The pursuit of high-performance is worth considerable effort in catalysis for energy efficiency and environmental sustainability. To develop redox catalysts with superior performance for soot combustion, a series of M...The pursuit of high-performance is worth considerable effort in catalysis for energy efficiency and environmental sustainability. To develop redox catalysts with superior performance for soot combustion, a series of Mn_(x)Co_(y) oxides were synthesized using MgO template substitution.This method greatly improves the preparation and catalytic efficiency and is more in line with the current theme of green catalysts and sustainable development. The resulting Mn_(1)Co_(2.3) has a strong activation capability of gaseous oxygen due to a high concentration of Co^(3+) and Mn^(3+). The Mn doping enhanced the intrinsic activity by prompting oxygen vacancy formation and gaseous oxygen adsorption. The nanosheet morphology with abundant mesoporous significantly increased the solid–solid contact efficiency and improved the adsorption capability of gaseous reactants. The novel design of Mn_(1)Co_(2.3)oxide enhanced its catalytic performance through a synergistic effect of Mn doping and the porous nanosheet morphology, showing significant potential for the preparation of high-performance soot combustion catalysts.展开更多
A feasible approach to rectify the world's energy demand using sustainable development of adequate energy generation and storage technologies in a single channel.In this respect,we made a holistic approach with a ...A feasible approach to rectify the world's energy demand using sustainable development of adequate energy generation and storage technologies in a single channel.In this respect,we made a holistic approach with a bifunctional electrode material to perform effectively in energy generation and storage applications.MoS_(2) nanosheets were produced by the eco-friendly method and reduced graphene oxide is used to prepared by carbon soot which is derived from castor oil.The prepared soot and rGO were combined with MoS_(2) nanosheets using a simple sonication method.The as-prepared sample was introduced in the supercapacitor and DSSC application.The combination MoS_(2)@rGO provides an enhanced conversion efficiency of 11.81%and the reproducibility of DSSC is also studied.Further,MoS_(2)@rGO is used to fabricate an asymmetric supercapacitor to investigate its real-time application.The device produced the maximum power density(1666.6 mW/kg)and energy density(25.69 mWh/Kg)at 1 A/g.The asymmetric supercapacitor device holds a cyclic stability of 81.4%for 5000 cycles and it powered up an LED device for 4 min.展开更多
The aim of this study was to investigate the oxidation reactivity and behavior of exhaust particulate matter(PM)from diesel engines.PM samples from two diesel engines(1K,CY4102)with different emission levels were coll...The aim of this study was to investigate the oxidation reactivity and behavior of exhaust particulate matter(PM)from diesel engines.PM samples from two diesel engines(1K,CY4102)with different emission levels were collected by a thermophoretic system and a quartz filter.The oxidation reactivity,oxidation behaviors,and physicochemical properties of the PM samples were analyzed using thermogravimetric analysis(TGA),high-resolution transmission electron microscopy(HRTEM),Fourier-transform infrared spectrometry(FTIR),and Raman spectroscopy.The results showed that there was a great difference in the oxidation reactivity of soot particles emitted by the two different diesel engines.A qualitative analysis of the factors influencing oxidation reactivity showed that the nanostructure,degree of graphitization,and relative concentration of aliphatic C—H functional groups were the most important factors,whereas no significant correlation was found between the primary particle size and activation energy of the diesel soot.Based on the oxidation behavior analysis,the diesel soot particles exhibited both internal and surface oxidation modes during the oxidation process.Surface oxidation was dominant during the initial stage,and as oxidation progressed,the mode gradually changed to internal oxidation.Internal oxidation mode of soot particles from the 1K engine was significantly higher than that of CY4102.展开更多
The composite oxides xAg/Co_(0.93)Ce_(0.07)(x=Ag/(Co+Ce) molar ratio),intended for use as high performance catalytic materials,were successfully prepared via citric acid complexation.The effects of silver on ...The composite oxides xAg/Co_(0.93)Ce_(0.07)(x=Ag/(Co+Ce) molar ratio),intended for use as high performance catalytic materials,were successfully prepared via citric acid complexation.The effects of silver on the performance of these substances during soot combustion were subsequently investigated.Under O_2,the 0.3Ag/Co_(0.93)Ce_(0.07) catalyst resulted in the lowest ignition temperature,T_(10),of197 ℃,while the minimum light-off temperature was obtained from both 0.2Ag/Co_(0.93)Ce_(0.07) and0.3Ag/Co_(0.93)Ce_(0.07) in the NO_x atmosphere.These materials were also characterized by various techniques,including H_2,soot and NO_x temperature programmed reduction,X-ray diffraction,and electron paramagnetic resonance,Raman,X-ray photoelectron,and Fourier transform infrared spectroscopic analyses.The results demonstrated that silver significantly alters the catalytic behavior under both O_2 and NO_x,even though the lattice structure of the mixed oxide is not affected.Surface silver oxides generated under the O_2 atmosphere favor soot combustion by participating in the redox cycles between soot and the silver oxide,whereas the AgNO_3 that forms in a NO_x-rich atmosphere facilitates soot abatement at a lower temperature.The inferior activity of AgNO_3 relative to that of Ag_2O results in the different catalytic performance in the presence of NO_x or O_2.展开更多
