A series of CrOx–CeO2/Ti-PILC(PILC is pillared interlayered clay)catalysts for n-butylamine oxidation were prepared using an impregnation method,and the structures,surface acidity distributions,and redox properties o...A series of CrOx–CeO2/Ti-PILC(PILC is pillared interlayered clay)catalysts for n-butylamine oxidation were prepared using an impregnation method,and the structures,surface acidity distributions,and redox properties of the catalysts were characterized using X-ray diffraction,X-ray photoelectron spectroscopy,transmission electron microscopy,H2temperature-programmed reduction,and NH3temperature-programmed desorption.The results show that addition of an appropriate amount of CeO2enhances the interactions between Cr and Ce,and this increases the acid strength and mobility of active oxygen species on the catalyst.8CrCe(6:1)/Ti-PILC(12,20)exhibits the best catalytic performance and control of NOxin n-butylamine oxidation.展开更多
The catalytic elimination of nitrogen-containing volatile organic compounds(NVOCs)still encounters bottlenecks in NO_(x)formation and low N_(2)selectivity.Here,a series of Cu-promoted Ce-Zr mixed oxide catalysts were ...The catalytic elimination of nitrogen-containing volatile organic compounds(NVOCs)still encounters bottlenecks in NO_(x)formation and low N_(2)selectivity.Here,a series of Cu-promoted Ce-Zr mixed oxide catalysts were synthesized using a simple precipitation approach,and n-butylamine was adopted as the probe pollutant to evaluate their catalytic performance.The Ce Cu_(10%)ZrO_(x)catalyst exhibited the best catalytic activity,with 100%n-butylamine conversion and 90%N_(2)selectivity at 250℃.Concurrently,this sample also displayed good water resistance.A detailed characterization of the catalyst was performed through a series of experimental studies and theoretical calculations.The addition of Cu increased the redox property and promoted the production of oxygen vacancies,all of which were favorable for the greatest nbutylamine selective catalytic oxidation performance.The changes of oxygen vacancies over Ce Cu_(10%)ZrO_(x)in reaction process were studied by in situ Raman spectra.Moreover,in situ diffuse reflectance infrared Fourier transform spectra(DRIFTs)and theoretical calculations were employed to explore the reaction mechanism of n-butylamine selective oxidation.The high activity and selectivity of this catalyst confirm the practical feasibility of the selective oxidation of n-butylamine to CO_(2)and N_(2),and the exploration of the reaction mechanism provides new insights into the further design of catalysts.展开更多
基金supported by the National Natural Science Foundation of China (21177110)
文摘A series of CrOx–CeO2/Ti-PILC(PILC is pillared interlayered clay)catalysts for n-butylamine oxidation were prepared using an impregnation method,and the structures,surface acidity distributions,and redox properties of the catalysts were characterized using X-ray diffraction,X-ray photoelectron spectroscopy,transmission electron microscopy,H2temperature-programmed reduction,and NH3temperature-programmed desorption.The results show that addition of an appropriate amount of CeO2enhances the interactions between Cr and Ce,and this increases the acid strength and mobility of active oxygen species on the catalyst.8CrCe(6:1)/Ti-PILC(12,20)exhibits the best catalytic performance and control of NOxin n-butylamine oxidation.
基金the R&D Program of Beijing Municipal Education Commission(No.KJZD20191443001)Beijing Municipal Science and Technology Commission(No.Z181100000118003)the Fundamental Research Funds for the Central Universities and Doctoral Research Start-up Fund Project of Taiyuan University of Science and Technology(No.20202053)。
文摘The catalytic elimination of nitrogen-containing volatile organic compounds(NVOCs)still encounters bottlenecks in NO_(x)formation and low N_(2)selectivity.Here,a series of Cu-promoted Ce-Zr mixed oxide catalysts were synthesized using a simple precipitation approach,and n-butylamine was adopted as the probe pollutant to evaluate their catalytic performance.The Ce Cu_(10%)ZrO_(x)catalyst exhibited the best catalytic activity,with 100%n-butylamine conversion and 90%N_(2)selectivity at 250℃.Concurrently,this sample also displayed good water resistance.A detailed characterization of the catalyst was performed through a series of experimental studies and theoretical calculations.The addition of Cu increased the redox property and promoted the production of oxygen vacancies,all of which were favorable for the greatest nbutylamine selective catalytic oxidation performance.The changes of oxygen vacancies over Ce Cu_(10%)ZrO_(x)in reaction process were studied by in situ Raman spectra.Moreover,in situ diffuse reflectance infrared Fourier transform spectra(DRIFTs)and theoretical calculations were employed to explore the reaction mechanism of n-butylamine selective oxidation.The high activity and selectivity of this catalyst confirm the practical feasibility of the selective oxidation of n-butylamine to CO_(2)and N_(2),and the exploration of the reaction mechanism provides new insights into the further design of catalysts.