Trends analysis of vegetation exposure indices in rural areas of the U.S.

In this work, statistical models based on a linear time term are tested to determine if they can adequately represent the behavior over time of indices that relate vegetation exposure to air pollutants at a large number of monitoring sites in the rural U.S. Three pollutants are addressed: ozone (O₃), sulfur dioxide (SO₂)and nitrogen dioxide (NO₂. The formulations selected to generate the values of the exposure indices were the sum of all hourly average concentrations (SUM0); in addition, for O₃, the sum of all hourly average concentrations weighted with a sigmoidal function, which assigned larger weights to the higher concentrations. The basic hourly average concentration data were selected from routine air monitoring stations of existing networks that met minimum criteria for quality assurance and data completeness. The statistical methodology used was based on a linear regression model which accounted for seasonality and changes in experimental procedures. An additional lag-one autoregressive term was added to the model for those stations which exhibited significant autocorrelation in the data, based on the Durbin-Watson statistic. Long-term analyses included data for 7 to 10 years; short-term analyses included data for 4 to 5 years. Results show that over rural areas of the U.S., these models do not adequately represent the behavior of vegetation exposure indices, both in the long-term and the short-term analyses; the majority of stations did not have statistically significant (5% level) coefficients for the term representing linear dependence on time. Emissions data for SO₂, NO_x and volatile organic compounds (VOC) over the same time period are also presented. Over the contiguous U.S., emissions between 1979 and 1987 have decreased by a maximum of 3%; emission changes for individual states have generally decreased between 1979 and 1987, but between 1983 and 1987 both increases and decreases have occurred.     

2013年1月华北地区重霾污染过程SO2和NOx的CMAQ源同化模拟研究

以2006年中国地区的INTEX-B排放清单为基础,采用CMAQ模式污染源同化方法,反演更新了2013年1月重霾污染过程华北地区的SO₂和NO_x排放源;应用WRF-CMAQ模式以及2006年INTEX-B初始排放源和2013年1月改进的排放源,分别模拟了1月9-15日和28-31日两次持续重霾污染过程的SO₂和NO₂浓度,并与华北地区47个环境监测站点实测值进行对比,重点分析了基于初始源和同化反演源的模拟效果及其改进原因;本文亦采用2012年清华大学编制的东亚地区MEIC排放清单评估了SO₂和NO_x同化反演源的合理性.分析结果表明:①CMAQ模式污染源同化方法可适用于重霾污染过程,即采用同化反演源模拟的SO₂、NO₂浓度时空变化特征与实测值较一致,而且可反映SO₂、NO_x排放源强的动态变化特征;②基于同化反演源的SO₂、NO₂浓度模拟效果明显优于2006年INTEX-B排放源,其时间变化趋势与实测值较一致,而且可模拟重霾污染过程SO₂、NO₂浓度的峰值;③采用反演源模拟的SO₂、NO₂浓度空间区分布特征与实测值较一致,而且可较好反映重污染区的极值分布特征;④经污染源同化改进后SO₂、NO₂模拟浓度与实测值的相关系数有所提高,误差明显减小;SO₂的改进效果略优于NO₂,这与污染源对两种污染物浓度的影响差异有关;⑤初始源中SO₂、NO_x排放源的空间分布和强度与2012年清华大学编制的排放源强差异较大,而同化反演源的空间分布和强度均接近于上述2012年排放源,较好反映出重点地区的高污染源分布特征.本文研究结果将为改进重霾污染过程的空气质量预报、减小自下而上建立的排放源清单不确定性、评估SO₂、NO_x等排放源的影响效应以及不同气象条件下区域排放源的动态调控等提供新技术途径和研究思路.     

Dispersion modelling of nitrogen oxides in the United Kingdom

This paper describes the construction and application of an Eulerian-dispersion model for the calculation of NO₂ and NO_x concentrations in the U.K. Model results are compared with measurements from 44 U.K. sites. The sensitivity of the model results to chemical and dispersion parameterisations is assessed. The model is also used to verify the validity of ‘instantaneous mixing’ assumptions used in trajectory models. Finally, the distribution of ground-level NO_x concentrations from power stations, motor vehicles and other stationary sources is calculated across the U.K., including a preliminary assessment of the possible contribution from natural sources.     

