大气14CO2的加速器质谱分析技术研究进展

利用加速器质谱技术测定大气¹⁴CO₂以示踪大气化石源CO₂成为当前减污降碳工作的热点。该文从加速器质谱¹⁴C分析基础出发,系统介绍了加速器质谱的工作原理、大气样品的采集及纯化、石墨化样品的制备和测定,阐述了大气碳监测领域14 CO₂测试的研究进展。随着加速器质谱技术的不断发展,大气¹⁴CO₂的研究将会更加广泛和深入,有助于进一步认识大气化石源CO₂的来源,更有针对性地开展减污降碳工作。未来应统一制定¹⁴CO₂监测方法标准,规范操作流程和质控手段,完善实验仪器配套设施,加快提升监测能力和水平。     

Study of urban atmospheric pollution in Navarre (Northern Spain)

An ambient air quality study was undertaken in two cities (Pamplona and Alsasua) of the Province of Navarre in northern Spain from July 2001 to June 2004. The data were obtained from two urban monitoring sites. At both monitoring sites, ambient levels of ozone, NO_x, and SO₂ were measured. Simultaneously with levels of PM₁₀ measured at Alsasua (using a laser particle counter), PM₁₀ levels were also determined at Pamplona (using a beta attenuation monitor). Mean annual PM₁₀ concentrations in Pamplona and Alsasua reached 30 and 28 μg m⁻³, respectively. These concentrations are typical for urban background sites in Northern Spain. By using meteorological information and back trajectories, it was found that the number of exceedances of the daily PM₁₀ limit as well as the PM₁₀ temporal variation was highly influenced by air masses from North Africa. Although North African transport was observed on only 9% of the days, it contributed the highest observed PM₁₀ levels. Transport from the Atlantic Ocean was observed on 68% of the days; transport from Europe on 13%; low transport and local influences on 7%; and transport from the Mediterranean region on 3% of the days. The mean O₃ concentrations were 45 and 55 μg m⁻³ in Pamplona and Alsasua, respectively, which were above the values reported for the main Spanish cities. The mean NO and NO₂ levels were very similar in both sites (12 and 26 μg m⁻³, respectively). Mean SO₂ levels were 8 μg m⁻³ in Pamplona and 5 μg m⁻³ in Alsasua. Hourly levels of PM₁₀, NO and NO₂ showed similar variations with the typically two coincident maximums during traffic rush hours demonstrating a major anthropogenic origin of PM₁₀, in spite of the sporadic dust outbreaks.     

Occurrence of Acid Rain over Delhi

Precipitation samples were collected as wet-fall only andprimarily on event basis in Delhi during the monsoon period of1995. Concentrations of major anions (SO₄ ^2-,NO₃ ^- and Cl^-) andcations (Ca²⁺, Mg²⁺,Na⁺ and K⁺) were determined. The pH of the rain waterwas found to be more than 5.6, showing alkalinity during theearly phase of monsoon, but during the late phase of monsoon pHtendency was towards acidity due to lack of proper neutralizationof acidic ions. Neutralization is not only due to the localprocess but also due to the pre-monsoon Andhi which bringsSuspended Particulate Matter (SPM) containing Ca²⁺,Mg²⁺, Na⁺ and K⁺ as well as the local emission ofNH₃. In the late monsoon the concentration of cations getsreduced because of heavy rainfall and relatively unfavourablecondition for their transport from the adjoining areas, whereasthe anion concentrations remain unchanged owing to theircontinuous emission.     

Inorganic constituents of urban air pollution in the Lazio region (Central Italy)

A field study was carried out at six locations in the Lazio region (Central Italy) aimed at characterising atmospheric particulate matter (PM₁₀ and PM_2.5) from the point of view of the chemical composition and grain size distribution of the particles, the mixing properties of the atmosphere, the frequency and relevance of natural events. The combination of four different analytical techniques (ion chromatography, X-ray fluorescence and ICP for inorganic components, thermo-optical analysis for carbon compounds) yielded sound results in terms of characterisation of the air masses. During the first three months of the study (October–December 2004), many pollution events of natural (sea-salt or desert dust episodes) or anthropogenic nature were identified and characterised. More than 90% of the collected mass was identified by chemical analysis. The central role played by the mixing properties of the lower atmosphere when pollution events occurred was highlighted. The results show a major impact of primary anthropogenic pollutants on traffic stations and a homogeneous distribution of secondary pollutants over the regional area. An evaluation of the sources of PM and an identification of possible reliable tracers were obtained using a chemical fractionation procedure.     

