A comparative study of US EPA 1996 and 1999 emission inventories in the west Gulf of Mexico coast region, USA

Emission inventory is one of the required inputs to air quality models. To assist in the urban and regional modeling efforts, United States Environmental Protection Agency (EPA) has compiled a National Emission Inventory (NEI) for criterion pollutants, and the precursors of ozone and particulate matter (PM). In December 2002, EPA released the 1999 NEI estimates (NEI99), which represent the most recent national emission data. However, the data sets are not in model-ready format for air quality simulations. This present work converts the NEI99 Final Version 2 data sets into Inventory Data Analyzer (IDA) format and processes the data using the Sparse Matrix Operator Kernel Emissions (SMOKE) modeling system to generate a gridded emission inventory in a domain covering the west Gulf Coast Region, USA. The spatial and diurnal emission characteristics of the gridded emission inventories are then assessed and compared with those of the National Emission Trend 1996 (NET96). The NEI99 database contains more complete emission records in both area and point sources. It is also found that NEI99 data exhibit greater emissions with respect to point and mobile sources but smaller emissions with respect to area sources when compared to the corresponding gridded NET96 data in the same study domain. The most distinct differences between the NEI99 and NET96 databases are CO emission of mobile sources, SO2 emissions of point sources, and VOC/PM/NH3/NOx emissions of area and non-road sources. The gridded NEI99 data show low VOC/NOx ratios (<2-5) in the urban areas of the study domain.     

Estimation of biogenic emissions with satellite-derived land use and land cover data for air quality modeling of Houston-Galveston ozone nonattainment area

The Houston-Galveston Area (HGA) is one of the most severe ozone non-attainment regions in the US. To study the effectiveness of controlling anthropogenic emissions to mitigate regional ozone nonattainment problems, it is necessary to utilize adequate datasets describing the environmental conditions that influence the photochemical reactivity of the ambient atmosphere. Compared to the anthropogenic emissions from point and mobile sources, there are large uncertainties in the locations and amounts of biogenic emissions. For regional air quality modeling applications, biogenic emissions are not directly measured but are usually estimated with meteorological data such as photo-synthetically active solar radiation, surface temperature, land type, and vegetation database. In this paper, we characterize these meteorological input parameters and two different land use land cover datasets available for HGA: the conventional biogenic vegetation/land use data and satellite-derived high-resolution land cover data. We describe the procedures used for the estimation of biogenic emissions with the satellite derived land cover data and leaf mass density information. Air quality model simulations were performed using both the original and the new biogenic emissions estimates. The results showed that there were considerable uncertainties in biogenic emissions inputs. Subsequently, ozone predictions were affected up to 10 ppb, but the magnitudes and locations of peak ozone varied each day depending on the upwind or downwind positions of the biogenic emission sources relative to the anthropogenic NOx and VOC sources. Although the assessment had limitations such as heterogeneity in the spatial resolutions, the study highlighted the significance of biogenic emissions uncertainty on air quality predictions. However, the study did not allow extrapolation of the directional changes in air quality corresponding to the changes in LULC because the two datasets were based on vastly different LULC category definitions and uncertainties in the vegetation distributions.     

Allocating anthropogenic pollutant emissions over space: application to ozone pollution management

An inventory of volatile organic compound (VOC) and nitrogen oxides (NOx) emissions is an important tool for the management of ground-level ozone pollution. This paper has two broad aims: it illustrates the potential of a geographic information system (GIS) for enhancing an existing spatially-aggregated, anthropogenic emissions inventory (EI) for Tucson, AZ, and it discusses the ozone-specific management implications of the resulting spatially-disaggregated EI. The main GIS-related methods include calculating emissions for specific features, spatially disaggregating region-wide emissions totals for area sources, and adding emissions from various point sources. In addition, temporal allocation factors enable the addition of a multi-temporal component to the inventory. The resulting inventory reveals that on-road motor vehicles account for approximately 50% of VOC and NOx emissions annually. On-road motor vehicles and residential wood combustion are the largest VOC sources in the summer and winter months, respectively. On-road motor vehicles are always the largest NOx sources. The most noticeable weekday vs. weekend VOC emissions differences are triggered by increased residential wood combustion and increased lawn and garden equipment use on weekends. Concerning the EI's uncertainties and errors, on-road mobile, construction equipment, and lawn and garden equipment are identified as sources in the most need of further investigation. Overall, the EIs spatial component increases its utility as a management tool, which might involve visualization-driven analyses and air quality modeling.     