Soot,a product of insufficient combustion,is usually in the form of aggregate. The multi-scattering of soot fractal aggregates has been proved to play an important role in studying the soot radiative properties,which ...Soot,a product of insufficient combustion,is usually in the form of aggregate. The multi-scattering of soot fractal aggregates has been proved to play an important role in studying the soot radiative properties,which is rarely considered in predicting the radiative heat transfer in combustion flame. In the present study,based on the weighted sum of gray soot fractal aggregate(WSGSA) model,which is used to predict the temperature field and soot aggregates in turbulent diffusion flame,the flame temperature distribution and soot volume fraction distribution under the conditions of the model without considering radiation,the default radiation model in Fluent software and the WSGSA model are calculated respectively. The results show that the flame temperature will be seriously overestimated without considering radiation and the maximum relative discrepancy of flame centerline temperature is about 64.5%. The accuracy will be improved by the default radiation model in the Fluent software,but the flame temperature is still overestimated and the maximum relative discrepancy of flame centerline temperature is about 42.1%. However,more satisfactory results can be obtained by the WSGSA model,and the maximum relative discrepancy of flame centerline temperature is no more than 15.3%. Similar conclusions can also be obtained in studying the temperature distribution along different flame heights. Moreover,the soot volume fraction can be predicted more accurately with the application of the WSGSA model. Both without considering radiation and using the default radiation model in the Fluent software will result in the underestimating of soot volume fraction. All the results reveal that the WSGSA model can be used to predict the temperature and soot aggregates in the CH/air turbulent diffusion flame.展开更多
Ag/LaCoO3 perovskite catalysts for soot combustion were prepared by the impregnation method.The structure and physicochemical properties of the catalysts were characterized using X-ray diffraction,N2 adsorption-desorp...Ag/LaCoO3 perovskite catalysts for soot combustion were prepared by the impregnation method.The structure and physicochemical properties of the catalysts were characterized using X-ray diffraction,N2 adsorption-desorption,H2 temperature-programmed reduction,soot temperatureprogrammed reduction,and X-ray photoelectron spectroscopy.The catalytic activity of the catalysts for soot oxidation was tested by temperature-programmed oxidation in air and in a NOx atmosphere.Metallic Ag particles were the main Ag species.Part of the Ag migrated from the surface to the lattice of the LaCoO3 perovskite,to form La(1-x)AgxCoO3.This increased the amount of oxygen vacancies in the perovskite structure during thermal treatment.Compared with unmodified LaCoO3,the maximum soot oxidation rate temperature(Tp) decreased by 50-70 ℃ in air when LaCoO3 was partially modified by Ag,depending on the thermal treatment temperature.The Tp of the Ag/LaCoO3catalyst calcined at 400℃ in a NOx atmosphere decreased to about 140℃,compared with that of LaCoO3.Ag particles and oxygen vacancies in the catalysts contributed to their high catalytic activity for soot oxidation.The stable catalytic activity of the Ag/LaCoO3 catalyst calcined at 700℃ in a NOx atmosphere was related to its stable structure.展开更多
Au/3DOM(three-dimensionally ordered macroporous) Al2O3 and Au/CeO2/3DOM Al2O3 were prepared using a reduction-deposition method and characterized using scanning electron microscopy,N2 adsorption-desorption,X-ray dif...Au/3DOM(three-dimensionally ordered macroporous) Al2O3 and Au/CeO2/3DOM Al2O3 were prepared using a reduction-deposition method and characterized using scanning electron microscopy,N2 adsorption-desorption,X-ray diffraction,transmission electron microscopy,ultraviolet-visible spectroscopy,temperature-programmed hydrogen reduction,and X-ray photoelectron spectroscopy.Au nanoparticles of similar sizes were well dispersed and supported on the inner walls of uniform macropores.The norminal Au loading is 2%.Al-Ce-O solid solution in CeO2/3DOM Al2O3 catalysts can be formed due to the incorporation of Al^3+ ions into the ceria lattice,which causes the creation of extrinsic oxygen vacancies.The extrinsic oxygen vacancies improved the oxygen-transport properties.The strong metal-support interactions between Au and CeO2 increased the amount of active oxygen on the Au nanoparticle surfaces,and this promoted soot oxidation.The activities of the Au-based catalysts were higher than those of the supports(Al2O3 or CeO2/3DOM Al2O3) at low temperature.Au/CeO2/3DOM Al2O3 had the highest catalytic activity for soot combustion,with T(10),T(50),and T(90) values of 273,364,and 412℃,respectively.展开更多
