Series of Mn/TiO2 catalysts modified with various contents of Nd for low-temperature SCR were synthesized.It can be found that the appropriate amount of Nd can markedly reduce the take-off temperature of Mn/TiO2 catal...Series of Mn/TiO2 catalysts modified with various contents of Nd for low-temperature SCR were synthesized.It can be found that the appropriate amount of Nd can markedly reduce the take-off temperature of Mn/TiO2 catalyst to 80℃and NOx conversion is stabilized over 90%in the wide temperature range of 100-2600 C.0.1 Nd-Mn/Ti shows higher N2 selectivity and better SO2 resistance than Mn/Ti catalyst.The results reveal that Nd-doped Mn/TiO2 catalyst exhibits larger BET surface area and better dispersion of active component Mn2O3.XPS results indicate that the optimal 0.1 Nd-Mn/Ti sample possesses higher concentration of Mn4+and larger amount of adsorbed oxygen at the surface compared with the unmodified counterpart.In situ DRIFTS show that the surface acidity is evidently increased after adding Nd,especially,the Lewis acid sites,and the intermediate(-NH2)is more stable.The reaction mechanism over Mn/Ti and 0.1 Nd-Mn/Ti catalysts obey the Eley-Rideal(E-R)mechanisms under low temperature reaction conditions.H2-TPR results show that Nd-Mn/TiO2 catalyst exhibits better lowtemperature redox properties.展开更多
The reduction kinetics and mechanisms of hematite ore with various particle sizes with hydrogen at low temperature were studied using the thermogravimetric analysis. At the same temperature, after the particle size of...The reduction kinetics and mechanisms of hematite ore with various particle sizes with hydrogen at low temperature were studied using the thermogravimetric analysis. At the same temperature, after the particle size of powder decreases from 107. 5μm to 2. 0 μm, the surface area of the powder and the contact area between the powder and gas increase, which makes the reduction process of hematite accelerate by about 8 times, and the apparent activation energy of the reduction reaction drops to 36.9 kJ/mol from 78. 3 kJ/mol because the activity of ore powder is improved by refining gradually. With the same reaction rate, the reaction temperature of 6.5 μm powder decreases by about 80 ℃ compared with that of 107. 5 μm powder. Thinner diffusion layer can also accelerate the reaction owing to powder refining. The higher the temperature, the greater is the peak of the reduction rate; at the same temperature, the greater the particle size, the smaller is the peak value of the reduction rate; both inner diffusion and interface chemical reaction play an important role in the whole reaction process.展开更多
A detailed mechanism covering 545 species and 3105 reactions for high-temperature combustion of n-propylcyclohexane（n-PCH）, generated via a mechanism generation program（ReaxGen） developed by our research group, wa...A detailed mechanism covering 545 species and 3105 reactions for high-temperature combustion of n-propylcyclohexane（n-PCH）, generated via a mechanism generation program（ReaxGen） developed by our research group, was validated in this study. A semi-detailed mechanism involved with 195 species and 573 reactions and a skeletal mechanism concerned with 108 species and 393 reactions were obtained by means of rate-of-production analysis and path flux analysis（PFA）, respectively. In order to validate the reliability of these mechanisms, ignition delay time, laminar flame speed and concentration profiles of important species were simulated with the help of CHEMKIN software. Numerically predicted results of our mechanisms are in very good agreement with available experimental data. Finally, major reaction pathways of n-PCH combustion and important reactions during the combustion process were investigated by reaction pathway analysis and sensitivity analysis, respectively. The results indicate that these mechanisms are reliable for describing the auto-ignition characteristics of n-PCH. These mechanisms would also be helpful to computational fluid dynamics（CFD） for engine design. Moreover, this systematic approach used in our study, which combines mechanism construction, simplification, validation and analysis for n-PCH, may also be employed to construct mechanisms for the high-temperature combustion of other cycloalkanes with one ring.展开更多
ZrB2 powders were synthesized via a borothermal reduction reaction of ZrO2 with the assistance of NaCl under a flowing Ar atmosphere. The optimal temperature and reaction time were 1223 K and 3 h, respectively. Compar...ZrB2 powders were synthesized via a borothermal reduction reaction of ZrO2 with the assistance of NaCl under a flowing Ar atmosphere. The optimal temperature and reaction time were 1223 K and 3 h, respectively. Compared with the reactions conducted without the addition of NaCl, those performed with the addition of an appropriate amount of NaCl finished at substantially lower temperatures. However, the addition of too much NaCl suppressed this effect. With the assistance of NaCl, a special morphology of polyhedral ZrB2 particles covered with ZrB2 nanosheets was obtained. Moreover, the experimental results revealed that the special morphology was the result of the combined effects of B2O3 and NaCl. The formation of the special microstructure is explained on the basis of the “dissolution–recrystallization” mechanism.展开更多