运用机器学习方法预测空气中臭氧浓度

臭氧(O_3)浓度变化与天然源、移动源和点源的排放量存在某些隐含的关联。根据臭氧浓度变化的特性,基于污染源在线排放数据、气象监测数据以及空气质量监测数据构造特征,运用机器学习方法进行逐小时臭氧浓度预测。该方法不仅充分利用了臭氧浓度变化时序数据,而且考虑了气象条件变化对污染物浓度变化的影响,最重要的是将点源排放氮氧化物这一臭氧生成的重要前体物纳入模型考虑。在金砖国家领导人厦门会晤前后(2017年8月31日至9月9日),运用该方法对厦门市溪东、洪文、鼓浪屿和湖里中学四个大气自动监测站的臭氧小时浓度平均值进行滚动预报,比较准确地模拟出臭氧浓度的日周期性变化,同时对峰值和低谷能够进行较为有效的捕捉和刻画。按照《环境空气质量标准》(GB3095—2012)臭氧日最大八小时浓度平均值进行评价,四个站点均取得了90%的预报等级准确率。     

资阳市大气污染源排放清单研究

采用实地调研、资料收集等方式获得了2017年资阳市典型污染源的活动水平数据,参照城市大气污染物排放清单编制技术手册建立了基于排放因子法和物料衡算法的资阳市大气污染源排放清单,分析了主要污染物的行业排放特征和空间分布特征。结果表明,2017年资阳市SO₂、NO_X、CO、PM₁₀、PM_2.5、VOCs、NH₃总排放量分别为3.58kt、13.91kt、94.91kt、25.51kt、8.67kt、23.84kt和46.44kt。SO₂排放主要来自工业源;NOX排放主要来自移动源;CO排放主要来自工业过程及移动源;PM₁₀和PM_2.5、排放来自扬尘源和露天秸秆焚烧;VOCs主要来自溶剂使用源;NH₃主要来自农业活动。资阳市主要污染物排放分布在工业点源较为集中的雁江区和安岳县,乐至县污染物排放量相对较小。     

Determination of volatile organic compound emissions and ozone formation from spraying solvent-based pesticides

Large-scale agricultural activities have come under scrutiny for possible contributions to the emission of ozone precursors. The San Joaquin Valley (SJV) of California is an area with intense agricultural activity that exceeds the federal ozone standards for more than 30 to 40 d yr(-1) and the more stringent state standards for more than 100 d yr(-1). Pesticides are used widely in both agricultural and residential subregions of the SJV, but the largest use, by weight of "active ingredient," is in agriculture. The objective of the study was to determine the role of pesticide application on airborne volatile organic compounds (VOC) concentrations and ozone formation in the SJV. The ozone formation from the pesticide formulation sprayed on commercial orchards was studied using two transportable smog chambers at four application sites during the summers of 2007 and 2008. In addition to the direct measurements of ozone formation, airborne VOC concentrations were measured before and after pesticide spraying using canister and sorbent tube sampling techniques. Soil VOC concentrations were also measured to understand the distribution of VOCs between different environmental compartments. Numerous VOCs were detected in the air and soil samples throughout the experiment but higher molecular weight aromatic hydrocarbons were the primary compounds observed in elevated concentrations immediately after pesticide spraying. Measurements indicate that the ozone concentration formed by VOC downwind of the orchard may increase up to 15 ppb after pesticide application, with a return back to prespray levels after 1 to 2 d.     