1997~2011年北京市空气中酸性物质与降水组分变化趋势的相关性分析

依据北京市环境保护监测中心1997～2011年降水监测资料、大气环境质量监测资料,结合北京经济发展和能源结构变化,分析了酸雨前体物的排放与环境空气中酸性物质及降水中组分的相关性,为政府部门评定大气污染治理效果,制定未来防控政策和规划提供科学决策依据.研究表明,环境空气中NO2、NOx、SO2年均浓度显著相关,说明北京地区环境空气中氮与硫的来源基本相同,均来自化石燃料燃烧排放,这也是酸雨形成的根本原因.北京市大气中的污染物主要来自局地排放源,而降水中硫、氮的湿沉降量与环境空气中SO2、NO2、NOx浓度变化趋势的相关性较差,表明降水中各离子浓度受局地源和外来大气输送共同作用的影响.同时发现降水中硝酸根浓度与机动车数量呈现相同变化趋势,反映出机动车尾气排放的NOx与降水中硝酸根浓度增长密切相关.     

Calculation of long-term averaged and episodic oxidant concentrations for the Netherlands

Ground-level ozone and oxidant (sum of O₃ and NO₂) concentrations in The Netherlands are calculated during the growing season (May–September) by means of a Lagrangian long-range transport model. Two air parcels—one representative of the mixed layer, the other representative of the polluted layer above the mixed layer (aged smog layer)—are followed along 96 h back trajectories. Long-term averaged and 98 percentile values of hourly averaged concentrations are estimated on the basis of concentrations calculated for four arrival times per day for all days in the period considered.In a number of sensitivity runs the influence of European anthropogenic NO_x and VOC emissions on the oxidant concentrations in The Netherlands has been investigated. In general, the influence of European emissions on the 98-percentile values is 2–3 times as large as on the averaged concentrations. This indicates that long-term averaged concentrations more strongly depend on the concentrations in the free troposphere whereas the episodic concentrations are determined by photochemical production over Europe. VOC emission reduction is more effective in lowering episodic concentrations than NO_x emission reduction. For long-term averaged concentrations, however, NO_x and VOC emission reduction of 50% or more are nearly equally effective.     

The stem-II regional scale acid deposition and photochemical oxidant model—IV. The impact of emission reductions on mesoscale acid deposition in the lower ohio river valley

Assessment of the effect of reduction in emissions of primary sources on eventual levels of pollutants, pH of precipitation and total wet deposition is crucial in designing acid-rain control strategies. The STEM-II/ASM model is used to investigate the effect of reduction in emissions on the ultimate deposition patterns and amounts of major acidic pollutants in a mesoscale region. This work also investigates the effect of background levels of primary pollutant species on the eventual levels and deposition amounts of SO₄⁼ and NO₃⁻. A series of mesoscale simulations were conducted in which emissions of primary sources of NO_x and SO₂ were reduced and/or background concentrations of certain key species were changed. The results indicate that the dominant effect on the eventual deposition amounts of SO₄⁼ and NO₃⁻ is due to background concentrations of key precursor species such as SO_x and NO_x. With relatively high background concentrations, reducing SO₂ emissions by 50% and NO_x emissions by 40% resulted in reductions of 2–3% for SO₄⁼ wet deposition aand about 15% for NO₃⁻ wet deposition. However, reducing the background concentrations of SO₂ and SO₄⁼ by 50% and NO, NO₂ and HNO₃ by 40% resulted in substantial reductions in wet deposition; SO₄⁼ deposition was reduced by 40–50% and NO₃⁻ deposition was reduced by approximately 35%.     

