Supported manganese oxide catalysts were prepared by incipient wetness impregnation method for methane catalytic combustion, and effects of the support （Al2O3, SiO2 and TiO2） and Mn loading were investigated. These ...Supported manganese oxide catalysts were prepared by incipient wetness impregnation method for methane catalytic combustion, and effects of the support （Al2O3, SiO2 and TiO2） and Mn loading were investigated. These catalysts were characterized with N2 adsorption, X-ray diffraction, X-ray photoelectron spectroscopy and temperature-programmed reduction techniques. Methane conversion varied in a large range depending on supports or Mn loading. Al2O3 supported 15% Mn catalyst exhibited better activity toward methane catalytic oxidation. The manganese state and oxygen species played an important role in the catalytic performance,展开更多
Silicalite-1(S1)foam was functionalized by supporting manganese-cobalt(Mn-Co)mixed oxides to develop the structured hierarchical catalyst(Mn-Co@SlF)for catalytic combustion for the first time.The self-supporting S1 fo...Silicalite-1(S1)foam was functionalized by supporting manganese-cobalt(Mn-Co)mixed oxides to develop the structured hierarchical catalyst(Mn-Co@SlF)for catalytic combustion for the first time.The self-supporting S1 foam with hierarchical porosity was prepared via hydrothermal synthesis with polyurethane(PU)foam as the template.Subsequently,Mn-Co oxide nano sheets were uniformly grown on the surface of S1 foams under hydrothermal conditions to prepare the structured hierarchical catalyst with specific surface area of 354 m^2·g^-1,micropore volume of 0.141 cm^3·g^-1 and total pore volume of 0.217 cm3·g^-1,as well as a good capacity to adsorb toluene(1.7 mmol·g^-1 at p/p0=0.99).Comparative catalytic combustion of toluene of over developed structured catalyst Mn-Co@SlF was performed against the control catalysts of bulk Mn-Co@S1(i.e.,the crushed Mn-Co@SlF)and unsupported Mn-Co oxides(i.e.,Mn-Co).Mn-Co@SlF exhibited comparatively the best catalytic performance,that is,complete and stable toluene conversion at 2480 C over 65 h due to the synergy between Mn-Co oxides and S1 foam,which provided a large number of oxygen vacancies,high redox capacity.In addition,the hierarchical porous structure also improved the accessibility of active sites and facilitated the global mass transfer across the catalyst bed,being beneficial to the catalysis and catalyst longevity.展开更多
A series of Mn-Cu mixed oxide catalysts were prepared by precipitation method. The catalysts were characterized by N2 adsorp- tion-desorption, H2-TPR and XPS. When the loading ratio of manganese oxides to copper oxide...A series of Mn-Cu mixed oxide catalysts were prepared by precipitation method. The catalysts were characterized by N2 adsorp- tion-desorption, H2-TPR and XPS. When the loading ratio of manganese oxides to copper oxides was 8：2 or 7：3, the catalysts possessed better catalytic activity, and benzene was converted completely at 558 K. Results of H2-TPR showed that the loading of a small amount of copper oxides decreased the reduction temperature of catalysts. Results of XPS showed that the loading of a small amount of copper oxides increased the proportion of manganese and defective oxygen on the surface of catalysts, and stabilized manganese at higher oxidation state. And the catalyst with the loading ratio 7：3 was a little worse than 8：2, since the interaction between manganese oxides and copper oxides is too strong, copper oxides migrate to the surface of catalysts and manganese oxides in excess are immerged.展开更多
