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1.
First-principles-based kinetic Monte Carlo simulation was used to track the elementary surface transformations involved in the catalytic decomposition of NO over Pt(100) and Rh(100) surfaces under lean-burn operating conditions. Density functional theory (DFT) calculations were carried out to establish the structure and energetics for all reactants, intermediates and products over Pt(100) and Rh(100). Lateral interactions which arise from neighbouring adsorbates were calculated by examining changes in the binding energies as a function of coverage and different coadsorbed configurations. These data were fitted to a bond order conservation (BOC) model which is subsequently used to establish the effects of coverage within the simulation. The intrinsic activation barriers for all the elementary reaction steps in the proposed mechanism of NO reduction over Pt(100) were calculated by using DFT. These values are corrected for coverage effects by using the parametrized BOC model internally within the simulation. This enables a site-explicit kinetic Monte Carlo simulation that can follow the kinetics of NO decomposition over Pt(100) and Rh(100) in the presence of excess oxygen. The simulations are used here to model various experimental protocols including temperature programmed desorption as well as batch catalytic kinetics. The simulation results for the temperature programmed desorption and decomposition of NO over Pt(100) and Rh(100) under vacuum condition were found to be in very good agreement with experimental results. NO decomposition is strongly tied to the temporal number of sites that remain vacant. Experimental results show that Pt is active in the catalytic reaction of NO into N2 and NO2 under lean-burn conditions. The simulated reaction orders for NO and O2 were found to be +0.9 and ?0.4 at 723?K, respectively. The simulation also indicates that there is no activity over Rh(100) since the surface becomes poisoned by oxygen.  相似文献   

2.
甲烷在逆流换热微燃烧器内催化燃烧的数值模拟   总被引:5,自引:0,他引:5  
本文联合使用CFD软件FLUENT和化学反应动力学软件DETCHEM对甲烷-空气混合物在有逆流换热的微燃烧器内的催化燃烧进行了数值模拟。计算中只考虑了甲烷在催化表面上的反应。燃料-空气混合物的当量比为0.4,燃烧器外壁面与环境采用对流换热边界条件。计算结果表明,同时采用逆流换热和表面催化燃烧可以实现常规方法无法实现的甲烷稳定、高效转变。  相似文献   

3.
A large eddy simulation (LES) was conducted of turbulent flow in a channel with a rough wall on one side and a free surface on the other by adopting an anisotropy-resolving subgrid-scale (SGS) model. A shear Reynolds number of Reτ = 395 was used based on the mean friction velocity and channel height. To investigate the grid dependency of the LES results caused by the SGS model, three grid resolutions were tested under the same definition of a roughness shape by using the immersed boundary method. The results obtained were compared with direct numerical simulation data with and without the wall roughness and those without the extra anisotropic term. The primary focus was on how the present anisotropic SGS model with coarser grid resolutions can properly provide the effects of roughness on the mean velocity and turbulent stresses, leading to a considerable reduction of the computational cost of LES.  相似文献   

4.
Fundamental understandings of surface chemistry and catalysis of solid catalysts are of great importance for the developments of efficient catalysts and corresponding catalytic processes, but have been remaining as a challenge due to the complex nature of heterogeneous catalysis. Model catalysts approach based on catalytic materials with uniform and well-defined surface structures is an effective strategy. Single crystals-based model catalysts have been successfully used for surface chemistry studies of solid catalysts, but encounter the so-called “materials gap” and “pressure gap” when applied for catalysis studies of solid catalysts. Recently catalytic nanocrystals with uniform and well-defined surface structures have emerged as a novel type of model catalysts whose surface chemistry and catalysis can be studied under the same operational reaction condition as working powder catalysts, and they are recognized as a novel type of model catalysts that can bridge the “materials gap” and “pressure gap” between single crystals-based model catalysts and powder catalysts. Herein we review recent progress of surface chemistry and catalysis of important oxide catalysts including CeO2, TiO2 and Cu2O acquired by model catalysts from single crystals to nanocrystals with an aim at summarizing the commonalities and discussing the differences among model catalysts with complexities at different levels. Firstly, the complex nature of surface chemistry and catalysis of solid catalysts is briefly introduced. In the following sections, the model catalysts approach is described and surface chemistry and catalysis of CeO2, TiO2 and Cu2O single crystal and nanocrystal model catalysts are reviewed. Finally, concluding remarks and future prospects are given on a comprehensive approach of model catalysts from single crystals to nanocrystals for the investigations of surface chemistry and catalysis of powder catalysts approaching the working conditions as closely as possible.  相似文献   