Source-receptor relationships for wet SO42− and NO3− production

Precipitation chemistry data for the years 1982–1985 from 110 stations distributed across the continental U.S. and southern Ontario Province are used to describe the geographic distributions of SO₄²⁻ and NO₃⁻ in precipitation. Volume-weighted, wet SO₄²⁻ and NO₃⁻ concentrations, averaged over the 4 years of observation by season and annullly, show coherent patterns with maxima in the northeastern U.S. and southeastern Canada about ten times greater than the minima observed in the Intermountain and Pacific Northwest regions.Tests for empirical source-receptor relationships indicate that, in land areas with relatively low emissions of SO₂ and NO_x, the associations between wet SO₄²⁻ concentrations and SO₂ emissions and between wet NO₃⁻ concentrations and NO_x emissions within 560 km of each precipitation chemistry station are weak or nonexistent (r²⩽0.42). The remaining land areas show moderate to strong associations between SO₂ and SO₄²⁻ and NO_x and NO₃⁻ during the spring and summer, but only weak to nonexistent associations during the winter. The associations between emissions and concentrations, e.g. SO₂ and SO₄²⁻, are equally well represented by either a linear or a power law function. However, at the level of aggregation employed, the data do not substantiate a linear-proportional relationship between concentrations and anthropogenic emissions. Furthermore, emissions of SO₂ and NO_x are highly correlated, as are the emissions of RHC and NO_x.     

A diffusion tube survey of NO2 levels in urban areas of the U.K.

A nationwide survey of ambient NO₂ concentrations has been carried out by Warren Spring Laboratory and AEA Technology, Harwell, in urban areas of the U.K. The survey utilised passive diffusion tube samplers, deployed at 363 existing smoke/SO₂ monitoring stations, and ran from July to December 1986.Although undertaken primarily to provide an independent check on the siting of monitoring stations to determine compliance with the European Community NO₂ Directive, the survey provides for the first time a nationwide picture of urban levels of this pollutant. London was found to experience the highest average NO₂ concentrations in the U.K., with these being highest close to busy roads. Concentrations were found to be only moderately higher in winter than in summer.Correlations between measurements of SO₂, smoke and NO₂ were examined. The closest correlation is observed between NO₂ and smoke, indicating traffic to be a dominant source of these pollutants. NO₂ data are also shown to correlate well with disaggregated NO_x emission data for the U.K.     

Evaluating the influence of air pollution on solar radiation observations over the coastal region of Alicante (Southeastern Spain)

The present study evaluates ground-based downward surface shortwave radiation (R_s) over the coastal region of Alicante (Southeastern Spain). Hourly measurements collected over the eleven-year period 2010-2020 are used. Two weather stations located over the region capital, Alicante, have been selected as representative of urban and suburban typologies. Two additional weather stations far from the city have been selected representing rural typologies. R_s is significantly reduced over the urban station during the morning hours within the winter season compared to the observations recorded over the suburban and rural stations, with a global mean difference of -81 and -120 W/m² at 10 LT, respectively. However, no significant differences are obtained during the midday sun, with a global mean difference of -20 W/m² between the urban and rural stations. With the aim of explaining these differences, the current paper investigates the relationship between R_s and different air pollutants: NO_x, SO₂, and fine particulate matter (PM_2.5 and PM₁₀) as well as the wind field measured at the urban and suburban stations. The results found in this work point towards a close relationship between R_s and NO_x concentrations annual cycles, which are also influenced by the prevailing wind circulations observed over the study area. A global mean NO_x concentration of 107 µg/m³ is observed over the urban station at 10 LT during the winter season. In contrast, these high concentrations are significantly reduced over the suburban station, with global mean value of 40 µg/m³ at 10 LT, for this period of the year.     

The impact of changing regional emissions on precipitation chemistry in the eastern United States

