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Engineering In-Co3O4/H-SSZ-39(OA) Catalyst for CH4-SCR of NOx: Mild Oxalic Acid (OA) Leaching and Co3O4 Modification

Guanyu Chen,Weixin Zhang,Rongshu Zhu,Yanpeng Chen,Minghu Zhao,Mei Hong

Zeolite-based catalysts efficiently catalyze the selective catalytic reduction of NOxwith methane (CH4-SCR) for the environmentally friendly removal of nitrogen oxides, but suffer severe deactivation in high-temperature SO2- and H2O-containing flue gas. In this work, SSZ-39 zeolite (AEI topology) with high hydrothermal stability is reported for preparing CH4-SCR catalysts. Mild acid leaching with oxalic acid (OA) not only modulates the Si/Al ratio of commercial SSZ-39 to a suitable value, but also removes some extra-framework Al atoms, introducing a small number of mesopores into the zeolite that alleviate diffusion limitation. Additional Co3O4modification during indium exchange further enhances the catalytic activity of the resulting In-Co3O4/H-SSZ-39(OA). The optimized sample exhibits remarkable performance in CH4-SCR under a gas hourly space velocity (GHSV) of 24,000 h−1and in the presence of 5 vol% H2O. Even under harsh SO2- and H2O-containing high-temperature conditions, it shows satisfactory stability. Catalysts containing Co3O4components demonstrate much higher CH4conversion. The strong mutual interaction between Co3O4and Brønsted acid sites, confirmed by the temperature-programmed desorption of NO (NO-TPD), enables more stable NxOyspecies to be retained in In-Co3O4/H-SSZ-39(OA) to supply further reactions at high temperatures.