Platinum/cerium-zirconium-sulfate(Pt/Ce-Zr-SO_4^(2-)) catalysts were prepared by wetness impregnation.Catalytic activities were evaluated from the combustion of propene and CO.Sulfate(SO_4^(2-))addition improv...Platinum/cerium-zirconium-sulfate(Pt/Ce-Zr-SO_4^(2-)) catalysts were prepared by wetness impregnation.Catalytic activities were evaluated from the combustion of propene and CO.Sulfate(SO_4^(2-))addition improved the catalytic activity significantly.When using Pt/Ce-Zr-SO_4^(2-) with 10 wt%SO_4^(2-),the temperature for 90%conversion of propene and CO decreased by 75℃ compared with Pt/Ce-Zr.The conversion exceeded 95%at 240℃ even after 0.02%sulfur dioxide poisoning for 20 h.Temperature-programmed desorption of CO and X-ray photoelectron spectroscopy analyses revealed an improvement in Pt dispersion onto the Ce-Zr-SO_4^(2-) support,and the increased number of Pt particles built up more Pt^(-)-(SO_4^(2-))^(-) couples,which resulted in excellent activity.The increased total acidity and new Bronsted acid sites on the surface provided the Pt/Ce-Zr-SO_4^(2-) with good sulfur resistance.展开更多
Decomposition mass loss and pyrolysis products analyses of particles sampled at various locations along the tailpipe of a Euro-IV diesel engine were performed using a thermo gravimetry in conjunction with Fourier tran...Decomposition mass loss and pyrolysis products analyses of particles sampled at various locations along the tailpipe of a Euro-IV diesel engine were performed using a thermo gravimetry in conjunction with Fourier transformation infrared spectrometrymass spectrum.Diesel particles were collected at the same location with and without diesel oxidation catalyst(DOC)mounted on the test engine separately.The three poles in thermal gravity-differential thermal gravity images suggested that the decomposition process of diesel particles could be divided into three stages which correspond to the decompositions of lower boiling substances,higher boiling substances and soot respectively.It is noticed that no matter whether DOC was mounted or not,the further the particles were sampled away from the engine block,the lower the peak temperatures and the heavier the mass losses within the first two stages,which indicated that the soluble organic fraction in the particle samples increased and therefore lowering the activation energy of thermal decomposition.Hydroxyl,ammonia,C_xH_y fragments,benzene,toluene,and phenol were found to be the primary products of particle decomposition,which didn’t change with the location of particle sample point.The employment of DOC increased the activation energy for particle oxidation and resulted in a higher peak temperature and lower mass loss within the first-stage.Moreover,the C=O stretching bands of aldehyde and ketone at 1771 cm-1 was only detected without a DOC,while the N02 peak at 1634 cm-1 was solely noticed with the presence of DOC.Compared to the first-stage pyrolysis products,more polycyclic aromatic hydrocarbons and less C_xH_y fragments were seen in the second-stage.展开更多
A series of Ce_(1-x)Ti_(x)O_(2)mixed oxide catalysts were synthesized by sol-gel method and then loading of noble metal(M=Pt,Rh,Ru)was used for soot oxidation.Ti-doped Ce_(1-x)Ti_(x)O_(2)catalysts(x is the molar ratio...A series of Ce_(1-x)Ti_(x)O_(2)mixed oxide catalysts were synthesized by sol-gel method and then loading of noble metal(M=Pt,Rh,Ru)was used for soot oxidation.Ti-doped Ce_(1-x)Ti_(x)O_(2)catalysts(x is the molar ratio of Ti/(Ti+Ce)and ranges from 0.1 to 0.5)exhibit much better oxidation performance than CeO_(2)catalyst,and the Ce_(0.9)Ti_(0.1)O_(2)catalyst calcined at 500℃has the best catalysis activity.Each noble metal(1 wt%)was supported on Ce_(0.9)Ti_(0.1)O_(2)(M/C9 T1)and the properties of the catalysts were characterized by X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),Raman,Brunauer-Emmett-Teller(BET)method,and H_(2)-temperature programmed reduction(H_(2)-TPR)results.Results show that the introduction of Ti into CeO_(2)forming Ti-O-Ce structure enhances the catalytic activity and increases the number of oxygen vacancies at the catalyst surface.The noble metal is highly dispersed over Ce_(0.9)Ti_(0.1)O_(2),and M/C9 T1 catalysts present enhanced activity in comparison to Ce_(0.9)Ti_(0.1)O_(2).It is found that noble metals can greatly increase the activity of the catalyst and the corresponding oxidation rate of soot can enhance the electron transfer capacity and oxygen adsorption capacity of the catalyst.A small amount of Ti doping in CeO_(2)can significantly improve the activity of the catalyst,while a large amount of Ti reduces the performance of the catalyst because a large amount of Ti is enriched on the surface of the catalyst,which hinders the contact and reaction between the catalyst and the soot.展开更多