Inorganic constituents of urban air pollution in the Lazio region (Central Italy)

A field study was carried out at six locations in the Lazio region (Central Italy) aimed at characterising atmospheric particulate matter (PM₁₀ and PM_2.5) from the point of view of the chemical composition and grain size distribution of the particles, the mixing properties of the atmosphere, the frequency and relevance of natural events. The combination of four different analytical techniques (ion chromatography, X-ray fluorescence and ICP for inorganic components, thermo-optical analysis for carbon compounds) yielded sound results in terms of characterisation of the air masses. During the first three months of the study (October-December 2004), many pollution events of natural (sea-salt or desert dust episodes) or anthropogenic nature were identified and characterised. More than 90% of the collected mass was identified by chemical analysis. The central role played by the mixing properties of the lower atmosphere when pollution events occurred was highlighted. The results show a major impact of primary anthropogenic pollutants on traffic stations and a homogeneous distribution of secondary pollutants over the regional area. An evaluation of the sources of PM and an identification of possible reliable tracers were obtained using a chemical fractionation procedure.     

北京城区降水对PM2.5和PM10清除作用分析

基于北京市PM_2.5和PM₁₀质量浓度、组分浓度以及降水数据,利用数理统计、相关性分析等方法分别从降水总量、降水时长和降水前颗粒物浓度3个角度研究降水对PM_2.5、PM₁₀的清除作用,同时以一次典型降水过程为例,具体分析降水对颗粒物的影响。结果表明：降水总量的增加有助于促进PM_2.5、PM₁₀的清除,随着降水总量增加,PM_2.5、PM₁₀的平均清除率提高,有效清除的比例增加;连续降水可增强对大气颗粒物的湿清除作用,连续降水达3d可有效降低PM_2.5、PM₁₀浓度;降水对PM_2.5、PM₁₀浓度的清除率和大气颗粒物前一日的平均浓度有较好的正相关性。降水对大气颗粒物的清除可分为清除、回升和平稳3个阶段,各个阶段大气颗粒物的变化趋势不同。降水对于大气气溶胶化学组分和酸碱性的改变具有明显作用,对于大气颗粒物各种组分的清除效果不完全相同。对于大气中OC、NO₃^-、SO₄^2-和NH₄⁺去除率较高,且这4种组分主要以颗粒态形式被冲刷进入降水中,加剧了北京市降水酸化程度。     

基于GOSAT卫星的中国CO2浓度时空特征分析

采用温室气体观测卫星(GOSAT) 傅里叶变换光谱仪(FTS)发布的CO₂柱浓度L₃级别数据集产品,利用TCCON地基站点的CO₂柱浓度数据对卫星遥感数据进行验证,分析中国CO₂柱浓度时空变化特征及其影响因素。研究结果表明,GOSAT卫星的CO₂柱浓度产品精度较高,线性回归的r²为0.99,线性方程斜率为0.98,平均偏差为0.11 mg/L。中国CO₂柱浓度呈现逐年增长的趋势,存在12个月的周期性季节性变化。2010、2020年区域年平均CO₂柱浓度分别约为389.30、412.62 mg/L,增长了23.32 mg/L,年平均增长率大约为0.58%。中国区域大气CO₂柱浓度的月变化存在明显的时空差异,最大值和最小值分别出现在4月和8月,2020年4月和8月的区域平均值分别为415.09、409.13 mg/L。中国区域CO₂柱浓度从东部沿海向西部逐级递减,且呈现明显的季节性变化,夏季高值主要集中在东南部沿海地区,冬季高值主要集中在华北地区。     

环境空气质量新标准对珠三角区域站空气质量评价的影响

利用粤港珠三角区域空气质量监控网中天湖、金果湾与万顷沙3个区域站2010年全年SO₂、NO₂、PM₁₀、O₃、PM_2.5与CO自动监测的数据,分析了实施环境空气质量新标准(GB 3095—2012)对这3个子站空气质量评价的影响。研究发现,若采用新标准,万顷沙的NO₂、PM₁₀和PM_2.5年均浓度将不同程度超标。这3个子站空气质量达标率下降7~28个百分点,空气污染指数从91%~99%下降至63%~91%;O₃的引入是导致空气质量达标率下降的最主要的原因;O₃将取代PM₁₀成为最主要的首要污染物,出现频率大于50%,且O₃(8 h)平均浓度的影响大于O₃ (1 h)浓度的影响。PM_2.5的纳入也是导致空气质量达标率下降的重要因素,其超标率为3%(金果湾)~16%(万顷沙)。NO₂标准的收严未对天湖与金果湾空气质量评价造成影响,但导致万顷沙NO₂的超标率从2%上升至10%,且NO₂作为首要污染物的比例达24%。     

