Abstract
Abstract Metal-incorporated SAPO-34 catalysts were prepared by one-step hydrothermal method. Effects of various parameters including the types of metal ions, Cu2+ sources, structure directing agents (SDAs), hydrothermal temperature and time on catalyst activity of the metal-incorporated SAPO-34 catalysts were investigated. Three types of metal-incorporated SAPO-34 catalysts (Cu/SAPO-34, Fe/SAPO-34 and Mn/SAPO-34) were successfully obtained. Compared with Fe/SAPO-34 and Mn/SAPO-34 catalysts, Cu/SAPO-34 catalyst revealed complete cubic-like microstructure, wide active temperature window and high conversion rate in selective catalytic reduction (SCR) of nitric oxide. After defined Cu2+ was the favorable active site of SAPO-34 catalyst, the effects of four Cu2+ sources on SCR performance were further investigated, and found Cu2+ sources did not produce significant influence on nitric oxide conversion rates. SDAs determined the formation of Cu/SAPO-34 catalyst, and the Cu/SAPO-34 catalyst adopting tetraethylenepentamine (TEPA) as SDA could maintain higher crystal integrity and active sites, which were in favor of the SCR reaction. Moreover, hydrothermal temperature and time had great influences on the formation of Cu/SAPO-34 catalyst. When the hydrothermal temperature was higher than 150 oC and the hydrothermal time was longer than 3 days, the Cu/SAPO-34 catalyst with a cubic-like structure and high catalyst activity could be obtained.
Highlights
Nitrogen oxides (NOx), as one of the major atmospheric pollutants, are mainly generated in the combustion of fossil fuels and biofuels, which have given rise to serious environmental problems including greenhouse effect, ozone depletion, acid rain[1,2,3,4,5]
Inspired from previous researches, here, we fabricated metal-incorporated SAPO-34 catalysts by one-step hydrothermal synthesis, investigated the effects of various parameters including the types of metal ions, copper ion sources, structure directing agents (SDAs), hydrothermal temperature and time on catalyst activity of metal-incorporated SAPO-34 catalysts, characterized the morphology, structure, and chemical composition of metal-incorporated SAPO-34 catalysts by scanning electron microscope (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and N2 adsorption techniques
After defined copper ions were the favorable active site of SAPO-34 catalyst, we further investigated the relationship between different Cu2+ sources (Cu(COOH)[2], CuSO4, CuCl2, Cu(NO3)[2], and) and selective catalytic reduction (SCR) performance
Summary
Nitrogen oxides (NOx), as one of the major atmospheric pollutants, are mainly generated in the combustion of fossil fuels and biofuels, which have given rise to serious environmental problems including greenhouse effect, ozone depletion, acid rain[1,2,3,4,5]. Wang et al.[26] adopted ion-exchange method to fabricate Cu/ SAPO-34 catalysts, which demonstrated Cu species existing as isolated ions were active sites for the SCR reaction. Liu et al.[27] reported their work on Cu/ SAPO-34 catalysts obtained by ion-exchange method They believed that the migration of surface CuO clusters into the ion-exchanged sites as isolated Cu2+ improved the activity at high temperatures, which suppressed the competitive oxidation of NH3. Inspired from previous researches, here, we fabricated metal-incorporated SAPO-34 catalysts by one-step hydrothermal synthesis, investigated the effects of various parameters including the types of metal ions, copper ion sources, SDAs, hydrothermal temperature and time on catalyst activity of metal-incorporated SAPO-34 catalysts, characterized the morphology, structure, and chemical composition of metal-incorporated SAPO-34 catalysts by SEM, XRD, XPS and N2 adsorption techniques
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