Designing efficient and facile recoverable
catalysts is desired for sustainable biomass valorization. This work
reports the one-pot synthesis of a novel magnetic Fe(NiFe)O4–SiO2 nanocatalyst for hydrogenation of biomass-derived
furfural into valuable furfuryl alcohol. Various techniques were used
to systematically analyze the physicochemical properties of the Fe(NiFe)O4–SiO2 nanocatalyst. Vibrating sample magnetometer
analysis reveals low coercivity of Fe(NiFe)O4–SiO2 (6.991 G) compared with that of Fe3O4–SiO2 (27.323 G), which is attributed to highly
dispersed Ni species in the Fe(NiFe)O4–SiO2 catalyst. HRTEM images indicated the nanosized nature of the Fe(NiFe)O4–SiO2 catalyst with an average diameter
of ∼14.32 nm. The Fe(NiFe)O4–SiO2 catalyst showed a superior BET surface area (259 m2/g),
which is due to the formation of nanosized particles. The magnetic
Fe(NiFe)O4–SiO2 nanocatalyst shows a
remarkable performance with 94.3 and 93.5% conversions of furfural
and ∼100% selectivity of furfuryl alcohol at 90 °C and
20 H2 bar and 250 °C and 5 H2 bar, respectively.
Using heptane as a solvent, the effect of temperature, pressure, reactant
amount, and catalyst loading were investigated to optimize the reaction
conditions. A probable mechanism via a non-hydrogen spillover route
was proposed for the hydrogenation of furfural to furfuryl alcohol
over the magnetic Fe(NiFe)O4–SiO2 nanocatalyst.
The efficiency of the magnetic Fe(NiFe)O4–SiO2 nanocatalyst is attributed to highly dispersed nickel species,
which plays a key role in the dissociation of H2 into a
proton and a hydride in the furfural hydrogenation. The superior performance
of the magnetic Fe(NiFe)O4–SiO2 nanocatalyst,
along with the advantages of low cost and easy recoverability, could
make it a new appealing catalyst in various selective hydrogenation
reactions.
Hierarchical ZnO/ZSM-5 catalysts were prepared by desilication and impregnation with 2 wt % metallic ZnO. X-ray diffraction and Fourier transform infrared (FTIR) results showed that the structures of the hierarchical zeolites were relatively preserved despite desilication but were accompanied with sequential loss in crystallinity, likewise Bro̷ nsted acidity causing decline in conversion or activity of the catalyst. However, pyridine FTIR shows enhancement of the Bro̷ nsted acidic sites. Throughout the activity test, the hierarchical ZnO/ZSM-5 catalysts showed an outstanding performance within 5 h on stream with the average aromatic (benzene, toluene, and xylenes) selectivity trend, represented by their NaOH concentrations 0.3 M > 0.4 M > 0.2 M > 0.1 M corresponding to 61.0, 53.5, 40.3, and 36.8%, respectively. Their average propane conversions within the same period followed a consecutive trend 0.1 M > 0.2 M > 0.3 M > 0.4 M conforming to 34.1, 24.8, 17.3, and 10.2%, respectively. These were compared with that of the reference (ZnO/ZSM-5), which exhibited an average aromatic selectivity of 25.2% and propane conversion of 39.7%. Furthermore, the hierarchical catalyst generally displayed a low amount of C9+ heavier aromatics with the ZnO/ZSM-5(0.3 M) catalyst having the lowest C9+ selectivity of 23.7% compared to the reference catalyst with 72.7% at the same time on stream.
Light alkane aromatization for aromatic compound production, used in petrochemical industries is an attractive area of research. The effect of second metal co-impregnation was investigated in stabilizing zinc on ZSM-5 in aromatization of propane. HZSM-5 was modified with zinc and iron metal by co wet-impregnation and characterized using XRF, XRD, BET, N2-adsorption, FTIR, FTIR-Pyridine, SEM, TEM, H2-TPR and XPS. The effect of different loadings of Iron on Zn/ZSM-5 was investigated on acidity, aromatic yield, product distribution and aromatization performance. Performance test was conducted in a fixed bed reactor at 540 °C, one atmosphere. GHSV of 1200 mL/g-h. Co-impregnation of Zn with Fe improved the catalytic activity and aromatic yield for 10 h time on stream as compared to parent HZSM-5 and Zn/ZSM-5 of very low aromatic yield and propane conversion. Impregnation of Zn as the dehydrogenating metal on HZSM-5 steadily increased aromatic yield from 5% on HZSM-5 to 25% and was steadily dropped to 20% after 10 h TOS. The co-impregnation of iron of 1–3 wt% loading as the second metal for zinc stability with 2 wt% Zn on ZSM-5 improved propane conversion and aromatic yield to 55% for the 10 h TOS. This further enhanced aromatic product distribution and minimized light gases.
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