北京市交通道路空气中NO_x的污染现状及时空变化规律研究

基于2008年及2009年分4个季节对北京市3种类型道路(开阔型、交叉路口型和峡谷型)空气中的NOx的现场监测结果,分析了3种类型道路空气中NOx的污染现状和时空变化规律及影响因素。实验结果表明,昼间北京市各类型街道空气中NOx浓度呈早晚浓度高、中午浓度低的变化规律,NOx浓度随季节和车流量变化较明显。交通道路空气中NO占NOx的分担率高,且有较好的相关性,而NO2分担率较低,与NOx相关性较差。     

南京北郊春季地面臭氧与氮氧化物浓度特征

2009年3—5月,采用NO-NO2-NH3分析仪和O3分析仪对南京市北郊大气O3、NO、NO2和NOx浓度进行连续观测,研究南京北郊春季大气臭氧与氮氧化物浓度变化特征。结果表明:O3浓度的日变化呈单峰型结构,白天较高,夜晚较低,在06:00左右出现最低值,14:00左右出现峰值,且工作日的O3浓度值明显高于周末的O3浓度值。NOx的日变化呈现双峰型变化规律,早上07:00左右出现第1个峰值,下午14:00—15:00左右达到最低值,午夜23:00左右出现第2个峰值。从3—5月份,NO浓度明显下降,3月份的变化幅度比较大;NO2浓度则明显上升,5月份变化幅度较大。3—5月NO与O3之间呈显著的负相关关系,4—5月NO2、NOx与O3呈显著的负相关关系。     

电弧放电产生NOx及其对亚硫酸铵的氧化

将脱硫塔产生的高浓度亚硫酸铵氧化为硫酸铵是氨法脱硫研究的一个难点.利用二氧化氮(NO2)的氧化性,可以有效氧化高浓度的亚硫酸铵.空气中电弧放电可以产生氮氧化物(NOx),本研究采用高频交流电源,不锈钢针-针电极,研究了放电间距、气体流量、湿度和O2含量等参数对产物NOx的浓度和NO2/NOx比值的影响,并对产物气体做了红外分析和光谱分析.实验结果表明,放电间距增大有利于NOx浓度和NO2/NOx的提高,气体流量和湿度的增大使NOx浓度和NO2/NOx降低,O2含量为50％和60％时NO2浓度和NO2/NOx分别达到最大值.产物NOx对亚硫酸铵的氧化速率最高可达0.0264 mol/(L·min).     

介质阻挡放电协同Ag/Al_2O_3对NO_x脱除的影响

为有效去除发电厂烟气中产生的NOx,利用介质阻挡放电(DBD)产生低温等离子体并结合催化剂Ag/Al2O3进行烟气脱硝实验,研究了在加入乙烯的条件下,平均负载量、催化温度和装置的布置方式对NOx脱除的影响。结果表明,随着负载的增多,NO脱除率呈现先增大后减小的趋势,5种负载量中最佳为1.76%;随着催化温度的升高,NO脱除率同样呈现先增大后减小的趋势,最佳的催化温度为150℃左右;3种不同布置方式对NO和NOx脱除有明显差别,单独催化剂在NO和NOx的脱除率都比较低;单独介质阻挡放电NO脱除率很高,但是NOx很却很低;而两者结合在NO和NOx都达到了很好的效果。     

中国山东电网燃煤锅炉NOx排放状况和治理技术试验研究

通过对山东电网所属发电厂锅炉NOx排放状况进行调查、测试,得出锅炉NOx排放量与煤种、炉型、燃烧器型式、运行中空气过剩系数、负荷等的关系.结果表明,山东省火力发电厂50 MW及以上容量机组2003年的NOx排放总量超过40万t(按NO2计算).控制和治理NOx排放已成为刻不容缓的重要工作.     

