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.     

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。     

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.     

广州南沙区O3浓度变化及其与气象因子的关系

利用广州南沙区气象探测基地2010年O3浓度和常规气象观测资料,分析了O3浓度变化特征及其气象因子的关系。结果表明,广州南沙区2010年O3浓度最高时均值的最大值出现在8月,超标时数最多的是9月;O3浓度日变化呈单峰型分布,O3浓度日变化最大的季节是秋季,其次为夏季、春季、冬季;O3浓度呈现秋季>春季>夏季>冬季的变化特征。气温、相对湿度、日照时数和云量与O3浓度相关系数大,是影响南沙O3浓度的主要气象因子。秋季O3浓度高,O3主要以局地光化学反应生成为主;春季、夏季和冬季O3主要以外来源的输送为主。气团后向轨迹分析表明南沙区秋季气团主要来自污染的大陆地区,春季、夏季和冬季气团主要是来自东南沿海附近或较为清洁的南海。     

基于水质水量的城镇污水处理厂工艺运行稳定性研究

采用四川省2座位于不同排水服务区域的城镇污水处理厂的样本数据,统计分析了日处理水量,COD、TN、TP浓度及负荷和C/N、C/P等统计量的累积频率分布规律,并分析了各统计量的分布特征对工艺运行稳定性的影响。结果表明,污水处理厂A进水污染物负荷的累积频率分布范围较大,其采用的周期循环活性污泥(CASS)工艺基本能适应进水水质的随机变化,但因存在碳源随机性不足情况,可能导致其脱氮稳定性降低;污水处理厂B进水污染物负荷的累积频率分布范围较小,虽然其采用的厌氧—缺氧—好氧(A2/O)工艺的调控能力较低,但也基本能适应其服务区域内进水水质的随机变化;2座污水处理厂的日处理水量累积频率分布与污染物浓度及负荷的累积频率分布之间均存在显著的差异,日处理水量的累积频率分布比较集中,而污染物浓度及负荷的累积频率分布的离散范围较大,这也潜在威胁到工艺运行的稳定性。总体来看,2座污水处理厂的处理工艺选择恰当,均能较好适应其服务区域的进水水质和水量的要求。     

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。     

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。     

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。     

太原市近地面臭氧浓度变化规律及其与气象要素的关系

臭氧(O3)是城市大气污染和气候变化促进的重要因子,对于城市大气污染与防治研究具有重要意义。本研究选取太原城区10个国控点O3日浓度变化,分析了其与相关气象因子(能见度、室外温度、室外湿度、风速和风向)的关系。研究结果表明,夏季O3浓度最高;春季O3浓度变化次之,冬季变化最小;城市新兴繁荣区和传统重工业区高浓度O3变化的时间跨度要明显高于过渡区域。城区O3和相关气象因子存在显著季节性变化特征。小波分析结果显示,城区O3时间序列相对较高能量的变化周期为主要以4 d的短周期为主(p0.05),与各气象因子存在8 d的显著的同步变化特征(p0.05),且在6—7月与室外温度和室外湿度还存在严格的线性同步变化特征,在11月则与可见度存在近似严格的线性同步变化特征。全年,西西北风对O3浓度影响频率达50%;而夏季受此影响频率高达60%,秋季西西北风和西北北风对O3浓度的影响频率相近(约40%)。研究结果将有助于为北方城市大气污染防治提供理论参考和实践指导。     

上海城市化对气象要素和臭氧浓度的影响

为探讨城市化引起的土地利用变化对上海近地面气象要素和臭氧(O3)浓度的影响,运用美国国家大气研究中心等机构共同开发的WRF-Chem模式,在考虑扩大城市用地、运用城市冠层模式以及城市人为热影响的基础上,针对上海地区2个不同发展时期的下垫面土地利用类型,就2007年3次高浓度O3天气过程,设置4组灵敏性试验进行模拟。结果表明,以虹桥机场站为代表的市区受城市化影响温度升高、相对湿度降低、风速减小,日平均温度最高上升3.5℃,日平均相对湿度最大降低20%,日平均风速最大减小1.5m/s;但以青浦站和川沙站为代表的郊区受城市化影响不明显。此外,以卢湾站为代表的市区,O3浓度普遍增加,日均值最高可增加8.3μg/m3;但以川沙站和淀山湖站为代表的郊区,O3浓度的变化随着个例的不同有增加也有减少。     

