
Enhancing the anisole hydrodeoxygenation activity over Ni/Nb2O5−x by tuning the oxophilicity of the support
- Author
- Hadia Ali (UGent) , Tom Vandevyvere (UGent) , Jeroen Lauwaert (UGent) , Sushil Kumar Kansal, Maarten Sabbe (UGent) , Shunmugavel Saravanamurugan and Joris Thybaut (UGent)
- Organization
- Project
- Abstract
- The present work focuses on designing a robust non-noble metal-based niobia-supported catalyst with a high number of oxygen vacancies for an efficient HDO activity of anisole. Various synthesis procedures, such as hydrothermal (Nb2O5-HT), precipitation (Nb2O5-P) and hydrolysis (Nb2O5-H), are adopted for the preparation of the Nb2O5 support, followed by 3 wt% Ni impregnation. As a benchmark, Ni has also been impregnated on commercial Nb2O5 (Nb2O5-C). The catalysts display a large discrepancy in surface areas, the crystallite size of Nb2O5 and NiOx, strong metal-support interaction (SMSI), active interfacial Ni-NbOx species and oxygen vacancies. In particular, Ni impregnated on Nb2O5-H (Ni/Nb2O5-H) possesses the highest amount of oxygen vacancies (202 mu mol g(-1)) (O-2-temperature programmed desorption), which is 1.1 and 3.5 fold higher than that for Ni/Nb2O5-HT and Ni/Nb2O5-P, respectively, indicating the importance of the synthesis procedure of the support. Interestingly Ni/Nb2O5-H has 200-fold higher oxygen vacancies than Ni/Nb2O5-C. Likewise, Ni/Nb2O5-H possesses a high Ni3+/Ni2+ and Nb4+/Nb5+ ratio, based on X-ray photoelectron spectroscopy, suggesting high dispersion of small NiOx particles on the NbOx surface, facilitating the redistribution of the electrons at the interface of NiO and Nb2O5 due to SMSI. This leads to the formation of active interfacial Ni-NbOx species and oxygen vacancies (confirmed by H-2-TPD and XPS), contributing to the activation of hydrogen and anisole adsorption and thereby improving HDO activity substantially. At similar conversions of anisole, Ni/Nb2O5-H exhibits the highest rate of HDO of 0.63 mmol min(-1) g(-1), which is 1.4 to 3.2 fold higher than those of the other catalysts, including Nb2O5-C. Under optimised reaction conditions, Ni/Nb2O5-H shows a remarkable activity towards HDO of anisole with an excellent selectivity to cyclohexane (96.5%) at the near-quantitative conversion of anisole (>98%) at 240 degrees C, 20 bar H-2, 2 h. Ni/Nb2O5-H also displays good to excellent activity towards various lignin-based model compounds, affording 50-96% cyclohexane yield.
- Keywords
- Catalysis, IMPROVED SOLAR ABSORPTION, CATALYTIC HYDRODEOXYGENATION, SELECTIVE, HYDRODEOXYGENATION, MODEL-COMPOUND, METAL, NB2O5, PHENOL, OXIDATION, BIOMASS, PT/TIO2
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Citation
Please use this url to cite or link to this publication: http://hdl.handle.net/1854/LU-01GV0P15V6NW8MABF20H0SNSBG
- MLA
- Ali, Hadia, et al. “Enhancing the Anisole Hydrodeoxygenation Activity over Ni/Nb2O5−x by Tuning the Oxophilicity of the Support.” CATALYSIS SCIENCE & TECHNOLOGY, vol. 13, no. 4, 2023, pp. 1140–53, doi:10.1039/d2cy01745h.
- APA
- Ali, H., Vandevyvere, T., Lauwaert, J., Kansal, S. K., Sabbe, M., Saravanamurugan, S., & Thybaut, J. (2023). Enhancing the anisole hydrodeoxygenation activity over Ni/Nb2O5−x by tuning the oxophilicity of the support. CATALYSIS SCIENCE & TECHNOLOGY, 13(4), 1140–1153. https://doi.org/10.1039/d2cy01745h
- Chicago author-date
- Ali, Hadia, Tom Vandevyvere, Jeroen Lauwaert, Sushil Kumar Kansal, Maarten Sabbe, Shunmugavel Saravanamurugan, and Joris Thybaut. 2023. “Enhancing the Anisole Hydrodeoxygenation Activity over Ni/Nb2O5−x by Tuning the Oxophilicity of the Support.” CATALYSIS SCIENCE & TECHNOLOGY 13 (4): 1140–53. https://doi.org/10.1039/d2cy01745h.