A facile procedure was carried out to prepare macroporous perovskite-type complex oxide catalysts of La1–xKxCo1–yFeyO3(x=0,0.1,y=0,0.1) by using the combined method of organic ligation and solution combustion.This m...A facile procedure was carried out to prepare macroporous perovskite-type complex oxide catalysts of La1–xKxCo1–yFeyO3(x=0,0.1,y=0,0.1) by using the combined method of organic ligation and solution combustion.This method could ensure the formation of the desired macroporous structures and the desired crystal phases of the prepared catalysts.It was found that the macroporous catalysts showed higher catalytic activities for soot combustion than that of the corresponding nanometric samples,and the macroporous ...展开更多
MnOx-CeO2 oxides prepared by complexation-combustion method were used for soot oxidation. The highest conversion rate of soot was obtained on a MnOx-CeO2 oxide prepared under mild acid condition of pH = 4, where the o...MnOx-CeO2 oxides prepared by complexation-combustion method were used for soot oxidation. The highest conversion rate of soot was obtained on a MnOx-CeO2 oxide prepared under mild acid condition of pH = 4, where the oxidation temperature corresponding to maximum activity was decreased more than 150 ℃ compared with that of un-catalytic soot oxidation. The structure and property of the catalysts were investigated by X-ray powder diffraction (XRD) and temperature programmed reduction (TPR). The results indicated that there were at least two kinds of Mn species present in MnOx-CeO2 catalysts, i.e. Mn ions within CeO2 lattice and high dispersion MnOx on the surface of CeO2. The presence of Mn ions in the CeO2 lattice improved the oxygen vacancy due to the charge difference, and the CeO2 considerably decreased the reduction temperature of MnOx. The capability to activate oxygen through the oxygen exchange between O2 in gas phase and lattice oxygen species in MnOx-CeO2 oxide contributed to the high catalytic activity for the reaction.展开更多
Three-dimensional ordered macroporous (3DOM) La1?xKxNiO3 perovskite-type catalysts were successfully prepared by a colloidal crystal template method and characterized by scanning electron microscopy, transmission elec...Three-dimensional ordered macroporous (3DOM) La1?xKxNiO3 perovskite-type catalysts were successfully prepared by a colloidal crystal template method and characterized by scanning electron microscopy, transmission electron microscopy, high-resolution transmission electron microscopy, energy-dispersive X-ray scattering elemental mapping, X-ray diffraction, Raman and X-ray photoelectron spectroscopy, and temperature-programmed reduction of H2. Further, their catalytic activity in soot combustion was determined by temperature-programmed oxidation reaction. K substitution into the LaNiO3 lattice led to remarkably improved catalytic activity of this catalyst in soot combustion. Amongst various catalysts, La0.95K0.05NiO3 exhibited the highest activity in soot combustion (with its T50 and CO2 S values being 338 °C and 98.2%, respectively), which is comparable to the catalytic activities of Pt-based catalysts under the condition of poor contact between the soot and the catalyst. K-substitution improves the valence state of Ni and increases the number of oxygen vacancies, thereby leading to increased density of surface-active oxygen species. The active oxygen species play a vital role in catalyzing the elimination of soot. The perovskite-type La1?xKxNiO3 nanocatalysts with 3DOM structure without noble metals have potential for practical applications in the catalytic combustion of diesel soot particles.展开更多
Nanostructure K2NiF4 type oxides La2-xKxCuO4 complex oxides were prepared using the Sol-Gel method, characterized by X-Ray Diffraction (XRD), Fourier Transform Infrared (FT-IR), and Scanning Electron Microscopy (...Nanostructure K2NiF4 type oxides La2-xKxCuO4 complex oxides were prepared using the Sol-Gel method, characterized by X-Ray Diffraction (XRD), Fourier Transform Infrared (FT-IR), and Scanning Electron Microscopy (SEM). The catalytic activity for soot combustion was evaluated by the Temperature-Programmed Reaction (TPO) technique. The results demonstrated that the substitution quality of K^+ for La^3+ at the A-site would increase the catalytic activities of La2-xKxCuO4 for soot combustion greatly; the substitution quality affected the structure and catalytic activity obviously. The La1.8K0.2CuO4 complex oxides with tetrahedral structures had the best catalytic activity for soot combustion, and the ignition temperature of soot combustion was lowered from 490 to 320 ℃.展开更多
