Statistical forecast models for daily air particulate iron and lead concentrations for Madrid,Spain

Statistical models that estimate the daily concentrations of air-particulate Fe and Pb (which are linked to natural and anthropogenic sources, respectively) in a semi-urban area of Madrid, Spain, have been specified. State-space modeling, coupled with Kalman filtering, and Box-Jenkins (transfer function and ARIMA) modeling has been used. Wind speed, which is related to the atmospheric diffusion, has been selected as an exogenous variable for the state-space and transfer function models. The adaptive state-space models do not seem to perform significantly better than the transfer function models but clearly do better than ARIMA models. One-day-lagged wind s̀peed and the persistence were the most important inputs for the proposed Fe and Pb concentration models. However, the predictions of daily Fe particle concentration appears to be better than those of Pb. The performance of the adaptive state-space models suggests that this kind of modeling can be suitable for particulate matter air quality forecasting.     

Potential bias from non-continuous monitoring of ambient ozone concentrations for characterizing hourly and daily 7- and 12-hour average concentrations

Researchers using chamber experiments to investigate O₃ effects on vegetation do not always monitor O₃ concentrations continuously. Errors introduced because of non-continuous monitoring during experimental treatments may result in the inadequate characterization of hourly average concentrations, with the consequence that summarized exposure indices may provide inaccurate linkages between experimental results and the standard-setting process. We have investigated the uncertainties associated with limited sampling to characterize (1) hourly average and (2) daily 7- and 12-h average O₃ concentrations. As expected, accuracy increased with increased sampling; over- and underestimation of hourly values was directly related to whether the actual concentrations were increasing, decreasing or stable from one hour to the next. When non-continuous sampling was used at sites experiencing small changes from one hour to the next, more than 85 and 60% of the estimated hourly average values were within ±5 and ±2.5 ppb of the actual values, respectively. For a site where average O₃ concentrations changed rapidly from one hour to the next, a greater error was observed. For the daily 7- and 12-h average values, when hourly average concentrations did not change rapidly from one hour to the next, 85% or more of the estimated values agreed within ±2 ppb, independent of sampling frequency. Greater uncertainty was experienced when hourly average concentrations changed at a faster rate. When considering the uncertainties associated with non-continuous sampling, investigators should specify the level of accuracy needed to characterize hourly average concentrations and then select the number of samples per hour required to meet that objective.     

长江三角洲城市臭氧数值预报与释用

应用华东区域大气环境数值预报业务系统对长江三角洲55个城市2019年逐日臭氧(O3)进行了数值预报,结果表明不同时效的预报效果非常稳定,预报与观测在相关系数、倍比等指标上体现出良好的一致性,绝大多数城市的相关系数高于0.7,但数值上存在系统性偏高.时间变化上的高度一致性决定了学习期为5～7d、截距为0的单因子动态适应学...     

利用人工神经网络对空气中O3浓度进行预测

将人工神经网络应用于对空气中O3的浓度预测,提出了完整的预测模型,选取风速、风向、相对湿度、云量、平均气温、最高气温等6项气象因子作为输入量,经过两个月的预测实验,结果表明,实测值与预测值的平均相对误差为21.49%,相关系数为0.837.表明人工神经网络对O3的浓度预测是一种有效的工具.     

Evaluation of a number of chemical mechanisms for their application in models describing the formation of photochemical ozone in Europe

A series of 24 chemical mechanisms from the literature are compared against each other using harmonized emissions, photolysis rate coefficients for simple inorganic chemistry and life cycle data for ozone, PAN and H₂O₂. The evaluation sought to understand the impact of parameterizing hydrocarbon oxidation on the peak concentrations of photochemically-generated secondary pollutants. Only seven of the 24 chemical mechanisms gave peak concentrations of ozone, PAN and H₂O₂ simultaneously in their respective central ranges. PAN and H₂O₂ were generally calculated with a much lower precision compared to ozone. Only 11 mechanisms out of 24 gave responses to both 50% hydrocarbons and NO_x emissions controls in their respective central bands. The lack of coordinated ozone, PAN and hydrogen peroxide measurements across Europe currently limits the adequacy of model comparisons and hence the confidence which may be placed in assessments of likely impacts of future control strategies.     