北京市机动车排放遥感监测分析

机动车排放遥感监测反映实际道路行驶中的排放状况,对全面分析排放水平有很强的统计意义。北京市机动车排放遥感监测的CO、HC和NOx的平均浓度分别为1.94%、388×10-6和700×10-6。北京市机动车排放的CO、HC和NOx中50%分别来自于15.90%、13.98%、11.13%的高排放车,但某车辆对于一种污染物出现高排放并不意味着它对其他污染物也是高排放。根据遥感监测得到北京市轻型汽油车基于油耗的CO、HC和NOx平均尾气管排放因子分别为200.1g/L、11.05 g/L和6.68 g/L。     

中国山东电网燃煤锅炉NOx排放状况和治理技术试验研究

通过对山东电网所属发电厂锅炉NOx排放状况进行调查、测试，得出锅炉NOx排放量与煤种、炉型、燃烧器型式、运行中空气过剩系数、负荷等的关系。结果表明，山东省火力发电厂50MW及以上容量机组2003年的NOx排放总量超过40万t（按NO2计算）。控制和治理NOx排放已成为刻不容缓的重要工作。     

东部沿海城市与西部半干旱地区近地层臭氧浓度观测研究

利用东部沿海城市天津大气边界层观测站(以下简称天津站)和西部兰州大学半干旱气候与环境观测站(SACOL)一年的臭氧和NOx体积浓度观测资料,对比分析了两观测站点近地层臭氧浓度的逐月变化、频率分布、日变化特征以及与NOx之间的相关关系.结果表明,两观测站点臭氧浓度月均值变化呈现出很好的一致性,均在4-7月出现高值,12月至次年2月出现低值,SACOL臭氧浓度月均值的最大值和最小值出现时间要比天津站推迟一个月.天津站臭氧体积浓度主要分布在10～50μL/m3,SACOL则集中在10～70 μL/m3,春、夏季两观测站点臭氧体积浓度低于10 μL/m3的频率均很小,秋、冬季两观测站点臭氧浓度频率分布特征类似.两观测站点臭氧浓度日变化在4个季节均呈现典型的单峰型分布,SACOL臭氧浓度日最大值出现时刻要比天津站晚2h.两观测站点臭氧浓度与NOx、NO2、NO的浓度之间均呈显著的负相关关系.天津站与臭氧浓度的相关性最强的为NO,而SACOL则是NOx.     

用活性填料催化氧化-硝酸吸收法脱除氮氧化物的研究

为了提高硝酸吸收氮氧化物的效率,对活性填料催化氧化-硝酸吸收NOx进行了研究.结果表明:活性填料能明显提高NOx的吸收效率;当NOx中NO2体积百分含量增加,其吸收效率增加;随进气浓度和液气比的增大,NOx吸收效率增加;随NO2浓度的增加,NO的吸收效率先增加后减少,在NO/NO2为3时,NO吸收效率最高;随NO的增加NO2的吸收效率先增加后减少,在NO/NO2为0.6～1之间,NO2的吸收效果较好.     

北京与伦敦空气中气态污染物的比对研究

城市空气质量问题已经引起广泛关注.通过对中英2个大城市北京与伦敦 2004 年 8 月～2005 年12 月空气中气态污染物 O3、NOx、SO2 和 CO 浓度变化的分析与对比发现:参照世界卫生组织空气质最准则、欧盟空气质量标准、美国国家空气质量标准或国家空气质量二级标准,北京O3、NO2、SO2和 CO 浓度的超标天数或时数明显高于伦敦.观测期内,北京 O3、NOx、SO2 和 CO 浓度明显高于伦敦,平均值分别是 17.9±22.1×10-9、72.4±76.1×10-9、19.5±21.8×10-9、2 004.6±1 509.8×10-9与10.8±9.9×10-9、54,6±38.9×10-9、1.8±2.2×10-9、372.3±235.0×10-9.两城市 O3 统计日变化形式均表现为白天高、夜晚低,峰值出现在午后 14:00 左右,日较差分别为 31.5±30.9×10-9与 11.1±7.7×10-9;NO、NO2、SO2 和 CO 呈双峰态日变化,峰值出现在交通的早高峰与晚高峰附近.北京 O3 最高值出现在夏季,而伦敦出现在春季;但两城市NOx、SO2 和 CO 最高值均出现在冬季.北京与伦敦的NO2与 NO 呈显著线性相关,且斜率与截距十分相似,分别是 1.25 和 1.28 与 28.1 和 23.2;同时两城市 CO/NOx 比率明显高于 SO2/NO 分别为 14.0、4.5 与 0.13、0.03.由此可以判断:对于两城市空气污染问题,交通源的贡献要远大于点源;但点源也对两城市空气质量造成影响.此外,连续逆温的天气是造成重污染事件的原因.     

