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Issue 4, 2011
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Gold catalysis at the gas–solid interface: role of the support in determining activity and selectivity in the hydrogenation of m-dinitrobenzene

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Abstract

The catalytic gas phase hydrogenation of m-dinitrobenzene (1 atm, 423 K) over laboratory synthesised (1 mol%) Au supported on Al2O3, TiO2, Fe2O3 and CeO2 and a reference Au/TiO2 (World Gold Council) has been investigated. The catalysts were prepared by deposition-precipitation (DP) and impregnation (IMP), where the former route generated smaller (surface area weighted) mean Au particle sizes (1.5–2.8 nm) compared with the IMP synthesis (3.5–9.0 nm). The catalysts have been characterized in terms of temperature programmed reduction (TPR), H2 chemisorption/temperature programmed desorption (TPD), BET area, powder X-ray diffraction (XRD) and high resolution transmission electron microscopy (HRTEM) analyses. Hydrogen consumption over the T range 371–457 K during activation of Au on TiO2, Al2O3 and CeO2 can be associated with Au3+ → Au0 reduction. XRD analysis demonstrated the presence of metallic gold in Au/Fe2O3pre-TPR. A partial and complete reduction of the hematite support to magnetite (Fe2O3 → Fe3O4) was observed post-TPR to 423 and 673 K, respectively; H2-TPD results suggest the participation of spillover hydrogen in this step. Exclusive –NO2group reduction and time invariant conversions were observed for all the catalysts considered in this study. An increase in the specific hydrogenation rate with a decrease in the mean Au size (from 9 to 3 nm) was observed. m-Nitroaniline was generated as the sole product over Au/TiO2 and Au/Fe2O3 whereas Au/CeO2 promoted the exclusive formation of m-phenylenediamine and a mixture of both products was obtained over Au/Al2O3. Our findings establish a basis for the development of a sustainable (clean and continuous) process for the hydrogenation of m-dinitrobenzene where product composition can be controlled through the choice of the oxide support.

Graphical abstract: Gold catalysis at the gas–solid interface: role of the support in determining activity and selectivity in the hydrogenation of m-dinitrobenzene

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Article information


Submitted
11 Feb 2011
Accepted
03 Apr 2011
First published
05 May 2011

Catal. Sci. Technol., 2011,1, 652-661
Article type
Paper

Gold catalysis at the gas–solid interface: role of the support in determining activity and selectivity in the hydrogenation of m-dinitrobenzene

F. Cárdenas-Lizana, S. Gómez-Quero, N. Perret and M. A. Keane, Catal. Sci. Technol., 2011, 1, 652
DOI: 10.1039/C1CY00051A

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