The catalytic performance of Pt-based catalysts for the total oxidation of hydrocarbons was investigated.The activity of supported Pt catalysts(Pt/Al2O3,Pt/ZrO2,Pt/TiO2,and Pt/H-ZSM-5)depends on the metal oxide suppor...The catalytic performance of Pt-based catalysts for the total oxidation of hydrocarbons was investigated.The activity of supported Pt catalysts(Pt/Al2O3,Pt/ZrO2,Pt/TiO2,and Pt/H-ZSM-5)depends on the metal oxide support.Pt/Al2O3 showed the highest catalytic activity when the catalysts were aged at 750°C for 50 h in air.The activity of Pt/Al2O3 was dependent on the valence state of the Pt surface.Pt/Al2O3 with the Pt surface in the metallic state was more active than with the surface in the cationic state.The surface density of acid and basic sites on the Al2O3 support controlled the valence state of the Pt surface and stability of the Pt particles in the highly dispersed state,respectively.展开更多
The effects of a diesel oxidation catalytic (DOC) converter on diesel engine emissions were investigated on a diesel bench at various loads for two steady-state speeds using diesel fuel and B20. The DOC was very eff...The effects of a diesel oxidation catalytic (DOC) converter on diesel engine emissions were investigated on a diesel bench at various loads for two steady-state speeds using diesel fuel and B20. The DOC was very effective in hydrocarbon (HC) and CO oxidation. Approximately 90%-95% reduction in CO and 36%-70% reduction in HC were realized using the DOC. Special attention was focused on the effects of the DOC on elemental carbon (EC) and organic carbon (OC) fractions in fine particles (PM2.5) emitted from the diesel engine. The carbonaceous compositions of PM2.5 were analyzed by the method of thermal/optical reflectance (TOR). The results showed that total carbon (TC), OC and EC emissions for PM2.5 from diesel fuel were generally reduced by the DOC. For diesel fuel, TC emissions decreased 22%-32% after the DOC depending on operating modes. The decrease in TC was attributed to 35%-97% decrease in OC and 3%-65% decrease in EC emissions. At low load, a significant increase in the OC/EC ratio of PMz.5 was observed after the DOC. The effect of the DOC on the carbonaceous compositions in PM2.5 from B20 showed different trends compared to diesel fuel. At low load, a slight increase in EC emissions and a significant decrease in OC/EC ratio of PM2.5 after DOC were observed for B20.展开更多
This study investigated the filtration and continuous regeneration of a particulate filter system on an engine test bench, consisting of a diesel oxidation catalyst(DOC) and a catalyzed diesel particulate filter(C...This study investigated the filtration and continuous regeneration of a particulate filter system on an engine test bench, consisting of a diesel oxidation catalyst(DOC) and a catalyzed diesel particulate filter(CDPF). Both the DOC and the CDPF led to a high conversion of NO to NO2 for continuous regeneration. The filtration efficiency on solid particle number(SPN) was close to100%. The post-CDPF particles were mainly in accumulation mode. The downstream SPN was sensitively influenced by the variation of the soot loading. This phenomenon provides a method for determining the balance point temperature by measuring the trend of SPN concentration.展开更多
The influence of sulfation on Pd/Ce0.75Zr0.25O2, Pd/Ce O2-Ti O2 and Pd/Ce O2 was investigated. Physical structure and chemical properties of different catalysts were characterized by N2 adsorption, X-ray diffraction(...The influence of sulfation on Pd/Ce0.75Zr0.25O2, Pd/Ce O2-Ti O2 and Pd/Ce O2 was investigated. Physical structure and chemical properties of different catalysts were characterized by N2 adsorption, X-ray diffraction(XRD), CO chemisorption, X-ray photoelectron spectroscopy(XPS), Fourier transform infrared spectroscopy(FT-IR) and X-ray fluorescence(XRF). After 10 h SO2 sulfation, it was found that the decrement on CO oxidation catalytic activity was limited on Pd/Ce0.75Zr0.25O2 compared to Pd/Ce O2-Ti O2 and Pd/Ce O2. It demonstrated that Pd/Ce0.75Zr0.25O2 was more sulfur resistant compared to the other two catalysts. After sulfur exposure, catalyst texture was not much influenced as shown by N2 adsorption and XRD, and surface Pd atoms were poisoned indicated by CO chemisorption results. Pd/Ce0.75Zr0.25O2 and Pd/Ce O2-Ti O2 exhibited less sulfur accumulation compared to Pd/Ce O2 in the sulfation process. Furthermore, XPS results clarified that surface sulfur amount, especially surface sulfates amount on the sulfated catalysts was more crucial for the deactivation in sulfur containing environment.展开更多
