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1.
Wet scrubbing combined with ozone oxidation has become a promising technology for simultaneous removal of SO2 and NOx in exhaust gas. In this paper, a new 20-species, 76-step detailed kinetic mechanism was proposed between O3 and NOx. The concentration of N2O5 was measured using an in-situ IR spectrometer. The numerical evaluation results kept good pace with both the public experiment results and our experiment results. Key reaction parameters for the generation of NO2 and N2O5 during the NO ozonation process were investigated by a numerical simulation method. The effect of temperature on producing NO2 was found to be negligible. To produce NO2, the optimal residence time was 1.25 sec and the molar ratio of O3/NO about 1. For the generation of N2O5, the residence time should be about 8 sec while the temperature of the exhaust gas should be strictly controlled and the molar ratio of O3/NO about 1.75. This study provided detailed investigations on the reaction parameters of ozonation of NOx by a numerical simulation method, and the results obtained should be helpful for the design and optimization of ozone oxidation combined with the wet flue gas desulfurization methods (WFGD) method for the removal of NOx.  相似文献   

2.
A laboratory-based atmospheric flow chamber, using realistic presentation rates of SO2, NO and NO2 pollutants directed to various dry and wetted surfaces, has been employed to quantify the effects of the individual pollutants and the role of ozone as an oxidant. For the individual pollutant gases reacting with stone surfaces coming to equilibrium with 84% relative humidity (r.h.), chemical reaction in the presence of a moisture film proceeds and the extent of this reaction is related to pollutant gas solubility in the moisture film, i.e. SO2 > NO2 > NO. After dissolution in the moisture film, the pollutant gases are oxidized in the presence of catalysts associated with the stones. The additional presence of ozone promotes oxidation of the pollutant gases and thus their reaction with the stones. For SO2 pollutant, oxidation in the gas phase is not significant compared with that in the moisture film, with enhanced oxidation in the presence of catalysts. Ozone increases oxidation of NO and NO2 pollutant gases in the gas phase and moisture film; however, the oxidation of SO2 in the moisture film is more significant than that of NO or NO2. Wetting of the stone surfaces, in the absence of ozone, reveals the consistently greatest chemical reaction with SO2 compared with NO and NO2, which is related to SO2 solubility, oxidation in the presence of catalysts and production of sulphuric acid. Generally similar behaviour is evident of NO and NO2, but NO shows a reduced extent of chemical reaction, implying that its oxidation in surface water, in the presence of catalytic species, is slow and hence the reactants are lost in the form of run-off. In the additional presence of ozone, the SO2 pollutant gas gives rise to enhanced chemical reaction, whereas both NO and NO2 show lower extents of chemical reaction than for the dry stones. This arises from the relatively slow conversion of N2O5 in the liquid phase to nitric acid, allowing loss of reactants in run-off.  相似文献   

3.
The rate of non-linear chemical reactions in a dispersing plume, such as the formation of NO2, is discussed on the basis of various models and measurements of the oxidation rate of NO. Results of calculations with four different reactive plume models are compared with a set of plume measuremeent and discussed in terms of the ration of the time scales of physical (Tp) and chemical processes (Tc), the Damköhler number:Tp/Tc. In modelling a fast non-linear chemical reaction an interaction between physical processes of dispersion and mixing and chemical reactions can be expected. Models may differ in that they assume either chemical equilibrium (Tp/Tc⪢1) or no chemical equilibbrium (Tp/Tc⪡1).From our study it is concluded that for the first 5 km from a stack concentrations in the plume change more rapidly by dilution due to dispersion of the plume than by chemical reactions. Farther off it is the other way around and the chemistry is fast enough to achieve chemical equilibrum in the plume parcels.Conversion of NO is then inhibited by the mixing rate of the plume with its surrounding air. To incorporate the mixing rate of the plume correctly into a model, in principle the concentration distribution in a momentary plume has to be used. If a non-linear chemical reaction is modelled it is therefore important to establish the averaging times on which the dispersion parameters in the model are based. The contribution of plume meandering to dispersion, which is especially important in the daytime, can be eliminated by taking shorter averaging times. This leads to a marked improvement of modelling results. Further research is required to investigate how the contribution of fluctuations in the concentrations around the mean has to be incorporated into a model of a chemically reactive plume.  相似文献   