From 1975 to 1987 a 19% change in SO₂ emissions a 16% change in NO_x emissions have occurred over the eastern and mid-western U.S. Six continental precipitation chemistry sites from the MAP3S network, plus the Hubbard Brook Experimental Forest, NH, show a direct relationship between emission levels and precipitation H⁺ and SO₄^2- concentrations, except for Penn State, PA. MAP3S sites at Illinois and Ohio, located closest to the major SO₂ source regions, demonstrates statiscally significant (P <0.05) linear regressions of SO₄^2- concentrations on SO₂ emissions. Whiteface Mt., NY, shows a weaker relationship (P <0.01), and Hubbard Brook shows the strongest relationship (P <0.01) between SO₂ emissions and SO₄^2- concentration in precipitation. No site shows a significant relationship (P <0.10) for NO_x emissions and NO₃⁻ concentrations in precipitation. Illinois, Ohio, Ithaca and Hubbard Brook show significant linear regressions of H⁺ concentrations on emissions of SO₂ + NO_x (P <0.10, 0.05, 0.01, and 0.01, respectively). Overall, for the entire region examined, decreasing SO₂ emissions levels appear to have decreased SO₄^2- concentrations with an efficiency of 74% ± 15% (s.e.). Decreasing SO₂ plus NO_x emissions (18%) have been accompanied by a decreasing H⁺ concentrations (18%) suggesting an efficiency of conversion of 100% ± 15% (s.e.) for the study region as a whole. While significant reductions in acid species have occured at Hubbard Brook, further reductions in excess of 50% of present deposition are necessary to protect acid-sensitive ecosystems.     

2010年广州亚运期间空气质量与污染气象条件分析

利用2010年11月4日～12月10日广州地区NO2、O3、SO2、PM、能见度实测资料,区域空气污染指数RAQI及大气输送扩散特征参数,分析广州亚运期间空气质量与气象条件变化特征.结果表明,亚运期间空气质量比亚运前后好,能见度比亚运前后大,PM1和PM2.5浓度比亚运前后小,能见度与PM1和PM2.5有较好的反相关;亚运期间NO2和SO2日均值和小时均值均达到国家一级标准,PM10日均值和O3小时均值均满足国家二级标准,污染物得到较好的控制;广州地区SO2受本地源和外地源远距离输送叠加影响,NO2受本地源影响较大;广州周边城市NO2、SO2和PM10有向广州输送的潜势,而广州O3有向其周边城市扩散的潜势;亚运期间污染气象条件比亚运前后有利,亚运期间污染物浓度降低得益于政府实施的减排措施及良好的气象条件.     

Studying high ozone concentrations by using the Danish Eulerian model

The long-range transport of air pollutants (LRTAP) over Europe is studied by a mathematical model based on a system of partial differential equations (PDEs). The number of PDEs is equal to the number of species studied and the model contains 35 species at present. Among the species are NO, NO₂, NO₃⁻, HNO₃, NH₃, NH₄⁺, O₃, PAN, SO₂, SO₄²⁻ and may hydrocarbons. Most of the 70 chemical reactions involved in the model are nonlinear (including here many photochemical reactions).The model requires large sets of input data. Emissions of SO₂, NO_x, NH₃ and both natural and anthropogenic volatile organic compounds (VOC) are needed in the model. The meteorological data consist of fields of wind velocities, precipitation, surface temperatures, temperatures of the boundary layer, relative humidities and cloud cover, which are read in the beginning of every 6-h interval. Both daytime and nighttime mixing heights are used in the model.Many of the species in the model vary on a diurnal basis. An investigation of the main mechanisms that determine the diurnal variation of the ozone concentrations is performed. One of the important conditions that is necessary if one wants to represent correctly the diurnal variations of the concentrations is to have access to meteorological data that vary diurnally. This is especially true for the temperature and the mixing height.The use of modern numerical algorithms (which are combined with vectorization of the most time-consuming numerical procedures) allows one to perform long-term runs with the model on several high-speed computers. Results obtained in runs with meteorological data for July 1985 and August–October 1989 are discussed. The computed concentrations and depositions are compared with measurements taken at stations located in different European countries. The agreement between calculated concentrations and measurements is reasonably good.Results obtained with several scenarios, in which the NO_x emission and/or the anthropogenic VOC emissions are varied, are presented. Several main conclusions are drawn by studying the results obtained during the comparisons. Some plans for future development of the models are discussed.     