中国农业与工程机械尾气减排控制措施的费效分析

移动源尾气排放已成为我国空气污染的主要来源之一,相比于道路移动源来说,非道路移动源尾气排放的减排控制工作仍处于初级阶段。本研究就非道路移动源尾气减排控制的三种主要措施——整车淘汰、发动机更换以及发动机维修,对中国非道路工程和农业机械进行费效分析,探讨经济可行的控制途径。研究假设农业和工程机械的使用年限分别为15年和10年,同时假设采取减排措施后所有机械均达到国IV排放标准。研究表明,采取减排措施后,农业机械每年可减排NOx 40万～45万t,但PM污染物减排效益不明显;工程机械每年可减排NOx约52万t,且PM污染物每年可减排量约16万t,但费用可高达2000亿～25 000亿元,且不同措施的差别巨大,以整车淘汰费用最高。多数农业机械发动机维修所需费用高于发动机更换,相反,工程机械发动机更换所需费用高于发动机维修。因此,在采用减排措施和制定政策时,需要根据实际情况进行调整。对农业机械,采用发动机更换的减排方式更经济;对工程机械,采用发动机维修的减排措施更实惠。     

Volatile organic compounds in the unsaturated zone from radioactive wastes

Volatile organic compounds (VOCs) are often comingled with low-level radioactive wastes (LLRW), but little is known about subsurface VOC emanations from LLRW landfills. The current study systematically quantified VOCs associated with LLRW over an 11-yr period at the USGS Amargosa Desert Research Site (ADRS) in southwestern Nevada. Unsaturated-zone gas samples of VOCs were collected by adsorption on resin cartridges and analyzed by thermal desorption and GC/MS. Sixty of 87 VOC method analytes were detected in the 110-m-thick unsaturated zone surrounding a LLRW disposal facility. Chlorofluorocarbons (CFCs) were detected in 100% of samples collected. Chlorofluorocarbons are powerful greenhouse gases, deplete stratospheric ozone, and are likely released from LLRW facilities worldwide. Soil-gas samples collected from a depth of 24 m and a horizontal distance 100 m south of the nearest waste-disposal trench contained >60,000 ppbv total VOCs, including >37,000 ppbv CFCs. Extensive sampling in the shallow unsaturated zone (0-2 m deep) identified areas where total VOC concentrations exceeded 5000 ppbv at the 1.5-m depth. Volatile organic compound concentrations exceeded background levels up to 300 m from the facility. Maximum vertical diffusive fluxes of total VOCs were estimated to be 1 g m yr. Volatile organic compound distributions were similar but not identical to those previously determined for tritium and elemental mercury. To our knowledge, this study is the first to characterize the unsaturated zone distribution of VOCs emanating from a LLRW landfill. Our results may help explain anomalous transport of radionuclides at the ADRS and elsewhere.     

Economic-environmental modeling of point source pollution in Jefferson County,Alabama, USA

This paper uses an integrated economic-environmental model to assess the point source pollution from major industries in Jefferson County, Northern Alabama. Industrial expansion generates employment, income, and tax revenue for the public sector; however, it is also often associated with the discharge of chemical pollutants. Jefferson County is one of the largest industrial counties in Alabama that experienced smog warnings and ambient ozone concentration, 1996-1999. Past studies of chemical discharge from industries have used models to assess the pollution impact of individual plants. This study, however, uses an extended Input-Output (I-O) economic model with pollution emission coefficients to assess direct and indirect pollutant emission for several major industries in Jefferson County. The major findings of the study are: (a) the principal emission by the selected industries are volatile organic compounds (VOC) and these contribute to the ambient ozone concentration; (b) the direct and indirect emissions are significantly higher than the direct emission by some industries, indicating that an isolated analysis will underestimate the emission by an industry; (c) while low emission coefficient industries may suggest industry choice they may also emit the most hazardous chemicals. This study is limited by the assumptions made, and the data availability, however it provides a useful analytical tool for direct and cumulative emission estimation and generates insights on the complexity in choice of industries.     