4.
夏季城市大气O3浓度影响因素及其相关关系   总被引:22,自引:3,他引:19  
利用2003年夏季济南市区近地面大气O3、相关前体物和气象因素等观测数据,研究了O3浓度的分布特征及时间变化规律,分析了7月份O3与NO、NO2和CO等前体物及太阳辐射和气温气象条件的相关性.结果表明,济南市区夏季O3污染比较严重,观测期间各污染物O3、NO、NO2、NOx和CO浓度都相对较高,昼间O3与各前体物的浓度呈较好的负相关关系,与太阳辐射具有非常明显的相关性,而与气温的相关性不明显.根据以上分析结果,利用回归分析方法,建立了昼间O3浓度与前体物、气象因子之间的相关模式,结果表明O3浓度的计算值与观测值符合性较好.  相似文献   

5.
The effect of concentration fluctuations on the modelling of non-linear chemical reactions in the atmosphere will be considerable when hourly mean dispersion parameters are used. This effect can be reduced by introducing instantaneous dispersion parameters, as will be shown in this paper for the modelling of the oxidation of NO emited into an O3 containing atmosphere.We used the results of atmospheric tracer gas experiments to derive the dimensions of the instanteneous plume. With these results model calculations were carried out for the NOO3 reaction. Results were compared with airborne measurements of NO oxidation in the plumes of Dutch power plants.The introduction of the instantaneous plume leads to better agreement between model calculations and measurements. It is also found that the deviation from photochemical equilibrium in the plume is considerably smaller when instantaneous, instead of hourly, mean dispersion parameters are used. The dimension of the instantaneous plume did not show a dependence on atmospheric stability.  相似文献   

6.
王峰  汪健伟  杨宁  翟菁  侯灿 《环境科学》2021,42(12):5713-5722
本文基于三维区域空气质量模式WRF-Chem,通过修改模式化学模块,量化输出过程量和诊断量,提供了一种定量分析挥发性有机化合物(VOCs)源强不确定性对O3生成影响的方法.为无法定量计算VOCs源强导致的臭氧生成率[P(O3)]偏差,以及由此对O3体积分数分布和污染控制相关联的VOCs敏感区和NOx 敏感区分布的误判提供了方法参考.采用标准统计参数对WRF-Chem模式的气象场与污染场模拟性能进行了评估,相关指标均优于前人结果.以INTEX-B(intercontinental chemical transport experiment-phase B)人为源、FINNv1(fire inventory from NCAR version 1)生物质燃烧源和 MEGAN(model of emissions of gases and aerosols from nature)生物源作为基准源,并以卫星观测数据作为约束,对排放源进行改进,评估了源改进前后臭氧生成率[P(O3)]、O3体积分数和O3控制敏感区指标(Ln/Q)的变化情况.仅人为VOCs(AVOCs)源增加68%后,P(O3)模拟峰值增升比例达13%~82%,以北京观测站点为例,P(O3)模拟月均峰值增加42%(22.5×10-9 h-1).对P(03)形成贡献比例最大的主要化学反应是HO2+NO(占比约68%),AVOCs源增加68%后,该反应贡献比例下降至65%.在改进源下,P(O3)普遍增加达到2×10-9~4×10-9h-O3各季节增幅较大的区域均主要集中在京津冀、长三角和珠三角中心城市及周边区域,与我国大型城市区基本都是VOCs敏感区的结论一致.整体而言,VOCs源强改进后,Nox敏感区O3体积分数增加幅度不大,不超过4×10-9,而部分VOCs敏感区增幅超过20 x10-9.VOCs源强的不确定性会影响O3形成过程中Nox和VOCs敏感区的判断,特别是VOCs源强明显低估会夸大VOCs敏感区的范围,从而降低O3调控对策的有效性.  相似文献   