Extreme Nitrogen Oxide and Ozone Concentrations in Athens Atmosphere in Relation to Meteorological Conditions

In the present study, we investigate the variation of NO _x (NO + NO₂) and O₃ concentrations and the relation between the extreme events (episodes) of NO _x and O₃ concentrations and the relevant meteorological conditions in the urban atmosphere of the Athens basin. Hourly data of NO, NO₂ and O₃ concentrations from 10 representative monitoring sites located in the Athens basin were used, covering the 10-year time period from 1994 to 2003. The results of our analysis show that the concentrations of air pollutants differ significantly from one monitoring site to another, due to the location and proximity of each station to the emission sources. For each site, there are also significant differences in NO _x and O₃ concentrations from day to day, as well as from month to month and/or from season to season. The annual and seasonal variations show higher NO values in winter and lower in summer. On the contrary, NO₂ and O₃ values are higher in summer (photochemical production of O₃) and lower in winter. These differences are attributed, to a large extent, to the prevailing synoptic and meteorological conditions, the most important between them being the wind direction and speed as well as the atmospheric pressure. Our analysis of the identified 179 extreme NO _x air pollution events shows that most of them took place under anticyclonic conditions, associated with calm or weak winds (speed <2.5 ms⁻¹) of mostly southern to southwestern directions, as well as with low air temperatures and intense stable surface atmospheric conditions. There exists a significant decreasing tendency in NO _x air pollution episodic events over the 10-year study period, resulting in very few to none events in the period from 2000 to 2003. As far as it concerns the extreme O₃ concentrations, 34 air pollution events were identified, occurring under high air temperatures, variable weak winds and intense solar irradiation. The trends of O₃ concentrations are stronger in suburban sites than in urban ones.     

臭氧前体物排放清单相关模型及应用

欧美等国家对于O_3污染的研究开展较早,已建立较成熟的O_3污染生成、扩散及空气质量等模型。文章主要介绍评述了美国环保局推荐使用的计算O_3前体物的相关模型(MOVES、NONROAD、SMOKE、EMFAC和EDMS),从基本原理和功能、污染源类型、研究尺度、所需参数等方面对比分析各模型的特点和适用范围,并综述其国内外研究应用情况;讨论了中国在这些模型的使用方面应该注意的问题,如加强开展模型计算结果验证和基础实验获得本土化的模型参数,以及中国开发的相关模型的优势和适用性等。     

Assessment of Ambient Air Quality in Urban Centres of Haryana (India) in Relation to Different Anthropogenic Activities and Health Risks

Considering the mounting evidences of the effects of air pollution on health, the present study was undertaken to assess the ambient air quality status in the fast growing urban centres of Haryana state, India. The samples were collected for total suspended particulate matter (TSPM), respirable suspended particulate matter (PM₁₀), sulfur dioxide (SO₂), and oxides of nitrogen (NO₂) during different seasons from 8 districts of Haryana during January, 1999 to September, 2000. The four types of sampling sites with different anthropogenic activities i.e. residential, sensitive, commercial and industrial were identified in each city. The ambient air concentration of TSPM and PM₁₀ observed was well above the prescribed standards at almost all the sites. The average ambient air concentrations of SO₂ and NO₂ were found below the permissible limits at all the centres. Comparatively higher concentration of SO₂ was observed during winter seasons, which seems to be related with the enhanced combustion of fuel for space heating and relatively stable atmospheric conditions. Air Quality Index (AQI) prepared for these cities shows that residential, sensitive and commercial areas were moderately to severely polluted which is a cause of concern for the residents of these cities. The high levels of TSPM and SO₂ especially in winter are of major health concern because of their synergistic action. The data from Hisar city reveals a significant increase in the total number of hospital visits/admissions of the patients with acute respiratory diseases during winter season when the level of air pollutants was high.     

Influence of Meteorological Parameters on Particulates and Atmospheric Pollutants at Taichung Harbor Sampling Site