A series of perovskite type oxides and supported Ag catalysts were prepared, and characterized by X ray diffraction (XRD) and X ray photoelectron spectroscopy (XPS). The catalytic activities of the catalyst...A series of perovskite type oxides and supported Ag catalysts were prepared, and characterized by X ray diffraction (XRD) and X ray photoelectron spectroscopy (XPS). The catalytic activities of the catalysts as well as influencing factors on catalytic activity have been investigated for the simultaneous removal of NOx and diesel soot particulate. An increase in catalytic activity for the selective reduction of NOx was observed with Ag addition in these perovskite oxides, especially with 5% Ag loading. This catalyst could be a promising candidate of catalytic material for the simultaneous elimination of NOx and diesel soot.展开更多
A model is proposed to describe soot formation and oxidation during bio-oil gasification.It is based on the description of bio-oil heating,devolatilization,reforming of gases and conversion of both char and soot solid...A model is proposed to describe soot formation and oxidation during bio-oil gasification.It is based on the description of bio-oil heating,devolatilization,reforming of gases and conversion of both char and soot solids.Detailed chemistry (159 species and 773 reactions) is used in the gas phase.Soot production is described by a single reaction based on C2H2species concentration and three heterogeneous soot oxidation reactions.To support the validation of the model,three sets of experiments were carried out in a lab-scale Entrained Flow Reactor (EFR) equipped with soot quantification device.The temperature was varied from 1000 to 1400 C and three gaseous atmospheres were considered:default of steam,large excess of steam(H2O/C=8),and the presence of oxygen in the O/C range of 0.075–0.5.The model is shown to accurately describe the evolution of the concentration of the main gas species and to satisfactorily describe the soot concentration under the three atmospheres using a single set of identified kinetic parameters.Thanks to this model the contribution of different mechanisms involved in soot formation and oxidation in various situations can be assessed.展开更多
To improve the tribological behavior of biodiesel soot(BDS) in liquid paraffin(LP), the order of biodiesel soot was increased through thermally oxidized treatment at 500 ℃, and the oil solubility was then improved th...To improve the tribological behavior of biodiesel soot(BDS) in liquid paraffin(LP), the order of biodiesel soot was increased through thermally oxidized treatment at 500 ℃, and the oil solubility was then improved through a modification using oleylamine(OLA). The BDS and thermally oxidized oleylamine-modified BDS(T-BDS-OLA)were characterized through various methods including the use of TG, FETEM, Raman spectroscopy, FTIR, and a zeta potentiometer. The tribological properties and mechanisms of the BDS before and after the thermally oxidized treatment modification were investigated using a ball-on-disc reciprocating tribometer, FESEM, 3 D laser-scanning microscopy, and Raman spectroscopy. The results showed that T-BDS-OLA has a higher degree of order than the BDS, with an onion-like microstructure. BDS and T-BDS-OLA can both improve the antifriction and antiwear properties of LP at a soot content of 0.1%-0.4%, while T-BDS-OLA in LP shows better antifriction and antiwear properties than BDS. The tribological mechanisms can be attributed to both types of soot acting as spacing and roll bearing between the friction surfaces. In addition, the exfoliated graphitic sheets from T-BDS-OLA can form a carbon lubrication layer providing easy sliding.展开更多
A computational study of soot formation in ethylene/air coflow jet diffusion flame at atmospheric pres-sure was conducted using a reduced mechanism and soot formation model. A 20-step mechanism was derived from the fu...A computational study of soot formation in ethylene/air coflow jet diffusion flame at atmospheric pres-sure was conducted using a reduced mechanism and soot formation model. A 20-step mechanism was derived from the full mechanism using sensitivity analysis,reaction path analysis and quasi steady state(QSS) approximation. The model in premixed flame was validated and with computing savings in diffusion flame was applied by incor-porating into a CFD code. Simulations were performed to explore the effect of coflow air on flame structure and soot formation. Thermal radiation was calculated by a discrete-ordinates method,and soot formation was predicted by a simple two-equation soot model. Model results are in good agreement with those from experiment data and detailed mechanism at atmospheric conditions. The soot nucleation,growth,and oxidation by OH are all enhanced by decrease in coflow air velocity. The peak soot volume fraction region appears in the lower annular region be-tween the peak flame temperature and peak acetylene concentration locations,and the high soot oxidation rate due to the OH attack occurs in the middle annular region because of high temperature.展开更多
基金supported by the top talent program of Henan Agricultural University[grant numbers 30501029].
