Molecular nitrogen promotes catalytic hydrodeoxygenation
Although molecular dinitrogen (N2) is widely used as a carrier or inert gas for many catalytic reactions, it is rarely considered as a catalytic promoter. Here, we report that N2 could be used to reduce the activation energy for catalytic hydrodeoxygenation over ruthenium-based catalysts. Specifical...
| 主要な著者: | , , , , , , , , , , , , , , , , , |
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| フォーマット: | Journal article |
| 言語: | English |
| 出版事項: |
Nature Research
2019
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| _version_ | 1826305020774055936 |
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| author | Duan, H Liu, J-C Xu, M Zhao, Y Ma, X-L Dong, J Zheng, X Zheng, J Allen, CS Danaie, M Peng, Y-K Issariyakul, T Chen, D Kirkland, AI Buffet, J-C Li, J Tsang, SCE O'Hare, D |
| author_facet | Duan, H Liu, J-C Xu, M Zhao, Y Ma, X-L Dong, J Zheng, X Zheng, J Allen, CS Danaie, M Peng, Y-K Issariyakul, T Chen, D Kirkland, AI Buffet, J-C Li, J Tsang, SCE O'Hare, D |
| author_sort | Duan, H |
| collection | OXFORD |
| description | Although molecular dinitrogen (N2) is widely used as a carrier or inert gas for many catalytic reactions, it is rarely considered as a catalytic promoter. Here, we report that N2 could be used to reduce the activation energy for catalytic hydrodeoxygenation over ruthenium-based catalysts. Specifically, we report a 4.3-fold activity increase in the catalytic hydrodeoxygenation of p-cresol to toluene over a titanium oxide supported ruthenium catalyst (Ru/TiO2) by simply introducing 6 bar N2 under batch conditions at 160 °C and 1 bar hydrogen. Detailed investigations indicate that N2 can be adsorbed and activated on the metallic ruthenium surface to form hydrogenated nitrogen species, which offer protic hydrogen to lower the activation energy of direct carbonaromatic–oxygen bond scission and the hydrogenation of hydroxy groups. Thus, by employing different ruthenium catalysts, including Ru/TiO2, Ru/Al2O3, Ru/ZrO2 and Ru/C, we demonstrate that N2 promotion of hydrodeoxygenation can be regarded as a general strategy. |
| first_indexed | 2024-03-07T06:26:32Z |
| format | Journal article |
| id | oxford-uuid:f47e5fa6-38fa-44a2-84d3-cc6711142886 |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-07T06:26:32Z |
| publishDate | 2019 |
| publisher | Nature Research |
| record_format | dspace |
| spelling | oxford-uuid:f47e5fa6-38fa-44a2-84d3-cc67111428862022-03-27T12:20:12ZMolecular nitrogen promotes catalytic hydrodeoxygenationJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:f47e5fa6-38fa-44a2-84d3-cc6711142886EnglishSymplectic Elements at OxfordNature Research2019Duan, HLiu, J-CXu, MZhao, YMa, X-LDong, JZheng, XZheng, JAllen, CSDanaie, MPeng, Y-KIssariyakul, TChen, DKirkland, AIBuffet, J-CLi, JTsang, SCEO'Hare, DAlthough molecular dinitrogen (N2) is widely used as a carrier or inert gas for many catalytic reactions, it is rarely considered as a catalytic promoter. Here, we report that N2 could be used to reduce the activation energy for catalytic hydrodeoxygenation over ruthenium-based catalysts. Specifically, we report a 4.3-fold activity increase in the catalytic hydrodeoxygenation of p-cresol to toluene over a titanium oxide supported ruthenium catalyst (Ru/TiO2) by simply introducing 6 bar N2 under batch conditions at 160 °C and 1 bar hydrogen. Detailed investigations indicate that N2 can be adsorbed and activated on the metallic ruthenium surface to form hydrogenated nitrogen species, which offer protic hydrogen to lower the activation energy of direct carbonaromatic–oxygen bond scission and the hydrogenation of hydroxy groups. Thus, by employing different ruthenium catalysts, including Ru/TiO2, Ru/Al2O3, Ru/ZrO2 and Ru/C, we demonstrate that N2 promotion of hydrodeoxygenation can be regarded as a general strategy. |
| spellingShingle | Duan, H Liu, J-C Xu, M Zhao, Y Ma, X-L Dong, J Zheng, X Zheng, J Allen, CS Danaie, M Peng, Y-K Issariyakul, T Chen, D Kirkland, AI Buffet, J-C Li, J Tsang, SCE O'Hare, D Molecular nitrogen promotes catalytic hydrodeoxygenation |
| title | Molecular nitrogen promotes catalytic hydrodeoxygenation |
| title_full | Molecular nitrogen promotes catalytic hydrodeoxygenation |
| title_fullStr | Molecular nitrogen promotes catalytic hydrodeoxygenation |
| title_full_unstemmed | Molecular nitrogen promotes catalytic hydrodeoxygenation |
| title_short | Molecular nitrogen promotes catalytic hydrodeoxygenation |
| title_sort | molecular nitrogen promotes catalytic hydrodeoxygenation |
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