基金supported by the National Natural Science Foundation of China(21506194,21676255)the Provincial Natural Science Foundation of Zhejiang Province(LY16B070011)the Commission of Science and Technology of Zhejiang Province(2017C33106,2017C03007)~~
文摘Platinum/cerium-zirconium-sulfate(Pt/Ce-Zr-SO_4^(2-)) catalysts were prepared by wetness impregnation.Catalytic activities were evaluated from the combustion of propene and CO.Sulfate(SO_4^(2-))addition improved the catalytic activity significantly.When using Pt/Ce-Zr-SO_4^(2-) with 10 wt%SO_4^(2-),the temperature for 90%conversion of propene and CO decreased by 75℃ compared with Pt/Ce-Zr.The conversion exceeded 95%at 240℃ even after 0.02%sulfur dioxide poisoning for 20 h.Temperature-programmed desorption of CO and X-ray photoelectron spectroscopy analyses revealed an improvement in Pt dispersion onto the Ce-Zr-SO_4^(2-) support,and the increased number of Pt particles built up more Pt^(-)-(SO_4^(2-))^(-) couples,which resulted in excellent activity.The increased total acidity and new Bronsted acid sites on the surface provided the Pt/Ce-Zr-SO_4^(2-) with good sulfur resistance.
基金supported by the Open Research Program of State Key Laboratory of Engine Combustion(No.K2018-11)the National Nature Science Foundation of China(No.51806015)the National Engineering Laboratory for Mobile Source Emission Control Technology(No.NELMS2018A17)
文摘Decomposition mass loss and pyrolysis products analyses of particles sampled at various locations along the tailpipe of a Euro-IV diesel engine were performed using a thermo gravimetry in conjunction with Fourier transformation infrared spectrometrymass spectrum.Diesel particles were collected at the same location with and without diesel oxidation catalyst(DOC)mounted on the test engine separately.The three poles in thermal gravity-differential thermal gravity images suggested that the decomposition process of diesel particles could be divided into three stages which correspond to the decompositions of lower boiling substances,higher boiling substances and soot respectively.It is noticed that no matter whether DOC was mounted or not,the further the particles were sampled away from the engine block,the lower the peak temperatures and the heavier the mass losses within the first two stages,which indicated that the soluble organic fraction in the particle samples increased and therefore lowering the activation energy of thermal decomposition.Hydroxyl,ammonia,C_xH_y fragments,benzene,toluene,and phenol were found to be the primary products of particle decomposition,which didn’t change with the location of particle sample point.The employment of DOC increased the activation energy for particle oxidation and resulted in a higher peak temperature and lower mass loss within the first-stage.Moreover,the C=O stretching bands of aldehyde and ketone at 1771 cm-1 was only detected without a DOC,while the N02 peak at 1634 cm-1 was solely noticed with the presence of DOC.Compared to the first-stage pyrolysis products,more polycyclic aromatic hydrocarbons and less C_xH_y fragments were seen in the second-stage.
基金Project supported by National Key Research and Development Program of China(2018YFC1801706-01)the Natural Science Foundation of China(21663009,2216020078)the Science and Technology Project of Guizhou Province(20192835,2021480)。
文摘A series of Ce_(1-x)Ti_(x)O_(2)mixed oxide catalysts were synthesized by sol-gel method and then loading of noble metal(M=Pt,Rh,Ru)was used for soot oxidation.Ti-doped Ce_(1-x)Ti_(x)O_(2)catalysts(x is the molar ratio of Ti/(Ti+Ce)and ranges from 0.1 to 0.5)exhibit much better oxidation performance than CeO_(2)catalyst,and the Ce_(0.9)Ti_(0.1)O_(2)catalyst calcined at 500℃has the best catalysis activity.Each noble metal(1 wt%)was supported on Ce_(0.9)Ti_(0.1)O_(2)(M/C9 T1)and the properties of the catalysts were characterized by X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),Raman,Brunauer-Emmett-Teller(BET)method,and H_(2)-temperature programmed reduction(H_(2)-TPR)results.Results show that the introduction of Ti into CeO_(2)forming Ti-O-Ce structure enhances the catalytic activity and increases the number of oxygen vacancies at the catalyst surface.The noble metal is highly dispersed over Ce_(0.9)Ti_(0.1)O_(2),and M/C9 T1 catalysts present enhanced activity in comparison to Ce_(0.9)Ti_(0.1)O_(2).It is found that noble metals can greatly increase the activity of the catalyst and the corresponding oxidation rate of soot can enhance the electron transfer capacity and oxygen adsorption capacity of the catalyst.A small amount of Ti doping in CeO_(2)can significantly improve the activity of the catalyst,while a large amount of Ti reduces the performance of the catalyst because a large amount of Ti is enriched on the surface of the catalyst,which hinders the contact and reaction between the catalyst and the soot.