基金Project supported by the Key Research and Development Projects of Jiangsu Province(BE2017716)National Key R&D Program of China(2017YFB0603201)Environmental Nonprofit Industry Research subject(2016YFC0208102)。
文摘Series of Mn/TiO2 catalysts modified with various contents of Nd for low-temperature SCR were synthesized.It can be found that the appropriate amount of Nd can markedly reduce the take-off temperature of Mn/TiO2 catalyst to 80℃and NOx conversion is stabilized over 90%in the wide temperature range of 100-2600 C.0.1 Nd-Mn/Ti shows higher N2 selectivity and better SO2 resistance than Mn/Ti catalyst.The results reveal that Nd-doped Mn/TiO2 catalyst exhibits larger BET surface area and better dispersion of active component Mn2O3.XPS results indicate that the optimal 0.1 Nd-Mn/Ti sample possesses higher concentration of Mn4+and larger amount of adsorbed oxygen at the surface compared with the unmodified counterpart.In situ DRIFTS show that the surface acidity is evidently increased after adding Nd,especially,the Lewis acid sites,and the intermediate(-NH2)is more stable.The reaction mechanism over Mn/Ti and 0.1 Nd-Mn/Ti catalysts obey the Eley-Rideal(E-R)mechanisms under low temperature reaction conditions.H2-TPR results show that Nd-Mn/TiO2 catalyst exhibits better lowtemperature redox properties.
基金Sponsored by National Natural Science Foundation of China(50474006)National Science and Technology Support Program for the 11th Five-Year Plan(2006BAE03A12,2006BAE03A05)
文摘The reduction kinetics and mechanisms of hematite ore with various particle sizes with hydrogen at low temperature were studied using the thermogravimetric analysis. At the same temperature, after the particle size of powder decreases from 107. 5μm to 2. 0 μm, the surface area of the powder and the contact area between the powder and gas increase, which makes the reduction process of hematite accelerate by about 8 times, and the apparent activation energy of the reduction reaction drops to 36.9 kJ/mol from 78. 3 kJ/mol because the activity of ore powder is improved by refining gradually. With the same reaction rate, the reaction temperature of 6.5 μm powder decreases by about 80 ℃ compared with that of 107. 5 μm powder. Thinner diffusion layer can also accelerate the reaction owing to powder refining. The higher the temperature, the greater is the peak of the reduction rate; at the same temperature, the greater the particle size, the smaller is the peak value of the reduction rate; both inner diffusion and interface chemical reaction play an important role in the whole reaction process.
基金Supported by the National Natural Science Foundation of China （No.91016002）.
文摘A detailed mechanism covering 545 species and 3105 reactions for high-temperature combustion of n-propylcyclohexane（n-PCH）, generated via a mechanism generation program（ReaxGen） developed by our research group, was validated in this study. A semi-detailed mechanism involved with 195 species and 573 reactions and a skeletal mechanism concerned with 108 species and 393 reactions were obtained by means of rate-of-production analysis and path flux analysis（PFA）, respectively. In order to validate the reliability of these mechanisms, ignition delay time, laminar flame speed and concentration profiles of important species were simulated with the help of CHEMKIN software. Numerically predicted results of our mechanisms are in very good agreement with available experimental data. Finally, major reaction pathways of n-PCH combustion and important reactions during the combustion process were investigated by reaction pathway analysis and sensitivity analysis, respectively. The results indicate that these mechanisms are reliable for describing the auto-ignition characteristics of n-PCH. These mechanisms would also be helpful to computational fluid dynamics（CFD） for engine design. Moreover, this systematic approach used in our study, which combines mechanism construction, simplification, validation and analysis for n-PCH, may also be employed to construct mechanisms for the high-temperature combustion of other cycloalkanes with one ring.
基金financially supported by the Fundamental Research Funds for the Central Universities, China (No. FRF-GF-17-B41)
文摘ZrB2 powders were synthesized via a borothermal reduction reaction of ZrO2 with the assistance of NaCl under a flowing Ar atmosphere. The optimal temperature and reaction time were 1223 K and 3 h, respectively. Compared with the reactions conducted without the addition of NaCl, those performed with the addition of an appropriate amount of NaCl finished at substantially lower temperatures. However, the addition of too much NaCl suppressed this effect. With the assistance of NaCl, a special morphology of polyhedral ZrB2 particles covered with ZrB2 nanosheets was obtained. Moreover, the experimental results revealed that the special morphology was the result of the combined effects of B2O3 and NaCl. The formation of the special microstructure is explained on the basis of the “dissolution–recrystallization” mechanism.