文摘The pursuit of high-performance is worth considerable effort in catalysis for energy efficiency and environmental sustainability. To develop redox catalysts with superior performance for soot combustion, a series of Mn_(x)Co_(y) oxides were synthesized using MgO template substitution.This method greatly improves the preparation and catalytic efficiency and is more in line with the current theme of green catalysts and sustainable development. The resulting Mn_(1)Co_(2.3) has a strong activation capability of gaseous oxygen due to a high concentration of Co^(3+) and Mn^(3+). The Mn doping enhanced the intrinsic activity by prompting oxygen vacancy formation and gaseous oxygen adsorption. The nanosheet morphology with abundant mesoporous significantly increased the solid–solid contact efficiency and improved the adsorption capability of gaseous reactants. The novel design of Mn_(1)Co_(2.3)oxide enhanced its catalytic performance through a synergistic effect of Mn doping and the porous nanosheet morphology, showing significant potential for the preparation of high-performance soot combustion catalysts.
基金financial support by MHRD-SPARC-890(2019)UAE for financial support+1 种基金the full financial support by MHRD-SPARC-890(2019)the instrumentation facility utilized from RUSA 2.0 grant No.F.24-51/2014-U,Policy(TNMultiGen)Govt of India Projects。
文摘A feasible approach to rectify the world's energy demand using sustainable development of adequate energy generation and storage technologies in a single channel.In this respect,we made a holistic approach with a bifunctional electrode material to perform effectively in energy generation and storage applications.MoS_(2) nanosheets were produced by the eco-friendly method and reduced graphene oxide is used to prepared by carbon soot which is derived from castor oil.The prepared soot and rGO were combined with MoS_(2) nanosheets using a simple sonication method.The as-prepared sample was introduced in the supercapacitor and DSSC application.The combination MoS_(2)@rGO provides an enhanced conversion efficiency of 11.81%and the reproducibility of DSSC is also studied.Further,MoS_(2)@rGO is used to fabricate an asymmetric supercapacitor to investigate its real-time application.The device produced the maximum power density(1666.6 mW/kg)and energy density(25.69 mWh/Kg)at 1 A/g.The asymmetric supercapacitor device holds a cyclic stability of 81.4%for 5000 cycles and it powered up an LED device for 4 min.
基金the SINOPEC(124015)and the State Key Laboratory of Engines at Tianjin University(No.K2022-06).
文摘The aim of this study was to investigate the oxidation reactivity and behavior of exhaust particulate matter(PM)from diesel engines.PM samples from two diesel engines(1K,CY4102)with different emission levels were collected by a thermophoretic system and a quartz filter.The oxidation reactivity,oxidation behaviors,and physicochemical properties of the PM samples were analyzed using thermogravimetric analysis(TGA),high-resolution transmission electron microscopy(HRTEM),Fourier-transform infrared spectrometry(FTIR),and Raman spectroscopy.The results showed that there was a great difference in the oxidation reactivity of soot particles emitted by the two different diesel engines.A qualitative analysis of the factors influencing oxidation reactivity showed that the nanostructure,degree of graphitization,and relative concentration of aliphatic C—H functional groups were the most important factors,whereas no significant correlation was found between the primary particle size and activation energy of the diesel soot.Based on the oxidation behavior analysis,the diesel soot particles exhibited both internal and surface oxidation modes during the oxidation process.Surface oxidation was dominant during the initial stage,and as oxidation progressed,the mode gradually changed to internal oxidation.Internal oxidation mode of soot particles from the 1K engine was significantly higher than that of CY4102.
