Abstract:
In response to the challenges associated with the synergistic removal of nitrogen oxides (NO
x) and chlorinated aromatic compounds from flue gases generated during steel sintering, waste incineration, and other processes, as well as the issues with existing commercial catalysts, such as a relatively high active temperature window and the tendency to produce highly toxic by-products, a study was conducted on the low-temperature synergistic removal performance of composite metal oxide catalysts, using chlorobenzene (CB) as a surrogate for chlorinated aromatic compounds. The research focused on a CeMnNb ternary composite metal oxide catalyst. Catalyst samples with varying Ce/Nb molar ratios were prepared via the co-precipitation method. The effects of operating parameters, including reaction temperature, ammonia-nitrogen ratio (NSR), O
2 volume fraction, and space velocity, were investigated using a fixed-bed activity testing system. Additionally, X-ray photoelectron spectroscopy (XPS) characterization was employed to explore the structural evolution and sulfur/water resistance mechanisms of the catalyst in the presence of H
2O and SO
2. Results demonstrate that under the optimized condition (a reaction temperature of 280 ℃, volume fractions of NH
3, NO, CB and O
2 of 600×10
-6, 600×10
-6, 300×10
-6, and 8%, respectively, and a space velocity of 60 000 h
-1), the CeMnNb catalyst with a Ce/Mn/Nb molar ratio of 1∶1∶2 can achieve a CB removal efficiency of 97.2% and a NO
x conversion efficiency of 88.3%. Both H
2O and SO
2 are found to inhibit the synergistic removal performance of the catalyst, with a more pronounced inhibitory effect observed when they coexist. Notably, the poisoning effect of SO
2 is irreversible. XPS characterization results reveal that the relative content of Mn
4+ in the catalyst decreases significantly under all three reaction conditions. In the presence of H
2O, Cl formes Mn-Cl bonds with low-valent Mn species. When SO
2 is present, the relative content of surface organic chlorine increases. However, when H
2O and SO
2 coexist, sulfates are readily formed, which is conductive to reduce the deposition of chlorinated compounds.