基金supported by the New Energy and Industrial Technology Development Organization(NEDO)
文摘The catalytic performance of Pt-based catalysts for the total oxidation of hydrocarbons was investigated.The activity of supported Pt catalysts(Pt/Al2O3,Pt/ZrO2,Pt/TiO2,and Pt/H-ZSM-5)depends on the metal oxide support.Pt/Al2O3 showed the highest catalytic activity when the catalysts were aged at 750°C for 50 h in air.The activity of Pt/Al2O3 was dependent on the valence state of the Pt surface.Pt/Al2O3 with the Pt surface in the metallic state was more active than with the surface in the cationic state.The surface density of acid and basic sites on the Al2O3 support controlled the valence state of the Pt surface and stability of the Pt particles in the highly dispersed state,respectively.
基金This work was financially supported by the National Science Fund for Distinguished Young Scholars of China (No. 20625722) and the National Natural Science Foundation of China (Grant No. 20807025). We would also like to thank Prof. Yunshan Ge from Beijing Institute of Technology for the significant in-kind support on the engine test and thank Mr. Charles N. Freed for useful comments on this work.
文摘The effects of a diesel oxidation catalytic (DOC) converter on diesel engine emissions were investigated on a diesel bench at various loads for two steady-state speeds using diesel fuel and B20. The DOC was very effective in hydrocarbon (HC) and CO oxidation. Approximately 90%-95% reduction in CO and 36%-70% reduction in HC were realized using the DOC. Special attention was focused on the effects of the DOC on elemental carbon (EC) and organic carbon (OC) fractions in fine particles (PM2.5) emitted from the diesel engine. The carbonaceous compositions of PM2.5 were analyzed by the method of thermal/optical reflectance (TOR). The results showed that total carbon (TC), OC and EC emissions for PM2.5 from diesel fuel were generally reduced by the DOC. For diesel fuel, TC emissions decreased 22%-32% after the DOC depending on operating modes. The decrease in TC was attributed to 35%-97% decrease in OC and 3%-65% decrease in EC emissions. At low load, a significant increase in the OC/EC ratio of PMz.5 was observed after the DOC. The effect of the DOC on the carbonaceous compositions in PM2.5 from B20 showed different trends compared to diesel fuel. At low load, a slight increase in EC emissions and a significant decrease in OC/EC ratio of PM2.5 after DOC were observed for B20.
基金supported by the National High Technology Research and Development Program of China(863)(No.2013AA065304)
文摘This study investigated the filtration and continuous regeneration of a particulate filter system on an engine test bench, consisting of a diesel oxidation catalyst(DOC) and a catalyzed diesel particulate filter(CDPF). Both the DOC and the CDPF led to a high conversion of NO to NO2 for continuous regeneration. The filtration efficiency on solid particle number(SPN) was close to100%. The post-CDPF particles were mainly in accumulation mode. The downstream SPN was sensitively influenced by the variation of the soot loading. This phenomenon provides a method for determining the balance point temperature by measuring the trend of SPN concentration.
基金supported by the Introduction of Talent and Technology Cooperation Plan of Tianjin(14RCGFGX00849)
文摘The influence of sulfation on Pd/Ce0.75Zr0.25O2, Pd/Ce O2-Ti O2 and Pd/Ce O2 was investigated. Physical structure and chemical properties of different catalysts were characterized by N2 adsorption, X-ray diffraction(XRD), CO chemisorption, X-ray photoelectron spectroscopy(XPS), Fourier transform infrared spectroscopy(FT-IR) and X-ray fluorescence(XRF). After 10 h SO2 sulfation, it was found that the decrement on CO oxidation catalytic activity was limited on Pd/Ce0.75Zr0.25O2 compared to Pd/Ce O2-Ti O2 and Pd/Ce O2. It demonstrated that Pd/Ce0.75Zr0.25O2 was more sulfur resistant compared to the other two catalysts. After sulfur exposure, catalyst texture was not much influenced as shown by N2 adsorption and XRD, and surface Pd atoms were poisoned indicated by CO chemisorption results. Pd/Ce0.75Zr0.25O2 and Pd/Ce O2-Ti O2 exhibited less sulfur accumulation compared to Pd/Ce O2 in the sulfation process. Furthermore, XPS results clarified that surface sulfur amount, especially surface sulfates amount on the sulfated catalysts was more crucial for the deactivation in sulfur containing environment.