4.8 Article

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

期刊

APPLIED CATALYSIS B-ENVIRONMENTAL
卷 232, 期 -, 页码 275-287

出版社

ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcatb.2018.03.029

关键词

Alumina; Silver oxide species; Copper oxide species; Selective ammonia oxidation; Reaction mechanism

资金

  1. Excellence Initiative of the German federal government in the frame of the Center for Automotive Catalytic Systems Aachen (ACA) at RWTH Aachen University
  2. Excellence Initiative of the German state government in the frame of the Center for Automotive Catalytic Systems Aachen (ACA) at RWTH Aachen University
  3. EPSRC (UK)

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XRD, BET, H-2-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 gamma-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 N-2 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 N-2 selectivity up to 500 degrees 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 N-2 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.

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