Calculation of long term averaged ground level ozone concentrations

Seasonal averaged ground level concentrations for O₃ have been calculated for The Netherlands by means of a two-layer Lagrangian long-range transport (LRT) model. The model includes emissions, nonlinear atmospheric chemistry, dry deposition, exchange between boundary layer (BL) and free troposphere (FT) and fumigation between a mixed layer and an aged smog layer. Concentrations of primary and secondary pollutants in the FT are obtained from a two-dimensional global model developed by Isaksen.In the reference calculation the modelled concentrations of Ox (sum of O₃ and NO₂) and O₃ are in fair agreement with measurements. The NO_x (sum of NO and NO₂) and NO₂ concentrations are under-estimated by the model but there is a good temporal correlation between calculated and measured concentrations. Validation of other components involved in the chemical scheme is hardly possible due to the paucity of measured data. It can only be stated that the results presented in this paper are not in disagreement with measured or modelled data presented in the literature.In a number of sensitivity runs the influence of European anthropogenic emissions of NO_x and volatile organic compounds (VOC) has been investigated. The calculations indicate that the influence of European emissions on the growing season, daytime averaged (May–September, 10–17 h) O₃ concentrations in The Netherlands is small. For European reductions in the order of tens of per cents a VOC emission reduction is more effective than a NO_x emission reduction in lowering the O₃ concentrations. For strong reductions (about 70%) VOC and NO_x are equally effective. The effects of the modelled underprediction of NO_x concentrations on the production of O₃ on a European scale are probably small. On a local scale the effects are more pronounced due to the NO/O₃ titration (photostationary equilibrium). Therefore, an empirical correction is applied on the modelled O₃ concentrations. After this correction, it is shown that daytime O₃ levels during the growing season increase when European NO_x emissions are reduced (2.0–7.7.% increase at 50% NO_x emission reduction). A reduction in VOC emission leads to decreasing O₃ levels (9% reduction for 40% VOC emission reduction, 16% reduction for 70% VOC emission reduction). For a combined reduction of both VOC and NO_x slightly decreasing ground level O₃ concentrations are expected.     

基于相似集合预报技术的臭氧预报释用研究

利用相似集合预报技术(An En),采用2a的睿图-化学子系统(RMAPS-CHEM)历史预报结果和观测资料,对2018年6月1日～9月30日模式在京津冀地区13个城市共70个国控站点逐小时预报的O3浓度进行了释用订正研究,结果表明:随着集合成员数的增加,An En方法的预报效果呈现出先上升后下降的趋势,并且越过临界集合成员数后,预报效果逐渐降低,因此确定14为最优集合成员数.不同预报因子的权重敏感性不同,其中以RMAPS-CHEM本身预报的O3权重最高,其它依次为2m温度、2m相对湿度、10m风速和边界层高度.经过An En方法的释用订正,有效降低了O3浓度的预报误差.An En方法对O3浓度的时空变化趋势以及浓度值大小都有很好的订正效果,从所有站点的检验结果来看,An En方法订正后的O3浓度与观测值之间的相关系数较模式结果提升68.6%,均方根误差降低25%.An En方法对O3预报释用订正的效果存在明显的区域特征和日变化特征,白天时段对预报的提升主要集中在京津冀东部地区和大城市地区,夜间主要是在城市地区更加显著;An En方法夜间的订正效果优于白天,部分站点夜间提升效果(相关系...     

2016年中国城市臭氧浓度的时空变化规律

随着城市化进程的加快和机动车保有量的急剧增加,导致我国很多地区臭氧（O₃）前体物（挥发性有机物和氮氧化物）排放量显著增加,臭氧污染现象日益突出.臭氧污染对人体健康、植被生长、生态环境等具有重要影响,已成为学术界研究的热点.为揭示全国尺度近地面臭氧的时空变化规律,本文基于2016年中国364个城市的监测数据分析了中国城市O₃浓度的时空变化特征,并采用Global Moran''s I和Getis-Ord G_i^*指数,揭示了2016年中国城市O₃污染的空间集聚和冷热点区域的时空特征.结果表明,在全国尺度上,2016年中国城市年均O₃浓度为100.2 μg·m^-3,北方城市和南方城市O₃浓度分别具有显著的倒"V"和"M"型月变化规律,且呈现夏季高、春秋季居中、冬季最低的特征;中国城市O₃浓度具有显著的空间分异规律,中部和东部是O₃污染的高发区,西部地区和黑龙江省的O₃污染处于较低水平;中国城市O₃浓度具有显著的集聚性特征,且呈现1-5月由南向北而6-12月由北向南扩展的年周期循环特征,热点地区主要集中在华北、华中和华东地区.     

