The effect of polycyclic aromatic hydrocarbons(PAHs)on the stability of the hydrogenation catalyst for production of ultra-low sulfur diesel was studied in a pilot plant using Ni-Mo-W/γ-Al_(2)O_(3)catalyst.The mechan...The effect of polycyclic aromatic hydrocarbons(PAHs)on the stability of the hydrogenation catalyst for production of ultra-low sulfur diesel was studied in a pilot plant using Ni-Mo-W/γ-Al_(2)O_(3)catalyst.The mechanisms of catalyst deactivation were analyzed by the methods of elemental analysis,nitrogen adsorption-desorption,thermogravimetry-mass spectrometry(TG-MS)technology,X-ray photoelectron spectroscopy(XPS)and high resolution transmission electron microscopy(HRTEM).The results demonstrated that PAHs had little effect on the activity of catalyst at the beginning of operation,during which the reaction temperature was increased by only 1-4℃.However,the existence of PAHs significantly accelerated the deactivation of catalyst and weakened the stability of catalyst.This phenomenon could be explained by the reason that the catalyst deactivation is not only related to the formation of carbon deposit,but is also closely related to the loss of pore volume and the decrease of Ni-W-S phase ratio after adding PAHs.展开更多
The deactivation of a Ni-Mo-W/Al_2O_3 catalyst during ultra-low-sulfur diesel production was investigated in a pilot plant. The reasons of catalyst deactivation were analyzed by the methods of elemental analysis, BET ...The deactivation of a Ni-Mo-W/Al_2O_3 catalyst during ultra-low-sulfur diesel production was investigated in a pilot plant. The reasons of catalyst deactivation were analyzed by the methods of elemental analysis, BET and TG-MS. The results showed that the catalyst deactivation rate was notable at the beginning of run, and then gradually reached a steady state after 448 h. In the initial period the catalyst deactivation may mainly be caused by the formation of the carbon deposits. The carbon deposits blocked the catalyst pores and the accessibility of active center decreased. The TG-MS analysis identified three types of carbon species deposited on the catalysts, viz.: the low temperature carbon deposit with high H/C atomic ratio, the medium temperature carbon deposit, and the high temperature carbon with low H/C atomic ratio. The amount of high temperature carbon deposits on the catalyst determined the overall activity and, therefore the high temperature carbon was a major contributor to the deactivation of Ni-Mo-W catalyst.展开更多
Number size distributions (NSDs, 10―487 nm) and composition of nanoparticle emitted from an engine fueled with ordinary diesel (OD) and low sulfur diesel (LSD) fuel were comparatively studied. The results indicate th...Number size distributions (NSDs, 10―487 nm) and composition of nanoparticle emitted from an engine fueled with ordinary diesel (OD) and low sulfur diesel (LSD) fuel were comparatively studied. The results indicate that, compared with the OD, the LSD was found to slightly decrease the mass concentration, and significantly reduce the number concentration of the total particles (10―487 nm), and the reduction of number increased with the speed and load of engine. The NSD for the two fuels showed a similar bimodal structure under all test engine conditions. Under the same engine conditions, the nucleation mode for LSD fuel was significantly lower than that of ordinary diesel. However, the accumulation mode for the two fuels showed little difference. The elements composition of exhaust particles included C, O, Cl, S, Si, Ca, Na, Al and K. The S element was not detected in LSD fuel case. The main component of soluble organic fraction (SOF) of exhaust particles for the two fuels included saturated alkane (C15―C26), ester and polycyclic aromatic hydrocarbons (PAHs). However, PAHs were not found in LSD fuel case.展开更多
In an urban-transit bus, fueled by biodiesel in Toledo, Ohio, single inhalable particle samples in October 2008 were collected and detected by scanning electron microscopy and energy dispersive X-ray spectrometry （SE...In an urban-transit bus, fueled by biodiesel in Toledo, Ohio, single inhalable particle samples in October 2008 were collected and detected by scanning electron microscopy and energy dispersive X-ray spectrometry （SEM/EDS）. Particle size analysis found bimodal distribution at 0.2 and 0.5 μm. The particle morphology was characterized by 14 different shape clusters： square, pentagon, hexagon, heptagon, octagon, nonagon, decagon, agglomerate, sphere, triangle, oblong, strip, line or stick, and unknown, by quantitative order. The square particles were common in the samples. Round and triangle particles are more, and pentagon, hexagon, heptagon, octagon, nonagon, decagon, strip, line or sticks are less. Agglomerate particles were found in abundance. The surface of most particles was coarse with a fractal edge that can provide a suitable chemical reaction bed in the polluted atmospheric environment. The three sorts of surface patterns of squares were smooth, semi-smooth, and coarse. The three sorts of square surface patterns represented the morphological characteristics of single inhalable particles in the air inside the bus in Toledo. The size and shape distribution results were compared to those obtained for a bus using ultra low sulfur diesel.展开更多
基金financially supported by the Hydrogenation Process and Hydrogenation Catalyst Laboratory (RIPP,SINOPEC)
文摘The effect of polycyclic aromatic hydrocarbons(PAHs)on the stability of the hydrogenation catalyst for production of ultra-low sulfur diesel was studied in a pilot plant using Ni-Mo-W/γ-Al_(2)O_(3)catalyst.The mechanisms of catalyst deactivation were analyzed by the methods of elemental analysis,nitrogen adsorption-desorption,thermogravimetry-mass spectrometry(TG-MS)technology,X-ray photoelectron spectroscopy(XPS)and high resolution transmission electron microscopy(HRTEM).The results demonstrated that PAHs had little effect on the activity of catalyst at the beginning of operation,during which the reaction temperature was increased by only 1-4℃.However,the existence of PAHs significantly accelerated the deactivation of catalyst and weakened the stability of catalyst.This phenomenon could be explained by the reason that the catalyst deactivation is not only related to the formation of carbon deposit,but is also closely related to the loss of pore volume and the decrease of Ni-W-S phase ratio after adding PAHs.
