介质阻挡放电中烟气相对湿度对脱硫脱硝的影响

为了深入了解NO和SO2在介质阻挡放电反应器中的反应机理,研究了烟气中水蒸气含量对脱硫脱硝效率以及功耗的影响.试验结果表明:烟气中水蒸气含量对介质阻挡放电脱硫脱硝的效率有较大的影响,在N2/NO/SO2/H2O体系中,水蒸气含量的增加会造成放电功耗增大,使NO脱除效率降低、SO2脱除效率明显提高,并对生成产物NO2的浓度也有一定的影响.利用红外光谱分析反应产物,发现NO和SO2在介质阻挡放电反应器中会生成NO2、N2O、HNO3、H2SO4、SO3等物质.     

柴油机排气组分对低温等离子体转化NO的影响

自制了介质阻挡放电型低温等离子体反应器,设计了低温等离子体柴油机模拟排气处理系统,研究了低温等离子体作用下O2、C3H6和水蒸气对NO氧化转化的影响及NO在N2中的还原转化.研究表明:NO在N2气氛中的还原转化率低,能耗大;模拟气中存在O2时,NO向N2的还原转化率降低,NO向NO2的氧化转化率大幅提高;排气中的H2O在低温等离子体作用下生成OH强氧化性粒子,促进NO向NO2的氧化转化;HC的存在可提高NO向NO2的氧化转化,并能有效降低NO向NO2的转化能耗.总之,在柴油机富氧排气环境中,低温等离子体很难直接将NO转化为N2,但可有效地将NO氧化为NO2及硝酸盐,为催化剂催化还原NOx创造条件.     

低温等离子体转化NO的反应动力学研究

针对含有和不含有O2的两种模拟柴油机尾气(NO+N2和NO+N2+O2)在介质阻挡放电反应器中脱除NO的机理进行了分析,建立了利用低温等离子体去除和转化NO的反应动力学模型,并对处理NO的化学过程进行了反应动力学模拟,将模拟结果与自行设计的介质阻挡放电低温等离子体试验装置的试验数据[1]进行对比,验证了该动力学模型的合理性和正确性,并利用该机理模型,对反应体系中其余主要反应物种的浓度进行了模拟研究,得到了这些物种的浓度随停留时间的变化曲线.     

温度对NTP喷射系统处理柴油机模拟排气的影响

为研究低温等离子体活性物质对柴油机有害排放物的去除效果,自行设计了介质阻挡放电型低温等离子体反应器。采用独立于柴油机排气管之外的低温等离子体喷射系统,研究其在不同的柴油机模拟排气温度下,对各排气成分的转化效果。研究结果表明:在低温等离子体环境下,NO主要转化为NO2;O3对NO和HC有较强的氧化作用;高温不利于NO的转化和O3的产生,但有利于HC的氧化,同时产生CO;温度和激励峰峰值电压的变化对CO2浓度基本没有影响。     

低温等离子体净化柴油机尾气中氮氧化物的试验研究

设计了介质阻挡放电试验装置,并分别进行了低温等离子体去除N_2+NO和N_2+NO+O_2两种模拟柴油机尾气中NO的试验研究,得到了NO的去除率以及NO_2、NO_x的浓度随NO的初始浓度、反应器的输入电压以及气体流量而变化的试验曲线,分析了O_2的存在对试验结果的影响。研究表明:利用脉冲放电产生低温等离子体净化模拟尾气,NO的去除率均较高,但在不存在O_2的情况下,NO主要转化成了N_2和O_2;而在存在O_2的情况下,NO主要转化成了NO_2。     

介质阻挡放电条件下添加乙烯对NO氧化影响的试验研究

采用小型试验装置模拟烟气C2H4、O2、N2和NO,利用介质阻挡放电对模拟烟气中的NO进行了氧化试验,并通过改变C2H4、O2的体积分数分析NO的氧化效果.结果表明：添加乙烯可以大幅度提高NO的氧化作用,且随着乙烯体积分数的增加,NO的脱除率逐渐增大;模拟烟气中氧气的体积分数对NO的氧化也有一定程度的影响,随着氧气体积分数的增加,NO的脱除率和NO2的生成率均呈递增的趋势;添加乙烯后,模拟烟气的氧化产物主要是CO;添加C2H4可以大幅度降低脱除NO的反应能耗.     

