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, 61 (3), 144-153

Solvent Free Synthesis of PdZn/TiO 2 Catalysts for the Hydrogenation of CO 2 to Methanol

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Solvent Free Synthesis of PdZn/TiO 2 Catalysts for the Hydrogenation of CO 2 to Methanol

Hasliza Bahruji et al. Top Catal.

Abstract

Catalytic upgrading of CO2 to value-added chemicals is an important challenge within the chemical sciences. Of particular interest are catalysts which are both active and selective for the hydrogenation of CO2 to methanol. PdZn alloy nanoparticles supported on TiO2 via a solvent-free chemical vapour impregnation method are shown to be effective for this reaction. This synthesis technique is shown to minimise surface contaminants, which are detrimental to catalyst activity. The effect of reductive heat treatments on both structural properties of PdZn/TiO2 catalysts and rates of catalytic CO2 hydrogenation are investigated. PdZn nanoparticles formed upon reduction showed high stability towards particle sintering at high reduction temperature with average diameter of 3-6 nm to give 1710 mmol kg-1 h of methanol. Reductive treatment at high temperature results in the formation of ZnTiO3 as well as PdZn, and gives the highest methanol yield.

Keywords: CO2 hydrogenation; Green methanol; Hydrogen storage; Methanol; PdZn alloy.

Figures

Fig. 1
Fig. 1
XRD of P25 and PdZn/TiO2 catalyst after hydrogen reduction at 400, 550 and 650 °C
Fig. 2
Fig. 2
XRD analysis of 7 and 10 wt% PdZn/TiO2 catalysts; and catalysts prepared via sequential CVI, 2Pd–1Zn–TiO2 and 2Zn–1Pd–TiO2 after hydrogen reduction at 400 °C
Fig. 3
Fig. 3
Pd 3d, Zn LMM Auger electron and O 1s XPS analysis of 5% PdZn/TiO2 following a calcination at 500 °C and subsequent reduction in H2 at b 400 °C and c 650 °C
Fig. 4
Fig. 4
Pd 3d, XPS analysis of a 7% PdZn/TiO2 and 10% PdZn/TiO2 following reduction in H2 at 400 °C and b catalysts prepared via sequential CVI, 2Pd–1Zn–TiO2 and 2Zn–1Pd–TiO2 after hydrogen reduction at 400 °C
Fig. 5
Fig. 5
CO DRIFTS spectra of 5% PdZn/TiO2 following reduction at 150 and 250 °C
Fig. 6
Fig. 6
TEM images and particle size distribution histograms for 5% PdZn/TiO2 following; a calcination at 500 °C and subsequent reduction in H2 at b 400 °C, c 550 °C and d 650 °C. e A HR-TEM image of PdZn nanoparticles in 5% PdZn/TiO2 following reduction at 400 °C, showing a d-spacing calculation
Fig. 7
Fig. 7
TEM images and particle size distribution of 7% PdZn/TiO2 and 10% PdZn/TiO2 after reduction at 400 °C

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