天津市秋季臭氧浓度影响因素及相关关系研究

选择天津市秋季典型重污染时期2005年11月2～7日近地面大气O3、NO、NO2、CO、紫外线(UV)强度和温度等观测数据,研究O3浓度的时间变化特征及其与相关前体物、气象条件的相关关系.结果表明,在观测期间O3浓度存在明显的日变化周期,在13:00～14:00时浓度最大,夜间变化平缓;O3浓度与NO、NO2、NOx和CO等前体物呈较好的负相关关系;温度和UV与O3浓度密切相关,昼间O3与UV呈相同变化趋势,相关系数达0.71,O3浓度变化滞后于UV变化,将O3浓度与前1小时的UV对比分析,相关系数提高到0.81.     

珠三角城市近地面臭氧污染分布特征及变化趋势

利用2013—2017年珠三角城市空气质量监测站的大气常规污染物逐时监测数据,探究珠三角区域臭氧(O3)污染年际变化、季节变化、日变化特征。结果表明,珠三角O3浓度秋季高冬春低,在一年之内呈现2月、5月、9—11月从低到高3个峰值;在一天之内呈现昼高夜低的单峰结构,峰值大多出现在午后15:00时。珠三角中部城市超标天数较多,沿海城市超标天数较少,大部分城市每年O3超标天数逐渐增多。O3月变化和日变化与NO2呈现负相关。总体而言,NO2平均浓度越高的城市,O3昼夜爬升值越高。     

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.     

一次光化学污染过程中O_3和NOx的垂直梯度观测研究

为了研究2008年北京奥运会前期污染物浓度变化特征,对北京气象塔3层高度上的大气污染物(NO2和O3)进行加强观测,分析其变化特征。观测结果表明,由于北京奥运会前期采取了严格的空气质量控制措施,NO2浓度相对车辆限行前下降了45.3%,且随着高度递增逐渐降低;O3浓度最大值和日均值有所降低,其最大值出现时间较10年前提前了1~2 h,且有4 h左右处于相对平稳状态。O3浓度峰值主要是受NO2的控制,O3浓度峰值出现时间提前反映出北京大气氧化效率不断提高。对于观测期间出现光化学污染事件,利用同期气象资料和大气污染监测数据分析,发现造成这次大气污染的主要原因是气象因子:地面多处于弱高压场控制中,大气层结稳定,风力较弱(小于2 m/s),并伴随着连续高温、强辐射和低湿。     

连云港地区近地面臭氧浓度月均浓度变化特征

利用2014—2018年连云港地区的监测资料,分析了O3的月变化特征,得出O3与NO2、CO呈负相关关系,并给出了相对合理的解释。     

一次光化学污染过程中O3和NOx的垂直梯度观测研究

为了研究2008年北京奥运会前期污染物浓度变化特征,对北京气象塔3层高度上的大气污染物（NO2和O3）进行加强观测,分析其变化特征。观测结果表明,由于北京奥运会前期采取了严格的空气质量控制措施,NO2浓度相对车辆限行前下降了45.3%,且随着高度递增逐渐降低;O3浓度最大值和日均值有所降低,其最大值出现时间较10年前提前了12 h,且有4 h左右处于相对平稳状态。O3浓度峰值主要是受NO2的控制,O3浓度峰值出现时间提前反映出北京大气氧化效率不断提高。对于观测期间出现光化学污染事件,利用同期气象资料和大气污染监测数据分析,发现造成这次大气污染的主要原因是气象因子：地面多处于弱高压场控制中,大气层结稳定,风力较弱（小于2 m/s）,并伴随着连续高温、强辐射和低湿。     

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.     

