Novel MnaZrbCrcOx catalysts for low temperature NH3-SCR derived from high H2O content flue gas via natural gas combustion
A series of Mn a Zr b Cr c O x catalysts with different Cr/Mn molar ratios were synthesized via co-precipitation for the selective catalytic reduction of NO x with NH 3 (NH 3 -SCR). It was found that a Mn 5 Zr 2 Cr 2.5 O x catalyst with a Mn:Zr:Cr ratio of 5:2:2.5 exhibited excellent low-temperature activity and the best levels of H 2 O resistance at a high weight hourly space velocity (WHSV) of 54,000 ml/(h·g). NO conversion levels were measured as greater than 87% within a temperature range of 150–250 °C, and catalytic performance levels reached 90% even 50 h after reactions occurred in the presence of 15% H 2 O at 230 °C. The characterization results show that strong interactions occurring between Mn, Zr and Cr oxides and higher quantities of Mn 4+ and Lewis acid sites improved the redox properties and facilitated H 2 O resistance. In situ diffuse reflectance infrared Fourier transform spectra ( in situ DRIFTS) show that coordinated NH 3 on Lewis acid sites and bidentate nitrates play important roles in SCR reactions and that such reactions follow both Langmuir-Hinshelwood (L-H) and Eley-Rideal (E-R) mechanisms. The competitive adsorption of H 2 O and NO may be the main cause of the adverse effects of H 2 O on catalytic performance.
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