Heterogeneous catalytic combustion provides a feasible technique for high efficient methane utilization.Perovskites ABO_3-type materials have received renewed attention as a potential alternative for noble metals supp...Heterogeneous catalytic combustion provides a feasible technique for high efficient methane utilization.Perovskites ABO_3-type materials have received renewed attention as a potential alternative for noble metals supported catalysts in catalytic methane combustion due to excellent hydrothermal stability and sulfur resistance. Recently, the emergence of nanostructured perovskite oxides（such as threedimensional ordered nanostructure, nano-array structure） with outstanding catalytic activity has further driven methane catalytic combustion research into spotlight. In this review, we summarize the recent development of nanostructured perovskite oxide catalysts for methane combustion, and shed some light on the rational design of high efficient nanostructured perovskite catalysts via lattice oxygen activation,lattice oxygen mobility and materials morphology engineering. The emergent issues needed to be addressed on perovskite catalysts were also proposed.展开更多
Constructing cerium and manganese bimetallic catalysts with excellent catalytic performance for soot combustion is the research frontier at present.In order to find out the key factors for catalytic soot combustion of...Constructing cerium and manganese bimetallic catalysts with excellent catalytic performance for soot combustion is the research frontier at present.In order to find out the key factors for catalytic soot combustion of Ce-Mn-O catalysts,a series of Ce-Mn-O catalysts with different Ce/Mn proportions were prepared by co-precipitation method.The activity test results show that it increases first and then decreases with the increase of Mn content.The best catalytic activity is obtained for Ce_(0.64)Mn_(0.36) catalyst,which shows a maximum rate temperature(T_(m)) at 306℃ for CO_(2) production in TPO curve.Compared with non-catalytic soot combustion,the T_(m) decreases by mo re than 270℃.Syste matical characte rization results suggest that when the adsorbed surface oxygen,lattice oxygen,specific surface area and total reduction amount of the catalysts reach a certain value,the key factors leading to the difference of catalytic activity become the readily reducible and highly dispersed surface manganese oxide species and contact performance of the external surface.The surface manganese oxide species is beneficial to improving the low-temperature reducibility of catalysts and the porous surface is conducive to the contact between catalyst and soot.Furthermore,for the soot combustion reaction containing only O_(2),the promoting effect of Mn^(4+)is not obvious.展开更多
Most of volatile organic compounds （VOCs） are harmful to the atmosphere and human health. Cata‐lytic combustion is an effective way to eliminate VOCs. The key issue is the availability of high per‐formance catalys...Most of volatile organic compounds （VOCs） are harmful to the atmosphere and human health. Cata‐lytic combustion is an effective way to eliminate VOCs. The key issue is the availability of high per‐formance catalysts. Many catalysts including transition metal oxides, mixed metal oxides, and sup‐ported noble metals have been developed. Among these catalysts, the porous ones attract much attention. In this review, we focus on recent advances in the synthesis of ordered mesoporous and macroporous transition metal oxides, perovskites, and supported noble metal catalysts and their catalytic oxidation of VOCs. The porous catalysts outperformed their bulk counterparts. This excel‐lent catalytic performance was due to their high surface areas, high concentration of adsorbed oxy‐gen species, low temperature reducibility, strong interaction between noble metal and support and highly dispersed noble metal nanoparticles and unique porous structures. Catalytic oxidation of carbon monoxide over typical catalysts was also discussed. We made conclusive remarks and pro‐posed future work for the removal of VOCs.展开更多
Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile...Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds(VOCs).In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom(Co_(1)Ni_(1)/meso-Cr_(2)O_(3))and bimetallic Co and Ni nanoparticle(Co_(NP)Ni_(NP)/mesoCr_(2)O_(3))catalysts adopting the one-pot polyvinyl pyrrolidone(PVP)-and polyvinyl alcohol(PVA)-protecting approaches,respectively.The results indicate that the Co_(1)Ni_(1)/meso-Cr_(2)O_(3)catalyst exhibited the best catalytic activity for n-hexane(C_(6)H_(14))combustion(T_(50%)and T_(90%)were 239 and 263℃ at a space velocity of 40,000 mL g^(-1)h^(-1);apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol^(-1)and 4.3×10^(-7)mol g^(-1)_(cat)s^(-1),respectively),which was associated with its higher(Cr^(5+)+Cr^(6+))amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni_(1) was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co_(1) preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen(MvK)mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→CO_x→CO_(2)and H_(2)O.展开更多
The metal oxides CuMnCe and CeY washcoats on cordierite were prepared using an impregnation method, and then used as support for the active Pt component to prepare the Pt/CuMnCe and Pt/CeY monolithic catalysts for the...The metal oxides CuMnCe and CeY washcoats on cordierite were prepared using an impregnation method, and then used as support for the active Pt component to prepare the Pt/CuMnCe and Pt/CeY monolithic catalysts for the deep oxidation of VOCs. In comparison with the Pt/CeY, CuMnCe, and CeY monolithic catalysts, the Pt/CuMnCe monolithic catalyst shows an excellent performance for toluene,ethyl acetate,and n-hexane oxidation and the Tis low to 216, 200 and 260 ℃,respectively. The active components Pt/PtO and CuMnCe result in a better synergetic interaction, which promote the catalyst reducibility, increase the oxygen mobility, and enhance the adsorption and activation of organic molecules.展开更多
Mo-modified Pd/Al2O3catalysts were prepared by an impregnation method and tested for the catalytic combustion of benzene. The catalysts were characterized by N2 isothermal adsorption, X-ray diffraction（XRD）, X-ray p...Mo-modified Pd/Al2O3catalysts were prepared by an impregnation method and tested for the catalytic combustion of benzene. The catalysts were characterized by N2 isothermal adsorption, X-ray diffraction（XRD）, X-ray photoelectron spectroscopy（XPS）, temperatureprogrammed desorption of NH3（NH3-TPD）, H2temperature-programmed reduction（H2-TPR）, and high-angle annular dark-field scanning transmission electron microscopy（HAADF-STEM）. The results showed that the addition of Mo effectively improved the activity and stability of the Pd/Al2O3catalyst by increasing the dispersion of Pd active components, changing the partial oxidation state of palladium and increasing the oxygen species concentration on the surface of catalyst. In the case of the Pd-Mo/Al2O3catalyst,benzene conversion of 90% was obtained at temperatures as low as 190°C, which was 45°C lower than that for similar performance with the Pd/Al2O3catalyst. Moreover, the 1.0% Pd-5% Mo/Al2O3catalyst was more active than the 2.0% Pd/Al2O3catalyst. It was concluded that Pd and Mo have a synergistic effect in benzene catalytic combustion.展开更多
in this study, cerarnics honeycomb-supported ABO_3 perovskite type oxides were preparedby changing the composition of A and B site cations, and observed their activities for lean CH.oxidation. In the case of change in...in this study, cerarnics honeycomb-supported ABO_3 perovskite type oxides were preparedby changing the composition of A and B site cations, and observed their activities for lean CH.oxidation. In the case of change in A site composition La_(0.3)Sr_(0.2)MnO_3 and La_(0.6)Sr_3MnO_3 is the mostactive catalysts for 1 v% CH_4 and 2 v% CH_4 respectively. But LaMn_(0.5)Co_(0.5)O_3 oxide is the best ac-tive catalyst for 1-2v% CH_4 among the oxides by changing B site compositions of LaBO_3 and su-perior to La_(0.3)Sr_(0.2)MnO_3 and La_(0.6)Sr_(0.4)MnO_3 catalysts.Adding trace Pd improved the activity and characteristics of space velocity for LaMn_(0.5)CO_(0.5)O_3and La_(0.3)Sr_(0.2)MnO_3 Although LaMn_(0.5)Co_(0.5)O_3 +Pd (0.03 wt%) was less active than the Pd catalyst,the activity was more than Pt catalyst at a conversion level below 90%.展开更多