Comparative study on estimation methods for NOx emissions from a roadway

In order to estimate NO_x concentration at road side areas, it is necessary to determine the NO_x emissions from the automobile passing a road. There are two methods for estimation of NO_x emission. One is calculated by the emission factor of automobile, driving mode and traffic volume. Another is a method based on the relation between NO_x and tracer gas concentration of diffusion experiment.First, diffusion experiments by air tracer were conducted. They were carried out at two areas, one of which was an open area and the other was a highly-built-up area. In the experiment, traffic volume, NO_x and tracer gas concentrations were measured simultaneously. However, the result obtained at the former area was used for this analysis.The NO_x emission rate of the automobile was calculated from the data of traffic survey and tracer gas experiments and both results were compared. Three methods for estimation of NO_x emission rate from traffic survey were employed in this study.From these results, it can be confirmed that both results are in agreement and well correlated, so these estimation methods are considered to be appropriate.     

Anthropogenic emissions of SO2 and NOx in Asia: emission inventories

The anthropogenic emissions of SO₂ and NO_x for 25 Asian countries east of Afghanistan and Pakistan have been calculated for 1975, 1980, 1986, 1986 and 1987 based on fuel consumption, sulfur content in fuels and emission factors for used fuels in each emission category. The provincial- and regional-based calculations have also been made for China and India. The total SO₂ emissions in these parts of Asia have been calculated to be 18.3 and 29.1 Tg in 1975 and 1987, respectively. The calculated total NO_x emissions were 9.4 and 15.5 Tg in 1975 and 1987, respectively. The SO₂ and NO_x emissions in East Asia (China, Japan, South Korea, North Korea and Taiwan) were 23.4 and 10.7 Tg in 1975 and 1987, respectively.     

Hydrogen peroxide levels in Los Angeles: A screening-level evaluation

The major factors affecting the diurnal variation of gaseous hydrogen peroxide were studied using a one-dimensional vertical gas-phase chemistry/transport screening model. The model which included diurnal variations of the inversion layer, surface emissions, dry deposition of air pollutants, and meteorological conditions such as solar radiation, temperature, relative humidity and wind speed, was used to evaluate the influence of the ratio of NMHC/NO_x, the emission rates of NO_x and NMHC, the deposition velocity of H₂O₂, and the height of inversion layer on the ground level gaseous H₂O₂ concentrations. The model was found to yield reasonable agreement with field data from the Carbonaceous Species Methods Comparison Study at Glendora, California, in 11–21 August 1986. Specifically, model predictions and field results all indicated that during clear skies, ambient H₂O₂ concentration was highest at about early afternoon when O₃ concentration was highest and NO_x was lowest. It was concluded that the predicted gaseous H₂O₂ concentration is most sensitive to the emission rate of NO_x and the ratio of NHMC/NO_x, but it is less sensitive to the deposition velocity, height of inversion layer, and the emission rate of NMHC.     

2020～2021年新冠疫情期间南京市PM2.5化学组成与来源变化特征

为了解新冠疫情期间极端减排情景下南京市PM_2.5的化学组成和来源变化,对南京市2020年1～3月和2021年6～8月两次疫情管控前后PM_2.5化学组分(水溶性无机离子、碳质组分和无机元素)的小时观测结果进行分析.结果表明,NO^-₃浓度在两次疫情管控期间比管控前分别下降52.9%和43.0%,高于NH⁺₄(46.4%和31.6%)和SO₄^2-(33.8%和16.5%).由于观测点位于交通干道附近,元素碳(EC)的下降幅度(35.4%和20.6%)高于有机碳(OC; 11.1%和16.2%).结合以上丰量组分特征比值的变化,推断疫情管控对交通排放的影响比工业活动更显著.各主要丰量组分浓度在疫情管控前后的连续变化过程表明,来自本地交通排放的NO_x对PM_2.5中NO^-₃的形成有重要贡献,并且是短期内本地PM_2.5...     

北京大气气溶胶部分无机组分及相关气体的浓度变化

利用SJAC-MOBIC在2000-05～2000-09的3个采样时段测量了北京大气中的气溶胶SO₄^2-、NO₃^-、NO₂^-、Cl^-及相关气体组分,得出了这些污染组分的逐时变化.结果表明气溶胶Cl^-、NO₂^-、NO₃^-及气体HCl、HNO₂和HNO₃有明显的变化规律,SO₂和气溶胶SO₄^2-的变化取决于SO₂的排放,SO₄^2-的峰值一般比SO₂的峰值晚2h左右.     

