The catalytic oxidation of toluene over Ag/SBA‐15synthesized under different pretreatment conditions,including O2at500°C(denoted O500),H2at500°C(H500),and O2at500°C followed by H2at300°C(O500‐H30...The catalytic oxidation of toluene over Ag/SBA‐15synthesized under different pretreatment conditions,including O2at500°C(denoted O500),H2at500°C(H500),and O2at500°C followed by H2at300°C(O500‐H300)was studied.The pretreated samples were investigated by N2physisorption,X‐ray diffraction,and ultraviolet‐visible diffuse reflectance.The pretreatment atmosphere greatly influences the status of the Ag and O species,which in turn significantly impacts the adsorption and catalytic removal of toluene.Ag2O and amorphous Ag particles,as well as a large amount of subsurface oxygen species,are formed on O500,and the subsurface oxygen enhances the interaction between Ag species and toluene,so O500shows good activity at higher temperature.However,its activity at lower temperature is not as high as expected,with a reduced presence of Ag2O and lower adsorption capacity for toluene.H2pretreatment at500°C is conducive to the formation of large Ag particles and yields the largest adsorption capacity for toluene,so H500exhibits the best activity at lower temperatures;however,because of poor interaction between Ag and toluene,its activity at higher temperature is modest.The O500‐H300sample exhibits excellent catalytic activity during the whole reaction process,which can be attributed to the small and highly dispersed Ag nanoparticles as well as the existence of subsurface oxygen.展开更多
Silver modified HZSM-5 （AgHZ） zeolite catalysts were prepared by ion exchange method and their catalytic properties in the l-butene cracking reaction were measured. The catalysts were characterized by infrared spec-...Silver modified HZSM-5 （AgHZ） zeolite catalysts were prepared by ion exchange method and their catalytic properties in the l-butene cracking reaction were measured. The catalysts were characterized by infrared spec- troscopy with pyridine adsorption （Py-IR）, N2 adsorption and X-ray diffraction （XRD）. The effects of Ag loading and steaming treatment on catalytic performances were studied. It is found that the activity ofHT_SM-5 （HZ） catalyst significantly decreases with the steaming time, whereas AgHZ catalysts show stable activity in the steaming time of 24-48 h and their activities increase with the Ag loading. When the steaming time is 24-48 h, the yield of propylene over HZ catalyst significantly decreases, whereas it is stable over AgHZ catalysts. The AgHZ catalysts with Ag loadings of 0.28%-0.43% （by mass） show similar propylene yields （-30%）, which are higher than that over the AgHZ catalyst with a Ag loading of 0.55% （by mass）. These results indicate that the steam-treated AgHZ catalysts with optimum Ag loadings have higher yield of propylene and are more stable than the steam- treated HZ catalyst. The regeneration stability measurement in butene cracking also shows that the AgHZ catalyst steam-treated under a suitable condition has better stability than the HZ catalyst.展开更多
基金supported by the National Natural Science Foundation of China(21377016,21577014)Program for Changjiang Scholars and Innovative Research Team in University(IRT_13R05)~~
文摘The catalytic oxidation of toluene over Ag/SBA‐15synthesized under different pretreatment conditions,including O2at500°C(denoted O500),H2at500°C(H500),and O2at500°C followed by H2at300°C(O500‐H300)was studied.The pretreated samples were investigated by N2physisorption,X‐ray diffraction,and ultraviolet‐visible diffuse reflectance.The pretreatment atmosphere greatly influences the status of the Ag and O species,which in turn significantly impacts the adsorption and catalytic removal of toluene.Ag2O and amorphous Ag particles,as well as a large amount of subsurface oxygen species,are formed on O500,and the subsurface oxygen enhances the interaction between Ag species and toluene,so O500shows good activity at higher temperature.However,its activity at lower temperature is not as high as expected,with a reduced presence of Ag2O and lower adsorption capacity for toluene.H2pretreatment at500°C is conducive to the formation of large Ag particles and yields the largest adsorption capacity for toluene,so H500exhibits the best activity at lower temperatures;however,because of poor interaction between Ag and toluene,its activity at higher temperature is modest.The O500‐H300sample exhibits excellent catalytic activity during the whole reaction process,which can be attributed to the small and highly dispersed Ag nanoparticles as well as the existence of subsurface oxygen.
基金Supported by the National Science Foundation of China(U1162129)the Science and Technology Department of Zhejiang Province(2009R50020)
文摘Silver modified HZSM-5 （AgHZ） zeolite catalysts were prepared by ion exchange method and their catalytic properties in the l-butene cracking reaction were measured. The catalysts were characterized by infrared spec- troscopy with pyridine adsorption （Py-IR）, N2 adsorption and X-ray diffraction （XRD）. The effects of Ag loading and steaming treatment on catalytic performances were studied. It is found that the activity ofHT_SM-5 （HZ） catalyst significantly decreases with the steaming time, whereas AgHZ catalysts show stable activity in the steaming time of 24-48 h and their activities increase with the Ag loading. When the steaming time is 24-48 h, the yield of propylene over HZ catalyst significantly decreases, whereas it is stable over AgHZ catalysts. The AgHZ catalysts with Ag loadings of 0.28%-0.43% （by mass） show similar propylene yields （-30%）, which are higher than that over the AgHZ catalyst with a Ag loading of 0.55% （by mass）. These results indicate that the steam-treated AgHZ catalysts with optimum Ag loadings have higher yield of propylene and are more stable than the steam- treated HZ catalyst. The regeneration stability measurement in butene cracking also shows that the AgHZ catalyst steam-treated under a suitable condition has better stability than the HZ catalyst.
