MnOx supported on hierarchical SAPO-34 for the low-temperature selective catalytic reduction of NO with nh3: Catalytic activity and SO2 resistance

Abstract

The ethanol dispersion method was employed to synthesize a series of MnOx/SAPO-34 catalysts using SAPO-34 with the hierarchical pore structure as the zeolite carrier, which were prepared by facile acid treatment with citric acid. Physicochemical properties of catalysts were characterized by XRD, XPS, BET, TEM, NH3-TPD, SEM, FT-IR, Py-IR, H2-TRP and TG/DTG. NH3-SCR performances of the hierarchical MnOx/SAPO-34 catalysts were evaluated at low temperatures. Results show that citric acid etching solution at a concentration of 0.1 mol/L yielded a hierarchical MnOx/SAPO-34-0.1 catalyst with ca.15 wt.% Mn loading, exhibiting optimal catalytic activity and SO2 tolerance at low temperatures. Almost 100% NO conversion and over 90% N2 selectivity at 120°C under a gas hourly space velocity (GHSV) of 40,000 h-1 could be obtained over this sample. Furthermore, the NO conversion was still higher than 65% when 100 ppm SO2 was introduced to the reaction gas for 4 h. These could be primarily attributed to the large specific surface area, high surface acidity concentration and abundant chemisorbed oxygen species provided by the hierarchical pore structure, which could also increase the mass transfer of the reaction gas. This finding suggests that the NH3-SCR activity and SO2 poisoning tolerance of hierarchical MnOx/SAPO-34 catalysts at low temperatures can be improved by controlling the morphology of the catalysts, which might supply a rational strategy for the design and synthesis of Mn-based SCR catalysts.