基金financially supported by the Hydrogenation Process and Hydrogenation Catalyst Laboratory (RIPP, SINOPEC)
文摘The deactivation of a Ni-Mo-W/Al_2O_3 catalyst during ultra-low-sulfur diesel production was investigated in a pilot plant. The reasons of catalyst deactivation were analyzed by the methods of elemental analysis, BET and TG-MS. The results showed that the catalyst deactivation rate was notable at the beginning of run, and then gradually reached a steady state after 448 h. In the initial period the catalyst deactivation may mainly be caused by the formation of the carbon deposits. The carbon deposits blocked the catalyst pores and the accessibility of active center decreased. The TG-MS analysis identified three types of carbon species deposited on the catalysts, viz.: the low temperature carbon deposit with high H/C atomic ratio, the medium temperature carbon deposit, and the high temperature carbon with low H/C atomic ratio. The amount of high temperature carbon deposits on the catalyst determined the overall activity and, therefore the high temperature carbon was a major contributor to the deactivation of Ni-Mo-W catalyst.
基金Supported by the Research Fund for The Doctoral Program of Higher Education of China (Grant No. 20070248024)
文摘Number size distributions (NSDs, 10―487 nm) and composition of nanoparticle emitted from an engine fueled with ordinary diesel (OD) and low sulfur diesel (LSD) fuel were comparatively studied. The results indicate that, compared with the OD, the LSD was found to slightly decrease the mass concentration, and significantly reduce the number concentration of the total particles (10―487 nm), and the reduction of number increased with the speed and load of engine. The NSD for the two fuels showed a similar bimodal structure under all test engine conditions. Under the same engine conditions, the nucleation mode for LSD fuel was significantly lower than that of ordinary diesel. However, the accumulation mode for the two fuels showed little difference. The elements composition of exhaust particles included C, O, Cl, S, Si, Ca, Na, Al and K. The S element was not detected in LSD fuel case. The main component of soluble organic fraction (SOF) of exhaust particles for the two fuels included saturated alkane (C15―C26), ester and polycyclic aromatic hydrocarbons (PAHs). However, PAHs were not found in LSD fuel case.
文摘In an urban-transit bus, fueled by biodiesel in Toledo, Ohio, single inhalable particle samples in October 2008 were collected and detected by scanning electron microscopy and energy dispersive X-ray spectrometry （SEM/EDS）. Particle size analysis found bimodal distribution at 0.2 and 0.5 μm. The particle morphology was characterized by 14 different shape clusters： square, pentagon, hexagon, heptagon, octagon, nonagon, decagon, agglomerate, sphere, triangle, oblong, strip, line or stick, and unknown, by quantitative order. The square particles were common in the samples. Round and triangle particles are more, and pentagon, hexagon, heptagon, octagon, nonagon, decagon, strip, line or sticks are less. Agglomerate particles were found in abundance. The surface of most particles was coarse with a fractal edge that can provide a suitable chemical reaction bed in the polluted atmospheric environment. The three sorts of surface patterns of squares were smooth, semi-smooth, and coarse. The three sorts of square surface patterns represented the morphological characteristics of single inhalable particles in the air inside the bus in Toledo. The size and shape distribution results were compared to those obtained for a bus using ultra low sulfur diesel.