Ventilation air methane is one of available resources with a massive reserve.However,most of ventilation air methane is discharged into the air and pollutes the environment.Catalysts with high temperature resistance(&...Ventilation air methane is one of available resources with a massive reserve.However,most of ventilation air methane is discharged into the air and pollutes the environment.Catalysts with high temperature resistance(>800℃)for ventilation air methane are very essential for utilization of the ventilation air methane.We mainly prepared catalysts CeO_(2)/La_(2)CoFeO_(6)and La_(2)CoFeO_(6)/CeO_(2)and comparative samples CeO_(2)and La_(2)CoFeO_(6)by the simple sol-gel method and calcined them under 9000C,and tested the catalytic performance of ventilation air methane combustion under the condition of 5 vol%H_(2)O.The experimental results show that the light-off temperature(T_(1O))and complete combustion temperature(T_(90))of the ventilation air methane combustion reaction of CeO_(2)/La_(2)CoFeO_(6)catalyst are 417.4 and 587.7℃,respectively.T_(1O)and Tgo of La_(2)CoFeO_(6)/CeO_(2)only reach 425.5 and 615.8℃.The T_(10)and T_(9O)of CeO_(2)/La_(2)CoFeO_(6)are 417.4 and 587.7℃,which are lower than those of La_(2)CoFeO_(6)[T_(10)=452.4℃and T_(90)=673.0℃)and La_(2)CoFeO_(6)/CeO_(2)(T_(10)=425.5℃and T_(90)=615.8℃).Therefore,the catalytic performance of the anti-supported rare earth oxide catalyst CeO_(2)/La_(2)CoFeO_(6)is better than that of La_(2)CoFeO_(6)and supported catalyst La_(2)CoFeO_(6)/CeO_(2).展开更多
A monolithic series of Cu-Mn-Ce oxides supported on cordierites with different Cu/Mn/Ce molar ratios were prepared by the in-situ sol-gel method without any binder. The catalysts were characterized by scanning electro...A monolithic series of Cu-Mn-Ce oxides supported on cordierites with different Cu/Mn/Ce molar ratios were prepared by the in-situ sol-gel method without any binder. The catalysts were characterized by scanning electron microscopy （SEM）, energy dispersive spectrometer （EDS）, X-ray diffraction （XRD）, and Brunauer-Emmett-Teller method （BET） and examined in the catalytic combustion of volatile organic compounds （VOCs）. The results showed that the well-dispersed nanometer particles of mixed oxides adhered firmly to the cordierite surface. Cu0.15Mn0.3Ce55/cordierite was identified as the most active catalyst. Compared with commercial Pd/Al2O3, Cu0.15Mn0.3Ce55/cordierite showed higher activities for the combustion of various types of VOCs, especially for oxy-derivative compounds which could be lighted off below 200 ℃.展开更多
This paper reviews several important factors that influence the synthesis of dumbbell‐like nanoparticles,which can significantly enhance the catalyst activity in catalytic combustion. The dumbbell‐like nanoparticles...This paper reviews several important factors that influence the synthesis of dumbbell‐like nanoparticles,which can significantly enhance the catalyst activity in catalytic combustion. The dumbbell‐like nanoparticles discussed in this article refer to a hetero‐structure with two nanoparticles of different materials in contact with each other. This nanostructure can be considered as a special intermediate between individual spherical nanoparticles and a core–shell nanostructure. Therefore,the synthesis of dumbbell‐like nanoparticles is more difficult than other structures. The controllability of the synthesis process, the nanoparticle size and size distribution, and the morphology of the final products depend on many factors： the seed size and size ratio could be used to influence the controllability of epitaxial growth. The component sizes and size distribution could be varied by carefully controlling the reaction temperature and reaction time. The morphology of the dumbbell‐like nanoparticles is closely related to the solvent polarity, the precursor ratio, the lattice mismatch between the two components, and the surfactant concentration. Some related synthesis methods are also briefly introduced in each section to facilitate understanding. This summary will benefit the development of new dumbbell‐like nanoparticles with various components, which have great potential in catalytic combustion of more dysoxidizable gases.展开更多
基金supported by the New Century Excellent Talent Project of China (NCET-05-0783).