基金supported by the National Natural Science Foundation of China(21577088)~~
文摘The composite oxides xAg/Co_(0.93)Ce_(0.07)(x=Ag/(Co+Ce) molar ratio),intended for use as high performance catalytic materials,were successfully prepared via citric acid complexation.The effects of silver on the performance of these substances during soot combustion were subsequently investigated.Under O_2,the 0.3Ag/Co_(0.93)Ce_(0.07) catalyst resulted in the lowest ignition temperature,T_(10),of197 ℃,while the minimum light-off temperature was obtained from both 0.2Ag/Co_(0.93)Ce_(0.07) and0.3Ag/Co_(0.93)Ce_(0.07) in the NO_x atmosphere.These materials were also characterized by various techniques,including H_2,soot and NO_x temperature programmed reduction,X-ray diffraction,and electron paramagnetic resonance,Raman,X-ray photoelectron,and Fourier transform infrared spectroscopic analyses.The results demonstrated that silver significantly alters the catalytic behavior under both O_2 and NO_x,even though the lattice structure of the mixed oxide is not affected.Surface silver oxides generated under the O_2 atmosphere favor soot combustion by participating in the redox cycles between soot and the silver oxide,whereas the AgNO_3 that forms in a NO_x-rich atmosphere facilitates soot abatement at a lower temperature.The inferior activity of AgNO_3 relative to that of Ag_2O results in the different catalytic performance in the presence of NO_x or O_2.
基金supported by the National Natural Science Foundation of China (No. 51806103)the Aeronautical Science Foundation of China (No.201928052002)the Fundamental Research Funds for the Central Universities(No.NT2021007)。
文摘Soot,a product of insufficient combustion,is usually in the form of aggregate. The multi-scattering of soot fractal aggregates has been proved to play an important role in studying the soot radiative properties,which is rarely considered in predicting the radiative heat transfer in combustion flame. In the present study,based on the weighted sum of gray soot fractal aggregate(WSGSA) model,which is used to predict the temperature field and soot aggregates in turbulent diffusion flame,the flame temperature distribution and soot volume fraction distribution under the conditions of the model without considering radiation,the default radiation model in Fluent software and the WSGSA model are calculated respectively. The results show that the flame temperature will be seriously overestimated without considering radiation and the maximum relative discrepancy of flame centerline temperature is about 64.5%. The accuracy will be improved by the default radiation model in the Fluent software,but the flame temperature is still overestimated and the maximum relative discrepancy of flame centerline temperature is about 42.1%. However,more satisfactory results can be obtained by the WSGSA model,and the maximum relative discrepancy of flame centerline temperature is no more than 15.3%. Similar conclusions can also be obtained in studying the temperature distribution along different flame heights. Moreover,the soot volume fraction can be predicted more accurately with the application of the WSGSA model. Both without considering radiation and using the default radiation model in the Fluent software will result in the underestimating of soot volume fraction. All the results reveal that the WSGSA model can be used to predict the temperature and soot aggregates in the CH/air turbulent diffusion flame.
文摘Ag/LaCoO3 perovskite catalysts for soot combustion were prepared by the impregnation method.The structure and physicochemical properties of the catalysts were characterized using X-ray diffraction,N2 adsorption-desorption,H2 temperature-programmed reduction,soot temperatureprogrammed reduction,and X-ray photoelectron spectroscopy.The catalytic activity of the catalysts for soot oxidation was tested by temperature-programmed oxidation in air and in a NOx atmosphere.Metallic Ag particles were the main Ag species.Part of the Ag migrated from the surface to the lattice of the LaCoO3 perovskite,to form La(1-x)AgxCoO3.This increased the amount of oxygen vacancies in the perovskite structure during thermal treatment.Compared with unmodified LaCoO3,the maximum soot oxidation rate temperature(Tp) decreased by 50-70 ℃ in air when LaCoO3 was partially modified by Ag,depending on the thermal treatment temperature.The Tp of the Ag/LaCoO3catalyst calcined at 400℃ in a NOx atmosphere decreased to about 140℃,compared with that of LaCoO3.Ag particles and oxygen vacancies in the catalysts contributed to their high catalytic activity for soot oxidation.The stable catalytic activity of the Ag/LaCoO3 catalyst calcined at 700℃ in a NOx atmosphere was related to its stable structure.