Characterization of Ozone During Consecutive Drought and Wet Years at a Rural West Virginia Site

Ozone concentrations at a rural-remote site in a forested region of north-central West Virginia were monitored during 1988 and 1989, a drought and wet year, respectively. During 1988, the absolute maximum average concentration for a single hour was 156 ppb, while it was only 107 ppb in 1989. Overall, the frequency of high concentrations was greater during 1988; the 120 ppb National Ambient Air Quality Standard was exceeded 17 times. The 7-h period encompassing the highest growing season concentrations for this site over the 2-yr period is 1100- 1759 h EST, rather than the period 0900-1559 h originally used by the National Crop Loss Assessment Network. The 7-h growing season means (0900-1559 h) of 52.6 ppb and 47.1 ppb for 1988 and 1989, respectively, compare well to those reported for the Piedmont/Mountain/Ridge-Valley area, but are higher than those for other surrounding areas. The diurnal ozone patterns, as well as the distribution of concentration ranges and timing of seasonal maxima, suggest that long-range transport of ozone and its precursors probably is an important factor at this site, given its remote and rural character.     

Impact of downward-mixing ozone on surface ozone accumulation in southern Taiwan

The ozone that initially presents in the previous day's afternoon mixing layer can remain in the nighttime atmosphere and then be carried over to the next morning. Finally, this ozone can be brought to the ground by downward mixing as mixing depth increases during the daytime, thereby increasing surface ozone concentrations. Variation of ozone concentration during each of these periods is investigated in this work. First, ozone concentrations existing in the daily early morning atmosphere at the altitude range of the daily maximum mixing depth (residual ozone concentrations) were measured using tethered ozonesondes on 52 experimental days during 2004-2005 in southern Taiwan. Daily downward-mixing ozone concentrations were calculated by a box model coupling the measured daily residual ozone concentrations and daily mixing depth variations. The ozone concentrations upwind in the previous day's afternoon mixing layer were estimated by the combination of back air trajectory analysis and known previous day's surface ozone distributions. Additionally, the relationship between daily downward-mixing ozone concentration and daily photochemically produced ozone concentration was examined. The latter was calculated by removing the former from daily surface maximum ozone concentration. The measured daily residual ozone concentrations distributed at 12-74 parts per billion (ppb) with an average of 42 +/- 17 ppb are well correlated with the previous upwind ozone concentration (R2 = 0.54-0.65). Approximately 60% of the previous upwind ozone was estimated to be carried over to the next morning and became the observed residual ozone. The daily downward-mixing ozone contributes 48 +/- 18% of the daily surface maximum ozone concentration, indicating that the downward-mixing ozone is as important as daily photochemically produced ozone to daily surface maximum ozone accumulation. The daily downward-mixing ozone is poorly correlated with the daily photochemically produced ozone and contributes significantly to the daily variation of surface maximum ozone concentrations (R2 = 0.19). However, the contribution of downward-mixing ozone to daily ozone variation is not included in most existing statistical models developed for predicting daily ozone variation. Finally, daily surface maximum ozone concentration is positively correlated with daily afternoon mixing depth, attributable to the downward-mixing ozone.     

Ground-Level Ozone in Eastern Canada: Seasonal Variations,Trends, and Occurrences of High Concentrations

Over the past few years, concern has increased in Canada over the health and environmental impacts of elevated concentrations of ground-level ozone. During the summer the most populated regions of Canada frequently record ozone concentrations that exceed the one-hour average maximum acceptable air quality objective of 32 parts per billion (ppb). In 1988 the Canadian Council of Ministers of the Environment agreed to develop a federal/provincial management plan to control nitrogen oxide and volatile organic compound emissions to reduce ozone concentrations in all affected regions of the country. In addition to the proposed interim control measures, the plan recommended that studies be undertaken to acquire the information necessary to develop sound control strategies. This report represents one of those studies and provides a summary of ground-level ozone measurements for eastern Canada for the 1980 to 1991 period with an emphasis on seasonal variations, trends, and occurrences of high concentrations.