7.
Most previous O3 simulations were based only on gaseous phase photochemistry. However, some aerosol-related processes, namely, heterogeneous reactions occurring on the aerosol surface and photolysis rate alternated by aerosol radiative influence, may affect O3 photochemistry under high aerosol loads. A three-dimensional air quality model, Models-3/Community Multi-scale Air Quality-Model of Aerosol Dynamics, Reaction, Ionization, and Dissolution, was employed to simulate the effects of the above-mentioned processes on O3 formation under typical high O3 episodes in Beijing during summer. Five heterogeneous reactions, i.e., NO2, NO3, N2O5, HO2, and O3, were individually investigated to elucidate their effects on O3 formation. The results showed that the heterogeneous reactions significantly affected O3 formation in the urban plume. NO2 heterogeneous reaction increased O3 to 90 ppb, while HO2 heterogeneous reaction decreased O3 to 33 ppb. In addition, O3 heterogeneous loss decreased O3 to 31 ppb. The effects of NO2, NO3, and N2O5 heterogeneous reactions showed opposite O3 concentration changes between the urban and extra-urban areas because of the response of the reactions to the two types of O3 formation regimes. When the aerosol radiative influence was included, the photolysis rate decreased and O3 decreased significantly to 73 ppb O3. The two aerosol-related processes should be considered in the study of O3 formation because high aerosol concentration is a ubiquitous phenomenon that affects the urban- and regional air quality in China.  相似文献   

8.
Large-eddy simulation (LES) is used to study the dispersion of a passive scalar downwind of a localized source in a convective boundary layer. The LES turbulent velocity statistics are compared with laboratory data and other LES studies. Two scalar source heights at 0.25 zi and 0.50 zi are considered, where zi is the inversion height, and the mean concentration fields are compared with the experimental data of Willis and Deardorf (1978, Atmospheric Environment12, 1305–1312; 1981, Atmospheric Environment15, 109–117). Emphasis is placed on the fluctuating component of the concentration field due to the random turbulent velocity fluctuations, and amplitudes, temporal and spatial scales, and probability distributions are examined. Concentration fluctuation intensity continually decreases downstream, suggesting zero intensity as the asymptotic limit. Vertical profiles of both mean concentration and fluctuation variance become well mixed downstream. Dissipation and correlation scales increase nearly in proportion to the plume width, so that time- and space-averaging the concentration is less effective in reducing the fluctuations further downstream. Concentration probability distributions show intermittency near the source but become nearly normal as the plume moves downstream. Results are compared and contrasted with the neutral flow study of Sykes and Henn (1992a, Atmospheric Environment26A, 3127–3144).  相似文献   

9.
Oxidation-absorption technology is a key step for NOx removal from low-temperature gas. Under the condition of low O3 concentration (O3/NO molar ratio = 0.6), F-TiO2 (F-TiO2), which is cheap and environmentally friendly, has been prepared as ozonation catalysts for NO oxidation. Catalytic activity tests performed at 120°C showed that the NO oxidation efficiency of F-TiO2 samples was higher than that of TiO2 (about 43.7%), and the NO oxidation efficiency of F-TiO2-0.15 was the highest, which was 65.3%. Combined with physicochemical characteristics of catalysts and the analysis of active species, it was found that there was a synergistic effect between F sites and oxygen vacancies on F-TiO2, which could accelerate the transformation of monomolecular O3 into multi-molecule singlet oxygen (1O2), thus promoting the selective oxidation of NO to NO2. The oxidation reaction of NO on F-TiO2-0.15 follows the Eley-Rideal mechanism, that is, gaseous NO reacts with adsorbed O3 and finally form NO2.  相似文献   