文摘Supported manganese oxide catalysts were prepared by incipient wetness impregnation method for methane catalytic combustion, and effects of the support （Al2O3, SiO2 and TiO2） and Mn loading were investigated. These catalysts were characterized with N2 adsorption, X-ray diffraction, X-ray photoelectron spectroscopy and temperature-programmed reduction techniques. Methane conversion varied in a large range depending on supports or Mn loading. Al2O3 supported 15% Mn catalyst exhibited better activity toward methane catalytic oxidation. The manganese state and oxygen species played an important role in the catalytic performance,
基金financial support from the Key Projects of Natural Science Foundation of Liaoning Province(2018010047-301)the Shenyang National Laboratory for Materials Science for his research(Y8L6641161)+1 种基金financial support from the National Key R&D Program of China(2016YFB0501303)funding from European Union's Horizon 2020 research and innovation programme under grant agreement No.872102。
文摘Silicalite-1(S1)foam was functionalized by supporting manganese-cobalt(Mn-Co)mixed oxides to develop the structured hierarchical catalyst(Mn-Co@SlF)for catalytic combustion for the first time.The self-supporting S1 foam with hierarchical porosity was prepared via hydrothermal synthesis with polyurethane(PU)foam as the template.Subsequently,Mn-Co oxide nano sheets were uniformly grown on the surface of S1 foams under hydrothermal conditions to prepare the structured hierarchical catalyst with specific surface area of 354 m^2·g^-1,micropore volume of 0.141 cm^3·g^-1 and total pore volume of 0.217 cm3·g^-1,as well as a good capacity to adsorb toluene(1.7 mmol·g^-1 at p/p0=0.99).Comparative catalytic combustion of toluene of over developed structured catalyst Mn-Co@SlF was performed against the control catalysts of bulk Mn-Co@S1(i.e.,the crushed Mn-Co@SlF)and unsupported Mn-Co oxides(i.e.,Mn-Co).Mn-Co@SlF exhibited comparatively the best catalytic performance,that is,complete and stable toluene conversion at 2480 C over 65 h due to the synergy between Mn-Co oxides and S1 foam,which provided a large number of oxygen vacancies,high redox capacity.In addition,the hierarchical porous structure also improved the accessibility of active sites and facilitated the global mass transfer across the catalyst bed,being beneficial to the catalysis and catalyst longevity.
基金Project supported by National Natural Science Foundation of China (20773090)the National High Technology Research and Development Program of China (863 Program, 2006AA06Z347)the Youth Fund of Sichuan University (2008119)
文摘A series of Mn-Cu mixed oxide catalysts were prepared by precipitation method. The catalysts were characterized by N2 adsorp- tion-desorption, H2-TPR and XPS. When the loading ratio of manganese oxides to copper oxides was 8：2 or 7：3, the catalysts possessed better catalytic activity, and benzene was converted completely at 558 K. Results of H2-TPR showed that the loading of a small amount of copper oxides decreased the reduction temperature of catalysts. Results of XPS showed that the loading of a small amount of copper oxides increased the proportion of manganese and defective oxygen on the surface of catalysts, and stabilized manganese at higher oxidation state. And the catalyst with the loading ratio 7：3 was a little worse than 8：2, since the interaction between manganese oxides and copper oxides is too strong, copper oxides migrate to the surface of catalysts and manganese oxides in excess are immerged.
基金the financial support from the Recruitment Program of Global Young Experts Start-up Fundthe Program of Introducing Talents of Discipline to Universities of China(111 Program, No. B17019)
文摘Heterogeneous catalytic combustion provides a feasible technique for high efficient methane utilization.Perovskites ABO_3-type materials have received renewed attention as a potential alternative for noble metals supported catalysts in catalytic methane combustion due to excellent hydrothermal stability and sulfur resistance. Recently, the emergence of nanostructured perovskite oxides（such as threedimensional ordered nanostructure, nano-array structure） with outstanding catalytic activity has further driven methane catalytic combustion research into spotlight. In this review, we summarize the recent development of nanostructured perovskite oxide catalysts for methane combustion, and shed some light on the rational design of high efficient nanostructured perovskite catalysts via lattice oxygen activation,lattice oxygen mobility and materials morphology engineering. The emergent issues needed to be addressed on perovskite catalysts were also proposed.