空气污染潜势-统计结合预报模型的建立及应用

建立了一个空气污染潜势预报和统计预报相结合的模型,该模型以特征气象因子和大气扩散清除因子为基础,并考虑不同因子的权重,定义空气污染潜势指数APPI.所考虑的因子包括:地面风速、混合层高度、混合层内平均风速、风向日变化、稳定度级数、垂直扩散系数、SO2干沉降速率、NO2干沉降速率、PM10干沉降速率、降水时长、地面天气形势.进一步利用统计方法建立空气污染指数API与APPI之间的关系.利用南京地区2009~2010年气象资料计算APPI,通过3项式拟合得到API与APPI的统计方程.结果表明,拟合得到的API与实际API相关系数为0.67,具有显著的相关性,且等级准确率为76.7%.进一步利用2011年1~12月中尺度气象模式WRF预报的气象场开展实况预报.研究表明,24h预报、48h预报、回顾预报的逐月等级正确率分别为44.4%~87.5%,46.4%~100%和63.0%~80.0%,年均等级正确率为60.6%,62.4%.和73.1%.若定义预报API与实际API相差±20以内为正确,则24h预报、48h预报、回顾预报的正确率分别为58.1%, 59.4%和63.8%.在IBM x3500并行集群服务器上计算,48h预报需要机时3h.可见,该模型具有较好的预报性能, 相对数值模型计算效率很高.     

盐城市地下水资源预测评价

盐城市是江苏省苏北沿海的新兴城市，区内从上至下分布有供水意义的含水层分别为中更新统第Ⅱ承压含水层，下更新统第Ⅲ承压含水层和中、上新统第Ⅳ承压含水层，其间以弱含水的粘性土层相分隔，并发生强烈的水力联系。本文将采用三维数值模型，在模型识别、验证的基础上，结合对地面沉降、咸水入侵等地质环境控制的要求，以2003年的地下水开采布局为基础。规划、预测了到2020年12月底，第Ⅱ承压含水层、第Ⅲ承压含水层和第Ⅳ承压含水层中的最低地下水位分别恢复到-20m、-30m和-40m时，各含水层中地下水的开采量及地下水的最优开采布局，并预测了未来各含水层地下水位降落漏斗趋于稳定的地下水开采量。     

The characterization and comparison of ozone exposure indices used in assessing the response of loblolly pine to ozone

Using the 1988 and 1989 experimental results obtained for two loblolly pine half-sibling families (GAKR 15–23 and GAKR 15–91) at the Auburn University intensive field research site, we: (1) explored the performance of a set of exposure indices; (2) characterized the ambient air and charcoal-filtered air treatments at Auburn and compared the values of the O₃ exposure indices with those values calculated for ambient O₃ monitors for a select set of sites; (3) identified and characterized O₃ treatments in the Auburn open-top exposure chambers where an adverse effect was noted; and (4) identified where such experimental exposure regimes occurred under ambient conditions. We found that the SUMO exposure index did not perform adequately. We were unable to distinguish among the performances of the SUM06, W126, and SUM08 exposure indices. The results of the analyses of six estimated logistic parameters for a model of diameter² × height (d²h) vs time indicated O₃ effects for both families. At pH 4.3 (near ambient conditions), a response to O₃ was detected in the NF × 2.5 treatments for both families for t₂, the approximate time of maximum growth during the second year. Using ln (final d²h), family 23 did not show O₃ effects. A comparison of the exposures experienced in the NF × 2.5 treatments with those occurring under ambient conditions at other locations showed that in 1983 and 1986, the San Bernardino County (CA) site experienced O₃ exposures similar to those values experienced at the NF × 2.5 treatments in 1989.     

On the mean daily and seasonal variations of the vertical ozone profiles in the lower troposphere

During the 15 year period that the Zugspitze cable car has operated between the valley (1 km a.s.l.) and Zugspitze peak (3 km a.s.l.) at the northern border of the Bavarian Alps, it has been used for investigating the profiles of meteorological and atmospheric electrical parameters, and Aitken nuclei. This cable railway is rather steep and is suspended mostly far away from the ground. From 1980 to 1982 nearly 2000 ozone profiles were additionalyrecorded. The data collected offer a profound basis in order to study the time variations of the lower tropospheric ozone profile depending on the hour of the day during all the seasons. In this paper the following are reported: the shape and time behaviour of ozone profiles in different seasons depending on the vertical mixing intensity, stratospheric intrusions and the penetration depth of the stratospheric O₃.     

