Highly efficient selective oxidation of 2-methylnaphthalene to vitamin K3 over mesoporous Al/Ti-SBA-15 catalysts: The effect of acid sites and textural property
[Display omitted] •Al/Ti-SBA-15 were synthesized in moderate acidic aqueous media and characterized by various methods.•Synthesized catalysts and commercial zeolites were applied in the selective oxidation of 2-methylnaphtalene to vitamin K3.•Al-SBA-15 with high Brönsted acid concentration shows out...
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Veröffentlicht in: | Molecular catalysis 2020-11, Vol.495, p.111158, Article 111158 |
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Sprache: | eng |
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•Al/Ti-SBA-15 were synthesized in moderate acidic aqueous media and characterized by various methods.•Synthesized catalysts and commercial zeolites were applied in the selective oxidation of 2-methylnaphtalene to vitamin K3.•Al-SBA-15 with high Brönsted acid concentration shows outstanding catalytic performance.•Kinetic models for oxidation of 2-methylnaphtalene over Al/Ti-SBA-15 were established.•DFT method was used to investigate the electronic properties of SBA-15 and Al-SBA-15.
Catalytic oxidation of 2-methylnaphthalene to 2-methyl-1,4-naphthoquinone (vitamin K3) is a significant pathway to produce vitamin groups K. High pollution and low-productivity of the traditional method require a greener catalyst and process. In this work, Al/Ti-SBA-15 with different nSi/nAl and nSi/nTi ratios were hydrothermally prepared in mild acidic condition and tested in partial oxidation of 2-methylnaphthalene. Commercial zeolites NaY, β and ZSM-5 were applied to investigate the influence of mass transfer resistance and acidity on catalytic performance. Catalysts were characterized by XRD, N2 adsorption-desorption, TEM, NH3-TPD, FTIR and Py-FTIR. We have found that the 2-methylnaphthalene conversion and vitamin K3 selectivity depend strongly on the mesoporous structure as well as Brönsted acid concentration and strength. Irregular micropores and strong acidity will accelerate the cleavage of C = C in aromatic rings, leading to the production of phthalic anhydride. DFT calculation reveals that incorporation of aluminum in SBA-15 can reduce the energy gap, facilitating the electron transfer. And as a consequence of the substitution of Al in tetrahedral positions in SBA-15, Al-SBA-15 (10) gives the best result with 72% yield to vitamin K3. This catalyst markedly reduces the activation energy due to the modified activated center. Repeated experiments recommend that Al-SBA-15 is a steady and high-efficiency catalyst for the production of vitamin K3. |
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ISSN: | 2468-8231 2468-8231 |
DOI: | 10.1016/j.mcat.2020.111158 |