Photocatalytic oxidation of nitrogen oxides using TiO2 loading on woven glass fabric

TiO2 loading on woven glass fabric is applied to treat nitrogen oxides (NOx) by photocatalytic oxidation (PCO). In this paper, the PCO behavior of NO at high concentrations was studied by PCO of NOx at source levels (20-168 ppm). The PCO efficiency reached 27% in this experiment, while the inlet NOx concentration was 168 ppm (147 ppm NO). The dependency of the reaction rate on several key influencing factors (relative humidity, space time, inlet concentration, oxygen percentage) was also studied. The results illustrate that the resulting hydroxyl radical and active oxide play an important role in the oxidation of NOx. The reactions are limited by the thermodynamic equilibrium after ca. 15s space time. A possible explanation for the catalyst deactivation is the accumulation of nitric acid and nitrous acid on the TiO2 surface during the PCO of NOx. However, the photocatalytic activity can be recovered with a simple heat treatment. The results from the study of the effect of the inlet concentration were described with the Langmuir-Hinshelwood model.     

Differences between weekday and weekend air pollutant levels in southern California

Ambient air quality data were analyzed to empirically evaluate the effects of reductions of volatile organic compounds (VOCs) and oxides of nitrogen (NOx) emissions on weekday and weekend levels of ozone (O3; 1991-1998) and particulate NO3- (1980-1999) in southern California. Despite significantly lower O3 precursor levels on weekends, 20 of 28 South Coast Air Basin (SoCAB) sites (28 of all 78 southern California sites) showed statistically significant higher mean O3 levels on Sundays than on weekdays (p < 0.01); 49 of the remaining 50 sites showed no significant differences between mean weekday and Sunday peak O3 levels. We also observed no statistically significant differences between mean weekday and weekend concentrations of particulate NO3- or nitric acid (HNO3, the precursor of particulate NO3-). Averaged over sites, the mean Sunday NOx and nonmethane hydrocarbon concentrations were 25-41% and 16-30% lower, respectively, than on weekdays. Site-to-site differences between weekend and weekday mean peak hourly O3 levels were related to whether O3 formation was limited by the availability of NOx. A thermodynamic equilibrium model predicts that particulate NO3- levels would decrease in response to a reduction of HNO3, and that particulate ammonium NO3- formation was not limited by the availability of ammonia. The similarity of mean weekday and weekend levels of NO3- therefore did not result from limitations on the formation of particulate NO3- from its precursor, HNO3.     

Modeling and direct sensitivity analysis of biogenic emissions impacts on regional ozone formation in the Mexico-U.S. border area