Relationships between synoptic-scale atmospheric circulation and ozone concentrations in Metropolitan Pittsburgh,Pennsylvania

A synoptic climatology demonstrates the relationships between the atmospheric circulation and surface ozone (O₃) concentrations. To deduce these associations, a subjective synoptic classification scheme is applied to 10 years' O₃ data from the Pittsburgh metropolitan area. The results focus on four aspects of the atmospheric circulation-O₃ relationship: average, extreme-event, between season and year-to year conditions. On average, each of the nine circulation types is related to a characteristic O₃ concentration level and cumulative O₃ dose. Extreme high-O₃ events are associated with either the western side of a slowly migrating anticyclone or a stagnating extended high-pressure ridge; low-O₃ events are experienced under cool and cloudy cyclonic conditions. Between-season variations in the average and extreme circulation-O₃ relationshipsare observed: the high-pressure features that produce the high st O₃ levels in summer are related to low levels in winter, while circulation patterns that contribute very little to summertime O₃ build-up are associated with the highest levels of wintertime O₃. The latter situation could be caused by tropopause folding and the introduction of stratospheric ozone in winter months. While zonal (meridional) circulation regimes tend to produce lower (higher) mean annual O₃ levels, such year-to-year changes in synoptic-type frequencies do not appear to be strongly related to interannual variations in O₃, and other non-climatic factors appear to be of greater importance.     

Regionalization based on spatial and seasonal variation in ground-level ozone concentrations across China

Owing to the vast territory of China and strong regional characteristic of ozone pollution,it's desirable for policy makers to have a targeted and prioritized regulation and ozone pollution control strategy in China based on scientific evidences. It's important to assess its current pollution status as well as spatial and temporal variation patterns across China.Recent advances of national monitoring networks provide an opportunity to insight the actions of ozone pollution. Here, we present rotated empirical orthogonal function(REOF)analysis that was used on studying the spatiotemporal characteristics of daily ozone concentrations. Based on results of REOF analysis in pollution seasons for 3 years' observations, twelve regions with clear patterns were identified in China. The patterns of temporal variation of ozone in each region were separated well and different from each other, reflecting local meteorological, photochemical or pollution features. A rising trend in annual averaged Eight-hour Average Ozone Concentrations(O_3-8 hr) from 2014 to 2016 was observed for all regions, except for the Tibetan Plateau. The mean values of annual and 90 percentile concentrations for all 338 cities were 82.6 ± 14.6 and 133.9 ± 25.8 μg/m~3,respectively, in 2015. The regionalization results of ozone were found to be influenced greatly by terrain features, indicating significant terrain and landform effects on ozone spatial correlations. Among 12 regions, North China Plain, Huanghuai Plain, Central Yangtze River Plain, Pearl River Delta and Sichuan Basin were realized as priority regions for mitigation strategies, due to their higher ozone concentrations and dense population.     

Sensitivity of future ozone concentrations in the northeast USA to regional climate change

An air quality modeling system was used to simulate the effects on ozone concentration in the northeast USA from climate changes projected through the end of the twenty-first century by the National Center for Atmospheric Research’s (NCAR’s) parallel climate model, a fully coupled general circulation model, under a higher and a lower scenario of future global changes in concentrations of radiatively active constituents. The air quality calculations were done with both a global chemistry-transport model and a regional air quality model focused on the northeast USA. The air quality simulations assumed no changes in regional anthropogenic emissions of the chemical species primarily involved in the chemical reactions of ozone creation and destruction, but only accounted for changes in the climate. Together, these idealized global and regional model simulations provide insights into the contribution of possible future climate changes on ozone. Over the coming century, summer climate is projected to be warmer and less cloudy for the northeast USA. These changes are considerably larger under the higher scenario as compared with the lower. Higher temperatures also increase biogenic emissions. Both mean daily and 8-h maximum ozone increase from the combination of three factors that tend to favor higher concentrations: (1) higher temperatures change the rates of reactions and photolysis rates important to the ozone chemistry; (2) lower cloudiness (higher solar radiation) increases the photolysis reaction rates; and (3) higher biogenic emissions increase the concentration of reactive species. Regional model simulations with two cumulus parameterizations produce ozone concentration changes that differ by approximately 10%, indicating that there is considerable uncertainty in the magnitude of changes due to uncertainties in how physical processes should be parameterized in the models. However, the overall effect of the climate changes simulated by these models – in the absence of reductions in regional anthropogenic emissions – would be to increase ozone concentrations.     

