运城大气污染物时空演化特征及源区分析

在复合型大气污染治理常态化背景下,联防联控的治理模式已经成为当今区域性大气污染的主要解决措施和根本途径。本文通过山西省运城市大气污染物监测站点监测到的大气数据,分析了2021年运城市大气污染物SO₂、NO₂、CO、O₃、PM_2.5、PM₁₀浓度的时空分布特征和与气象因素的相关性,通过分析运城市污染物的排放清单计算出了大气污染物的排放指标和排放量,从时间和空间的角度对其防控管理工作提出了建议,以期为同行今后工作提供一定的参考和借鉴。     

基于无人机的大气细颗粒物与臭氧污染探测与溯源研究进展

近年来,中国大气细颗粒物(PM_2.5)污染的治理已取得阶段性成效,但臭氧(O₃)污染快速上升,实现PM_2.5和O₃协同控制的基础与关键是针对大气污染物的精细化探测和污染溯源.随着无人机技术和传感器技术的迅速发展,基于无人机平台的大气污染探测可以有效获得近地层的PM_2.5和O₃结构特征,并结合计算机算法对大气污染事件进行精准溯源,具有高时效性、高灵活性和高时空分辨率的特征,有助于研究人员了解区域污染物的分布、变化以及来源,为大气复合污染的协同控制提供科学依据.通过回顾传统的大气污染探测方法,总结了污染探测领域常用的无人机飞行平台类型和探测仪器,归纳了基于无人机的PM_2.5和O₃污染探测应用与相关溯源算法,并展望了无人机大气探测的未来研究方向.     

“大气十条”实施结束川南城市群秋季霾污染过程中水溶性离子特征

为了解《大气污染防治行动计划》（“大气十条”）实施结束后川南城市群大气PM_2.5的污染状况,于2018年11月7～19日在内江、自贡、宜宾和泸州这4个城市同步采集PM_2.5样品,结合天气形势分析了秋季PM_2.5及主要水溶性离子的污染特征,并利用后向轨迹聚类分析探讨了区域输送对该地区大气污染的影响.结果表明,川南城市群秋季大气平均ρ(PM_2.5)为（67.2±38.3）μg·m^-3,泸州最高而内江最低;SNA(SO^2-₄、 NO^-₃和NH⁺₄)在PM_2.5中占比为33.3%,其中NO^-₃为首要离子组分;由“大气十条”实施中期（2015年）至实施结束（2018年）,内江、宜宾和泸州秋季ρ(PM_2.5)分别增加了13.8%、 47.2%和69.1%,自贡持平;由于大气...     

气候变化对浙江省大气污染的影响

开展气候变化对大气污染影响的研究有利于加深对大气污染形成机理的认识.利用1996-2015年浙江省大气成分、气象观测资料,分析气候变化对大气污染的影响.结果表明,近20 a来浙江省呈年高压天气日数增多、年均气温升高、降水集中及年均净辐射、日照时数、风速、气温日较差和水汽蒸发量都下降的气候变化事实.气候变化引起大气污染扩散能力下降,1996-2015年杭州市和浙江省年均大气扩散指数分别下降了0.55和0.81,降幅分别达35.71%和42.69%.大气扩散指数与ρ（PM₁₀）、ρ（PM_2.5）及年霾日数之间呈显著负相关,当大气扩散指数增大时,大气颗粒物浓度和年霾日数均下降,反之亦然.杭州市大气扩散指数与ρ（PM₁₀）、ρ（PM_2.5）之间的相关系数分别为0.73和0.76.杭州市和浙江省大气扩散指数与年霾日数之间的相关系数分别达到0.77和0.78,T检验值则分别为28.88和30.81,说明由气候变化引起的大气扩散能力改变是影响大气污染的重要原因,但不同大气成分受气候变化的影响程度不同.影响ρ（PM₁₀）的关键气候要素是降水量、风速及相对湿度等,影响ρ（PM_2.5）的主要是辐射、气温,影响ρ（SO₂）的主要是气温,影响ρ（NO₂）及ρ（NO₃-）、ρ（NH₄+）的主要是辐射.总体来说,浙江省近20 a的气候变化事实可能有利于促进ρ（PM₁₀）、ρ（PM_2.5）、ρ（NO₂）及ρ（O₃）等上升,促进ρ（SO₂）、ρ（NO₃-）、ρ（SO₄2-）、ρ（NH₄+）等下降.      