A spatially and temporally resolved biogenic hydrocarbon and nitrogen oxides (NOx) emissions inventory has been developed for a region along the Mexico-U.S. border area. Average daily biogenic non-methane organic gases (NMOG) emissions for the 1700 x 1000 km2 domain were estimated at 23,800 metric tons/day (62% from Mexico and 38% from the United States), and biogenic NOx was estimated at 1230 metric tons/day (54% from Mexico and 46% from the United States) for the July 18-20, 1993, ozone episode. The biogenic NMOG represented 74% of the total NMOG emissions, and biogenic NOx was 14% of the total NOx. The CIT photochemical airshed model was used to assess how biogenic emissions impact air quality. Predicted ground-level ozone increased by 5-10 ppb in most rural areas, 10-20 ppb near urban centers, and 20-30 ppb immediately downwind of the urban centers compared to simulations in which only anthropogenic emissions were used. A sensitivity analysis of predicted ozone concentration to emissions was performed using the decoupled direct method for three dimensional air quality models (DDM-3D). The highest positive sensitivity of ground-level ozone concentration to biogenic volatile organic compound (VOC) emissions (i.e., increasing biogenic VOC emissions results in increasing ozone concentrations) was predicted to be in locations with high NOx levels, (i.e., the urban areas). One urban center--Houston--was predicted to have a slight negative sensitivity to biogenic NO emissions (i.e., increasing biogenic NO emissions results in decreasing local ozone concentrations). The highest sensitivities of ozone concentrations to on-road mobile source VOC emissions, all positive, were mainly in the urban areas. The highest sensitivities of ozone concentrations to on-road mobile source NOx emissions were predicted in both urban (either positive or negative sensitivities) and rural (positive sensitivities) locations.     

Modeling analyses of the effects of changes in nitrogen oxides emissions from the electric power sector on ozone levels in the eastern United States

In this paper, we examine the changes in ambient ozone concentrations simulated by the Community Multiscale Air Quality (CMAQ) model for summer 2002 under three different nitrogen oxides (NOx) emission scenarios. Two emission scenarios represent best estimates of 2002 and 2004 emissions; they allow assessment of the impact of the NOx emissions reductions imposed on the utility sector by the NOx State Implementation Plan (SIP) Call. The third scenario represents a hypothetical rendering of what NOx emissions would have been in 2002 if no emission controls had been imposed on the utility sector. Examination of the modeled median and 95th percentile daily maximum 8-hr average ozone concentrations reveals that median ozone levels estimated for the 2004 emission scenario were less than those modeled for 2002 in the region most affected by the NOx SIP Call. Comparison of the "no-control" with the "2002" scenario revealed that ozone concentrations would have been much higher in much of the eastern United States if the utility sector had not implemented NOx emission controls; exceptions occurred in the immediate vicinity of major point sources where increased NO titration tends to lower ozone levels.     

Evaluation of ozone-nitrogen oxides-volatile organic compound sensitivity of Cincinnati, Ohio

Ambient concentrations of ozone (O3), nitrogen oxides (NOx), total reactive nitrogen (NOy), nitric acid (HNO3), and hydrogen peroxide (H2O2) were measured during September 2003 at an urban site of Cincinnati, OH. The aim of this study was two-fold: to investigate whether O3 formation in this population exposure-type site is NOx, sensitive or volatile organic compound (VOC) sensitive and to test the practicality of using two combined observational-based methods to identify the sensitivity of O3 formation in midlevel polluted locations. The evaluation of the indicator species: NOy, O3/NOy, O3/HNO3, H2O2/ HNO3, and O3/(estimated NOx reaction products), as well as the combined hypothesis testing analysis of the weekend/weekday (WE/WD) differences of 1-hr and 8-hr average maximum O3 and of the 6:00 a.m.-9:00 a.m. average nitric oxide and NOx concentrations, show evidence that Cincinnati is likely VOC sensitive. Average WE 1-hr and 8-hr maximum O3, as well as duration of WE O3 accumulation, were not lower than the corresponding WD levels in spite of the observed significant reduction in NO, emissions on WE, a typical situation in VOC-sensitive locations. The possibility that the seasonal transition from summer to autumn could have influenced the results was also investigated through an exploratory analysis of the afternoon O3 maximum/NOx measured and of the WE/WD differences of peak O3 and morning average NO and NO, concentrations observed at this site from June through September 2003. The results suggest that a VOC-sensitive chemistry regime dominated along the summer season. The findings of this study suggest that additional reductions in regional NO, emissions in Cincinnati, a potential nonattainment area under the 8-hr O3 standard, may cause an increase in local O3. Future strategies to reduce O3 in Southwest Ohio should be further evaluated carefully. The combination of observational-based methods might provide a consistent complementary approach in the identification of the NO,-VOC sensitive characteristics of mid-to-moderate polluted urban areas.     

