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Both the grand canonical Monte Carlo and molecular dynamics simulation methods are used to investigate the adsorption and diffusion of carbon dioxide confined in a 1.86 nm slit carbon pore at 4 temperatures from subcritical (120 K) to supercritical (313 K) conditions. Layering transition, capillary condensation and adsorption hysteresis are found at 120 K. The microstructure of carbon dioxide fluid in the slit carbon pore is analyzed. The diffusion coefficients of carbon dioxide parallel to the slit wall are significantly larger than those normal to the slit wall. 相似文献
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以MCM-22和MCM-56分子筛为研究对象,考察烃类均三甲苯在MWW型分子筛上的吸附和扩散,同时对分子筛进行XRD、N2吸附和TEM等表征,探究分子筛的结构特性与吸附和扩散之间的关系。研究表明,均三甲苯在MWW型分子筛中的吸附和扩散位置为外表面半超笼。单层和错层结构使MCM-56较MCM-22分子筛拥有更多的外表面酸性位,有利于均三甲苯的吸附。与MCM-22相比,MCM-56分子筛片层结构较薄,焙烧导致晶体外部结构的卷曲使烃类大分子均三甲苯在MCM-56分子筛中的扩散受阻。 相似文献
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氧和氮在炭分子筛上的吸附与扩散 总被引:1,自引:0,他引:1
用重量法研究了氧、氮在两种空分用炭分子筛上的吸附与扩散。结果表明,氧和氮在炭分子筛中的扩散是活化扩散,该过程可用双孔模型进行描述。求得了氧、氮的扩散系数。 相似文献
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《工业催化》2016,(10)
基于巨正则蒙特卡洛和分子动力学,对NH_3-SCR反应体系中吸附质分子(NO与NH_3)在不同拓扑结构沸石分子筛(LTL、FER、LEV、BEA、MOR、FAU、CHA和MFI)上的吸附和扩散特性进行系统研究。结果表明,对于全硅分子筛而言,其分子筛的拓扑结构影响NO与NH_3在分子筛上的吸附,综合吸附量及吸附作用能发现,MFI和LEV分子筛对NO具有较优的吸附特性;MFI和BEA分子筛对NH_3具有较优的吸附特性。研究了Si与Al物质的量比对BEA分子筛吸附性能影响,结果表明,随着Si与Al物质的量比降低,分子筛自由体积逐渐增加,进而有助于分子筛催化剂对NO和NH_3的吸附。采用分子动力学模拟计算NO与NH_3在不同构型全硅分子筛上的扩散系数,发现具有三维直通道且孔径较大的分子筛催化剂有利于NO和NH_3在其孔道内部的扩散,MFI虽然具备三维孔道结构,但由于存在Z型交叉通道,一定程度阻碍了反应物分子的扩散。 相似文献
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分子筛催化过程中反应物、产物以及中间体等分子在分子筛孔道内的扩散行为显著影响催化剂择形催化性能、限域效应、产物选择性和稳定性等.本文总结了近二十年来分子模拟技术在分子筛扩散研究中的应用进展.首先简单介绍以分子动力学模拟为代表的分子筛扩散研究方法,然后介绍了包括烷烃、烯烃和芳烃在内的单组分以及多组分碳氢化合物在分子筛中的... 相似文献
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通过实验测定了二氧化硫(SO2)在HZSM-5型分子筛中的吸附性能,采用巨正则系综Monte Carlo方法建立相应的吸附模型,模拟计算相应的吸附行为。在实验与模拟结果相吻合的基础上,进一步模拟计算了SO2在HZSM-5型分子筛中的吸附等温线、吸附微观构型及吸附热等性质。结果表明:随着硅铝比(摩尔比)的增大,分子筛对SO2的吸附量降低,当硅铝比大于191时,硅铝比对SO2的吸附量影响很小。SO2分子主要吸附在氢离子和Al原子周围。在Al原子周围,SO2分子比较集中,同时发现氢离子的存在会阻碍SO2的扩散。在吸附量相同的条件下,SO2在HZSM-5型分子筛的吸附热随着硅铝比的升高而降低。 相似文献
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B. Montanari A. Vaccari M. Gazzano P. Kßner H. Papp J. Pasel R. Dziembaj W. Makowski T. Lojewski 《Applied catalysis. B, Environmental》1997,13(3-4):205-217
Cu/Mg/Al mixed oxides (CuO = 4.0–12.5 wt%), obtained by calcination of hydrotalcite-type (HT) anionic clays, were investigated in the selective catalytic reduction (SCR) of NO by NH3, either in the absence or presence of oxygen, and their behaviours were compared with that of a CuO-supported catalyst (CuO = 10.0 wt%), prepared by incipient wetness impregnation of a Mg/Al mixed oxide also obtained by calcination of an HT precursor. XRD analysis, UV-visible-NIR diffuse reflectance spectra and temperature-programmed reduction analyses showed the formation, in the mixed oxide catalysts obtained from HT precursors, mainly of octahedrally coordinated Cu2+ ions, more strongly stabilized than Cu-containing species in the supported catalyst, although the latter showed a lower percentage of reduction. The presence of well dispersed Cu2+ ions improved the catalytic performances, although similar behaviours were observed for all catalysts in the absence of oxygen. On the contrary, when the mixture with excess oxygen was fed, very interesting catalytic performances were obtained for the catalyst richest in copper (CuO = 12.5 wt%). This catalyst exhibited a behaviour comparable to that of a commercial V2O5–WO3TiO2 catalyst, without any deactivation phenomena after four consecutive cycles and following 8 h of time-on-stream at 653 K. Decreasing the copper content or increasing the calcination time and temperature led to considerably poorer performances and catalytic behaviours similar to that of the CuO-supported catalyst, due to the side-reaction of NH3 combustion on the free Mg/Al mixed oxide surface. 相似文献
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An IR and microcalorimetric study of adsorption and in situ reaction at room temperature of NO, O2, NO2 and NH3 provides evidence of the involvement of surface nitrate species in this reaction. On the basis of this new experimental evidence a mechanism is proposed for the low temperature SCR reaction of NO by NH3 over titanium silicalites (TS-1). 相似文献
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氨选择性催化还原(NH_3-SCR)是控制NO_x排放的有效手段,对Fe-ZSM-5、Cu-ZSM-5、Mn-ZSM-5及多金属负载的ZSM-5分子筛催化剂在NH_3-SCR脱除NO_x中的性能及影响因素进行总结,并展望ZSM-5分子筛在NO_x脱除中的发展方向。 相似文献