我国大气污染协同防控理论框架初探

我国大气污染防治工作在“十三五”期间取得了可喜成绩,PM_2.5浓度及重污染天数大幅降低,与此同时,我国城市地区臭氧(O₃)污染问题凸显,说明我国大气污染格局发生了深刻变化. 当前,PM_2.5与O₃成为影响我国城市和区域空气质量的主要因子,二者的协同控制是我国持续改善空气质量的焦点,也成为我国“十四五”期间大气污染防治工作的重点. 本文通过对国内外PM_2.5和O₃协同控制进展的梳理,总结我国大气复合污染协同治理的现状与挑战,从协同防控目标、核心协同任务、重点支撑保障等角度提出大气复合污染协同治理的理论框架,并对我国PM_2.5与O₃协同控制工作提出以下几点建议:①坚持科学精准治气;②坚持综合系统治气;③坚持严格依法治气;④坚持多维协同治气.      

安徽省大气污染物时空分布特征及演化规律

在区域复合型大气污染逐渐常态化之下,联防联控治理的新模式已成为解决区域性大气污染的根本途径和有效措施.利用2015年冬季（2015年11月8日—2016年1月20日）、2016年冬季（2016年11月8日—2017年1月20日）安徽省16个城市大气污染物（NO₂、SO₂、CO、O₃、PM₁₀、PM_2.5）浓度数据,结合耦合协调度模型、探索性空间数据分析和障碍度模型,分析大气污染物的时空格局特征,描述其演变规律和总体走向,诊断区域大气污染物中的首要障碍因子.结果表明:①安徽省大气污染物浓度水平具有时间波动性和空间非均衡性,NO₂、O₃、PM₁₀和PM_2.5指数水平表现为递增态势,整体呈现“两高一低”,即皖北高（0.050 3）、中部地区高（0.050 1）和皖南低（0.040 5）的态势,年际变化呈增长趋势,空间分异度变化较大;②安徽省大气污染物耦合度较高,基本维持在拮抗阶段（2015年冬季和2016年冬季耦合度年均值分别为0.480、0.479）,皖北呈增加态势,而中、南部城市主要呈略微降低趋势;包括极度失调和严重失调两种类型（2015年冬季和2016年冬季协调度平均值分别为0.114、0.123）;③安徽省内各城市大气污染物在全省范围内热、冷点分布迥异,2015年冬季和2016年冬季主要经历了聚拢（NO₂、O₃向中部城市聚拢）和北迁（PM₁₀、PM_2.5往北迁）两个过程.研究显示,结合安徽省大气污染物障碍度测量分析,优化和量化区域大气污染物中的首要障碍因子,可为有效开展地区大气污染的防控治理及区域联动提供有利保障.      

哈尔滨冬季积雪中多环芳烃同大气污染物的关系及其潜在源区分析

源于燃烧释放的多环芳烃(PAHs)易于吸附在大气颗粒物上,通过降雪清除效应累积于积雪中,是区域大气污染的良好指示器.于2020年底采集哈尔滨市积雪样本,结合前期逐日大气污染物监测数据(AQI、PM_2.5、PM₁₀、NO₂、SO₂、CO),明确哈尔滨市冬季大气污染类型与污染特征和积雪PAHs空间分布特征与来源,定量解析积雪PAHs同大气污染物的关系,揭示其对大气污染的指示意义,识别哈尔滨市冬季大气污染物的潜在源区.结果表明：研究期内存在3次以PM_2.5为主要污染物的中度污染天气,ρ(PM_2.5)/ρ(PM₁₀)比值表明区域受细颗粒物影响显著,为偏二次污染类型,ρ(NO₂)/ρ(SO₂)和ρ(CO)/ρ(SO₂)比值表明本地固定污染源和外来传输源贡献均呈加强趋势.积雪中Σ16PAHs浓度为1705～7243 ng·L^-1,中高环PAHs浓度属强变异,区...     

雾霾频发区域典型城市大气PM2.5中金属污染特征及来源分析

吸附在大气细颗粒物PM_2.5中的金属元素具有强稳定性和富集性,随着城市大气PM_2.5污染加剧,对公众健康构成极大的威胁。为了解大气PM_2.5中金属污染的地区特征,选取中国雾霾发生频次较高区域中典型城市作为研究对象,概述了2013—2017年城市大气PM_2.5中金属污染水平、时空分布特征及其主要来源。经分析,地区气象条件、工业布局和污染源的差别是各城市大气PM_2.5中金属元素污染水平及时空分布存在较大差异的主要原因。二次气溶胶、燃煤和生物质燃烧在研究城市大气PM_2.5金属元素来源中占据主要贡献,其他源类在各个地区贡献率有所不同。未来的工作应进一步探讨工业布局的改变对大气PM_2.5及其中金属元素污染及来源的影响,以期为环保部门制定有效的大气污染防治措施提供参考。     

基于PM2.5浓度达标约束和区域联防联控的河南省地级市大气环境容量研究

为研究以河南省为代表的受大气污染传输影响显著省份的大气环境容量,本文基于CMAQ模型,采用嵌套迭代模拟的方法,计算了在周边省份区域联防联控的前提下河南省PM_2.5浓度达标(GB 3095-2012《环境空气质量标准》二级标准限值)时17个地级市SO₂、NO_x、一次PM_2.5和NH₃的大气环境容量.结果表明：(1)省外传输对河南省PM_2.5浓度的贡献率为50.29%,其中周边7个省份传输贡献率为36.19%,可见周边省份实施大气污染联防联控是河南省实现空气质量达标的必要条件.(2)在省级PM_2.5浓度达标时,河南省周边7个省份SO₂、NO_x、一次PM_2.5和NH₃的大气环境容量分别为279.07×10⁴、465.61×10⁴、172.67×10⁴和182.96×10⁴     

基于APEI的2013—2018年福建省大气污染评价

为了在区(县、市)级尺度上准确衡量福建省大气污染情况,构建大气污染评价APEI指数。基于高分辨率大气污染数据集和夜间灯光数据,分析2013—2018年福建省78个县市大气污染程度时空变化特征及其影响因素的时空异质性。结果表明：1)福建省中心偏北县市大气污染程度小,东部沿海县市大气污染严重。近6年福建省78.21%的县市大气污染程度减弱;2)全省东部沿海区域空气污染严重,主要表现在NO₂和PM₁₀这2种大气污染物,均超过全省平均水平;3)从大气污染物时序变化趋势看,PM_2.5和PM₁₀变化相似,自2014年起逐年下降,到2018年分别下降约23.15%和12.21%,SO₂和NO₂分别下降明显。O₃呈U形变化,而CO则呈倒U形变化;4)全省6种大气污染物均呈现较明显的季节性波动特征;5)采用时空加权回归(STWR)模型分析夜间灯光对APEI影响的时空异质性,发现2014—2018年负向影响区域持续扩大;全省34个县市5年回归系数均为正值...     

京津冀区域PM2.5污染相互输送特征

基于CAMx-PSAT空气质量模型,对2015年京津冀区域PM_(2.5)污染及相互输送特征进行定量模拟,建立了京津冀13个城市的PM_(2.5)传输矩阵.结果表明,在年均尺度上京津冀区域PM_(2.5)以本地污染源贡献为主(21.49%~68.74%),传输贡献为辅,其中区域内传输贡献约为13.31%~54.62%,区外贡献约为13.32%~45.02%.PM_(2.5)传输特征呈现显著的时空差异性,区域中部城市唐山、北京、天津、保定和石家庄PM_(2.5)受本地贡献主导,在冬季尤其明显,而受传输影响较大的城市多分布在区域边界且在南部集中.区内作为汇的城市有廊坊、衡水、承德、秦皇岛和邢台,作为源的城市有天津、沧州、唐山、北京、石家庄和邯郸,张家口和保定对区内城市输出和受区内输入基本持平.典型城市分析证明城市间PM_(2.5)污染交互影响,北京与廊坊、保定、承德、天津和沧州等城市之间,天津与廊坊、唐山、北京、沧州和保定等城市之间,石家庄与邢台、衡水、保定、邯郸和廊坊之间均存在显著的PM_(2.5)相互输送.     

Spatial and temporal variation of particulate matter and gaseous pollutants in 26 cities in China

O3and PM2.5were introduced into the newly revised air quality standard system in February 2012, representing a milestone in the history of air pollution control, and China's urban air quality will be evaluated using six factors(SO2, NO2, O3, CO, PM2.5and PM10) from the beginning of 2013. To achieve the new air quality standard, it is extremely important to have a primary understanding of the current pollution status in various cities. The spatial and temporal variations of the air pollutants were investigated in 26 pilot cities in China from August 2011 to February 2012, just before the new standard was executed. Hourly averaged SO2, NO2and PM10were observed in 26 cities, and the pollutants O3, CO and PM2.5were measured in 15 of the 26 cities. The concentrations of SO2and CO were much higher in the cities in north China than those in the south. As for O3and NO2, however, there was no significant diference between northern and southern cities. Fine particles were found to account for a large proportion of airborne particles, with the ratio of PM2.5to PM10ranging from 55% to 77%. The concentrations of PM2.5(57.5 μg/m3) and PM10(91.2 μg/m3) were much higher than the values(PM2.5: 11.2 μg/m3; PM10 : 35.6 μg/m3) recommended by the World Health Organization. The attainment of the new urban air quality standard in the investigated cities is decreased by 20% in comparison with the older standard without considering O3, CO and PM2.5, suggesting a great challenge in urban air quality improvement, and more eforts will to be taken to control air pollution in China.     

Atmospheric trace compounds at a European coastal site—application to CO2, CH4 and COS flux determinations

The variations of CO₂, CH₄, COS, and NMHC concentrations, and of ²²²Rn activity were studied simultaneously in the boundary layer in a littoral site in Brittany, France. Various meteorological conditions occurred during the experiment allowing determination of trace gas concentrations characteristic of air masses having either dominant continental or oceanic influence. The relative NMHC concentration of the air reflects the origin of the air masses. Oceanic air is characterized by high proportions of alkenes, whereas the alkanes concentration is higher in continental air masses.In 1986 alternate sea- and land-breeze conditions allowed measurement of the evolution of the composition of an oceanic air mass under continental influence. By using the variabilities of ²²²Rn activities measured during the experiment, as well as the estimation of its mean flux over continents, we deduced the mean regional fluxes of CO₂, CH₄ and COS to be 5.8, 0.07 and −36 × 10⁻⁶ m mol m⁻² h⁻¹, respectively.     

