CeO2–TiO2composite supports with different Ce/Ti molar ratios were prepared by a homogeneous precipitation method, and V2O5–WO3/CeO2–TiO2catalysts for the selective catalytic reduction(SCR) of NOx with NH3 were prepared by an incipient-wetness impregnation method. These catalysts were characterized by means of BET, XRD, UV–Vis,Raman and XPS techniques. The results showed that the catalytic activity of V2O5–WO3/TiO2 was greatly enhanced by Ce doping(molar ratio of Ce/Ti = 1/10) in the TiO2 support.The catalysts that were predominantly anatase TiO2 showed better catalytic performance than the catalysts that were predominantly fluorite CeO2. The Ce additive could enhance the surface adsorbed oxygen and accelerate the SCR reaction. The effects of O2 concentration, ratio of NH3/NO, space velocity and SO2 on the catalytic activity were also investigated. The presence of oxygen played an important role in NO reduction. The optimal ratio of NH3/NO was 1/1 and the catalyst had good resistance to SO2 poisoning.
Kai ChengJian LiuTao ZhangJianmei LiZhen ZhaoYuechang WeiGuiyuan JiangAijun Duan
A series of LaxKl xCoO3 nanorod oxides with perovskite structure were synthesized by sol-gel method using polyvinyl al- cohol (PVA) as additive. These perovskite-type complex oxide catalysts were characterized by the techniques of X-ray diffraction (XRD), infrared (IR), Brumauer-Emmett-Teller (BET) and scanning electron microscopy (SEM). And the results showed that nano- rods of La1-xKxCoO3 perovskite-type complex oxides were fabricated by sol-gel method when the mass concentration of PVA was 4% and the calcined temperature kept at 700 ℃ for 4 h. The catalytic results of CO oxidation showed that the LaxK1-xoO3 catalysts had high activity. LaCoO3 nanorods exposed more {110} plane than LaCoO3 nanoparticles, which was beneficial to the catalytic oxi- dation of CO. LaCoO3 nanorods had the best catalytic performance for the oxidation of CO. At 200 ℃, the CO conversion could reach 100%.
A series of meso-microporous Cu-SAPO-34 catalysts were successfully synthesized by a one-pot hydrothermal crystallization method, and these catalysts exhibited excellent NH3-SCR performance at low temperature. Their structure and physic chemical properties were characterized by means of X-ray diffraction patterns (XRD), Scanning electron microscopy (SEM), Transmission electron microscopy (TEM), N2 sorption-desorption, nuclear magnetic resonance (NMR), Inductively Coupled Plasma-Atomic Emission spectrometer (ICP-AES), X-ray absorption spectroscopy (XPS), Temperature-programmed desorption of ammonia (NH3-TPD), Ultraviolet visible diffuse reflectance spectroscopy (UV-Vis DRS) and Temperature programmed reduction (TPR). The analysis results indicate that the high activities of Cu-SAPO-34 catalysts could be attributed to the enhancement of redox property, the formation of mesopores and the more acid sites. Furthermore, the kinetic results verify that the formation of mesopores remarkably reduces diffusion resistance and then improves the accessibility of reactants to catalytically active sites. The 1.0-Cu-SAPO-34 catalyst exhibited the high NO conversion (〉90%) among the wide activity temperature window in the range of 150- 425℃.
Jixing LiuFuhong YuJian LiuLifeng CuiZhen ZhaoYuechang WeiQianyao Sun
A series of meso‐microporous copper‐supporting chabazite molecular sieve(CuSAPO‐34) catalysts with excellent performance in low‐temperature ammonia selective catalytic reduction(NH3‐SCR)have been synthesized via a one‐pot hydrothermal crystallization method. The physicochemical properties of the catalysts were characterized by scanning electron microscopy, transmission electron microscopy, N2 adsorption‐desorption measurements, X‐ray diffraction, 27 Al magic angle spinning nuclear magnetic resonance, diffuse reflectance ultraviolet‐visible spectroscopy, inductively coupled plasma‐atomic emission spectroscopy, X‐ray photoelectron spectroscopy, temperature‐programmed reduction measurements, and electron paramagnetic resonance analysis. The formation of micro‐mesopores in the Cu‐SAPO‐34 catalysts decreases diffusion resistance and greatly improves the accessibility of reactants to catalytic active sites. The main active sites for NH3‐SCR reaction are the isolated Cu^2+ species displaced into the ellipsoidal cavity of the Cu‐SAPO‐34 catalysts.
Selective catalytic reduction technology using NH3 as a reducing agent(NH3-SCR) is an effective control method to remove nitrogen oxides. TiO2-supported vanadium oxide catalysts with different levels of Ce and Sb modification were prepared by an impregnation method and were characterized by X-ray diffractometer(XRD), Brunauer-Emmett-Teller(BET), Transmission electron microscopy(TEM), Fourier transform infrared spectroscopy(FT-IR), UV-Vis diffuse reflectance spectroscopy(UV-Vis DRS), Raman and Hydrogen temperature-programmed reduction(H2-TPR). The catalytic activities of V5 CexS by/TiO2 catalysts for denitration were investigated in a fixed bed flow microreactor. The results showed that cerium, vanadium and antimony oxide as the active components were well dispersed on TiO2, and the catalysts exhibited a large number of d-d electronic transitions, which were helpful to strengthen SCR reactivity. The V5 CexS by/TiO2 catalysts exhibited a good low temperature NH3-SCR catalytic activity. In the temperature range of 210 to 400℃, the V5 CexS by/TiO2 catalysts gave NO conversion rates above 90%. For the best V5Ce35Sb2/TiO2 catalyst, at a reaction temperature of 210℃, the NO conversion rate had already reached 90%. The catalysts had different catalytic activity with different Ce loadings. With the increase of Ce loading, the NO conversion rate also increased.
Chi XuJian LiuZhen ZhaoFei YuKai ChengYuechang WeiAijun DuanGuiyuan Jiang
SBA-15 supported Mo catalysts (Moy/SBA-15) were prepared by an ultrasonic assisted incipient-wetness impregnation method. The physical and chemical properties of the catalysts were characterized by means of N2-adsorption-desorption, XRD, TEM, UV-Vis, Raman, XANES and H2-TPR. The results showed that a trace amount of MoO3 was produced on high Mo content samples. Tum-over frequency (TOF) and product selectivity are dependent on the molybdenum content. Both Mo0.75/SBA-15 and Mo1.75/SBA-15 catalysts give the higher catalytic activity and the selectivity to the total aldehydes for the selective oxidation of C2H6. At the reaction temperature of 625℃, the maximum yield of aldehydes reached 4.2% over Mo0.75/SBA-15 catalyst. The improvement of the activity and selectivity was related with the state of MoOx species.