The aim of this paper is to analyze the change in the active structure of lignite during the process of lowtemperature oxidation by constructing a molecular structure model for lignite. Using quantum computation combi...The aim of this paper is to analyze the change in the active structure of lignite during the process of lowtemperature oxidation by constructing a molecular structure model for lignite. Using quantum computation combined with experimental results of proximate analysis, ultimate analysis, Fourier transform infrared spectroscopy(FTIR) and X-ray photoelectron spectroscopy(XPS), a structural model for the large molecular structure was constructed. By analyzing the bond lengths in the model molecule, the evolution law for the active structure of lignite was predicted for the process of low-temperature oxidation. In low-temperature oxidation,alkanes and hydroxyls are the primary active structures observed in lignite, though ether may also react. These active functional groups react with oxygen to release heat, thereby speeding up the reaction between coal and oxygen. Finally, the content of various functional groups in the process of lignite low-temperature oxidation was analyzed by infrared analysis, and the accuracy of the model was verified.展开更多
Cu-Mn, Cu-Mn-Ce, and Cu-Ce mixed-oxide catalysts were prepared by a citric acid sol-gel method and then characterized by XRD, BET, H_2-TPR and XPS analyses. Their catalytic properties were investigated in the toluene ...Cu-Mn, Cu-Mn-Ce, and Cu-Ce mixed-oxide catalysts were prepared by a citric acid sol-gel method and then characterized by XRD, BET, H_2-TPR and XPS analyses. Their catalytic properties were investigated in the toluene combustion reaction. Results showed that the Cu-Mn-Ce ternary mixed-oxide catalyst with 1:2:4 mole ratios had the highest catalytic activity, and 99% toluene conversion was achieved at temperatures below 220°C. In the Cu-Mn-Ce catalyst, a portion of Cu and Mn species entered into the Ce O2 fluorite lattice, which led to the formation of a ceria-based solid solution. Excess Cu and Mn oxides existed on the surface of the ceria-based solid solution. The coexistence of Cu-Mn mixed oxides and the ceria-based solid solution resulted in a better synergetic interaction than the Cu-Mn and Cu-Ce catalysts, which promoted catalyst reducibility, increased oxygen mobility, and enhanced the formation of abundant active oxygen species.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
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
As the emission control regulations get stricter,the NO;reduction in the sintering process becomes an important environmental concern owing to its role in the formation of photochemical smog and acid rain.The NOxemiss...As the emission control regulations get stricter,the NO;reduction in the sintering process becomes an important environmental concern owing to its role in the formation of photochemical smog and acid rain.The NOxemissions from the sintering machine account for 48% of total amount from the iron and steel industry.Thus,it is essential to reduce NO;emissions from the sintering machine,for the achievement of clean production of sinter.Ca-Fe oxides,serving as the main binding phase in the sinter,are therefore used as additives into the sintering mixture to reduce NOxemissions.The results show that the NO;reduction ratio achieves 27.76% with 8% Ca-Fe oxides additives since the Ca-Fe oxides can advance the ignition and inhibit the nitrogen oxidation compared with the conventional condition.Meanwhile,the existence of Ca-Fe oxides was beneficial to the sinter quality since they were typical low melting point compounds.The optimal mass fraction of Ca-Fe oxides additives should be less than 8%since the permeability of sintering bed was significantly decreased with a further increase of the Ca-Fe oxides fines,inhibiting the mineralization reaction of sintering mixture.Additionally,the appropriate particle size can be obtained when mixing an equal amount of Ca-Fe oxides additives of-0.5 mm and 0.5-3.0 mm in size.展开更多
基金Supported by the Fundamental Research Funds for the Central Universities(2017XKQY066)
文摘The aim of this paper is to analyze the change in the active structure of lignite during the process of lowtemperature oxidation by constructing a molecular structure model for lignite. Using quantum computation combined with experimental results of proximate analysis, ultimate analysis, Fourier transform infrared spectroscopy(FTIR) and X-ray photoelectron spectroscopy(XPS), a structural model for the large molecular structure was constructed. By analyzing the bond lengths in the model molecule, the evolution law for the active structure of lignite was predicted for the process of low-temperature oxidation. In low-temperature oxidation,alkanes and hydroxyls are the primary active structures observed in lignite, though ether may also react. These active functional groups react with oxygen to release heat, thereby speeding up the reaction between coal and oxygen. Finally, the content of various functional groups in the process of lignite low-temperature oxidation was analyzed by infrared analysis, and the accuracy of the model was verified.
基金the financial support from the Natural Science Foundation of China (No. 21107096)Zhejiang Provincial Natural Science Foundation of China (No. Y14E080008)+1 种基金the Commission of Science and Technology of Zhejiang province (No. 2013C03021)the Specialized Research Fund for the Doctoral Program of Higher Education (No. 20133317110004)
文摘Cu-Mn, Cu-Mn-Ce, and Cu-Ce mixed-oxide catalysts were prepared by a citric acid sol-gel method and then characterized by XRD, BET, H_2-TPR and XPS analyses. Their catalytic properties were investigated in the toluene combustion reaction. Results showed that the Cu-Mn-Ce ternary mixed-oxide catalyst with 1:2:4 mole ratios had the highest catalytic activity, and 99% toluene conversion was achieved at temperatures below 220°C. In the Cu-Mn-Ce catalyst, a portion of Cu and Mn species entered into the Ce O2 fluorite lattice, which led to the formation of a ceria-based solid solution. Excess Cu and Mn oxides existed on the surface of the ceria-based solid solution. The coexistence of Cu-Mn mixed oxides and the ceria-based solid solution resulted in a better synergetic interaction than the Cu-Mn and Cu-Ce catalysts, which promoted catalyst reducibility, increased oxygen mobility, and enhanced the formation of abundant active oxygen species.
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As the emission control regulations get stricter,the NO;reduction in the sintering process becomes an important environmental concern owing to its role in the formation of photochemical smog and acid rain.The NOxemissions from the sintering machine account for 48% of total amount from the iron and steel industry.Thus,it is essential to reduce NO;emissions from the sintering machine,for the achievement of clean production of sinter.Ca-Fe oxides,serving as the main binding phase in the sinter,are therefore used as additives into the sintering mixture to reduce NOxemissions.The results show that the NO;reduction ratio achieves 27.76% with 8% Ca-Fe oxides additives since the Ca-Fe oxides can advance the ignition and inhibit the nitrogen oxidation compared with the conventional condition.Meanwhile,the existence of Ca-Fe oxides was beneficial to the sinter quality since they were typical low melting point compounds.The optimal mass fraction of Ca-Fe oxides additives should be less than 8%since the permeability of sintering bed was significantly decreased with a further increase of the Ca-Fe oxides fines,inhibiting the mineralization reaction of sintering mixture.Additionally,the appropriate particle size can be obtained when mixing an equal amount of Ca-Fe oxides additives of-0.5 mm and 0.5-3.0 mm in size.