攀枝花市区及盐边县城区城市臭氧污染状况研究

攀枝花市区臭氧污染负荷逐年上升,盐边县城区近年来臭氧污染负荷均高于20%,臭氧污染已成为影响城市空气质量的重要因素。对2017年1月~2020年2月攀枝花市区和盐边县城区臭氧污染物浓度时空变化规律和相关性进行了研究,并结合攀枝花各地太阳能和天气网记录的气象数据,统计了太阳辐射强度、紫外线辐射强度、日最高气温、日平均风向、季节气候等气象要素与出现臭氧污染的概率。研究表明,攀枝花市区和盐边县城区两地春、夏季较易出现臭氧污染,春季臭氧浓度持续高值时数最多,夏季臭氧浓度持续高值影响时数次之,两地臭氧污染物浓度变化有极强相关性。此外,臭氧浓度与气象条件密切关系,当紫外辐射强度大于30W/m²时,臭氧污染的几率为5%~8%,最高日气温值29℃~36℃之间时易出现臭氧污染,攀枝花市区臭氧污染受西向气流影响最重,盐边县城区臭氧污染受南向气流影响最重,盐边城区臭氧污染主要受攀枝花市区影响。根据臭氧污染物浓度时空变化规律和气象条件,开展区域臭氧前体物排放调控,将有效改善地区环境空气质量。     

Photochemical model evaluation of the surface ozone impact of a power plant in a heavily industrialized area of southwestern Spain

The characterization and evaluation of the impact that an industry is likely to have on the surrounding ozone levels is one of many problems confronting air quality managers and should be taken into consideration when authorizing its installation. The correct management of an environment, in terms of monitoring existing industries and planning new activities, requires adequate knowledge of the processes sustained by the industrial emissions therein.This paper explores the improvements in air quality management arising from taking into account the uncertainties involved in the photochemical modeling of the impact of an industry on surface ozone levels.For this, we evaluate the impact on ozone levels of a power plant located in an industrial area of southwestern Spain (Huelva). The evaluation takes into account the effects of both emissions' uncertainty and the non-linear chemistry between ozone and its precursors, thus providing a probable range of increase over the normative values (hourly and 8-hourly maximums) defined in the European Directive. The proposed methodology is easily applicable by air quality managers.Advanced modeling techniques were used for the power plant assessment, MM5 atmospheric modeling system, and air quality model CAMx. The results from meteorology and ozone forecasts have shown acceptable agreement with the observations.The spatial distribution of the impact is found to be strongly determined by mesoscale meteorological processes, which are reinforced by the local orography; there is also a marked temporal evolution. The industrial plume is observed to induce a decrease (or maintenance) of the ozone levels near the emission source (0–10 km), and an increase in the ozone concentrations farther away (with maximums between 10 and 50 km). In fact, in the meteorological episodes with a predominance of local breeze circulations, impacts have been detected at distances of more than 100 km from the emission source.Sensitivity of the power plant impact to variations in ozone precursor emissions is described, and the scenarios and the points in the domain presenting higher sensitivity and registering larger impacts are also identified. The results show that the largest impacts take place in emission scenarios where the NO_x has been reduced with respect to the base case scenario. In contrast, in scenarios where the VOC emissions are reduced with respect to the base case scenario, the impact is smaller or remains unchanged. This is important in areas like the study case, where there is a high percentage of biogenic VOC emissions and the industrial areas are close to natural protected areas and agricultural fields.     

