TY - JOUR
T1 - Hydrodeoxygenation of isoeugenol over Ni-SBA-15: Kinetics and modelling
AU - Tieuli, Sebastiano
AU - Mäki-Arvela, Päivi
AU - Peurla, Markus
AU - Eränen, Kari
AU - Wärnå, Johan
AU - Cruciani, Giuseppe
AU - Menegazzo, Federica
AU - Murzin, Dmitry
AU - Signoretto, Michela
N1 - tk.
25 June 2019
accepted manuscript
24 months
CC BY-NC-ND
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Har kontaktat paivi.maki-arvela@abo.fi den 20.2.2020/LN
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PY - 2019
Y1 - 2019
N2 - Hydrodeoxygenation (HDO) of isoeugenol has been investigated over Ni-SBA-15 and Ni-SZ-SBA-15 containing sulfated ZrO2 with Si/Zr molar ratio of 8.4. The catalysts were prepared via incipient wetness method and characterized by N2 adsorption, AAS, TPR, X-ray diffraction (XRD), thermal gravimetric/differential thermal analyses (TG-DTA), organic elemental analysis, pyridine adsorption-desorption with Fourier-transform infrared spectroscopy (FTIR) and transmission electron microscopy (TEM). The results revealed that 75% yield of propylcyclohexane was obtained over a non acidic Ni-SBA-15 in isoeugenol HDO at 300 °C under 3 MPa H2 using dodecane as a solvent. Ni-SZ-SBA-15 gave only very low HDO activity, which is explained by location of the acid sites both inside and outside SBA-15, whereas nickel particles were partially located inside the SBA-15 structure. On the other hand Ni particles in Ni-SBA-15 with the size of 20 nm were located outside SBA-15 promoting HDO. The kinetic model was developed for HDO of isoeugenol based on the proposed reaction network, which took into account formation of intermediate products as well as oligomers. The developed kinetic model was capable of describing well the experimental data with the degree of explanation equal to 91%. The activation energy for hydrogenation of propylcyclohexene and for demethoxylation of dihydroeugenol to 4-propylphenol are equal to 92 kJ/mol and 62 kJ/mol, respectively.
AB - Hydrodeoxygenation (HDO) of isoeugenol has been investigated over Ni-SBA-15 and Ni-SZ-SBA-15 containing sulfated ZrO2 with Si/Zr molar ratio of 8.4. The catalysts were prepared via incipient wetness method and characterized by N2 adsorption, AAS, TPR, X-ray diffraction (XRD), thermal gravimetric/differential thermal analyses (TG-DTA), organic elemental analysis, pyridine adsorption-desorption with Fourier-transform infrared spectroscopy (FTIR) and transmission electron microscopy (TEM). The results revealed that 75% yield of propylcyclohexane was obtained over a non acidic Ni-SBA-15 in isoeugenol HDO at 300 °C under 3 MPa H2 using dodecane as a solvent. Ni-SZ-SBA-15 gave only very low HDO activity, which is explained by location of the acid sites both inside and outside SBA-15, whereas nickel particles were partially located inside the SBA-15 structure. On the other hand Ni particles in Ni-SBA-15 with the size of 20 nm were located outside SBA-15 promoting HDO. The kinetic model was developed for HDO of isoeugenol based on the proposed reaction network, which took into account formation of intermediate products as well as oligomers. The developed kinetic model was capable of describing well the experimental data with the degree of explanation equal to 91%. The activation energy for hydrogenation of propylcyclohexene and for demethoxylation of dihydroeugenol to 4-propylphenol are equal to 92 kJ/mol and 62 kJ/mol, respectively.
U2 - 10.1016/j.apcata.2019.04.028
DO - 10.1016/j.apcata.2019.04.028
M3 - Artikel
SN - 0926-860X
VL - 580
SP - 1
EP - 10
JO - Applied Catalysis A: General
JF - Applied Catalysis A: General
ER -