Atmospheric aerosol particles and metallic concentrations, ionic species were monitored at the Experimental harbor of Taichung sampling site in this study. This work attempted to characterize metallic elements and ionic species associated with meteorological conditions variation on atmospheric particulate matter in TSP, PM_2.5, PM_2.5–10. The concentration distribution trend between TSP, PM_2.5, PM_2.5–10 particle concentration at the TH (Taichung harbor) sampling site were also displayed in this study. Besides, the meteorological conditions variation of metallic elements (Fe, Mg, Cr, Cu, Zn, Mn and Pb) and ions species (Cl⁻, NO₃ ⁻, SO₄ ²⁻, NH₄ ⁺, Mg²⁺, Ca²⁺ and Na⁺) concentrations attached with those particulate were also analyzed in this study. On non-parametric (Spearman) correlation analysis, the results indicated that the meteorological conditions have high correlation at largest particulate concentrations for TSP at TH sampling site in this study. In addition, the temperature and relative humidity of meteorological conditions that played a key role to affect particulate matter (PM) and have higher correlations then other meteorological conditions such as wind speed and atmospheric pressure. The parameter temperature and relative humidity also have high correlations with atmospheric pollutants compared with those of the other meteorological variables (wind speed, atmospheric pressure and prevalent wind direction). In addition, relative statistical equations between pollutants and meteorological variables were also characterized in this study.     

2001年～2008年及奥运会期间天津市大气污染特征分析

根据天津市大气质量监测数据,对2001年～2008年及奥运会期间天津市大气污染特征和主要大气污染物的变化规律进行了分析。结果表明,2001年～2008年天津市的PM10、SO2和NO2污染总体呈下降趋势,但质量浓度仍相对较高。2008年8月奥运会期间天津市PM10和SO2质量浓度达到国家空气质量二级标准,NO2质量浓度达到国家空气质量一级标准,空气质量良好。天津市PM10污染相对稳定,SO2和NO2的污染分布呈现明显的季节性,时间上表现为冬强夏弱。气象条件对污染物浓度影响明显,沙尘、大雾等天气可使污染物浓度急剧升高。     

宁波市区冬季大气颗粒物及其主要组分的污染特征分析

为了更好地研究影响宁波市区环境空气质量的污染物变化特征,于2010年1月20—30日进行了加强监测。研究结果表明,宁波市区大气中PM₁₀和PM_2.5质量浓度较高,其中PM_2.5/PM₁₀为0.5~0.85。对PM₁₀和PM_2.5采样膜分析,水溶性粒子和含碳组分分别占PM₁₀和PM_2.5质量浓度的56.7%和66.9%,其中二次污染的水溶性离子SO₄^2-、NO₃^-和NH₄⁺是PM₁₀和PM_2.5中浓度较高的离子组分;PM_2.5样品中OC与EC的相关性较好,表明OC与EC的来源相对一致,可能主要来自机动车尾气的贡献;但PM₁₀样品中OC与EC的相关性较差,表明其来源相对复杂;其中SOC的浓度占OC的13%~35%,说明宁波市区冬季导致二次污染的光化学反应不活跃。     

大同市大气颗粒物浓度与水溶性离子季度分布特征

为研究大同市大气颗粒物质量浓度与水溶性离子组成特征,于2013年2、7、9、12月,分别对大同市及其对照点庞泉沟国家大气背景点进行了PM2.5及PM10的采样,通过超声萃取-IC法测定了样品中的9种水溶性离子,结果表明,大同市大气颗粒物污染1、4季度重于2、3季度,PM2.5季度均值全年均未超标,PM10仅第1季度超标1.4倍,污染状况总体良好,PM2.5与PM10相关系数R为0.75,说明大同市颗粒物污染有较为相近的来源,且不同季节均以粗颗粒物为主;大同市PM2.5中水溶性离子浓度分布为SO2-4、NO-3、NH+4Cl-、Ca2+K+、Na+F-、Mg2+,PM10中Ca2+浓度仅次于SO2-4、NO-3,控制扬尘将有效降低PM10的浓度;PM2.5及PM10中的9种水溶性离子在不同季度的浓度与颗粒物浓度分布规律类似,1、4季度较高,2、3季度较低;由阴阳离子平衡计算结果可知,相关性方程的斜率K为1.045,表明大同市大气颗粒物中阳离子相对亏损,大气细粒子组分偏酸性。NO-3与SO2-4浓度比值均小于1,大同市以硫酸型污染为主,大气中的SO2-4主要来源于人类活动排放。     

烟花爆竹禁燃对春节期间东北地区空气质量影响评估

利用2015—2017年春节期间东北地区主要大气污染物(PM_(10)、PM_(2.5)、SO_2、NO_2、CO和O3)质量浓度监测资料及相应气象因子(温度、湿度、风速和气压)观测资料,分析了春节期间烟花爆竹禁燃对东北地区空气质量的影响。结果表明:随着东北地区主要城市禁燃力度的增强,空气质量逐年提升,PM_(2.5)和SO_2浓度逐年大幅度下降。禁燃可明显降低城区PM_(2.5)浓度,而由于春节期间污染源整体减少,城区和城郊监测点PM_(2.5)浓度值差异减小。烟花爆竹对PM_(10)和PM_(2.5)浓度影响高于对气体污染物SO_2、NO_2和CO的影响。此外,气象条件对东北地区春节期间禁燃改善空气质量的效果也有明显影响。因此,结合春节期间的气象条件,在东北地区实施禁燃政策动态调整非常必要。     