基金Projects supported by the National Natural Science Foundation of China (21962021)Yunnan Fundamental Research Projects(202001AU070121)。
文摘Constructing cerium and manganese bimetallic catalysts with excellent catalytic performance for soot combustion is the research frontier at present.In order to find out the key factors for catalytic soot combustion of Ce-Mn-O catalysts,a series of Ce-Mn-O catalysts with different Ce/Mn proportions were prepared by co-precipitation method.The activity test results show that it increases first and then decreases with the increase of Mn content.The best catalytic activity is obtained for Ce_(0.64)Mn_(0.36) catalyst,which shows a maximum rate temperature(T_(m)) at 306℃ for CO_(2) production in TPO curve.Compared with non-catalytic soot combustion,the T_(m) decreases by mo re than 270℃.Syste matical characte rization results suggest that when the adsorbed surface oxygen,lattice oxygen,specific surface area and total reduction amount of the catalysts reach a certain value,the key factors leading to the difference of catalytic activity become the readily reducible and highly dispersed surface manganese oxide species and contact performance of the external surface.The surface manganese oxide species is beneficial to improving the low-temperature reducibility of catalysts and the porous surface is conducive to the contact between catalyst and soot.Furthermore,for the soot combustion reaction containing only O_(2),the promoting effect of Mn^(4+)is not obvious.
基金supported by the National High Technology Research and Development Program (863 Program,2015AA034603)the National Natural Science Foundation of China (21377008,201077007,20973017)+1 种基金Foundation on the Creative Research Team Construction Promotion Project of Beijing Municipal InstitutionsScientific Research Base Construction-Science and Technology Creation Platform National Materials Research Base Construction~~
文摘Most of volatile organic compounds （VOCs） are harmful to the atmosphere and human health. Cata‐lytic combustion is an effective way to eliminate VOCs. The key issue is the availability of high per‐formance catalysts. Many catalysts including transition metal oxides, mixed metal oxides, and sup‐ported noble metals have been developed. Among these catalysts, the porous ones attract much attention. In this review, we focus on recent advances in the synthesis of ordered mesoporous and macroporous transition metal oxides, perovskites, and supported noble metal catalysts and their catalytic oxidation of VOCs. The porous catalysts outperformed their bulk counterparts. This excel‐lent catalytic performance was due to their high surface areas, high concentration of adsorbed oxy‐gen species, low temperature reducibility, strong interaction between noble metal and support and highly dispersed noble metal nanoparticles and unique porous structures. Catalytic oxidation of carbon monoxide over typical catalysts was also discussed. We made conclusive remarks and pro‐posed future work for the removal of VOCs.
基金supported by the National Natural Science Committee of China-Liaoning Provincial People's Government Joint Fund(U1908204)National Natural Science Foundation of China(21876006,21976009,and 21961160743)+2 种基金Foundation on the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions(IDHT20190503)Natural Science Foundation of Beijing Municipal Commission of Education(KM201710005004)Development Program for the Youth Outstanding-Notch Talent of Beijing Municipal Commission of Education(CIT&TCD201904019)。
文摘Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds(VOCs).In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom(Co_(1)Ni_(1)/meso-Cr_(2)O_(3))and bimetallic Co and Ni nanoparticle(Co_(NP)Ni_(NP)/mesoCr_(2)O_(3))catalysts adopting the one-pot polyvinyl pyrrolidone(PVP)-and polyvinyl alcohol(PVA)-protecting approaches,respectively.The results indicate that the Co_(1)Ni_(1)/meso-Cr_(2)O_(3)catalyst exhibited the best catalytic activity for n-hexane(C_(6)H_(14))combustion(T_(50%)and T_(90%)were 239 and 263℃ at a space velocity of 40,000 mL g^(-1)h^(-1);apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol^(-1)and 4.3×10^(-7)mol g^(-1)_(cat)s^(-1),respectively),which was associated with its higher(Cr^(5+)+Cr^(6+))amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni_(1) was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co_(1) preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen(MvK)mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→CO_x→CO_(2)and H_(2)O.