5.
刘瑞芬  惠治鑫  熊科诏  曾春华 《物理学报》2018,67(16):160501-160501
建立含有关联噪声的双分子-单分子(DM)表面催化反应延迟反馈模型,该模型能同时显示一级和二级非平衡动力学相变,即在一级和二级非平衡动力学相变之间的反应窗口展现.讨论双分子在DM延迟反馈模型中两种吸附机制,即局域和随机吸附模型.研究结果表明:1)外部噪声及两噪声关联性致使反应窗口的宽度收缩;2)内部噪声对非平衡动力学相变行为的影响依赖两噪声关联性,即当两噪声负关联,内部噪声致使反应窗口的宽度变宽;而当两噪声正关联时,内部噪声致使反应窗口的宽度收缩;3)关联噪声致使反应窗口变化对DM模型中一级和二级非平衡动力学相变研究具有重要的科学意义.  相似文献   

6.
This work reports the research carried out by studying aliquots extracted at different axial coordinates from Three Way Catalyst (TWC) monoliths aged under real traffic conditions. Our study focused on the catalytic properties and on several chemical and physical effects caused in the Front and Rear monolith washcoat surfaces by vehicle aging after 60,000 km. Regarding the catalytic properties, all the used aliquots showed poorer activity than their corresponding fresh counterparts. The strongest deactivation was detected for NO and hydrocarbon conversion. CO conversion was less affected and the Rear monolith was as deactivated as the Front one. The characterisation techniques (TXRF, N2 adsorption-desorption isotherms, XRD and H2-TPR) detected - (i) the deposition of P, Zn and Pb; (ii) the formation of CePO4 on account of the Ce from the washcoat; (iii) thermal sintering; (iv) inhibition of the reducibility of Ce oxides - as the main effects brought about by vehicle aging conditions. The deactivation observed at the beginning of the Front monolith was the result of a combination of the former effects. When moving downstream to higher axial coordinates, Pb accumulation and the loss of specific area appeared to be the only probable sources of deactivation.  相似文献   

7.
一种风沙运动的颗粒动力学静电起电模型   总被引:4,自引:0,他引:4       下载免费PDF全文
鲁录义  顾兆林  罗昔联  雷康斌 《物理学报》2008,57(11):6939-6945
基于水的电离理论和颗粒动力学理论,提出了一种风沙运动颗粒碰撞的静电起电模型:颗粒表面覆盖有水分子薄层,颗粒间的碰撞导致能量转移和颗粒温度变化;水电离生成H3O+和OH-离子,当两个温度不同或水分子薄层正(负)离子浓度不同的颗粒相接触时,H3O+比OH-以更快地速度从浓度高的地方向浓度低的地方迁移. 在动力学的模拟计算中采用0.1mm,0.2mm和0.4mm三种粒径的沙粒以示沙 关键词: 风沙运动 静电 颗粒动力学 尘卷风  相似文献   

8.
We study the phase structure of a surface model by using the canonical Monte Carlo simulation technique on triangulated, fixed connectivity, and spherical surfaces with many fine holes. The size of a hole is assumed to be of the order of lattice spacing (or bond length) and hence can be negligible compared to the surface size in the thermodynamic limit. We observe in the numerical data that the model undergoes a first-order collapsing transition between the smooth phase and the collapsed phase. Moreover the Hasudorff dimension H remains in the physical bound, i.e., H < 3 not only in the smooth phase but also in the collapsed phase at the transition point. The second observation is that the collapsing transition is accompanied by a continuous transition of surface fluctuations. This second result distinguishes the model in this paper and the previous one with many holes, whose size is of the order of the surface size, because the previous surface model with large-sized holes has only the collapsing transition and no transition of surface fluctuations.  相似文献   

9.
The planar-type surface wave plasma (SWP) device permits the generation of high-density and uniform processing plasmas via 2.45-GHz microwave power without the application of an external magnetic field. In the present study, the discharge characteristics in the SWP device were analyzed using a two-dimensional numerical simulation code, and the results were compared with experimental observations. The simulation code is based on the finite-difference time-domain (FDTD) method for the microwave field and on the electron fluid model for the argon discharge plasma. Experimental measurements were performed, and they showed that the surface-wave discharge at a filling pressure of 10-100 mtorr has characteristic electron-density distributions that have a peak at approximately 2 cm from the surface. This characteristic of the electron density profiles, as well as the electron temperature profiles in the plasma, is reproduced by the simulation code, albeit with some discrepancies. In order to reduce the effects of these discrepancies, intentional changes in the electron heat conductivity were introduced, and the adiabatic assumption was found to result in a reasonable electron temperature profile. The effects of the alumina window thickness were also investigated in the simulation.  相似文献   

10.
李劲  刘红侠  李斌  曹磊  袁博 《中国物理 B》2010,19(10):107301-107301
Based on the exact resultant solution of two-dimensional Poisson’s equation in strained Si and Si1-X GeX layer, a simple and accurate two-dimensional analytical model including surface channel potential, surface channel electric field, threshold voltage and subthreshold swing for fully depleted gate stack strained Si on silicon-germanium-on-insulator (SGOI) MOSFETs has been developed. The results show that this novel structure can suppress the short channel effects (SCE), the drain-induced barrier-lowering (DIBL) and improve the subthreshold performance in nanoelectronics application. The model is verified by numerical simulation. The model provides the basic designing guidance of gate stack strained Si on SGOI MOSFETs.  相似文献   

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