带CrO_3氧化管的库仑法测定NO_x总量

程祖良等建立了库仑法测定NO_2的方法。由于一般废气同时含有NO和NO_2,上述方法不能测定NOx总量。我们在库仑仪电解池前加一个CrO_3氧化管,预先将废气中的NO氧化成NO_2,然后将分析气样通入电解池进行测定。关于CrO_3氧化管氧化NO的应用虽已比较成熟,国内外也不少报导,但都是测定大气中NOx,NOx浓度较低时使用。对污染源中用CrO_3氧化管氧化NO的工作国内外都没     

新疆干旱区城市对流层NO_2垂直柱浓度的时空分布

基于地基多轴差分吸收光谱仪(MAX-DOAS),分析2014年3月至2016年2月新疆干旱区城市(中等城市库尔勒市和小城市博乐市)对流层NO2垂直柱浓度(VCD)变化规律、分布特征及其影响因素。结果表明:(1)新疆干旱区城市对流层NO_2 VCD采暖期是非采暖期的4倍左右,且有显著的季节特征,表现为冬季秋季春季夏季,库尔勒市的对流层NO_2 VCD年均值大于博乐市,两市对流层NO2VCD日变化峰值在8:00(冬季峰值在9:00)和20:00左右,且晚上的峰值高于早上;(2)库尔勒市和博乐市的对流层NO_2 VCD高值分别达到2.540×1015~4.450×1015、1.630×1015~2.620×1015 molec/cm~2,高值区均集中在商业、工业区,对流层NO_2 VCD低值分别为2.300×1014~1.920×1015、6.000×1014~1.390×1015 molec/cm~2,低值区均集中在居民区、学校周边;(3)库尔勒市和博乐市对流层NO_2 VCD对气象因子有不同程度的响应,其与气压呈正相关,与气温、相对湿度、云量和风速呈负相关。     

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。     

Weekday/Weekend differences in ambient air pollutant concentrations in atlanta and the southeastern United States

The authors quantified changes between mean weekday and weekend ambient concentrations of ozone (O3) precursors (volatile organic compounds [VOC], carbon monoxide [CO], nitric oxide, and oxides of nitrogen [NOx]) in Atlanta and surrounding areas to observe how weekend precursor emission levels influenced ambient O3 levels. The authors analyzed CO, nitric oxide (NO), and NO, measurements from 1998 to 2002 and speciated VOC from 1996 to 2003. They observed a strong weekend effect in the Atlanta region, with median daytime (6:00 a.m. to 3:00 p.m. Eastern Standard Time) decreases of 62%, 57%, and 31%, respectively, in the ambient levels of NO, NOx, and CO from Wednesdays to Sundays, during the ozone season (March to October). They also observed significant decreases in ambient VOC levels between Wednesdays and Sundays, with decreases of 28% for the sum of aromatic compounds and 19% for the sum of Photochemical Assessment Monitoring Stations target compounds. Despite large reductions in O3 precursor levels on weekends, day-of-week differences in O3 mixing ratios in and near Atlanta were much smaller. Averaging overall O3-season days, the 1-hr and 8-hr mean peak daily O3 maxima on Sundays were 4.5% and 2.3% lower, respectively, than their mean levels on Wednesdays (median of 14 site differences), with no sites showing statistically significant Wednesday-to-Sunday differences. When restricted to high-O3 days (highest 3 peak O3 days per day of week per site per year), the 1-hr and 8-hr Sunday O3 mixing ratios were 11% and 10% lower, respectively, than their mean peak levels on Wednesdays (median of 14 site differences), with 6 of 14 sites showing statistically significant Wednesday-to-Sunday differences. The analyses of weekday/weekend differences in O3 precursor concentrations show that different emission reductions than normally take place each weekend will be required to achieve major reductions in ambient ozone levels in the Atlanta area.     

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.     

The Steubenville Comprehensive Air Monitoring Program (SCAMP): analysis of short-term and episodic variations in PM2.5 concentrations using hourly air monitoring data