基金Project supported by the National Natural Science Foundation of China(21506194,21676255)the Natural Science Foundation of Zhejiang Province(Y16B070011)the Commission of Science and Technology of Zhejiang Province(2017C03007,2017C33106)
文摘The metal oxides CuMnCe and CeY washcoats on cordierite were prepared using an impregnation method, and then used as support for the active Pt component to prepare the Pt/CuMnCe and Pt/CeY monolithic catalysts for the deep oxidation of VOCs. In comparison with the Pt/CeY, CuMnCe, and CeY monolithic catalysts, the Pt/CuMnCe monolithic catalyst shows an excellent performance for toluene,ethyl acetate,and n-hexane oxidation and the Tis low to 216, 200 and 260 ℃,respectively. The active components Pt/PtO and CuMnCe result in a better synergetic interaction, which promote the catalyst reducibility, increase the oxygen mobility, and enhance the adsorption and activation of organic molecules.
基金supported by the National High-Tech Research and Development Program (863) of China (No. 2008AA06XK1480855)
文摘Mo-modified Pd/Al2O3catalysts were prepared by an impregnation method and tested for the catalytic combustion of benzene. The catalysts were characterized by N2 isothermal adsorption, X-ray diffraction（XRD）, X-ray photoelectron spectroscopy（XPS）, temperatureprogrammed desorption of NH3（NH3-TPD）, H2temperature-programmed reduction（H2-TPR）, and high-angle annular dark-field scanning transmission electron microscopy（HAADF-STEM）. The results showed that the addition of Mo effectively improved the activity and stability of the Pd/Al2O3catalyst by increasing the dispersion of Pd active components, changing the partial oxidation state of palladium and increasing the oxygen species concentration on the surface of catalyst. In the case of the Pd-Mo/Al2O3catalyst,benzene conversion of 90% was obtained at temperatures as low as 190°C, which was 45°C lower than that for similar performance with the Pd/Al2O3catalyst. Moreover, the 1.0% Pd-5% Mo/Al2O3catalyst was more active than the 2.0% Pd/Al2O3catalyst. It was concluded that Pd and Mo have a synergistic effect in benzene catalytic combustion.
文摘in this study, cerarnics honeycomb-supported ABO_3 perovskite type oxides were preparedby changing the composition of A and B site cations, and observed their activities for lean CH.oxidation. In the case of change in A site composition La_(0.3)Sr_(0.2)MnO_3 and La_(0.6)Sr_3MnO_3 is the mostactive catalysts for 1 v% CH_4 and 2 v% CH_4 respectively. But LaMn_(0.5)Co_(0.5)O_3 oxide is the best ac-tive catalyst for 1-2v% CH_4 among the oxides by changing B site compositions of LaBO_3 and su-perior to La_(0.3)Sr_(0.2)MnO_3 and La_(0.6)Sr_(0.4)MnO_3 catalysts.Adding trace Pd improved the activity and characteristics of space velocity for LaMn_(0.5)CO_(0.5)O_3and La_(0.3)Sr_(0.2)MnO_3 Although LaMn_(0.5)Co_(0.5)O_3 +Pd (0.03 wt%) was less active than the Pd catalyst,the activity was more than Pt catalyst at a conversion level below 90%.
