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. 2019 Jan 29;12(3):413.
doi: 10.3390/ma12030413.

Magnetic Fe₂O₃⁻SiO₂⁻MeO₂⁻Pt (Me = Ti, Sn, Ce) as Catalysts for the Selective Hydrogenation of Cinnamaldehyde. Effect of the Nature of the Metal Oxide

Robinson Dinamarca  1 , Rodrigo Espinoza-González  2 , Cristian H Campos  3 , Gina Pecchi  4   5
Affiliations

Magnetic Fe₂O₃⁻SiO₂⁻MeO₂⁻Pt (Me = Ti, Sn, Ce) as Catalysts for the Selective Hydrogenation of Cinnamaldehyde. Effect of the Nature of the Metal Oxide

Robinson Dinamarca et al. Materials (Basel). .

Abstract

The type of metal oxide affects the activity and selectivity of Fe₂O₃⁻SiO₂⁻MeO₂⁻Pt (Me = Ti, Sn, Ce) catalysts on the hydrogenation of cinnamaldehyde. The double shell structure design is thought to protect the magnetic Fe₂O₃ cores, and also act as a platform for depositing a second shell of TiO₂, SnO₂ or CeO₂ metal oxide. To obtain a homogeneous metallic dispersion, the incorporation of 5 wt % of Pt was carried out over Fe₂O₃⁻SiO₂⁻MeO₂ (Me = Ti, Sn, Ce) structures modified with (3-aminopropyl)triethoxysilane by successive impregnation-reduction cycles. The full characterization by HR-TEM, STEM-EDX, XRD, N₂ adsorption isotherm at -196 °C, TPR-H₂ and VSM of the catalysts indicates that homogeneous core-shell structures with controlled nano-sized magnetic cores, multi-shells and metallic Pt were obtained. The nature of the metal oxide affects the Pt nanoparticle sizes where the mean Pt diameter is in the order: ⁻TiO₂⁻Pt > ⁻SnO₂⁻Pt > ⁻CeO₂⁻Pt. Among the catalysts studied, ⁻CeO₂⁻Pt had the best catalytic performance, reaching the maximum of conversion at 240 min. of reaction without producing hydrocinnamaldehyde (HCAL). It also showed a plot volcano type for the production of cinnamic alcohol (COL), with 3-phenyl-1-propanol (HCOL) as a main product. The ⁻SnO₂⁻Pt catalyst showed a poor catalytic performance attributable to the Pt clusters' occlusion in the irregular surface of the ⁻SnO₂. Finally, the ⁻TiO₂⁻Pt catalyst showed a continuous production of COL with a 100% conversion and 65% selectivity at 600 min of reaction.

Keywords: core shell; hydrogenation; nanocatalyst.

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Conflict of interest statement

The authors declare no conflict of interest.

Figures

Scheme 1
Scheme 1
Cinnamaldehyde (CAL) hydrogenation pathways.
Scheme 2
Scheme 2
Fe2O3–SiO2–MeO2–Pt (Me = Sn, Ce, Ti) synthesis pathways.
Figure 1
Figure 1
HR-TEM characterization for the synthetized core-shell materials. (a–c) HR-TEM micrographs and (d–f) STEM-EDX Fe (black), Si (blue), MeO2; Me = Ti, Sn, Ce (green) for the –MeO2 (Me = Ti, Sn, Ce) structures.
Figure 2
Figure 2
HR-TEM characterization for the synthetized Pt catalysts. (a–c) HR-TEM micrographs and (d–f) Pt particle size distribution.
Figure 3
Figure 3
XRD patterns of Pt and non-Pt content of Fe2O3–SiO2–MeO2 (Me = Ti, Sn, Ce) materials.
Figure 4
Figure 4
TPR-H2 profile of Fe2O3–NPs and Fe2O3–SiO2–MeO2–Pt (Me = Ti, Sn, Ce) catalysts.
Figure 5
Figure 5
Magnetic measurements of Fe2O3–SiO2–MeO2 and Fe2O3–SiO2–MeO2–Pt (Me = Ti, Sn, Ce) materials. Inset zoom of the hysteresis loop.
Figure 6
Figure 6
Catalytic evaluation of Fe2O3–SiO2–MeO2–Pt (Me = Ti, Sn, Ce) in CAL Hydrogenation. (a) Conversion curves and (b) Pseudo-first order kinetic model adjustment.
Figure 7
Figure 7
Product distribution during CAL hydrogenation on (a) Fe2O3–SiO2–TiO2–Pt, (b) Fe2O3–SiO2–SnO2–Pt and (c) Fe2O3–SiO2–CeO2–Pt catalysts.
See this image and copyright information in PMC

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