One-hour average ambient concentrations of particulate matter (PM) with an aerodynamic diameter < 2.5 microm (PM2.5) were determined in Steubenville, OH, between June 2000 and May 2002 with a tapered element oscillating microbalance (TEOM). Hourly average gaseous copollutant [carbon monoxide (CO), sulfur dioxide (SO2), nitrogen oxide (NOx), and ozone (O3)] concentrations and meteorological conditions also were measured. Although 75% of the 14,682 hourly PM2.5 concentrations measured during this period were < or = 17 microg/m3, concentrations > 65 microg/m3 were observed 76 times. On average, PM2.5 concentrations at Steubenville exhibited a diurnal pattern of higher early morning concentrations and lower afternoon concentrations, similar to the diurnal profiles of CO and NO(x). This pattern was highly variable; however, PM2.5 concentrations > 65 microg/m3 were never observed during the mid-afternoon between 1:00 p.m. and 5:00 p.m. EST. Twenty-two episodes centered on one or more of these elevated concentrations were identified. Five episodes occurred during the months June through August; the maximum PM2.5 concentration during these episodes was 76.6 microg/m3. Episodes occurring during climatologically cooler months often featured higher peak concentrations (five had maximum concentrations between 95.0 and 139.6 microg/m3), and many exhibited strong covariation between PM2.5 and CO, NO(x), or SO2. Case studies suggested that nocturnal surface-based temperature inversions were influential in driving high nighttime concentrations of these species during several cool season episodes, which typically had dramatically lower afternoon concentrations. These findings provide insights that may be useful in the development of PM2.5 reduction strategies for Steubenville, and suggest that studies assessing possible health effects of PM2.5 should carefully consider exposure issues related to the intraday timing of PM2.5 episodes, as well as the potential for toxicological interactions among PM2.5, and primary gaseous pollutants.     

Measurements of nitrogen dioxide concentrations at rural sites in the United Kingdom using diffusion tubes

Nitrogen dioxide concentrations have been measured at rural sites in the United Kingdom and have revealed a marked spatial variation. The annual mean NO2 concentration varies from approximately 1 microg Nm-3 in Northern Ireland to approximately 7 microg Nm-3 in East Anglia. Though the temporal resolution of the diffusion tube method is limited by exposure periods of 2-4 weeks, it was possible to detect a marked seasonal variation in NO2 concentration at all sites, with higher values in the winter than in the summer. This is in contrast to the small seasonal variation previously observed at sites in London. Sulphur dioxide concentrations were measured daily using a bubbler method and, if expressed in terms of mass of sulphur and nitrogen, the SO2 and NO2 annual mean concentrations were similar. This is in contrast to an S/N ratio of greater than 3 in total UK emissions of SO2 and NOx. It seems likely that this difference is due to a combination of the different spatial distributions and heights of emissions of SO2 and NOx, the influence of local sources of NOx, and the smaller S/N ratio in Continental European emissions.     

Defining the photochemical contribution to particulate matter in urban areas using time-series analysis

The objective of this project is to demonstrate how the ambient air measurement record can be used to define the relationship between O3 (as a surrogate for photochemistry) and secondary particulate matter (PM) in urban air. The approach used is to develop a time-series transfer-function model describing the daily PM10 (PM with less than 10 microm aerodynamic diameter) concentration as a function of lagged PM and current and lagged O3, NO or NO2, CO, and SO2. Approximately 3 years of daily average PM10, daily maximum 8-hr average O3 and CO, daily 24-hr average SO2 and NO2, and daily 6:00 a.m.-9:00 a.m. average NO from the Aerometric Information Retrieval System (AIRS) air quality subsystem are used for this analysis. Urban areas modeled are Chicago, IL; Los Angeles, CA; Phoenix, AZ; Philadelphia, PA; Sacramento, CA; and Detroit, MI. Time-series analysis identified significant autocorrelation in the O3, PM10, NO, NO2, CO, and SO2 series. Cross correlations between PM10 (dependent variable) and gaseous pollutants (independent variables) show that all of the gases are significantly correlated with PM10 and that O3 is also significantly correlated lagged up to two previous days. Once a transfer-function model of current PM10 is defined for an urban location, the effect of an O3-control strategy on PM concentrations is estimated by calculating daily PM10 concentrations with reduced O3 concentrations. Forecasted summertime PM10 reductions resulting from a 5 percent decrease in ambient O3 range from 1.2 microg/m3 (3.03%) in Chicago to 3.9 microg/m3 (7.65%) in Phoenix.     

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.     

