宝鸡市秋季清洁和污染时段水溶性离子污染特征及来源解析

为探究宝鸡市秋季大气PM_2.5中水溶性离子的污染特征及来源,于2019年10月15日至11月14日分别对宝鸡市监测站、文理学院和陈仓区环保局的3个站点进行PM_2.5样品采集,通过离子色谱仪得到水溶性离子质量浓度,分析了3个站点水溶性离子在清洁时段和污染时段的变化特征及来源.结果表明,三站点PM_2.5的质量浓度陈仓区环保局>文理学院>宝鸡市监测站.清洁时段和污染时段PM_2.5平均质量浓度分别为40.0μg·m^-3和100.1μg·m^-3,水溶性离子平均质量浓度分别为（13.7±7.7）μg·m^-3和（57.8±15.0）μg·m^-3.污染时段NO₃-/SO₄2-值是清洁时段的1.6—1.8倍.污染越重,SNA（NO₃-、SO₄2-和NH₄⁺）质量浓度越大,占总水溶性离子和P...     

疫情常态化管控下济南市春节前后PM2.5中二次组分变化特征

为研究新冠肺炎疫情常态化管控下,济南市春节前后PM_2.5中二次组分的变化特征、气粒分配规律及其影响因素,本文对2021年2月1-27日春节前、春节期间和春节后的3个时段济南市区在线监测的水溶性离子、碳组分及气态前体物质量浓度小时数据进行分析.结果表明,2021年疫情常态化管控下济南市春节前后二次组分浓度与2020年同比均明显下降,ρ(NO₃^-)、ρ(SO₄^2-)、ρ(NH₄⁺)和ρ(SOA)分别下降53.09%、58.32%、51.17%和61.84%,其中二次无机组分(NO₃^-、SO₄^2-、NH₄⁺之和)和SOA在PM_2.5中的占比分别为54.07%和8.20%,春节期间PM_2.5及二次组分在10—18时浓度较低,与春节期间白天人为活动相对减少,机动车、建筑工...     

城市森林大气PM2.5中水溶性无机离子沉降特征

森林被誉为"地球之肺",在防霾治污方面有其独特不可替代的作用,不同树种沉降PM_2.5的功能有很大差别.本文选取代表性城市森林——奥林匹克森林公园为研究对象,设置垂直监测塔观测大气PM_2.5的浓度垂直分布,以考察不同季节城市森林对PM_2.5中各组分的影响.在冬季、春季和夏季各采集PM_2.5样品,分析并计算PM_2.5中Na⁺、NH₄⁺、K⁺、Mg2⁺、Ca2⁺、Cl^-、NO₃^-和SO₄^2-等典型水溶性无机离子的浓度.结果表明,PM_2.5中水溶性无机离子总浓度呈规律性变化特征:冬季((56.90±27.38)μg·m-3)>春季((46.69±12.24)μg·m^-3)>夏季((23.16±8.75)μg·m^-3).其中SO₄^2-和NO₃^-浓度和占PM_2.5主要水溶性无机离子总浓度的50%以上.3个季节中,除冬季外,在春季和夏季,8种离子有明显的垂直方向上的沉降,夏季的沉降速率高于春季,但是春季由于大气颗粒物浓度高,沉降通量高于夏季.NO₃^-和SO₄^2-垂直方向的沉降量在所有可溶性无机离子中最高.植被密度、叶面积指数、气象条件等因素对于PM_2.5的沉降特征有明显影响.     