介质特性对介质阻挡放电脱除NO影响试验研究

在介质阻挡气体放电等离子体条件下,研究阻挡介质特性对NO脱除的影响规律。首先建立了介质阻挡放电等离子体脱硝试验系统,实验研究了Al2O3、CaO、MgO和玻璃等不同介质阻挡下NO的脱除效果,并对此影响规律进行了理论分析。实验结果及理论分析表明,不同阻挡介质所形成的气体放电的电场强度不同,提供给活性粒子的能量也不同,从而对NO的脱除效果具有不同的影响。     

双介质NTP反应器性能试验及空气放电产生NO_x的机理分析

为研究双介质阻挡放电型低温等离子体反应器的性能,对自行设计的双介质阻挡放电型低温等离子体反应器进行静态试验,分析了不同空气流量和工作电压对放电区域温度、NO、NO_2体积分数的影响,采集了不同空气流量和工作电压时放电区域的光谱信息,探讨了低温等离子体化学反应机理。研究结果表明:相同空气流量时,放电区域温度及光谱强度均随工作电压增大而增大,NO体积分数随工作电压呈线性增长关系,NO_2体积分数在空气流量为2L/min和4L/min时随工作电压增大而增大,在6L/min、8L/min和10L/min时几乎保持不变。相同工作电压时,放电区域温度随空气流量增大而减小,光谱强度几乎不随空气流量的改变而改变,NO体积分数随空气流量增大而减小,NO_2体积分数先随空气流量增大而减小,当空气流量大于6L/min后趋于稳定。     

介质阻挡放电低温等离子体对柴油机排放物的影响

以介质阻挡放电(DBD)理论对低温等离子体净化试验装置进行了探讨分析,设计出介质阻挡放电低温等离子体试验装置．利用自制的介质阻挡放电试验装置,采用交流高压、高频电源产生等离子体,对柴油机排放物进行后处理净化试验．结果表明,使用介质阻挡放电低温等离子体可有效脱除柴油机颗粒物(PM),脱除效率可达79％,总碳氢化合物(THC)脱除效率将近20％,同时氮氧化合物(NOx)也有所降低．扫描电子显微镜(SEM)观测结果显示,多数颗粒物的粒径都有所减小．     

等离子体NOx脱除技术概述

等离子体NOx脱除技术作为一种脱硝新工艺,受到世界各国的广泛关注.在叙述了等离子体脱硝的的两种反应机理、等离子体NOx脱除的主要方法(电子束照射法、高压脉冲电晕法、高压直流电晕法、介质阻挡放电法和介质填充床放电法)和等离子体脱硝的反应器结构的基础上,指出了等离子体脱硝方法中的不足,并对等离子体脱硝技术做了展望.     

停留时间对微细化煤焦再燃还原NO效率的影响

以4种细度的混煤(烟煤与褐煤)煤焦作为再燃燃料,用N_2、O_2、CO_2和NO配制模拟烟气,在1300℃的立式管式携带炉中,对停留时间与再燃还原NO效率的关系进行了实验研究,分析了停留时间对再燃还原NO效率的影响机制。结果表明,随着再燃停留时间的延长,NO还原效率增大;煤焦再燃还原NO的适宜停留时间约为0.8～1.0s.     

Mechanism study of nitric oxide reduction by light gases from typical Chinese coals

Coal devolatilization plays an important role in NO formation and reduction. In this study, the coal pyrolysis experiment was performed in an entrained flow reactor to obtain the light gas release characteristics. Six typical Chinese coals with volatile content ranged from 8.8% to 38.3% were studied. The pyrolysis temperature was in the range from 600 to 1200 °C. A significant rank dependence of HCN, CO and C₂H₂/C₂H₄/C₂H₆ was observed and their release for high volatile coals was higher than that for low volatile coals. The HCN–N/NH₃–N ratio ranged from 0.00 to 0.66 for anthracite coals and ranged from 1.63 to 3.90 for high volatile coals. Based on the experimental results, the effect of coal pyrolysis gas on NO reduction in a plug flow reactor at reducing atmosphere was kinetically calculated. The optimal excess air ratio(α_opt) corresponding to the maximum NO removal efficiency decreased with an increase in reduction temperature. For the light gas from the HL coal pyrolyzed at 800 °C, the α_opt decreased from 0.73 to 0.17 when the reduction temperature increased from 927 to 1327 °C. The rate of production analysis indicated that NO removal efficiency was determined by 3 competing reaction paths: NO reduction, NO formation and oxygen consumption by combustible species.     

