></i> ions proved to be the best anchors to prevent V leaching, while <i>Al<sup>III</sup></i> and <i>Zr<sup>IV</sup></i> ions were the best to improve selective conversion of the substrates. The active sites in these catalysts are shown to be 2D VO<sub>x</sub> layers stabilized on the anchors. In a screen of twelve solvents, weakly polar solvents like toluene were found to be most suitable for this reaction, as was environmentally friendly ethyl acetate. The above properties, together with the high selectivity for C–C bond cleavage, advocate for a heterogeneous catalytic pathway, intrinsically different from that reported previously for molecular oxovanadium (V) catalysts.https://www.mdpi.com/2073-4344/11/8/901mesoporous silicaheterogeneous catalysisoxidative C–C bond cleavagevanadiumlignin model |
| spellingShingle | Xinnan Lu Roxanne Clément Yong Lu Belén Albela R. Tom Baker Laurent Bonneviot Selective C–C Bond Cleavage in Diols and Lignin Models: High-Throughput Screening of Metal Oxide-Anchored Vanadium in Mesoporous Silica Catalysts mesoporous silica heterogeneous catalysis oxidative C–C bond cleavage vanadium lignin model |
| title | Selective C–C Bond Cleavage in Diols and Lignin Models: High-Throughput Screening of Metal Oxide-Anchored Vanadium in Mesoporous Silica |
| title_full | Selective C–C Bond Cleavage in Diols and Lignin Models: High-Throughput Screening of Metal Oxide-Anchored Vanadium in Mesoporous Silica |
| title_fullStr | Selective C–C Bond Cleavage in Diols and Lignin Models: High-Throughput Screening of Metal Oxide-Anchored Vanadium in Mesoporous Silica |
| title_full_unstemmed | Selective C–C Bond Cleavage in Diols and Lignin Models: High-Throughput Screening of Metal Oxide-Anchored Vanadium in Mesoporous Silica |
| title_short | Selective C–C Bond Cleavage in Diols and Lignin Models: High-Throughput Screening of Metal Oxide-Anchored Vanadium in Mesoporous Silica |
| title_sort | selective c c bond cleavage in diols and lignin models high throughput screening of metal oxide anchored vanadium in mesoporous silica |
| topic | mesoporous silica heterogeneous catalysis oxidative C–C bond cleavage vanadium lignin model |
| url | https://www.mdpi.com/2073-4344/11/8/901 |
| work_keys_str_mv | AT xinnanlu selectiveccbondcleavageindiolsandligninmodelshighthroughputscreeningofmetaloxideanchoredvanadiuminmesoporoussilica AT roxanneclement selectiveccbondcleavageindiolsandligninmodelshighthroughputscreeningofmetaloxideanchoredvanadiuminmesoporoussilica AT yonglu selectiveccbondcleavageindiolsandligninmodelshighthroughputscreeningofmetaloxideanchoredvanadiuminmesoporoussilica AT belenalbela selectiveccbondcleavageindiolsandligninmodelshighthroughputscreeningofmetaloxideanchoredvanadiuminmesoporoussilica AT rtombaker selectiveccbondcleavageindiolsandligninmodelshighthroughputscreeningofmetaloxideanchoredvanadiuminmesoporoussilica AT laurentbonneviot selectiveccbondcleavageindiolsandligninmodelshighthroughputscreeningofmetaloxideanchoredvanadiuminmesoporoussilica |