城市空气质量达标规划编制中的关键技术及其案例应用

本文结合重庆市空气质量限期达标规划编制案例,介绍了城市空气质量达标规划编制中的几个关键技术及其具体应用,包括本地化污染源排放清单编制、污染物来源解析、污染物排放形势预测与减排潜力分析以及大气环境容量核算等。本地化污染源排放清单是城市空气质量达标规划编制的基础,针对现有污染源制定科学合理的减排方案是达标规划的核心内容。分析不同区域的污染物组分浓度特征、污染源贡献以及未来污染排放形势预测,有助于识别出制约未来空气质量达标的关键因素及污染源。基于污染源减排潜力和污染传输矩阵制定的污染源减排方案更具合理性和可行性,应用空气质量模型估算大气环境容量可为规划目标可达性提供依据。     

成都市大气中O3污染水平及来源分析

根据2009年夏季成都市区大气中O3的监测结果,对大气中O3的浓度、分布进行了分析,并与2001年夏季成都市区的监测结果比较,分析臭氧污染水平的变化。结合同期NO2、VOCs监测结果,研究O3与两种前体物之间的相互关系。结果表明,近年来成都市区O3浓度呈上升趋势;O3浓度与NO2浓度变化趋势相反,表现为消耗NO2型光化学污染。     

固定源NO_x排放控制技术研究进展

有效控制固定源NOx排放是解决我国NOx污染的关键之一。本文论述了各种烟气脱硝技术的特点,主要讨论了其中应用最为广泛的NH3-SCR技术的研究进展,包括反应动力学、反应机理以及NH3-SCR的金属氧化物催化剂、分子筛类催化剂和碳基催化剂的研究现状。     

Ground-level ozone in the Pearl River Delta and the roles of VOC and NO(x) in its production

In many regions of China, very rapid economic growth has been accompanied by air pollution caused by vehicle emissions. In one of these regions, the Pearl River Delta, the variations of ground-level ozone and its precursors were investigated. Overall, the ambient concentrations of NO(2) increased quickly between 1995 and 1996, but then slightly decreased due to stringent nitrogen oxide (NO(x)) emission controls. Nonetheless, ambient NO(2) levels in the Pearl River Delta remained high. The regional average concentrations of volatile organic compounds (VOCs) were 290 ppbC in summer and 190 ppbC in autumn. Local emissions and long-distance transportation of pollutants play important roles in the regional distribution of VOCs. Ambient O(3) production is significant in urban areas and also downwind of cities. The relative incremental reactivities (RIRs), determined by an observation-based model, showed that ground-level ozone formation in the Guangzhou urban area is generally limited by the concentrations of VOCs, but there are also measurable impacts of NO(x).     

长沙城区大气中二氧化碳浓度变化及与其它污染物相关性分析

利用长沙市城区2011年及2012年连续自动监测获得的CO2数据,两年的平均值为412．2×10^-6,高于世界本底站青海瓦里关5．6％,与临安、无锡相当,略高于乌鲁木齐,而低于北京、上海。冬季CO2浓度日小时变化呈现双峰形态,峰值出现在上午9时及晚上19时～21时。夏季日小时变化为单峰形态,峰值出现在上午8时。冬季CO2浓度日均值为420．3×10^-6,比夏季高3．4％。CO2除与O3呈负相关以外,与其它污染物均呈现显著性正相关,特别是与CO、NO、NO2、NOx、SO2的相关性最强,而与颗粒物（PM10、PM25）的相关性稍差。     

气温和湿度在泸州市城区对臭氧浓度预测的运用研究

气温和湿度均为影响臭氧生成的要素,通过分析泸州市国控点数据,找出气温和湿度与臭氧浓度的关系,从而建立气温和湿度为变量的臭氧浓度预测模型.选取2019年泸州市主城区的气温和湿度数据,将气温按日最高温(Tmax)、日最低温(Tmin)和日平均气温(Tmean)划分,将湿度按四季划分,分别统计其与臭氧浓度的相关性.发现臭氧浓...     