Southwestern Ontario experiences the highest maximum hourly ozone concentrations and the greatest frequency of hours greater than the 82 ppb acceptable objective. Urban sites have the highest frequencies of ozone concentration measurements in the < 10 ppb range, while rural and remote sites show peaks in frequency distribution in the 20 to 30 ppb range. Trend analysis of summertime (May to September) average daily maximum ozone concentration showed no consistent pattern for eastern Canadian sites during 1980 to 1991. Sites in Montreal showed statistically insignificant downward trends while sites in Toronto showed small but statistically significant upward trends. These ozone-increasing trends are associated with reductions in nitric oxide concentrations. At all sites there was large year-to-year variability in peak ozone levels and in the frequency of hours with ozone concentrations above the maximum acceptable objective.     

Evaluating the performance of regional-scale photochemical modeling systems: Part II—ozone predictions

In this paper, the concept of scale analysis is applied to evaluate ozone predictions from two regional-scale air quality models. To this end, seasonal time series of observations and predictions from the RAMS3b/UAM-V and MM5/MAQSIP (SMRAQ) modeling systems for ozone were spectrally decomposed into fluctuations operating on the intra-day, diurnal, synoptic and longer-term time scales. Traditional model evaluation statistics are also presented to illustrate how the scale analysis approach can help improve our understanding of the models’ performance. The results indicate that UAM-V underestimates the total variance (energy) of the ozone time series when compared with observations, but shows a higher mean value than the observations. On the other hand, MAQSIP is able to better reproduce the average energy and mean concentration of the observations. However, both modeling systems do not capture the amount of variability present on the intra-day time scale primarily due to the grid resolution used in the models. For both modeling systems, the correlations between the predictions and observations are insignificant for the intra-day component, high for the diurnal component because of the inherent diurnal cycle but low for the amplitude of the diurnal component, and highest for the synoptic and baseline components. This better model performance on longer time scales suggests that current regional-scale models are most skillful in characterizing average patterns over extended periods, rather than in predicting concentrations at specific locations, during 1–2 day episodic events. In addition, we discuss the implications of these results to using the model-predicted daily maximum ozone concentrations in the regulatory framework in light of the uncertainties introduced by the models’ poor performance on the intra-day and diurnal time scales.     

Trends and variability of ground-level O3 in Connecticut over the period 1981-1997

The temporal and spatial characteristics of ground-level (tropospheric) O3 measured at 10 monitoring stations in Connecticut were studied from 1981 to 1997. To detect the O3 trend caused by changes in precursor emissions, moving average filters and a linear least-squared regression model were used to eliminate the short-term variation and effects of temperature from raw time-series O3 data. The results showed a significant decrease in the number of days exceeding the National Ambient Air Quality Standards (NAAQS) and a small change in total O3 concentration. The analysis indicated that the variation of daily maximum O3, caused by changes in emissions, explained more than 10% of the total O3 variation in Bridgeport and East Hartford during the past 17 years. Meanwhile, a strong weekly cycle was also found in O3 time-series data, resulting in lower O3 concentration in urban areas than in nonurban areas, implying that land use and land cover have impacts on the spatial distribution of ground-level O3 in Connecticut.     

Analysis of air pollution in two major Korean cities: trends, seasonal variations, daily 1-hour maximum versus other hour-based concentrations, and standard exceedances

This study considers the characteristics of carbon monoxide (CO), nitrogen dioxide (NO(2)), ozone (O(3)) and sulfur dioxide (SO(2)) in two major South Korean cities, including the capital city of Seoul, over a time period of 7-8 years. Changes in the annual mean and percentiles of the daily 1-h maximum and other hour-based concentrations varied according to the compound and city type. Seasonal variations varied according to the compound, yet not with the city type. Both Seoul and Taegu exhibited lower O(3) concentrations in July compared to other summer months. There was a high degree of correlation between the daily 1- and 8-h maximum or daily mean concentrations of all compounds in both cities, with an R(2) of 0.66-0.90 at p<0.0001. It was indicated that for CO and O(3), the 8-h standard was more stringent than the 1-h standard, while for NO(2) and SO(2), the 1-h standard was more stringent than the 24-h standard. The correlation coefficients between the daily 1-h maximum and daily mean concentrations decreased as the maximum concentration values of NO(2), O(3 ), and SO(2) increased in the two cities. For all the target compounds, Seoul recorded a substantially higher frequency of days with concentrations above the relevant 1-, 8-, and 24-h standards compared to Taegu.     