- Chicago author-date (all authors)
- Ali, Hadia, Tom Vandevyvere, Jeroen Lauwaert, Sushil Kumar Kansal, Maarten Sabbe, Shunmugavel Saravanamurugan, and Joris Thybaut. 2023. “Enhancing the Anisole Hydrodeoxygenation Activity over Ni/Nb2O5−x by Tuning the Oxophilicity of the Support.” CATALYSIS SCIENCE & TECHNOLOGY 13 (4): 1140–1153. doi:10.1039/d2cy01745h.
- Vancouver
- 1.Ali H, Vandevyvere T, Lauwaert J, Kansal SK, Sabbe M, Saravanamurugan S, et al. Enhancing the anisole hydrodeoxygenation activity over Ni/Nb2O5−x by tuning the oxophilicity of the support. CATALYSIS SCIENCE & TECHNOLOGY. 2023;13(4):1140–53.
- IEEE
- [1]H. Ali et al., “Enhancing the anisole hydrodeoxygenation activity over Ni/Nb2O5−x by tuning the oxophilicity of the support,” CATALYSIS SCIENCE & TECHNOLOGY, vol. 13, no. 4, pp. 1140–1153, 2023.
@article{01GV0P15V6NW8MABF20H0SNSBG, abstract = {{The present work focuses on designing a robust non-noble metal-based niobia-supported catalyst with a high number of oxygen vacancies for an efficient HDO activity of anisole. Various synthesis procedures, such as hydrothermal (Nb2O5-HT), precipitation (Nb2O5-P) and hydrolysis (Nb2O5-H), are adopted for the preparation of the Nb2O5 support, followed by 3 wt% Ni impregnation. As a benchmark, Ni has also been impregnated on commercial Nb2O5 (Nb2O5-C). The catalysts display a large discrepancy in surface areas, the crystallite size of Nb2O5 and NiOx, strong metal-support interaction (SMSI), active interfacial Ni-NbOx species and oxygen vacancies. In particular, Ni impregnated on Nb2O5-H (Ni/Nb2O5-H) possesses the highest amount of oxygen vacancies (202 mu mol g(-1)) (O-2-temperature programmed desorption), which is 1.1 and 3.5 fold higher than that for Ni/Nb2O5-HT and Ni/Nb2O5-P, respectively, indicating the importance of the synthesis procedure of the support. Interestingly Ni/Nb2O5-H has 200-fold higher oxygen vacancies than Ni/Nb2O5-C. Likewise, Ni/Nb2O5-H possesses a high Ni3+/Ni2+ and Nb4+/Nb5+ ratio, based on X-ray photoelectron spectroscopy, suggesting high dispersion of small NiOx particles on the NbOx surface, facilitating the redistribution of the electrons at the interface of NiO and Nb2O5 due to SMSI. This leads to the formation of active interfacial Ni-NbOx species and oxygen vacancies (confirmed by H-2-TPD and XPS), contributing to the activation of hydrogen and anisole adsorption and thereby improving HDO activity substantially. At similar conversions of anisole, Ni/Nb2O5-H exhibits the highest rate of HDO of 0.63 mmol min(-1) g(-1), which is 1.4 to 3.2 fold higher than those of the other catalysts, including Nb2O5-C. Under optimised reaction conditions, Ni/Nb2O5-H shows a remarkable activity towards HDO of anisole with an excellent selectivity to cyclohexane (96.5%) at the near-quantitative conversion of anisole (>98%) at 240 degrees C, 20 bar H-2, 2 h. Ni/Nb2O5-H also displays good to excellent activity towards various lignin-based model compounds, affording 50-96% cyclohexane yield.}}, author = {{Ali, Hadia and Vandevyvere, Tom and Lauwaert, Jeroen and Kansal, Sushil Kumar and Sabbe, Maarten and Saravanamurugan, Shunmugavel and Thybaut, Joris}}, issn = {{2044-4753}}, journal = {{CATALYSIS SCIENCE & TECHNOLOGY}}, keywords = {{Catalysis,IMPROVED SOLAR ABSORPTION,CATALYTIC HYDRODEOXYGENATION,SELECTIVE,HYDRODEOXYGENATION,MODEL-COMPOUND,METAL,NB2O5,PHENOL,OXIDATION,BIOMASS,PT/TIO2}}, language = {{eng}}, number = {{4}}, pages = {{1140--1153}}, title = {{Enhancing the anisole hydrodeoxygenation activity over Ni/Nb2O5−x by tuning the oxophilicity of the support}}, url = {{http://doi.org/10.1039/d2cy01745h}}, volume = {{13}}, year = {{2023}}, }
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