Characteristics of major secondary ions in typical polluted atmospheric aerosols during autumn in central Taiwan

In autumn of 2008, the chemical characteristics of major secondary ionic aerosols at a suburban site in central Taiwan were measured during an annually occurring season of high pollution. The semicontinuous measurement system measured major soluble inorganic species, including NH(4)(+), NO(3)(-), and SO(4)(2-), in PM(10) with a 15 min resolution time. The atmospheric conditions, except for the influences of typhoons, were dominated by the local sea-land breeze with clear diurnal variations of meteorological parameters and air pollutant concentrations. To evaluate secondary aerosol formation at different ozone levels, daily ozone maximum concentration (O(3,daily max)) was used as an index of photochemical activity for dividing between the heavily polluted period (O(3,daily max) ≧80 ppb) and the lightly polluted period (O(3,daily max)<80 ppb). The concentrations of PM(10), NO(3)(-), SO(4)(2-), NH(4)(+) and total major ions during the heavily polluted period were 1.6, 1.9, 2.4, 2.7 and 2.3 times the concentrations during the lightly polluted period, respectively. Results showed that the daily maximum concentrations of PM(10) occurred around midnight and the daily maximum ozone concentration occurred during daytime. The average concentration of SO(2) was higher during daytime, which could be explained by the transportation of coastal industry emissions to the sampling site. In contrast, the high concentration of NO(2) at night was due to the land breeze flow that transport inland urban air masses toward this site. The simulations of breeze circulations and transitions were reflected in transports and distributions of these pollutants. During heavily polluted periods, NO(3)(-) and NH(4)(+) showed a clear diurnal variations with lower concentrations after midday, possibly due to the thermal volatilization of NH(4)NO(3) during daytime and transport of inland urban plume at night. The diurnal variation of PM(10) showed the similar pattern to that of NO(3)(-) and NH(4)(+) aerosols. This indicated that the formatted secondary aerosols in the inland urban area could be transported to the coastal area by the weak land breeze and deteriorated the air quality in the coastal area at night.     

臭氧同时脱硫脱硝技术研究进展

对利用臭氧同时脱硫脱硝技术进行了综述，分析了臭氧对NOx的脱除机理。臭氧同时脱硫脱硝技术具有明显的一体化脱除特性，但臭氧的发生费用却制约了它的应用。介绍了目前国外在工程上应用的低温氧化技术（LOTOX），分析了其脱除效果及优缺点。     

Abundances and flux estimates of volatile organic compounds from a dairy cowshed in Germany

Animal husbandry and manure treatment have been specifically documented as significant sources of methane, ammonia, nitrous oxide, and particulate matter. Although volatile organic compounds (VOCs) are also produced, much less information exists concerning their impact. We report on chemical ionization mass spectrometry and photo-acoustic spectroscopy measurements of mixing ratios of VOCs over a 2-wk measurement period in a large cowshed at the Federal Agricultural Research Centre (FAL) in Mariensee, Germany. The high time resolution of these measurements enables insight into the sources of the emissions in a typical livestock management setting. During feeding hours and solid manure removal, large mixing ratio spikes of several VOCs were observed and correlated with simultaneous methane, carbon dioxide, and ammonia level enhancements. The subsequent decay of cowshed concentration due to passive cowshed ventilation was used to model emission rates, which were dominated by ethanol and acetic acid, followed by methanol. Correlations of VOC mixing ratios with methane or ammonia were also used to calculate cowshed emission factors and to estimate potential nationwide VOC emissions from dairy cows. The results ranged from around 0.1 Gg carbon per year (1 Gg = 10(9) g) for nonanal and dimethylsulfide, several Gg carbon per year for volatile fatty acids and methanol, to over 10 Gg carbon per year of emitted ethanol. While some estimates were not consistent between the two extrapolation methods, the results indicate that animal husbandry VOC emissions are dominated by oxygenated compounds and may be a nationally but not globally significant emission to the atmosphere.