HDN催化剂氧化烧炭条件的考察

对使用过的工业粒度ＭｏＮｉＰ／Ａｌ２Ｏ３重油加氢脱氮（ＨＤＮ）催化剂，考察了温度、氧含量及气体空速对烧炭速率、烧炭程度和催化剂比表面和孔结构的影响，给出了最佳的烧炭条件和结果。实验表明，常压下，气体空速为１２００ｍｌ·ｇ１·ｈ１时，用含４％Ｏ２的氮气烧炭最佳温度为５００℃，用空气烧炭的最佳温度为４５０℃。即使脱炭率达到９７％，烧炭后的催化剂比表面也比新鲜催化剂的比表面低些。

Synthesis of K-doped three-dimensionally ordered macroporous Mn_(0.5)Ce_(0.5)O_δ catalysts and their catalytic performance for soot oxidation

A series of K-doped Mn0.5Ce0.5Oδ （K-MCO） catalysts with three-dimensionally ordered macroporous （3DOM） structure and different K loadings were successfully synthesized using simple methods. These catalysts exhibited well-defined 3DOM nanostructure, which consisted of extensive interconnecting networks of spherical voids. The effects of the calcination temperature and calcination time on the morphological characteristics and crystalline forms of the catalysts were systematically studied. The catalysts showed high catalytic activity for the combustion of soot. 3DOM 20% K-MCO-4h catalyst, in particular, showed the highest catalytic activity of all of the catalysts studied （e.g., Ts0 = 331 ~C and Smco2 = 95.3%）. The occurrence of structural and synergistic effects among the K, Mn, and Ce atoms in the catalysts was favorable for enhancing their catalytic activity towards the combustion of diesel soot. Furthermore, the temperatures required for the complete combustion of the soot （〈400 ℃） were well within the exhaust temperature range （175-400 ℃）, which means that the accumulated soot can be removed under the conditions of the diesel exhaust gas. These catalysts could therefore be used in numerous practical applications because they are easy to synthesize, exhibit high catalytic activity, and can be made from low cost materials.

Effects of Au-Ce strong interactions on catalytic activity of Au/CeO_2/3DOM Al_2O_3 catalyst for soot combustion under loose contact conditions

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.

Fabrication of ultrafine Pd nanoparticles on 3D ordered macroporous TiO_2 for enhanced catalytic activity during diesel soot combustion

Nanocatalysts consisting of three‐dimensionally ordered macroporous(3DOM)TiO2‐supported ultrafine Pd nanoparticles(Pd/3DOM‐TiO2‐GBMR)were readily fabricated by gas bubbling‐assisted membrane reduction(GBMR)method.These catalysts had a well‐defined and highly ordered macroporous nanostructure with an average pore size of 280 nm.In addition,ultrafine hemispherical Pd nanoparticles(NPs)with a mean particle size of 1.1 nm were found to be well dispersed over the surface of the 3DOM‐TiO2 support and deposited on the inner walls of the material.The nanostructure of the 3DOM‐TiO2 support ensured efficient contact between soot particles and the catalyst.The large interface area between the ultrafine Pd NPs and the TiO2 also increased the density of sites for O2 activation as a result of the strong metal(Pd)‐support(TiO2)interaction(SMSI).A Pd/3DOM‐TiO2‐GBMR catalyst with ultrafine Pd NPs(1.1 nm)exhibited higher catalytic activity during diesel soot combustion compared with that obtained from a specimen having relatively large Pd NPs(5.0 nm).The T10,T50 and T90 values obtained from the former were 295,370 and 415°C.Both the activity and nanostructure of the Pd/3DOM‐TiO2‐GBMR catalyst were stable over five replicate soot oxidation trials.These results suggest that nanocatalysts having a 3DOM structure together with ultrafine Pd NPs can decrease the amount of Pd required,and that this approach has potential practical applications in the catalytic combustion of diesel soot particles.

Three-dimensionally ordered macroporous CeO_2/Al_2O_3-supported Au nanoparticle catalysts: Effects of CeO_2 nanolayers on catalytic activity in soot oxidation

A series of catalysts consisting of three‐dimensionally ordered macroporous(3DOM)x‐CeO2/Al2O3‐supported Au nanoparticles(x=2,10,20,and40wt%)were successfully synthesized using a reduction‐deposition method.These catalysts were characterized using scanning electron microscopy,the Brunauer‐Emmett‐Teller method,X‐ray diffraction,transmission electron microscopy,ultraviolet‐visible spectroscopy,and temperature‐programmed reduction by H2.Au nanoparticles of mean particle size5nm were well dispersed and supported on the inner walls of uniform macropores.The3DOM structure improved the contact efficiency between soot and the catalyst.An Al‐Ce‐O solid solution was formed in the multilayer support,i.e.,x‐CeO2/Al2O3,by the incorporation of Al3+ions into the CeO2lattice,which resulted in the creation of extrinsic oxygen vacancies.Strong interactions between the metal(Au)and the support(Ce)increased the amount of active oxygen species,and this promoted soot oxidation.The catalytic performance in soot combustion was evaluated using a temperature‐programmed oxidation technique.The presence of CeO2nanolayers in the3DOM Au/x‐CeO2/Al2O3catalysts clearly improved the catalytic activities in soot oxidation.Among the prepared catalysts,3DOM Au/20%CeO2/Al2O3showed high catalytic activity and stability in diesel soot oxidation.

Spontaneous coal combustion producing carbon dioxide and water

Gas products from the process of coal oxidization and spontaneous combustion have been studied at different temperatures with FTI spectroscopic tests. With temperatures rising to about 30~100 ℃, water and carbon dioxide gas were formed and from about 105~150 ℃, carbon monoxide was produced. Using the DFT B3LYP method with a 6-311G basis set, the reaction system, where spontaneous combustion between coal and oxygen occurs and produces water and monoxide, has been studied, with the geometric configuration for all stagnation points on the potential reaction energy surface optimized. With a frequency analysis and an IRC method, transient formations were tested. Our results indicate that in the reaction of coal oxidization and spontaneous com-bustion producing carbon dioxide and water, oxygen molecules attack carbon atoms of the terminal of the propyl alcohol group on the lateral chain of benzene rings, which causes this propyl alcohol group to produce the acid (-CH2-CH2-COOH) group and water. This acid group continues its break up into carbon dioxide and the (-CH2-CH3) ethyl group. We have come to the conclusion that this water-and-carbon dioxide-production reaction is spontaneous, based on the observation of the energy released by the reaction.

Experimental Research and Mathematical Modelling for Coal Reburning in Furnace

Reburning technology is one of the most cost-effective NOx reduction strategies for coal combustion systems. In this paper, a nitric oxide submodel incorporated into a comprehensive coal combustion model was developed for predicting NOx reduction in a 93 kW laboratory-scale coal combustion furnace by reburning. This NO submodel, including reburning mechanism, requires the solution of only two transport equations to model the behavior of NO reduction in the reburning process. A number of experiments have been performed in the same furnace, and the experimental data obtained from the optimized reburn configuration was used to validate the model. Measurements and predictions both show above 50% reduction of NO emissions for the optimized reburning process. Profile comparisons show that the predicted temperature and oxygen concentration match well with the measurements, and the general trend of predicted NO concentration is very similar to that measured. The results of this study show that the present nitric oxide submodel depicts quite well the observed behaviour of NO annihilation in the reburning process. It is expected that this usable and computationally economic model represents a useful tool to simulate the gaseous fuel reburning process for the researchers concerned with practical combustors.