我国日化用品使用挥发性有机物(VOCs)排放及臭氧生成潜势研究

溶剂使用源是挥发性有机物(VOCs)的重要排放源之一.近年来,VOCs排放清单中对工业生产类溶剂的VOCs排放估算较多,但对于生活类溶剂使用的研究有所欠缺.本研究以日化用品为研究对象,基于产品消费量、产品中的溶剂含量及其挥发特性,建立了我国2000-2017年日化用品使用的VOCs排放清单,并基于最大增量反应活性值(M...     

南京地区近地面臭氧浓度与气象条件关系研究

通过分析2013—2015年南京地区相关气象要素对近地面臭氧浓度的影响,建立了用于不同季节高浓度臭氧污染事件的预报预警模型,并归纳总结了南京地区高浓度臭氧出现的天气形势.结果表明,近地面臭氧浓度的变化与气象要素密切相关,气温、能见度、日照小时、总(净)辐射辐照度等要素与O_3浓度呈显著正相关,与相对湿度、总(低)云量呈负相关.高浓度臭氧污染是多因子综合作用的结果,典型气象条件表现为:太阳辐射强,低云量少,相对湿度适宜,地面小风速及特定的风向.通过定义高浓度臭氧潜势指数HOPI和风向指数WDI,并综合考虑14:00地面气温、相对湿度及8:00各标准层的相关气象要素,建立了逐季节多指标叠套的高浓度臭氧预报方程.采用2016年资料对其进行检验,发现预报值与观测值的相关系数分别达0.72(冬季)、0.76(春季)和0.73(夏季),说明方程具有较好的拟合效果和可预报性.通过普查历史天气图,归纳了伴随南京地区高浓度臭氧事件出现的8种主要天气形势,即高压类(高压中心G0、高压后部G1)、低压类(低压底部D0、低压前部D1、低压倒槽D2)、均压类(高压相关的均压JG、低压相关的均压JD、其它均压J).其中,以高压后部地面形势出现概率最大,低压前部均压场出现时对应臭氧平均浓度最高.     

A characterization of the spatiotemporal variability of non-urban ozone concentrations over the eastern United States

The spatial and temporal variability of the daily 1-h maximum O₃ concentrations over non-urban areas of the eastern United States of America was examined for the period 1985–1990 using principal component analysis. Utilization of Kaiser's Varimax orthogonal rotation led to the delineation of six contiguous subregions or “influence regimes” which together accounted for 64.02% of the total variance. Each subregion displayed statistically unique O₃ characteristics and corresponded well with the path and frequency of anticyclones. When compared to the entire domain, the mid-Atlantic and south subregions observe higher mean daily 1-h maximum concentrations. Concentrations are near the domain average for the northeast and southwest subregions and are lowest in the Great Lakes and Florida subregions. The percentage of observations exceeding 120 ppb were greates in the mid-Atlantic and southwest subregions, near the domain average in the northeast and south subregions, and lowest in the Great Lakes and Florida subregions.Examination of the time series of the principal component scores associated with the subregions indicated that Great Lakes and mid-Atlantic subregions tend to observe a stronger seasonal cycle, with maximum concentrations occurring during the last week in June and first week in July, respectively. The strength of this seasonality is weakened for the northeast and south subregions and its timing delayed, until the end of July and the first of August, respectively. The southwest subregion experiences a greatly diminished seasonality, with maximum concentrations delayed until the middle of August. The seasonality found in the Florida subregion is unique in both its strength and timing, as the highest concentrations consistently occur during the months of April and May. The time series were then deseasonalized and autocorrelations and spectral density estimates calculated, revealing that persistence is much more prevalent in the Florida (autocorrelation significant to a lag of 4 days), south (3 days) and southwest (3 days) subregions. Conversely, autocorrelations are only significant to a lag of one day in the northeast and two days for the Great Lakes and mid-Atlantic subregions.