基金supported by the National Natural Science Foundation of China (21477146,21303263)the National High Technology Research and Development Program of China (863 Program,2015AA034603)+2 种基金Beijing Nova Program (Z141109001814072)the Specialized Research Fund for the Doctoral Program of Higher Education of China (20130007120011)the Science Foundation of China University of Petroleum-Beijing (YJRC-2013-13,2462013BJRC003)~~
文摘Au/3DOM(three-dimensionally ordered macroporous) Al2O3 and Au/CeO2/3DOM Al2O3 were prepared using a reduction-deposition method and characterized using scanning electron microscopy,N2 adsorption-desorption,X-ray diffraction,transmission electron microscopy,ultraviolet-visible spectroscopy,temperature-programmed hydrogen reduction,and X-ray photoelectron spectroscopy.Au nanoparticles of similar sizes were well dispersed and supported on the inner walls of uniform macropores.The norminal Au loading is 2%.Al-Ce-O solid solution in CeO2/3DOM Al2O3 catalysts can be formed due to the incorporation of Al^3+ ions into the ceria lattice,which causes the creation of extrinsic oxygen vacancies.The extrinsic oxygen vacancies improved the oxygen-transport properties.The strong metal-support interactions between Au and CeO2 increased the amount of active oxygen on the Au nanoparticle surfaces,and this promoted soot oxidation.The activities of the Au-based catalysts were higher than those of the supports(Al2O3 or CeO2/3DOM Al2O3) at low temperature.Au/CeO2/3DOM Al2O3 had the highest catalytic activity for soot combustion,with T(10),T(50),and T(90) values of 273,364,and 412℃,respectively.
基金supported by the National Natural Science Foundation of China (20833011 and 20803093)the 863 Project of China (2006AA06Z346)
文摘A facile procedure was carried out to prepare macroporous perovskite-type complex oxide catalysts of La1–xKxCo1–yFeyO3(x=0,0.1,y=0,0.1) by using the combined method of organic ligation and solution combustion.This method could ensure the formation of the desired macroporous structures and the desired crystal phases of the prepared catalysts.It was found that the macroporous catalysts showed higher catalytic activities for soot combustion than that of the corresponding nanometric samples,and the macroporous ...
基金supported by the Key Project of National Natural Science Foundation of China (No. 20603016)Liaoning Provincial Science &Technology Project of China (No. 20071074) for financial support of this research
文摘MnOx-CeO2 oxides prepared by complexation-combustion method were used for soot oxidation. The highest conversion rate of soot was obtained on a MnOx-CeO2 oxide prepared under mild acid condition of pH = 4, where the oxidation temperature corresponding to maximum activity was decreased more than 150 ℃ compared with that of un-catalytic soot oxidation. The structure and property of the catalysts were investigated by X-ray powder diffraction (XRD) and temperature programmed reduction (TPR). The results indicated that there were at least two kinds of Mn species present in MnOx-CeO2 catalysts, i.e. Mn ions within CeO2 lattice and high dispersion MnOx on the surface of CeO2. The presence of Mn ions in the CeO2 lattice improved the oxygen vacancy due to the charge difference, and the CeO2 considerably decreased the reduction temperature of MnOx. The capability to activate oxygen through the oxygen exchange between O2 in gas phase and lattice oxygen species in MnOx-CeO2 oxide contributed to the high catalytic activity for the reaction.
基金supported by the National Natural Science Foundation of China(21673142)National Engineering Laboratory for Mobile Source Emission Control Technology(NELMS2017A05)+1 种基金PetroChina Innovation Foundation(2018D-5007-0505)Science Foundation of China University of Petroleum,Beijing(242017QNXZ02,2462018BJC005)~~
文摘Three-dimensional ordered macroporous (3DOM) La1?xKxNiO3 perovskite-type catalysts were successfully prepared by a colloidal crystal template method and characterized by scanning electron microscopy, transmission electron microscopy, high-resolution transmission electron microscopy, energy-dispersive X-ray scattering elemental mapping, X-ray diffraction, Raman and X-ray photoelectron spectroscopy, and temperature-programmed reduction of H2. Further, their catalytic activity in soot combustion was determined by temperature-programmed oxidation reaction. K substitution into the LaNiO3 lattice led to remarkably improved catalytic activity of this catalyst in soot combustion. Amongst various catalysts, La0.95K0.05NiO3 exhibited the highest activity in soot combustion (with its T50 and CO2 S values being 338 °C and 98.2%, respectively), which is comparable to the catalytic activities of Pt-based catalysts under the condition of poor contact between the soot and the catalyst. K-substitution improves the valence state of Ni and increases the number of oxygen vacancies, thereby leading to increased density of surface-active oxygen species. The active oxygen species play a vital role in catalyzing the elimination of soot. The perovskite-type La1?xKxNiO3 nanocatalysts with 3DOM structure without noble metals have potential for practical applications in the catalytic combustion of diesel soot particles.