Ozone in the urban southeastern United States

Ozone measurements (daily maximum values) from the Aerometric Information Retrieval System database are analyzed for selected sites, during 1980 to 1988, in southeastern USA. Frequency distributions, for most sites during most years, show a typical bell-shaped curve with the higher frequency around the yearly daily maximum ozone mean of about 100 to about 110 microg m(-3) (50-55 ppbv). Abnormal years in ozone concentration may skew the distribution as the mean shifts. A correlation of daily maximum ozone concentrations above 140 microg m(-3) (70 ppbv) between sites shows a division between the sites in the northern protion of the region and those in the southern portion of the region. Variations in ozone levels are well correlated over distances of several hundred kilometers, suggesting that high values are associated with synoptic scale episodes. An ozone exposure analysis also shows higher ozone exposures (250-300 ppm days) in the northerly sites as compared to the southerly sites (150-170 ppm days).     

Surface ozone exposures measured at clean locations around the world

For assessing the effects of air pollution on vegetation, some researchers have used control chambers as the basis of comparison between crops and trees grown in contemporary polluted rural locations and those grown in a clean environment. There has been some concern whether the arbitrary ozone level of 0.025 ppm and below, often used in charcoal-filtration chambers to simulate the natural background concentration of ozone, is appropriate. Because of the many complex and man-made factors that influence ozone levels, it is difficult to determine natural background. To identify a range of ozone exposures that occur at 'clean' sites, we have calculated ozone exposures observed at a number of 'clean' monitoring sites located in the United States and Canada. We do not claim that these sites are totally free from human influence, but rather than the ozone concentrations observed at these 'clean' sites may be appropriate for use by vegetation researchers in control chambers as pragmatic and defensible surrogates for natural background. For comparison, we have also calculated ozone exposures observed at four 'clean' remote sites in the Northern and Southern Hemispheres and at two remote sites (Whiteface Mountain, NY and Hohenpeissenberg, FRG) that are considered to be more polluted. Exposure indices relevant for describing the relationship between ozone and vegetation effects were applied. For studying the effects of ozone on vegetation, the higher concentrations are of interest. The sigmoidally-weighted index appeared to best separate those sites that experienced frequent high concentration exposures from those that experienced few high concentrations. Although there was a consistent seasonal pattern for the National Oceanic and Atmospheric Administration (NOAA) Geophysical Monitoring for Climate Change (GMCC) sites indicating a winter/spring maximum, this was not the case for the other remote sites. Some sites in the continental United States and southern Canada experienced ozone exposures in the range between those values experienced at the South Pole and Mauna Loa NOAA GMCC sites. The 7-month average of the daily 7 h average ozone concentration at 'clean' sites located in the continental United States and southern Canada ranged from 0.028 to 0.050 ppm. Our analysis indicates that seasonal 7 h average values of 0.025 ppm and below, used by some vegetation researchers as a reference point, may be too low and that estimates of crop losses and tree damage in many locations may have been too high. Our analysis indicates that a more appropriate reference point in North America might be between 0.030 and 0.045 ppm. We have observed that the subtle effects of changing distribution patterns of hourly average ozone concentrations may be obscured with the use of exposure indices such as the monthly average. Future assessments of the effects associated with ground-level ozone should involve the use of exposure indices sensitive to changes in the distribution patterns of hourly average ozone concentrations.     

Secondary ozone maxima in a very stable nocturnal boundary layer: observations from the Lower Fraser Valley,BC

The relationship between near-surface ozone concentration and the structure of the nocturnal boundary layer was investigated during a field campaign conducted in 1998 in the Lower Fraser Valley (LFV), British Columbia Canada. Despite the spatial and temporal variation in frequency and morphology, secondary nocturnal ozone maxima were shown to be an important feature of the diurnal ozone cycle throughout the LFV, and localised increases in ozone occasionally exceeded more than half the previous day's maximum concentration.Turbulence in the nocturnal boundary layer was shown to be weak and intermittent. Vertical profiles of Richardson number and ozone concentration indicated that the temporary turbulent coupling of the residual layer to the surface layer facilitated the transport of ozone stored aloft to the surface. Despite the overall complexity of the system, results show that seven out of the 19 ozone spikes observed at the Aldergrove site coincided with turbulence associated with the development of the down-valley wind system. A further nine spikes occurred during periods when a low-level jet was identified aloft. Significantly, ozone concentrations were shown to be highly variable in the residual layer and played an important role in determining the morphology of secondary ozone maxima at the surface. Largest increases in surface ozone concentration occurred when turbulence coincided with periods when ozone concentrations in excess of 80 ppb were observed aloft.