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Ag-Cu based catalysts for the selective ammonia oxidation into nitrogen and water vapour

DOI: 10.1016/j.apcatb.2018.03.029 DOI Help

Authors: Magdalena Jablonska (RWTH Aachen University) , Andrew Beale (University College London; Research Complex at Harwell) , Marek Nocun (AGH University of Science and Technology) , Regina Palkovits (RWTH Aachen University)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Applied Catalysis B: Environmental

State: Published (Approved)
Published: March 2018
Diamond Proposal Number(s): 14834

Abstract: XRD, BET, H2-TPR, UV-vis-DRS, XPS and XAFS were used to characterize a series of Ag and/or Cu – Ag (1-5%), Cu (10-15%) or Ag-Cu (1-1, 1-10, 1.5-10, 5-5% of metal) – supported on γ-Al2O3. Correlation between physicochemical properties, catalytic activity and selectivity in NH3-SCO were thoroughly investigated. Silver species mainly in the form of Ag2O on the Ag/Al2O3 catalysts led to enhanced activity together with drop in N2 selectivity with increasing silver loading up to 5%. A mixture of CuO and CuAl2O4 formed on the Cu/Al2O3 catalysts. Easily reducible highly dispersed CuOx promoted the activity of the catalysts, while bulk CuOx and CuAl2O4 decreased N2 selectivity up to 500 °C. The activity of all Cu-containing materials was inferior to Ag-containing ones. Thus, the gap between the high conversion temperature over Cu/Al2O3 and low N2 selectivity over Ag/Al2O3 was bridged by applying the Ag-Cu/Al2O3 catalysts, with the optimum loading of 1.5 and 10 wt.% for silver and copper, respectively. NH3-TPD, NH3-TPSR and in situ FTIR were used to determine the in situ selective catalytic reduction (i-SCR) mechanism over 1.5% Ag/Al2O3, 10% Cu/Al2O3 and 1.5% Ag-10% Cu/Al2O3 respectively. The i-SCR mechanism involved the partial oxidation of NH3 into NOx species, along with adsorbed NOx species interacting with adsorbed ammonia (NHx species) and being reduced to reaction products.

Journal Keywords: Alumina; Silver oxide species; Copper oxide species; Selective ammonia oxidation; Reaction mechanism

Subject Areas: Chemistry

Instruments: B18-Core EXAFS

Other Facilities: ESRF

Added On: 14/03/2018 08:56

Discipline Tags:

Physical Chemistry Catalysis Chemistry

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS)