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.     

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.     

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.     

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。