2018年成都市PM2.5中水溶性无机离子污染特征及来源解析

为了探究成都市PM_2.5水溶性无机离子的污染特征与来源贡献,于2018年1月1日—12月31日利用高分辨率的MARGA对PM_2.5组分展开在线监测,结合同一点位的气态污染物、气象参数监测数据进行分析.结果表明,水溶性无机离子与PM_2.5具有相同的月变化趋势,水溶性无机离子月均浓度为10.35-39.60μg·m^-3,在PM_2.5中的占比为31%—51%,水溶性无机离子是PM_2.5的重要组成部分.NO₃^-在水溶性无机离子中月均占比以12月最高,8月最低,SO₄^2-刚好与之相反.大气长期处于富氨状态,二次离子主要以（NH₄）₂SO₄、NH₄NO₃、NH₄Cl的形式存在,SOR在冬季12月与夏季8月分别出现高值0.61与0.5,但NOR只在冬季出...     

济南市PM2.5中二次组分的时空变化特征及其影响因素

为分析济南市PM_2.5中二次组分的时空变化和影响因素,对济南市春季(2019年5月16—25日)、秋季(2019年10月15—24日)和冬季(2019年12月17—2020年1月16日)4个典型点位的PM_2.5样品进行连续采样,并测定了PM_2.5中水溶性离子、有机碳(OC)和元素碳(EC)的含量。结果表明:物流交通区的二次组分质量浓度最高(56.13μg·m^?3),钢铁工业区的二次组分浓度比城市市区高,但是二次组分占比较城市市区低,清洁对照点的浓度和占比最低;济南市4个功能区SO₄^2?和NO₃^?转化率均高于0.1,除清洁对照点外,城市市区、钢铁工业区和物流交通区的SO₄^2?转化率明显高于NO₃^?转化率;济南市春季、秋季和冬季的ρ(NO₃^?)/ρ(SO₄^2?)分别为0.67、2.57和1.98,春季PM_2.5浓度以固定源贡献为主,秋季和冬季以移动源贡献为主;运用ISORROPIA热力学模型分析了含水量和pH对二次组分生成的影响,含水量会随着污染增大而增大,酸度和含水量对二次无机组分的转化机理产生影响,酸度会抑制二次无机组分的生成,而含水量会促进二次组分的生成;后向轨迹聚类分析结果表明,占比最高的轨迹(29.2%)来自东北方向的滨州和东营,基于潜在源贡献因子(WPSCF)和浓度权重轨迹(WCWT)分析PM_2.5中二次组分质量浓度的潜在污染源区域,SO₄^2?的主要贡献源区在济南市区北部的济阳区和东北方向的滨州、东营等,NO₃^?和NH₄⁺的主要贡献源区在济南市区北方向的济阳区、东北方向的章丘区和南方向的莱芜区等。该研究结果可为中国北方城市细颗粒物进一步的治理和防控提供数据支撑和理论依据。     

嘉善冬季PM2.5化学组分特征及来源分析

为研究嘉兴地区嘉善冬季污染时段和清洁时段PM_2.5化学组分特征,结合气象数据对2019年1月嘉兴市嘉善县善西超级站在线自动监测PM_2.5及化学组分数据、气态污染物(NO₂和SO₂)进行了分析.结果表明,2019年1月嘉善善西超级站污染时段PM_2.5浓度(97.18μg·m^-3)为清洁时段(36.77μg·m^-3)的2.6倍.污染时段水溶性离子浓度(41.58μg·m^-3)较清洁时段(19.82μg·m^-3)高21.76μg·m^-3,但占比有所降低,含碳组分比例增加.OC;EC比值为3.93,可能受到燃煤及机动车排放的共同影响.低风速及高湿有利于NO₂和SO₂等气态污染物进行二次转化,污染时段硫转化率和氮转化率均比清洁时段高,分别增高7.93%和54.11%,说明NOx向硝酸盐二次转化较为明显,导致颗粒物浓度升高.聚类分析结果显示67.34%气流来自北方,且相应的气流轨迹上污染物浓度比周边高,说明污染物存在一定的长距离输送.结合风玫瑰图可以看出,污染主要为本地及其周边的输送,污染物的长距离输送在短时会使污染浓度突增.因此,在重点关注本地及周边污染的同时,偏北气流下的污染物区域输送不可忽视.     