基金Beijing Municipal Education Committee Program (KM200710017006)
文摘Nanostructure K2NiF4 type oxides La2-xKxCuO4 complex oxides were prepared using the Sol-Gel method, characterized by X-Ray Diffraction (XRD), Fourier Transform Infrared (FT-IR), and Scanning Electron Microscopy (SEM). The catalytic activity for soot combustion was evaluated by the Temperature-Programmed Reaction (TPO) technique. The results demonstrated that the substitution quality of K^+ for La^3+ at the A-site would increase the catalytic activities of La2-xKxCuO4 for soot combustion greatly; the substitution quality affected the structure and catalytic activity obviously. The La1.8K0.2CuO4 complex oxides with tetrahedral structures had the best catalytic activity for soot combustion, and the ignition temperature of soot combustion was lowered from 490 to 320 ℃.
文摘A series of perovskite type oxides and supported Ag catalysts were prepared, and characterized by X ray diffraction (XRD) and X ray photoelectron spectroscopy (XPS). The catalytic activities of the catalysts as well as influencing factors on catalytic activity have been investigated for the simultaneous removal of NOx and diesel soot particulate. An increase in catalytic activity for the selective reduction of NOx was observed with Ag addition in these perovskite oxides, especially with 5% Ag loading. This catalyst could be a promising candidate of catalytic material for the simultaneous elimination of NOx and diesel soot.
基金the financial support from EnerBio Program of Fondation Tuck France,and express their gratitude to Mr
文摘A model is proposed to describe soot formation and oxidation during bio-oil gasification.It is based on the description of bio-oil heating,devolatilization,reforming of gases and conversion of both char and soot solids.Detailed chemistry (159 species and 773 reactions) is used in the gas phase.Soot production is described by a single reaction based on C2H2species concentration and three heterogeneous soot oxidation reactions.To support the validation of the model,three sets of experiments were carried out in a lab-scale Entrained Flow Reactor (EFR) equipped with soot quantification device.The temperature was varied from 1000 to 1400 C and three gaseous atmospheres were considered:default of steam,large excess of steam(H2O/C=8),and the presence of oxygen in the O/C range of 0.075–0.5.The model is shown to accurately describe the evolution of the concentration of the main gas species and to satisfactorily describe the soot concentration under the three atmospheres using a single set of identified kinetic parameters.Thanks to this model the contribution of different mechanisms involved in soot formation and oxidation in various situations can be assessed.
基金supported by the National Natural Science Foundation of China (Grant No. 51675153)the Major Science and Technology Special Project in Anhui (Grant No. 17030901084)
文摘To improve the tribological behavior of biodiesel soot(BDS) in liquid paraffin(LP), the order of biodiesel soot was increased through thermally oxidized treatment at 500 ℃, and the oil solubility was then improved through a modification using oleylamine(OLA). The BDS and thermally oxidized oleylamine-modified BDS(T-BDS-OLA)were characterized through various methods including the use of TG, FETEM, Raman spectroscopy, FTIR, and a zeta potentiometer. The tribological properties and mechanisms of the BDS before and after the thermally oxidized treatment modification were investigated using a ball-on-disc reciprocating tribometer, FESEM, 3 D laser-scanning microscopy, and Raman spectroscopy. The results showed that T-BDS-OLA has a higher degree of order than the BDS, with an onion-like microstructure. BDS and T-BDS-OLA can both improve the antifriction and antiwear properties of LP at a soot content of 0.1%-0.4%, while T-BDS-OLA in LP shows better antifriction and antiwear properties than BDS. The tribological mechanisms can be attributed to both types of soot acting as spacing and roll bearing between the friction surfaces. In addition, the exfoliated graphitic sheets from T-BDS-OLA can form a carbon lubrication layer providing easy sliding.
基金Supported by the National Natural Science Foundation of China(50806023 50721005 50806024) Program of Introducing Talents of Discipline to Universities of China(“111” Project B06019)
文摘A computational study of soot formation in ethylene/air coflow jet diffusion flame at atmospheric pres-sure was conducted using a reduced mechanism and soot formation model. A 20-step mechanism was derived from the full mechanism using sensitivity analysis,reaction path analysis and quasi steady state(QSS) approximation. The model in premixed flame was validated and with computing savings in diffusion flame was applied by incor-porating into a CFD code. Simulations were performed to explore the effect of coflow air on flame structure and soot formation. Thermal radiation was calculated by a discrete-ordinates method,and soot formation was predicted by a simple two-equation soot model. Model results are in good agreement with those from experiment data and detailed mechanism at atmospheric conditions. The soot nucleation,growth,and oxidation by OH are all enhanced by decrease in coflow air velocity. The peak soot volume fraction region appears in the lower annular region be-tween the peak flame temperature and peak acetylene concentration locations,and the high soot oxidation rate due to the OH attack occurs in the middle annular region because of high temperature.