Ozone air quality over North America: part I--a review of reported trends

Ozone and precursor trends can be used to measure the effectiveness of regulatory programs that have been implemented. In this paper, we review trends in the concentrations of O3 NOx, and HCs over North America that have been reported in the literature. Although most existing trend studies are confounded by meteorological variability, both the raw data trends and the trends adjusted for meteorology collectively indicate a general decreasing trend in O3 concentrations in most areas of the United States during 1985-1996. In Canada, mean daily maximum 1-hr O3 concentrations at urban sites show mixed trends with a majority of sites showing an increase from 1980 to 1993. Mean daily maximum 1-hr O3 at most regionally representative Canadian sites appears to decrease from 1985 to 1993 or shows no significant change. There are far fewer data and analyses of NOx and HC trends. Available studies covering various ranges of years indicate decreases in ambient NO and HC concentrations in Los Angeles, CA, decreases in HC concentrations in northeastern U.S. cities, and decreases in NOx concentrations in Canadian cities. Two key needs are long-term HC and NOx measurements, particularly at rural sites, and a systematic comparison of trend detection techniques on a reference data set.     

Evolution of the magnitude and spatial extent of the weekend ozone effect in California's South Coast Air Basin, 1981-2000

Since the mid-1970s, ozone (O3) levels in portions of California's South Coast Air Basin (SoCAB) on weekends have been as high as or higher than levels on weekdays, even though emissions of O3 precursors are lower on weekends. Analysis of the ambient data indicates that the intensity and spatial extent of the weekend O3 effect are correlated with-day-of-week variations in the extent of O3 inhibition caused by titration with nitric oxide (NO), reaction of hydroxyl radical (OH) with nitrogen dioxide (NO2), and rates of O3 accumulation. Lower NO mixing ratios and higher NO2/oxides of nitrogen (NOx) ratios on weekend mornings allow O3 to begin accumulating approximately an hour earlier on weekends. The weekday/weekend differences in the duration of O3 accumulation remained relatively constant from 1981 to 2000. In contrast, the rate of O3 accumulation decreased by one-third to one-half over the same period; the largest reductions occurred in the central basin on weekdays. Trends in mixing ratios of O3 precursors show a transition to lower volatile organic compound (VOC)/NOx ratios caused by greater reductions in VOC emissions. Reductions in VOC/NOx ratios were greater on weekdays, resulting in higher VOC/NOx ratios on weekends relative to weekdays. Trends in VOC/NOx ratios parallel the downward trend in peak O3 levels, a shift in the location of peak O3 from the central to the eastern portion of the basin, and an increase in the magnitude and spatial extent of the weekend O3 effect.     

On the local and regional influence on ground-level ozone concentrations in Hong Kong

Hong Kong is a densely populated city situated in the fast developing Pearl River Delta of southern China. In this study, the recent data on ozone (O3) and related air pollutants obtained at three sites in Hong Kong are analyzed to show the variations of O3 in urban, sub-urban and rural areas and the possible regional influences. Highest monthly averaged O3 was found at a northeastern rural site and lowest O3 level was observed at an urban site. The levels of NOx, CO, SO2 and PM10 showed a different spatial pattern with the highest level in the urban site and lowest at the rural site. Analysis of chemical species ratios such as SO2/NOx and CO/NOx indicated that the sites were under the influences of local and regional emissions to varying extents reflecting the characteristics of emission sources surround the respective sites. Seasonal pattern of O3 is examined. Low O3 level was found in summer and elevated levels occurred in autumn and spring. The latter appears different from the previous result obtained in 1996 indicating a single maximum occurring in autumn. Principal component analysis was used to further elucidate the relationships of air pollutants at each site. As expected, the O3 variation in the northeastern rural area was largely determined by regional chemical and transport processes, while the O3 variability at the southwestern suburban and urban sites were more influenced by local emissions. Despite the large difference in O3 levels across the sites, total potential ozone (O3+NO2) showed little variability. Cases of high O3 episodes were presented and elevated O3 levels were formed under the influence of tropical cyclone bringing in conditions of intense sunlight, high temperature and light winds. Elevated O3 levels were also found to correlate with enhanced ratio of SO2 to NOx, suggesting influence of regional emissions from the adjacent Pearl River Delta region.