水蒸气对金属铁与丙烯还原NO的影响

实验研究了水蒸气对丙烯在金属铁作用下还原NO的影响。研究了陶瓷管流动反应器在300~1 100℃时不同条件下水蒸气对脱硝效率的影响,采用XRD对反应后铁样品表面的组分进行分析。结果表明,在N_2氛围条件下,水蒸气使NO的还原效率有所降低。在模拟烟气条件下,水蒸气使NO的还原效率增加,如ξ1=0.9,在1 000℃时,烟气中含有体积分数为7.00%的水蒸气时,NO的还原效率为93.0%,而无水蒸气时NO的还原效率为85.5%。在湿烟气条件SO_2对丙烯在金属铁表面还原NO的效率影响不大,可以忽略。在N_2氛围,有水蒸气时,丙烷在金属铁表面还原NO的效率高于丙烯。但在模拟烟气条件下,有水蒸气时,丙烯在富燃料条件下在金属铁表面还原NO的效率高于丙烷,在富氧条件下则相反。     

Coupling a stochastic soot population balance to gas-phase chemistry using operator splitting

The feasibility of coupling a stochastic soot algorithm to a deterministic gas-phase chemistry solver is investigated for homogeneous combusting systems. A second-order splitting technique was used to decouple the particle population and gas phase in order to solve. A numerical convergence study is presented that demonstrates convergence with splitting step size and particle count for a batch reactor and a perfectly stirred reactor. Simulation results are presented alongside experimental data for a plug flow reactor (PFR) and are compared to a method of moments simulation of a perfectly stirred reactor. Coupling of the soot and chemistry solvers is shown to converge for both systems; however, numerical instabilities present significant challenges in the PSR case. Comparison with the experimental data for a PFR showed good agreement of the soot mass and reasonable agreement of the particle size distribution. Two different soot particle models were used to simulate the PFR: a spherical particle model and a surface-volume model that takes some account of particle shape. The results for the two models are compared. Additionally, the stochastic soot solver is used to track the evolution of the C/H ratio of individual soot particles in the PFR for the first time.     

Nitrogen oxides reduction by liquid petroleum gas over Co–Ce–Ti catalysts in a simulated rotary reactor

Hydrocarbons could be used as the reductant for elimination of NO_x emissions. Liquid petroleum gas, with higher carbon hydrocarbons and cheaper costs, may be of practical value as reducing agents. Due to the consumption of hydrocarbons by oxygen, the NO_x reduction efficiency is significantly inhibited by oxygen in the flue gas. In this research, a novel rotary reactor, realizing the alternating cycle of adsorption zone and reduction zone, was proposed to overcome this negative effect. Co–Ce–Ti mixed oxide catalysts synthesized by a sol–gel method were tested in a simulated rotary reactor for NO_x removal by liquid petroleum gas and characterized by SEM, BET, XRD and XPS. The results showed that catalysts exhibited better NO conversion efficiency at higher temperature but were highly susceptible to oxygen. Catalysts achieved nearly full removal of NO_x from flue gas at 300 °C in a simulated rotary reactor, and 300 °C is considered to be the most optimum temperature with lower energy consumption and excellent flue gas purification performance.     

再燃过程中HCN对NOx还原的重要性

在降低ＮＯｘ排放的一系列方法中,燃料再燃是重要措施之一。通过对再燃区不同的空气过量系数和再燃温度条件下的数值计算,研究了天然气（ＣＨ４）作为再燃燃料时ＨＣＮ对ＮＯ再燃过程和再燃率的影响。再燃区模拟烟气成分为：ＣＯ２＝１６．８％,Ｏ２＝２％,ＮＯ＝０．１％和平衡气体Ｎ２。研究发现,再燃燃料中含氮组分的存在,以及再燃区的工况条件都对ＮＯｘ的再燃率有很大的影响。因此,在实施降低ＮＯｘ排放的再燃技术过程中     

Research on the dynamic process of NO heterogeneous and homogeneous reduction with cement raw meal in vertical tubular reactor

