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Carbon dioxide hydrogenation over supported Au nanoparticles: effect of the support

Vourros A., Garagounis Ioannis, Kyriakou Vasileios, Carabineiro, Sónia Alexandra Correia, Maldonado-Hódar, Francisco Jose, Marnellos, Geōrgios E, Konsolakis Michail

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URI: http://purl.tuc.gr/dl/dias/60EEBA1D-B7DB-4BDC-B18A-CDA3F3BF5146
Year 2017
Type of Item Peer-Reviewed Journal Publication
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Bibliographic Citation A. Vourros, I. Garagounis, V. Kyriakou, S.A.C. Carabineiro, F. J. Maldonado-Hódar, G. E. Marnellos and M. Konsolakis, "Carbon dioxide hydrogenation over supported Au nanoparticles: effect of the support," J. CO2 Util., vol. 19, pp. 247-256, May 2017. doi: 10.1016/j.jcou.2017.04.005 https://doi.org/10.1016/j.jcou.2017.04.005
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Summary

The present work aims to explore the impact of the support (MxOy: Al2O3, TiO2, Fe2O3, CeO2, ZnO) on the CO2 hydrogenation activity of supported gold nanoparticles (Au/MxOy) at atmospheric pressure. The textural, redox and surface properties of Au/MxOy catalysts were evaluated by various characterisation methods, namely N2 adsorption-desorption at -196 °C, temperature-programmed reduction in H2, high resolution transmission electron microscopy and X-ray photoelectron spectroscopy. The results revealed a strong influence of the support both on CO2 conversion and on products distribution. Gold nanoparticles supported on ZnO and CeO2 were highly selective towards methanol. TiO2- and Fe2O3-based samples demonstrated high CO2 conversion, leading, however, almost exclusively to CO and/or CH4. Au/Al2O3 was practically inactive in the investigated temperature range (200-350 °C). The following activity order, in terms of methanol formation rate, was obtained: Au/CeO2 > Au/ZnO > Au/Fe2O3 > Au/TiO2 > Au/Al2O3. Au/CeO2 exhibited a methanol formation rate of 4.1 × 10-6 mol s-1 gAu -1 at 250 °C, which is amongst the highest reported at ambient pressure, in spite of the chemical inertness of bare ceria. In view of the characterisation results, the superiority of the Au/CeO2 sample could be mainly ascribed to a synergistic effect linked to the Au-ceria interactions.

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