10.
A kinetic model for the Ti(IV)-catalyzed H2O2/O3 process was established, and the experimental results demonstrated that the model could well describe this ozone-based oxidative system mathematically and chemically.  相似文献   

11.
北京城区夏季O3化学生成过程   总被引:3,自引:2,他引:1  
选取2007年7月1日—8月31日中的21个晴空日,利用观测资料和光化学箱模式计算了北京城区测点的O3生成速率G(O3)和O3生成效率OPE.结果表明,21个晴空日中G(O3)日最高小时值分布在(18~82)×10-9h-1之间;在O3污染和非污染日G(O3)最高值的平均水平无显著差异,且与Ox浓度之间不存在一致的对应关系,表明O3化学生成过程不能全面解释地面O3浓度的累积,物理传输过程对测点O3实测浓度有显著作用;各个化学过程对G(O3)的贡献率对比结果显示,HO2 在 NO向NO2的转化中贡献最大;OPE值分布在2.8~5.8之间,总体水平为4.1±0.1;OPE值与NOx浓度之间为非线性关系,OPE值随NOx浓度的增加而减少,表明消减测点附近VOCs排放能有效降低O3浓度.  相似文献   

12.
During the experimental field program that was conducted in October 1985 ton study the physics and chemistry of the Le Havre power plant plume, joints flights were performed with two aircraft from EDF and KEMA. The two episodes with very different meteorological conditions were investigated. The first episode was characterized by fairly constant wind speed and direction with altitude, low solar irradiation and neutral vertical dispersion conditions. The second episode was characterized by low wind speed and changing wind direction, high solar irradiation and stable vertical dispersion conditions. During the latter episode, the concentrations of emitted gases, SO2 and NOx remained high, even at several tens of km downwind of the stock. Increased SO42- and NO3- concentrations were detected in the power plant plume. In addition, important photochemical activity took p-lace in the plume of a nearby industrial area. The former episode showed more significantly vertical dilution and oxidation of NO but did not reveal any contribution of the power plant plume to aerosol formation.  相似文献   

13.
2020年8月利用化学放大法对合肥市西郊大气总过氧自由基RO*2·(RO2·+HO2·)体积分数进行监测,并结合O3和其前体物,分析了过氧自由基体积分数、O3生成速率和O3生成对前体物的敏感性.结果表明,观测期间总过氧自由基体积分数的日均值呈典型的单峰型变化,12:00左右出现最高值,日间峰值体积分数为43.8×10-12,日间RO*2·与太阳辐射强度、温度和O3呈明显的相关性.利用实测RO*2·和NO,获得合肥市西郊夏季O3生成速率,日间峰值为10.6×10-9h-1,O3生成速率对NO变化更为敏感.基于大气自由基和NOx(NO+NO2)反应去除速率占比(Ln/Q),对合肥...  相似文献   

14.
北京大气中NO、NO2和O3浓度变化的相关性分析   总被引:26,自引:8,他引:18  
臭氧(O3)是城市污染大气中的首要光化学污染物,其变化规律与氮氧化物(NOx=NO+NO2)关系密切.采用49C臭氧分析仪和42CTL氮氧化物分析仪对北京城区O3和NOx浓度进行了连续观测,时间为2004-08~2005-07.结果显示,O3和OX(O3+NO2)浓度在午后15:00左右出现峰值,NOx呈双峰态日变化,在07:00和23:00左右出现峰值.不同季节污染物的浓度变化存在差异,O3和NOx浓度分别在夏季和冬季达到最大.NOx浓度存在100×10-9(体积分数)的“分界点”,NOx低浓度时以NO2为主,NOx高浓度时NO占大部分.OX区域贡献和局地贡献存在明显的季节变化,前者主要受区域背景O3的影响,在春季最大,后者主要受局地NOx光化学反应的制约,在夏季最强,同时OX组分呈现显著的昼夜差异.  相似文献   

