Tunable gas phase hydrogenation of m-dinitrobenzene over alumina supported Au and Au-Ni

Fernando Cárdenas-Lizana, Santiago Gómez-Quero, Christopher J. Baddeley, Mark A. Keane

Research output: Contribution to journalArticle

48 Citations (Scopus)

Abstract

The gas phase hydrogenation of m-dinitrobenzene (m-DNB) has been investigated over alumina supported Au (1 mol%), Ni (10 mol%) and Au-Ni (Au/Ni mol ratio = 1/10). Au/Al2O3 delivered a time invariant exclusive formation of m-nitroaniline (partial reduction), Ni/Al 2O3 promoted total nitro-group reduction to give m-phenylenediamine as the sole product and Au-Ni/Al2O3 generated both products (partial and complete hydrogenation); Ni/Al 2O3 and Au-Ni/Al2O3 exhibited a temporal decline in activity. A physical mixture of Au/Al2O 3 + Ni/Al2O3 delivered a hydrogenation rate and product composition that was equivalent to that obtained with Ni/Al 2O3, i.e. Au/Al2O3 had a negligible contribution to the catalytic process, which was governed by the Ni component in the mixture. The catalysts have been characterized in terms of temperature-programmed reduction (TPR), H2 chemisorption/temperature- programmed desorption (TPD), BET area/pore volume, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), diffuse reflectance UV-vis (DRS UV-vis) and HRTEM-EDX measurements. The presence of zero valent Au and Ni is established post-TPR where EDX mapping has revealed a close surface proximity of both metals (mean particle size = 9 nm) in Au-Ni/Al2O3 with evidence (from XPS) of electron donation from Ni to Au. While the addition of Au to Ni/Al2O3 served to suppress H2 chemisorption post-TPR, H2-TPD revealed a more facile release of a greater amount of hydrogen from Au-Ni/Al2O3 relative to Ni/Al2O3, which we attribute to surface Au-Ni interaction that is also manifest in the hydrogenation activity/selectivity response. Our results establish the feasibility of controlling product distribution through the application of mono- (Au or Ni) and bimetallic (Au-Ni) catalysts. © 2010 Elsevier B.V. All rights reserved.

Original languageEnglish
Pages (from-to)155-165
Number of pages11
JournalApplied Catalysis A: General
Volume387
Issue number1-2
DOIs
Publication statusPublished - 20 Oct 2010

Keywords

  • Au-Ni/Al 2 O 3
  • Au/Al 2 O 3
  • m-Dinitrobenzene
  • Ni/Al 2 O 3
  • Reductive deposition of Au on Ni
  • Selective hydrogenation

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