Analysis of photochemical pollution in summer and winter using a photochemical box model in the center of Tokyo, Japan.

In order to give an effective and rapid analysis of the photochemical pollution and information for emission control strategies, a photochemical box model (PBM) was applied to one moderate summer episode, 11 July 1996, and one typical winter episode, 3 December 1996, in the center of Tokyo, Japan. The box model gave a good prediction of the photochemical pollution with minimal investment. As expected, the peak ozone in summer is higher than in winter. The NOx concentrations in winter are higher than those in summer. In summer, NO and NO2 have one peak in the morning. In winter, NO and NO2 show two peaks during the day. Three model runs including no reactions, a zero ozone boundary condition and dark reactions were conducted to understand the photochemical processes. The effects of emission reduction on the formation of the photochemical pollution in the center of Tokyo have been studied. The results show that the reduction of NMHC emission can decrease the ozone, however, the reduction of NOx emission can increase the ozone. It can be concluded that if the NOx emission are reduced, the reduction of NMHC should be more emphasized in order to decrease the ozone concentration in the center of Tokyo, Japan, especially the reduction of the NMHC from stationary source emission.     

Quantifying NOx for industrial combustion processes

The objectives of this paper are to (1) identify the problems with many of the units that are used to report and regulate NOx, (2) show how to properly correct NOx measurements for oxygen-enhanced combustion, and (3) recommend a preferred type of NOx unit. The current variety of NOx units make comparisons difficult and can cause considerable confusion. NOx may be measured on a wet or dry basis, but it is commonly reported on a dry basis. The reported NOx may differ from the actual measurements, which may be converted to a specific O2 basis level. Nearly all of the measured NOx from industrial combustion systems is in the form of NO, which is converted to NO2 in the atmosphere. However, when given on a mass basis, the measured NO is commonly reported as NO2 for regulatory purposes, but may be reported as NO, NO2, or simply NOx in technical papers. Some existing regulations may penalize combustion technologies with higher efficiencies and lower flue gas volumes, such as oxygen-enhanced combustion. Confusion may occur when applying some of the "conventional" NOx units to oxygen-enhanced processes. A better unit is the mass of NOx generated per unit of production, which also incorporates the overall process efficiency into the emissions. That unit does not penalize more efficient processes that may generate more NOx on a volume basis, but less NOx on a production basis.     

Associations between particle number and gaseous co-pollutant concentrations in the Los Angeles Basin

Continuous measurements of particle number (PN), particle mass (PM10), and gaseous pollutants [carbon monoxide (CO), nitric oxide (NO), oxides of nitrogen (NOx), and ozone (O3)] were performed at five urban sites in the Los Angeles Basin to support the University of Southern California Children's Health Study in 2002. The degree of correlation between hourly PN and concentrations of CO, NO, and nitrogen dioxide (NO2) at each site over the entire year was generally low to moderate (r values in the range of 0.1-0.5), with a few notable exceptions. In general, associations between PN and O3 were either negative or insignificant. Similar analyses of seasonal data resulted in levels of correlation with large variation, ranging from 0.0 to 0.94 depending on site and season. Summertime data showed a generally higher correlation between the 24-hr average PN concentrations and CO, NO, and NO2 than corresponding hourly concentrations. Hourly correlations between PN and both CO and NO were strengthened during morning rush-hour periods, indicating a common vehicular source. Comparing hourly particle number concentrations between sites also showed low to moderate spatial correlations, with most correlation coefficients below 0.4. Given the low to moderate associations found in this study, gaseous co-pollutants should not be used as surrogates to assess human exposure to airborne particle number concentrations.