Abstract
Direct decomposition of NO into N2 and O2 is an ideal technology for NOx removal. Catalyst deactivation by sulfur poisoning is the major obstacle for practical application. This paper focuses on strengthening the SO2 resistance of metal-exchanged HZSM-5 catalysts, by investigating the metals, promoters, preparation methods, metal-to-promoter molar ratios, Si/Al ratios and metal loadings. The results show that in the presence of SO2 (500 ppm), Fe is the best compared with Co, Ni and Cu. Cs, Ba and K modification enhanced the low-temperature activity of the Fe-HZSM-5 catalyst for NO decomposition, which can be further improved by increasing the exchanged-solution concentration and Fe/Cs molar ratio or decreasing the Si/Al molar ratio. Interestingly, Cs-doped Fe-HZSM-5 exhibited a high NO conversion and low NO2 selectivity but a high SO2 conversion within 10 h of continuous operation. This indicates that Cs-Fe-HZSM-5 has a relatively high SO2 resistance. Combining the characterization results, including N2 physisorption, XRD, ICP, XRF, UV–Vis, XPS, NO/SO2-TPD, H2-TPR and HAADF-STEM, SO42− was found to be the major sulfur species deposited on the catalyst’s surface. Cs doping inhibited the SO2 adsorption on Fe-HZSM-5, enhanced the Fe dispersion and increased the isolated Fe and Fe-O-Fe species. These findings could be the primary reasons for the high activity and SO2 resistance of Cs-Fe-HZSM-5.
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