Assessing the surface modifications following the mechanochemical preparation of a Ag/Al2O3 selective catalytic reduction catalyst

Kathryn Ralphs*, Carmine D'Agostino, Robbie Burch, Sarayute Chansai, Lynn F. Gladden, C. Hardacre, Stuart L. James, Jonathan Mitchell, Sarah F. R. Taylor

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

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Abstract

The surface modification of a mechanochemically prepared Ag/Al O catalyst compared with catalysts prepared by standard wet impregnated methods has been probed using two-dimensional T -T NMR correlations, HO temperature programmed desorption (TPD) and DRIFTS. The catalysts were examined for the selective catalytic reduction of NO using n-octane in the presence and absence of H. Higher activities were observed for the ball milled catalysts irrespective of whether H was added. This higher activity is thought to be related to the increased affinity of the catalyst surface towards the hydrocarbon relative to water, following mechanochemical preparation, resulting in higher concentrations of the hydrocarbon and lower concentrations of water at the surface. DRIFTS experiments demonstrated that surface isocyanate was formed significantly quicker and had a higher surface concentration in the case of the ball milled catalyst which has been correlated with the stronger interaction of the n-octane with the surface. This increased interaction may also be the cause of the reduced activation barrier measured for this catalyst compared with the wet impregnated system. The decreased interaction of water with the surface on ball milling is thought to reduce the effect of site blocking whilst still providing a sufficiently high surface concentration of water to enable effective hydrolysis of the isocyanate to form ammonia and, thereafter, N. This journal is © The Royal Society of Chemistry.
Original languageEnglish
Pages (from-to)531-539
Number of pages9
JournalCatalysis, Science & technology
Volume4
Issue number2
Early online date03 Dec 2013
DOIs
Publication statusPublished - 01 Feb 2014

Keywords

  • SILVER-ALUMINA CATALYSTS
  • LEAN-BURN CONDITIONS
  • HIGHER HYDROCARBONS
  • GOLD CLUSTERS
  • NOX REDUCTION
  • SILVER/ALUMINA CATALYST
  • MECHANISTIC ASPECTS
  • AEROBIC OXIDATION
  • LOW-TEMPERATURES
  • NMR RELAXATION

ASJC Scopus subject areas

  • Catalysis

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