京津冀燃煤工业和生活锅炉的技术分布与大气污染物排放特征

燃煤工业和生活锅炉(下称燃煤锅炉)是京津冀地区大气污染控制的重点,分析其污染物排放特征对燃煤锅炉的污染控制具有重要意义. 对京津冀地区燃煤锅炉的容量、锅炉种类、除尘方式、实际除尘效率等技术分布信息进行了统计,在此基础上建立了基于技术分布信息的2012年京津冀地区燃煤锅炉大气污染物排放清单,并分析了技术特征对燃煤锅炉大气污染物排放的影响. 结果表明:京津冀地区燃煤锅炉以10 t/h及以下的小容量锅炉为主,主要炉型为层燃炉,除尘方式以湿式除尘及多管旋风除尘为主;2012年京津冀地区燃煤锅炉的SO₂、NO_x、颗粒物、PM₁₀和PM_2.5排放量分别为90.81×104、30.88×104 、31.46×104、14.64×104和8.07×104 t,排放主要集中于10 t/h及以下和35 t/h以上的锅炉;天津、石家庄、保定、唐山是锅炉污染物排放量最大的城市;供热、食品、化工、造纸是燃煤锅炉排放最集中的行业. 京津冀地区不同城市锅炉的容量及行业分布差异明显,各城市对燃煤锅炉应因地制宜采取天然气替代、集中供热等措施,以控制燃煤锅炉的污染物排放.      

Transported acid aerosols measured in southern Ontario

During the period 29 June 1986–9 August 1986, a field health study assessing the acute health effects of air pollutants on children was conducted at a summer girls' camp on the northern shore of Lake Erie in SW Ontario. Continuous air pollution measurements of SO₂, O₃, NO_x, particulate sulfates, light scattering, and meteorological measurements including temperature, dew point, and wind speed and direction were made. Twelve-hour integrated samples of size fractioned particles were also obtained using dichotomous samplers and Harvard impactors equipped with an ammonia denuder for subsequent hydrogen ion determination. Particulate samples were analyzed for trace elements by X-ray fluorescence and Neutron Activation, and for organic and elemental carbon by a thermal/optical technique. The measured aerosol was periodically very acidic with observed 12-h averaged H⁺ concentrations in the range < 10–560 nmoles m⁻³. The aerosol H⁺ appeared to represent the net strong acidity after H₂SO₄ reaction with NH₃(g). Average daytime concentrations were higher than night-time for aerosol H⁺, sulfate, fine mass and ozone. Prolonged episodes of atmospheric acidity, sulfate, and ozone were associated with air masses arriving at the measurement site from the west and from the southwest over Lake Erie. Sulfate concentrations measured at the lakeshore camp were more than twice those measured at inland sites during extreme pollution episodes. The concentration gradient observed with onshore flow was potentially due to enhanced deposition near the lakeshore caused by discontinuities in the meteorological fields in this region.     

金鱼藻对14CO2的吸收和积累动态

为了探明14CO2(14C)在环境中的行为,采用同位素示踪技术研究了金鱼藻对14CO2的吸收和积累动态,并探讨了金鱼藻作为监测大气14CO2污染指示植物的可能性.结果表明,生长在水中的金鱼藻会通过某些途径吸收空气中14CO2并形成积累趋势,吸收途径主要是金鱼藻通过光合作用从水体中吸收游离14CO2和H14CO3-.金鱼...     

Simultaneous monitoring of PCB profiles in the urban air of Dalian, China with active and passive samplings

The concentration of polychlorinated biphenyls (PCBs) in the urban air of Dalian, China was monitored from November 2009 to October 2010 with active high-volume sampler and semipermeable membrane device (SPMD) passive sampler. The concentration of PCBs (particle + gas) ( ∑ PCBs) ranged from 18.6 to 91.0 pg/m 3 , with an average of 50.9 pg/m 3 , and the most abundant dioxin-like PCB (DL-PCBs) was PCB118. The WHO-TEQ values of DL-PCBs were 3.6-22.1 fg/m3 , with an average of 8.5 fg/m 3 , and PCB126 was the maximum contributor to ∑ TEQ. There was a much larger amount of PCBs in the gas phase than in the particulate phase. The dominant PCB components were lower and middle molecular weight PCBs. With increasing chlorination level, the concentration of the PCB congeners in the air decreased. The gas-particulate partitioning of PCBs was different for the four seasons. The gas- particulate partitioning coefficients (logK p ) vs. subcooled liquid vapor pressures (logP L 0 ) of PCBs had reasonable correlations for different sampling sites and seasons. The absorption mechanism contributed more to the gas-particulate partitioning process than adsorption. Correlation analysis of meteorological parameters with the concentration of PCBs was conducted using SPSS packages. The ambient temperature and atmospheric pressure were important factors influencing the concentration of PCBs in the air. The distribution pattern of the congeners of PCBs and the dominant contributors to DL-PCBs and TEQ in active samples and SPMDs passive samples were similar. SPMD mainly sequestrated gas phase PCBs.     

