A series of Fe‐Mn/Al2O3 catalysts were prepared and studied for low temperature selective catalytic reduction （SCR） of NO with NH3 in a fixed‐bed reactor. The effects of Fe and Mn on NO conversion and the deactiva...A series of Fe‐Mn/Al2O3 catalysts were prepared and studied for low temperature selective catalytic reduction （SCR） of NO with NH3 in a fixed‐bed reactor. The effects of Fe and Mn on NO conversion and the deactivation of the catalysts were studied. N2 adsorption‐desorption, X‐ray diffraction, transmission electron microscopy, energy dispersive spectroscopy, H2 temperature‐programmed reduction, NH3 temperature‐programmed desorption, X‐ray photoelectron spectroscopy （XPS）, thermal gravimetric analysis and Fourier transform infrared spectroscopy were used to character‐ize the catalysts. The 8Fe‐8Mn/Al2O3 catalyst gave 99%of NO conversion at 150？？ and more than 92.6%NO conversion was obtained in a wide low temperature range of 90–210？？. XPS analysis demonstrated that the Fe3＋was the main iron valence state on the catalyst surface and the addition of Mn increased the accumulation of Fe on the surface. The higher specific surface area, enhanced dispersion of amorphous Fe and Mn, improved reduction properties and surface acidity, lower binding energy, higher Mn4＋/Mn3＋ratio and more adsorbed oxygen species resulted in higher NO conversion for the 8Fe‐8Mn/Al2O3 catalyst. In addition, the SCR activity of the 8Fe‐8Mn/Al2O3 cata‐lyst was only slightly decreased in the presence of H2O and SO2, which indicated that the catalyst had better tolerance to H2O and SO2. The reaction temperature was crucial for the SO2 resistance of catalyst and the decrease of catalytic activity caused by SO2 was mainly due to the sulfate salts formed on the catalyst.展开更多
Transition metal catalysts M-N-C（M = Co,Fe,Mn） were synthesized by a template-free method by heating meso-tetraphenyl porphyrins（i.e.CoTPP,FeTPPCl,MnTPPCl） precursors.The catalysts were characterized by N2 adsorpt...Transition metal catalysts M-N-C（M = Co,Fe,Mn） were synthesized by a template-free method by heating meso-tetraphenyl porphyrins（i.e.CoTPP,FeTPPCl,MnTPPCl） precursors.The catalysts were characterized by N2 adsorption-desorption,thermogravimetry,high-resolution transmission electron microscopy,and Raman and X-ray photoelectron spectroscopy.The selective oxidation of ethylbenzene with molecular oxygen under a solvent-free condition was carried out to explore the catalytic performance of the M-N-Cs,which exhibited different catalytic performance.That was ascribed to the difference in M（Co,Fe,Mn） and different graphitization degree forming during the heating process,in which M（Co,Fe,Mn） might have different catalytic activity on the formation of the M-N-C catalyst.All the M-N-C composites had remarkable recyclability in the selective oxidation of ethylbenzene.展开更多
基金supported by the National High Technology Research and Development Program of China (863 Program,2015AA03A401)the National Natural Science Foundation of China (51276039)+1 种基金the Fundamental Research Funds for the Central Universities (020514380020,020514380030)the Postdoctoral Science Foundation of Jiangsu Province,China (1501033A)~~
文摘A series of Fe‐Mn/Al2O3 catalysts were prepared and studied for low temperature selective catalytic reduction （SCR） of NO with NH3 in a fixed‐bed reactor. The effects of Fe and Mn on NO conversion and the deactivation of the catalysts were studied. N2 adsorption‐desorption, X‐ray diffraction, transmission electron microscopy, energy dispersive spectroscopy, H2 temperature‐programmed reduction, NH3 temperature‐programmed desorption, X‐ray photoelectron spectroscopy （XPS）, thermal gravimetric analysis and Fourier transform infrared spectroscopy were used to character‐ize the catalysts. The 8Fe‐8Mn/Al2O3 catalyst gave 99%of NO conversion at 150？？ and more than 92.6%NO conversion was obtained in a wide low temperature range of 90–210？？. XPS analysis demonstrated that the Fe3＋was the main iron valence state on the catalyst surface and the addition of Mn increased the accumulation of Fe on the surface. The higher specific surface area, enhanced dispersion of amorphous Fe and Mn, improved reduction properties and surface acidity, lower binding energy, higher Mn4＋/Mn3＋ratio and more adsorbed oxygen species resulted in higher NO conversion for the 8Fe‐8Mn/Al2O3 catalyst. In addition, the SCR activity of the 8Fe‐8Mn/Al2O3 cata‐lyst was only slightly decreased in the presence of H2O and SO2, which indicated that the catalyst had better tolerance to H2O and SO2. The reaction temperature was crucial for the SO2 resistance of catalyst and the decrease of catalytic activity caused by SO2 was mainly due to the sulfate salts formed on the catalyst.
基金supported by the National Natural Science Foundation of China (21103045, 1210040, 1103312)State Key Laboratory of Heavy Oil at China University of Petroleum (SKCHOP201504)Key Laboratory of Mineralogy and Metallogeny of the Chinese Academy of Sciences at Guangzhou Institute of Geochemistry(KLMM20150103)~~
文摘Transition metal catalysts M-N-C（M = Co,Fe,Mn） were synthesized by a template-free method by heating meso-tetraphenyl porphyrins（i.e.CoTPP,FeTPPCl,MnTPPCl） precursors.The catalysts were characterized by N2 adsorption-desorption,thermogravimetry,high-resolution transmission electron microscopy,and Raman and X-ray photoelectron spectroscopy.The selective oxidation of ethylbenzene with molecular oxygen under a solvent-free condition was carried out to explore the catalytic performance of the M-N-Cs,which exhibited different catalytic performance.That was ascribed to the difference in M（Co,Fe,Mn） and different graphitization degree forming during the heating process,in which M（Co,Fe,Mn） might have different catalytic activity on the formation of the M-N-C catalyst.All the M-N-C composites had remarkable recyclability in the selective oxidation of ethylbenzene.