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Manganese–cerium mixed oxide catalysts with different molar ratio Mn/(Mn + Ce) (0, 0.25, 0.50, 0.75, 1) were prepared by citric acid method and investigated concerning their adsorption behavior, redox properties and behavior in the selective catalytic reduction of NOx by NH3. The studies based on pulse thermal analysis combined with mass spectroscopy and FT-IR spectroscopy uncovered a clear correlation between the dependence of these properties and the mixed oxide composition. Highest activity to nitrogen formation was found for catalysts with a molar ratio Mn/(Mn + Ce) of 0.25, whereas the activity was much lower for the pure constituent oxides. Measurements of adsorption uptake of reactants, NOx (NO, NO2) and NH3, and reducibility showed similar dependence on the mixed oxide composition indicating a clear correlation of these properties with catalytic activity. The adsorption studies indicated that NOx and NH3 are adsorbed on separate sites. Consecutive adsorption measurements of the reactants showed similar uptakes as separate measurements indicating that there was no interference between adsorbed reactants. Mechanistic investigations by changing the sequence of admittance of reactants (NOx, NH3) indicated that at 100–150 °C nitrogen formation follows an Eley–Rideal type mechanism, where adsorbed ammonia reacts with NOx in the gas phase, whereas adsorbed NOx showed no significant reactivity under conditions used. 相似文献
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The catalytic performance of the natural zeolite mined from Youngil, Korea was investigated when two types of reductant such as NH3 and hydrocarbons were employed for the reduction of NO. The determination of the structure of the natural zeolite has also been made to identify the type of zeolite and to examine its use as a catalytic material for NO removal reaction. The elementary analysis and electron probe microanalysis of the zeolite revealed that it typically consisted of an aluminosilicate. Although it mainly contains mordenite-type zeolite, heulandite was also included as well as the phases of quartz and feldspar as an impurity in the zeolite. This result could be also confirmed by the X-ray diffraction (XRD) and differential scanning calorimetry (DSC) analyses. It should be noted that the acid treatment of the natural zeolite for its use as a catalytic material is essential for the high performance of NO reduction by selective catalytic reduction (SCR) technology. Copper ion-exchanged natural zeolite catalyst (CuNZA) exhibits a competitive NO reducing activity for the reduction of NO by NH3 as well as hydrocarbons. It can be regarded as a promising catalytic system by NH3 and hydrocarbons for the removal of NOx from stationary and mobile sources. 相似文献
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采用浸渍法制备Re(x)Cu/HZSM-5(Re=La,Ce,Pr,Nd;x=0.5,1,2)系列催化剂。采用XRD和H_2-TPR等对催化剂进行表征,在微型固定床反应器中评价催化剂低温NH_3选择还原NO的催化活性。结果表明,Re(x)Cu/HZSM-5(Re=La,Ce,Pr,Nd;x=0.5,1,2)催化剂具有较好的低温NH_3选择还原NO催化活性,以La为助剂和添加质量分数1%的La(1)Cu/HZSM-5催化剂低温脱硝活性较好,T85和T95分别为153℃和164℃,活性温度窗口宽,(153~362)℃时,NO转化率超过95%。 相似文献
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Photoassisted selective catalytic reduction (photo-SCR) of NO with NH3 in the presence of O2 takes place at room temperature over TiO2 photocatalyst. From the results of photo-SCR reaction over various TiO2, we found that JRC-TIO-11 exhibited the best activity. The reaction activity correlated to the amount of acid sites of TiO2, but did not depend on the specific surface area and crystal diameter. The mixture of rutile and anatase shows higher activity than any of the corresponding TiO2 single phase catalyst. 相似文献
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Katariina Rahkamaa-Tolonen Teuvo Maunula Mari Lomma Mika Huuhtanen Riitta L. Keiski 《Catalysis Today》2005,100(3-4):217-222
The activity of fresh and hydrothermally aged zeolite-based catalysts in the NH3-selective catalytic reduction (SCR) reaction with excess of oxygen were studied. In addition, the effect of NO2 in the gas feed as well as the acidity of the catalysts for the SCR activity was investigated. The studied catalysts were hydrogen, copper, iron and silver ion exchanged ZSM-5, mordenite, beta, ferrierite, and Y-zeolites. The investigation verifies that the zeolite-based catalysts are very promising for the ammonia SCR reaction. Especially, the activity at low and high temperatures was higher than the activity of commercial vanadia-based catalysts. From the studied catalysts, Fe-beta was the most potential one. The presence of NO2 in the inlet flow enhanced significantly the catalytic activity of fresh and hydrothermally aged zeolite catalysts. This suggests that the oxidation of NO to NO2 is probably the rate-determining step for the SCR reaction. 相似文献