30年来中国民航运输行业的大气污染物排放

民航是我国重要的交通运输方式之一,但我国民航运输行业的大气污染物排放问题报道较少.根据中国民航统计部门逐年统计数据,采用基于燃料消耗量的排放因子法,估算了1980～2009年中国民航飞机的大气污染物排放量,并分析了大气污染物排放强度及其变化.结果表明,30年来中国民航飞机SO2、CO、NOx和HC排放量逐年增多,分别由1980年的0.031、0.189、0.225和0.314万t增至2009年的1.183、7.298、8.705和12.159万t,排放量年均增加分别为0.039 7、0.245、0.292和0.408万t.SO2、CO、NOx和HC的排放强度呈降低趋势,其值分别由1980年的0.624、3.806、4.53和6.322 g.(t.km)-1降至2009年的0.275、1.697、2.025和2.828 g.(t.km)-1.中国民航运输行业所排放的SO2、CO、NOx占全国总排放量的比重很低,与其他行业排放量相比,中国民航运输行业所排放的大气污染物量也较小.     

Wintertime peroxyacetyl nitrate (PAN) in the megacity Beijing: Role of photochemical and meteorological processes

Previous measurements of peroxyacetyl nitrate(PAN) in Asian megacities were scarce and mainly conducted for relative short periods in summer. Here, we present and analyze the measurements of PAN, O3, NOx, etc., made at an urban site(CMA) in Beijing from 25 January to 22 March 2010. The hourly concentration of PAN averaged 0.70 × 10 9mol/mol(0.23 × 10 9–3.51 × 10 9mol/mol) and was well correlated with that of NO2but not O3, indicating that the variations of the winter concentrations of PAN and O3in urban Beijing are decoupled with each other. Wind conditions and transport of air masses exert very significant impacts on O3, PAN, and other species. Air masses arriving at the site originated either from the boundary layer over the highly polluted N-S-W sector or from the free troposphere over the W-N sector. The descending free-tropospheric air was rich in O3, with an average PAN/O3ratio smaller than 0.031, while the boundary layer air over the polluted sector contained higher levels of PAN and primary pollutants, with an average PAN/O3ratio of 0.11. These facts related with transport conditions can well explain the observed PAN-O3decoupling. Photochemical production is important to PAN in the winter over Beijing. The concentration of the peroxyacetyl(PA) radical was estimated to be in the range of 0.0014 × 10 12–0.0042 × 10 12 mol/mol. The contributions of the formation reaction and thermal decomposition to PAN's variation were calculated and found to be significant even in the colder period in air over Beijing, with the production exceeding the decomposition.     

北京雾霾天大气颗粒物中微生物气溶胶的浓度及粒谱特征

于2013年1月8日~2013年2月4日雾霾频繁暴发期间,使用定量空气微生物采样器和气溶胶粒谱测试仪测试并比较了雾霾天和之后的清朗天气下细菌、真菌气溶胶浓度变化、粒谱分布及不同粒径大小颗粒物的数量浓度差异和粒谱分布特征.结果表明,采样周期内真菌气溶胶小于5μm的粒子(可吸入肺粒子)所占百分比显著高于细菌气溶胶小于5μm的粒子百分比.雾霾过后的晴朗天气下细菌、真菌气溶胶浓度高于雾霾天气时的浓度,而颗粒物浓度则相反.无论雾霾天或晴朗天微生物气溶胶的粒谱分布无显著差别,空气中的颗粒物以PM1.0占绝大多数.