广州市氮氧化物的数值模拟及暴露影响评价

主要介绍了大气暴露风险评价ADMER模式的模块组成及其主要功能,并利用该模式对广州地区常规的氮氧化物进行了暴露风险评价研究.利用中尺度气象模式模拟的5km气象场数据和收集整理的年平均污染排放源资料进行了大气污染扩散模拟计算.结果表明,无论是氮氧化物的浓度值还是其时空变化趋势,ADMER模式模拟的结果与实际观测均较一致,相关系数达0.76.氮氧化物的浓度高值出现在冬春季节,夏季的浓度相对较低,这主要是受气象场条件的影响.空间场上,氮氧化物的高值区位于广州地区的西南和中部,与工业大点源以及地面源排放的分布一致,而广州地区东北部氮氧化物的浓度值相对较低.在浓度评估的基础上,对暴露人口也进行了估算.由于广州是广东省的主要人口密集区,所以,定量化暴露人口对于进一步开展污染控制减排策略有一定的指示意义.     

夏季长三角地区臭氧非线性响应曲面模型的建立及应用

2013年8月上旬,长三角地区发生了一次大范围高浓度臭氧污染事件.本研究基于WRF-CMAQ空气质量模型系统,结合长三角地区大气污染物排放清单,构建了臭氧与其前体物之间的非线性响应曲面模型(Response surface modeling,RSM).基于RSM探讨了长三角地区O_3化学的敏感性特征,分析了上海市O_3的来源并预测不同情景下O_3的变化,提出O_3污染的最优控制方案.研究结果表明,长三角地区夏季O3主控因素区域差别较大,上海环科院、杭州卧龙桥、南京玄武湖等城区点位属于VOC控制型;徐州铜山、合肥肥西、丽水青田等郊区属于NOx控制型.O_3的敏感性特征在不同浓度水平下也呈现较大差异,随着O_3浓度水平的升高,各地区NOx敏感性均有所增加.从区域来源来看,远距离传输对平日上海O_3贡献较大,占50%以上;而在O_3污染日,本地及区域贡献为72.1%,而远距离传输贡献下降至27.9%.快速预测了110组减排情景,表明在本地及区域前体物均减排70%的情况下,2013年8月上海O_3浓度能完全达标.     

Chemical and optical properties of aerosols and their interrelationship in winter in the megacity Shanghai of China

A field campaign on air quality was carried out in Shanghai in winter of 2012. The concentrations of NO, NO₂, NO_x, SO₂, CO, and PM_2.5 increased during haze formation. The average masses of SO₄^2-, NO₃^- and NH₄⁺ were 10.3, 11.7 and 6.7 μg/m³ during the haze episodes, which exceeded the average (9.2, 7.9, and 3.4 μg/m³) of these components in the non-haze days. The mean values for the aerosol scattering coefficient (b_sp), aerosol absorption coefficient (b_ap) and single scattering albedo (SSA) were 288.7, 27.7 and 0.91 Mm^-1, respectively. A bi-peak distribution was observed for the mass concentrations of CO, NO, NO₂, and NO_x. More sulfate was produced during daytime than that in the evening due to photochemical reactions. The mass concentration of NH₄⁺ achieved a small peak at noontime. NO₃^- showed lower concentrations in the afternoon and higher concentrations in the early morning. There were obvious bi-peak diurnal patterns for bsp and bap as well as SSA. bsp and bap showed a positive correlation with PM_2.5 mass concentration. (NH₄)₂SO₄, NH₄NO₃, organic mass, elemental carbon and coarse mass accounted for 21.7%, 19.3%, 31.0%, 9.3% and 12.3% of the total extinction coefficient during non-haze days, and 25.6%, 24.3%, 30.1%, 8.1% and 8.2% during hazy days. Organic matter was the largest contributor to light extinction. The contribution proportions of ammonium sulfate and ammonium nitrate to light extinction were significantly higher during the hazy time than during the non-haze days.