A certain amount of coal is supplied at the outlet of cyclone suspension preheater C5 to reduce NO_x through homogenous and heterogenous reduction. Subsequently, char enters into precalciner and burnt out, while volatiles are burnt out after being exposed to over-fire air. Such process, i.e. the high-order reduction of NO_x, has been verified as a high-efficiency control mean for NO_x emission in cement industry. The dynamic processes of NO reduction by volatiles and coal in absence of O₂ have been studied in the vertical tubular reactor. The effects of cement raw meal and reaction temperature on NO heterogenous and homogeneous reduction were analyzed. The results suggested that the reactions were classified into two types (the homogeneous and the heterogeneous reactions), characterizing the reactions in the gas phase and the reactions between the gas phase and the particle surfaces, respectively. Homogeneous reduction was the critical mechanism during the earlier stage of reaction. Then, the char reduction mechanism became more efficient. Raw meal could promote NO heterogeneous reduction because CaO, as the carrier, could accelerate the transfer of oxygen atom. However, raw meal could significantly inhibit NO homogeneous reduction. CaO, as reactant, could change the pathways of cleavage reaction; the products of new reaction path contained a neutral molecule and an anion, instead of unstable free radicals which are actually vital to reduce NO in the gas phase. High temperature could facilitate homogeneous and heterogenous NO reduction. The catalysis of CaO on heterogenous had the optimum temperature (850 °C), and it could restrain the effect of heat inactivation. And CaO could significantly inhibit NO homogeneous reduction at the whole operation temperature.     

吸附协同等离子体作用的顺序式锅炉烟气脱硫脱硝工艺

针对锅炉（烟厂用锅炉等）烟气，提出了一种具有高脱除率和低能耗的顺序式烟气脱硫脱硝工艺。即在吸附剂颗粒表面利用活性N原子还原NO产生的活性0原子来继续氧化二氧化硫生成SO3，并通过化学反应动力学模拟研究了该工艺的可行性。NO／SO2/N2系统等离子体脱硫脱硝的模拟结果显示：NO有显著的脱除效果，SO2有少量转化为SO3，SO2脱除率随停留时间增加而增加。研究结果表明顺序式烟气脱硫脱硝是可行的，关键在于选用合适吸附剂来控制其表面的O2浓度和停留时间。     

A novel process simulation model for hydrogen production via reforming of biomass gasification tar

Process modeling and simulation are very important for new designs and estimation of operating variables. This study describes a new process for the production of hydrogen from lignocellulosic biomass gasification tars. The main focus of this research is to increase hydrogen production and improve the overall energy efficiency of the process. In this study, Aspen HYSYS software was used for simulation. The integration structure presented in this research includes sections like tar reforming and ash separation (Ash), combined heat and power cycle (CHP), hydrogen sulfide removal unit (HRU), water-gas shift (WGS) reactor, and gas compression as well as hydrogen separation from a mixture of gases in pressure swing adsorption (PSA). It was found that the addition of CHP cycle and the use of the plug flow reactor (PFR) model, firstly, increased the overall energy efficiency of the process by 63% compared to 29.2% of the base process. Secondly it increased the amount of hydrogen production by 0.518 kmol (H2)/kmol Tar as compared with 0.475 of the base process. Process analysis also demonstrated that the integrated process of hydrogen production from biomass gasification tars is carbon neutral.     

Catalytic reduction of nitrogen oxide by carbon monoxide,methane and hydrogen over transition metals supported on BEA zeolites

Different metals were impregnated onto BEA zeolites supports by ion-exchanging method to prepare catalysts for NO reduction. Activities of the prepared catalysts were then examed in a fixed bed reactor for NO reduction by CO, H₂, and CH₄. Experimental results indicated that Cu-BEA shows high catalytic activity for NO reduction by CO and H₂ at 300 °C–500 °C, while Co-BEA shows high catalytic activity of NO reduction by CH₄ at 400 °C–500 °C. Activities of all the catalysts increase as the temperature rises. Then characterization of H₂-TPR, XED, XPS and BET were conducted used to investigate the physical and chemical properties of these BEA catalysts. In-situ Fourier transform-infrared spectroscopy was also used to study the mechanism of the reaction of NO reduction by CO, CH₄ and H₂. The reason of different activities over different BEA catalysts was then carefully explored.