成都市夏季近地面臭氧污染气象特征

利用2016年7月成都市8个环境监测站点的臭氧、NO_2的监测资料以及成都市国家基准气象站和基本气象站的观测资料,对成都市夏季臭氧、NO_2浓度和气象要素的日变化特征和臭氧污染过程进行了分析。研究结果表明:成都市臭氧污染受综合气象条件和NO_2浓度的影响,高温、低湿、强辐射有利于臭氧大量生成,NO_2浓度高低决定了臭氧浓度的峰值大小;在污染期间,大气边界层高度远高于本地平均水平,数值约为平均水平的2～3倍;成都市臭氧污染的主要影响因子存在地区差异,成都市区的臭氧主要来自于自身的光化学反应,而灵岩寺地区的臭氧来自于VOCs和大气水平输送。     

Outdoor-indoor air quality in Riyadh: SO2, NH3, and HCHO

A funded research project was conducted during the period July1992 through November 1994. The project was designed to evaluateindoor and ambient air quality in and around buildings of different types and uses in Riyadh, the capital of Saudi Arabia.Thirty intercity buildings and two outercity (background) siteswere carefully selected and monitored for air quality. Ten airpollutants, together with relevant meteorological parameters, were monitored indoor and outdoor at each site continuously andsimultaneously for a period of two weeks covering summer and winter seasons.This article discusses the results obtained for sulfur dioxide (SO₂), ammonia (NH₃) and formaldehyde (HCHO). Results of this investigation revealed that most sites had on the averageexceeded the recommended standards for SO₂ and NH₃ bothindoor and outdoor, with indoor levels being worse than outdoorduring winter time. Several sites also showed high levels of HCHO, with outdoor levels being consistently higher than indoor.Statistical and frequency analyses were performed on the collected data, showing seasonal and sector by sector variability, and outdoor-indoor correlations.     

Chemical Constituents of Fugitive Dust

Wind erosion selectively winnows the fine, most chemically concentrated portions of surface soils and results in the inter-regional transport of fugitive dust containing plant nutrients, trace elements and other soil-borne contaminants. We sampled and analyzed surface soils, sediments in transport over eroding fields, and attic dust from a small area of the Southern High Plains of Texas to characterize the physical nature and chemical constituents of these materials and to investigate techniques that would allow relatively rapid, low cost techniques for estimating the chemical constituents of fugitive dust from an eroding field. From chemical analyses of actively eroding sediments, it would appear that Ca is the only chemical species that is enriched more than others during the process of fugitive dust production. We found surface soil sieved to produce a sub-sample with particle diameters in the range of 53–74 μm to be a reasonably good surrogate for fugitive dust very near the source field, that sieved sub-samples with particle diameters <10 μm have a crustal enrichment factor of approximately 6, and that this factor, multiplied by the chemical contents of source soils, may be a reasonable estimator of fugitive PM₁₀ chemistry from the soils of interest. We also found that dust from tractor air cleaners provided a good surrogate for dust entrained by tillage and harvesting operations if the chemical species resulting from engine wear and exhaust were removed from the data set or scaled back to the average of enrichment factors noted for chemical species with no known anthropogenic sources. Chemical analyses of dust samples collected from attics approximately 4 km from the nearest source fields indicated that anthropogenic sources of several environmentally important nutrient and trace element species are much larger contributors, by up to nearly two orders of magnitude, to atmospheric loading and subsequent deposition than fugitive dust from eroding soils.     

北京地区不同季节PM2.5和PM10浓度对地面气象因素的响应

利用2013年1月—2014年12月北京地区PM_(2.5)和PM_(10)监测数据和同期近地面气象观测数据,采用非参数分析法(Spearman秩相关系数)研究了北京地区PM_(2.5)和PM_(10)的浓度对不同季节地面气象因素的响应。结果表明:北京地区大气颗粒物浓度水平具有明显的季节特征,冬季大气颗粒物污染最严重,夏季最轻。不同季节影响颗粒物浓度水平的气象因素各不相同,其中风速和日照时数为主要影响因素。PM_(2.5)和PM_(10)质量浓度对气象因素变化的响应程度也有较大区别,PM_(2.5)/PM_(10)比值冬季最高,PM_(2.5)影响最大,春季最低,PM_(10)影响最大。这些结论可对制订科学有效的大气污染控制策略提供参考。