基金Project supported by the National Natural Science Foundation of China(21263008)Inner Mongolia Autonomous Region Innovation Guidance Foundation of China(20170934).
文摘Ventilation air methane is one of available resources with a massive reserve.However,most of ventilation air methane is discharged into the air and pollutes the environment.Catalysts with high temperature resistance(>800℃)for ventilation air methane are very essential for utilization of the ventilation air methane.We mainly prepared catalysts CeO_(2)/La_(2)CoFeO_(6)and La_(2)CoFeO_(6)/CeO_(2)and comparative samples CeO_(2)and La_(2)CoFeO_(6)by the simple sol-gel method and calcined them under 9000C,and tested the catalytic performance of ventilation air methane combustion under the condition of 5 vol%H_(2)O.The experimental results show that the light-off temperature(T_(1O))and complete combustion temperature(T_(90))of the ventilation air methane combustion reaction of CeO_(2)/La_(2)CoFeO_(6)catalyst are 417.4 and 587.7℃,respectively.T_(1O)and Tgo of La_(2)CoFeO_(6)/CeO_(2)only reach 425.5 and 615.8℃.The T_(10)and T_(9O)of CeO_(2)/La_(2)CoFeO_(6)are 417.4 and 587.7℃,which are lower than those of La_(2)CoFeO_(6)[T_(10)=452.4℃and T_(90)=673.0℃)and La_(2)CoFeO_(6)/CeO_(2)(T_(10)=425.5℃and T_(90)=615.8℃).Therefore,the catalytic performance of the anti-supported rare earth oxide catalyst CeO_(2)/La_(2)CoFeO_(6)is better than that of La_(2)CoFeO_(6)and supported catalyst La_(2)CoFeO_(6)/CeO_(2).
基金Project supported by National Natural Science Foundation of China (21107096)Zhejiang Provincial Natural Science Foundation (Y5090202)
文摘A monolithic series of Cu-Mn-Ce oxides supported on cordierites with different Cu/Mn/Ce molar ratios were prepared by the in-situ sol-gel method without any binder. The catalysts were characterized by scanning electron microscopy （SEM）, energy dispersive spectrometer （EDS）, X-ray diffraction （XRD）, and Brunauer-Emmett-Teller method （BET） and examined in the catalytic combustion of volatile organic compounds （VOCs）. The results showed that the well-dispersed nanometer particles of mixed oxides adhered firmly to the cordierite surface. Cu0.15Mn0.3Ce55/cordierite was identified as the most active catalyst. Compared with commercial Pd/Al2O3, Cu0.15Mn0.3Ce55/cordierite showed higher activities for the combustion of various types of VOCs, especially for oxy-derivative compounds which could be lighted off below 200 ℃.
基金supported by the National Natural Science Foundation of China(51376171)Science and Technological Fund of Anhui Province for Outstanding Youth(1508085J01)~~
文摘This paper reviews several important factors that influence the synthesis of dumbbell‐like nanoparticles,which can significantly enhance the catalyst activity in catalytic combustion. The dumbbell‐like nanoparticles discussed in this article refer to a hetero‐structure with two nanoparticles of different materials in contact with each other. This nanostructure can be considered as a special intermediate between individual spherical nanoparticles and a core–shell nanostructure. Therefore,the synthesis of dumbbell‐like nanoparticles is more difficult than other structures. The controllability of the synthesis process, the nanoparticle size and size distribution, and the morphology of the final products depend on many factors： the seed size and size ratio could be used to influence the controllability of epitaxial growth. The component sizes and size distribution could be varied by carefully controlling the reaction temperature and reaction time. The morphology of the dumbbell‐like nanoparticles is closely related to the solvent polarity, the precursor ratio, the lattice mismatch between the two components, and the surfactant concentration. Some related synthesis methods are also briefly introduced in each section to facilitate understanding. This summary will benefit the development of new dumbbell‐like nanoparticles with various components, which have great potential in catalytic combustion of more dysoxidizable gases.