15.
氮氧化物(NOx)是造成细颗粒物、近地面臭氧等大气污染问题的重要前体物.随着大气污染治理行动的深入,对工业锅炉/窑炉烟气排放的NOx进行控制十分重要.采用不同方法制备了一系列Co_3O_4催化剂,考察了不同制备方法对CO选择性催化还原NO(CO-SCR)反应活性的影响,通过BET、XRD、Raman、HR-TEM和SEM等技术对该系列催化剂进行了表征.活性测试表明,以硫酸钴为前驱体用固态研磨法制备的Co_3O_4-S催化剂具有更优异的CO-SCR反应活性,且表现出较好的抗水蒸气性能,以醋酸钴为前驱体用固态研磨法制备的Co_3O_4-C催化剂显示出较好的抗水性能. NO氧化结果显示,催化剂的NO氧化效果越好,CO-SCR活性也越好. Raman表征结果显示,Co_3O_4-S表面可能含有更多的Co2+离子,从而有利于形成氧空位. H2-TPR结果表明,Co_3O_4-S催化剂的氧化还原性较好. HR-TEM表征发现Co_3O_4-S和Co_3O_4-O主要暴露(111)和(220)晶面,而更多(220)晶面的暴露可能更有利于反应的进行.  相似文献   

16.
A photochemistry coupled computational fluid dynamics (CFD) based numerical model has been developed to model the reactive pollutant dispersion within urban street canyons, particularly integrating the interrelationship among diurnal heating scenario (solar radiation affections in nighttime, daytime, and sun-rise/set), wind speed, building aspect ratio (building-height-to-street-width), and dispersion of reactive gases, specifically nitric oxide (NO), nitrogen dioxide (NO2) and ozone (O3) such that a higher standard of air quality in metropolitan cities can be achieved. Validation has been done with both experimental and numerical results on flow and temperature fields in a street canyon with bottom heating, which justifies the accuracy of the current model. The model was applied to idealized street canyons of different aspect ratios from 0.5 to 8 with two different ambient wind speeds under different diurnal heating scenarios to estimate the influences of different aforementioned parameters on the chemical evolution of NO, NO2 and O3. Detailed analyses of vertical profiles of pollutant concentrations showed that different diurnal heating scenarios could substantially affect the reactive gases exchange between the street canyon and air aloft, followed by respective dispersion and reaction. Higher building aspect ratio and stronger ambient wind speed were revealed to be, in general, responsible for enhanced entrainment of O3 concentrations into the street canyons along windward walls under all diurnal heating scenarios. Comparatively, particular attention can be paid on the windward wall heating and nighttime uniform surface heating scenarios.  相似文献   

17.
基于DOAS地空观测的典型热带地区臭氧敏感性研究   总被引:1,自引:0,他引:1       下载免费PDF全文
为实现中国节能减排与产业经济协调发展的目标,本研究选取中国碳排放重要来源之一的能源密集型产业,采用空间全局自相关,标准差椭圆,空间局部自相关以及空间杜宾模型等方法对2007—2016年中国30个省域能源密集型产业格局、碳排放强度时空演变特征进行了分析,在空间溢出视角下对能源密集型产业结构演变的碳排放效应进行了探讨.结果表明:①空间自相关Moran''s I检验表明碳排放强度与能源密集型产业集聚均存在显著的空间正相关.②标准差椭圆表明,能源密集型产业有重心迁移的现象,但迁移效果不明显.③空间杜宾结果显示,能源密集型产业集聚与碳排放强度呈现"N"型曲线关系,能源密集型产业的集聚对碳排放强度的影响存在明显的空间溢出效应,人口数量和外商投资会显著抑制碳排放强度.  相似文献   

18.
The study shows the variation of surface ozone concentrations for six selected sites between 410 and 3569 m elevation. The annual mean values in 1987 for these sites ranged from 10 to 50 ppb. Mean values of ozone as well as frequency of peak values are clearly dependent on the elevation of the site. Apart from elevation the influences of the specific location and exposure to pollutants such as NO and NO2 are considered. The ratio of the daily means of NO and NO2 is very well suited to indicate local sources. Mean diurnal concentration variations of nitric oxide and ozone on a slope show a significant influence of topography.  相似文献   

19.
This paper describes an evaluation of the performance of a detailed gas-phase reaction mechanism in simulating the results of 561 experiments carried out in four different environmental chambers. The experiments included background air, NOx-air, CONOx-air and aldehyde-air irradiations used for chamber characterization, NOx-air irradiations of single organics as well as simple and complex organic mixtures, and irradiations of auto exhaust. The methods used to represent the major chamber effects and the lighting characteristics in the model simulations of the experiments are described and their associated uncertainties are discussed. Statistical measures of the performance of the mechanism in simulating results of the various types of experiments are summarized and discussed. The mechanism was able to predict maximum ozone yields and rates of NO oxidation to within ±30% for 63% of the experiments modeled, and to within ±50% for 85% of the runs. There is a slight bias (∼15%) towards overprediction of ozone in mixture runs. Although there are cases where the simulations suggest possible problems with the gas-phase mechanism, much of the variability in the goodness of the fits could be attributed to uncertainties in chamber effects. It is concluded that better characterization of chamber conditions are needed if more comprehensive tests of atmospheric photochemical mechanisms are desired.  相似文献   

20.
为了解我国不同气候背景城市O3污染及其与前体物的关系,选取北京市、沈阳市、银川市、成都市、南京市和广州市作为典型代表城市,基于这6个城市2014-2016年ρ(O3)、ρ(NO2)和ρ(CO)资料对O3与其前体物质量浓度变化特征及二者相关性进行研究.结果表明:①2014-2016年6个城市ρ(O3)年均值大小顺序依次为南京市>沈阳市>北京市>银川市>成都市>广州市,ρ(NO2)年均值大小顺序依次为北京市>成都市>南京市>沈阳市>广州市>银川市,ρ(CO)年均值大小顺序依次为北京市>银川市>成都市>沈阳市>南京市>广州市.2014-2016年除广州市ρ(O3)下降、沈阳市变化不明显外,其他城市ρ(O3)总体呈上升趋势;各城市ρ(NO2)和ρ(CO)普遍呈下降趋势.②广州市ρ(O3)夏季最高、春季最低,其他城市四季ρ(O3)大小顺序依次为夏季>春季>秋季>冬季;北京市、沈阳市和银川市四季ρ(NO2)和ρ(CO)大小顺序依次为冬季>秋季>春季>夏季,成都市、广州市和南京市为冬季>春季>秋季>夏季.各城市ρ(O3)和ρ(Ox)日变化呈单峰型,ρ(NO2)和ρ(CO)日变化呈双峰型.③6个城市城区ρ(O3)均低于清洁对照点,城区ρ(NO2)和ρ(CO)均高于清洁对照点,并且城区与清洁对照点O3及其前体物质量浓度差值随城市和月份变化存在一定的差异.④各城市ρ(O3)与ρ(NO2)和ρ(CO)均呈负相关,与ρ(Ox)呈显著正相关;城区ρ(O3)与ρ(NO2)和ρ(CO)的相关性均好于清洁对照点,清洁对照点ρ(O3)与ρ(Ox)的相关性则好于城区.⑤各城市ρ(O3)超标率随ρ(NO2)和ρ(CO)的增加均呈先迅速上升再快速减小,之后缓慢变化的特征,但ρ(O3)超标率峰值对应的ρ(NO2)和ρ(CO)有所差异.研究显示,日照条件较好的银川市、北京市和沈阳市O3与其前体物相关性较成都市、南京市和广州市强.   相似文献   

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