中国典型沿海城市冬季PM2.5中碳组分的污染特征及来源解析

为研究中国典型沿海城市冬季PM_2.5中碳组分的污染特征及来源,于2018年12月5日—2019年1月30日分别在天津(TJ)、上海(SH)和青岛(QD)同步采集PM_2.5样品。结果表明,天津、上海和青岛PM_2.5的平均浓度分别为(116.96±66.93)、(31.21±25.62)、(74.93±54.60)μg·m^-3,OC和EC的空间分布均为天津(18.69±7.95)μg·m^-3和(4.98±2.08)μg·m^-3>青岛(16.45±8.94)μg·m^-3和(2.01±1.04)μg·m^-3>上海(7.28±3.11)μg·m^-3和(1.05±1.25)μg·m^-3。3个站点的OC和EC均呈现较好的相关性,表明OC和EC具有相似的来源;OC/EC比值范围在2.37—7.53、5.47—46.41和4.77—13.36之间,证明各采样点均存在二次有机碳(SOC)的生成;采用最小R²法(MRS)估算SOC浓度,得到3个采样点SOC的平均质量浓度为(5.09±4.68)、(3.90±1.65)、(4.21±4.31)μg·m^-3,分别占OC总量的27.2%、55.8%和19.5%,其中上海的SOC在OC中的占比最大,说明上海二次有机碳污染较为严重,这主要归因于冬季严重污染源排放和有利的二次转化气象条件,而天津和青岛的碳组分主要来自污染源的直接排放。主成分分析(PCA)结果发现,天津PM_2.5中碳组分主要来源于道路尘、生物质燃烧和机动车尾气,上海PM_2.5中碳组分主要来源于生物质燃烧、道路扬尘和机动车尾气。青岛PM_2.5中碳组分主要来源于道路扬尘、机动车尾气。后向轨迹聚类分析表明,来自西北方向的气团对天津的影响较大,PM_2.5和碳组分的浓度值最大;而对上海而言,主要受北方气溶胶经过海面又传输回上海的气团的影响;青岛站点主要受华北地区污染物和本地排放源的影响。     

天津市2018—2020年春节PM2.5中水溶性无机离子特征及重污染过程分析

为阐明大气污染重点整治和新冠疫情影响下我国华北地区城市春节期间重污染过程PM_2.5中水溶性无机离子变化特征及其影响因素,本研究结合气态前体物浓度和气象要素,对天津市2018—2020年连续3年春节假期的2次重污染过程PM_2.5中主要水溶性无机离子(WSIIs)浓度进行对比分析.结果表明,2018年和2020年春节假期PM_2.5平均浓度(98.32μg·m^-3和137.7μg·m^-3)显著高于2019年(49.97μg·m^-3).PM_2.5平均浓度在污染期Ⅱ(2020年为206.5μg·m^-3)是污染期Ⅰ(2018年98.32μg·m^-3)的2.1倍;2次污染事件中NO₂浓度变化不大,而SO₂浓度在污染期Ⅱ(14.89μg·m^-3)是污染期Ⅰ(30.04μg·m^-3)的49.6%.SNA在WSIIs中占比超...     

保定市污染天气PM2.5中水溶性离子的特征和源解析

采集了2018年保定市污染天气的PM_2.5样品,采用离子色谱法测定了PM_2.5样品中的水溶性离子（WSIs）,分析了不同季节PM_2.5及其水溶性离子的分布特征,并采用PMF模型对PM_2.5进行了源解析.结果表明,采样期间保定市的PM_2.5浓度为18.4—258.0μg·m^-3,年均值为（91.5±62.5）μg·m^-3;季节规律是冬季(160.6μg·m^-3)>秋季(105.3μg·m^-3)>春季(57.6μg·m^-3)>夏季(53.2μg·m^-3).WSIs年均值为49.20μg·m^-3,占PM_2.5.的63.95%,WSIs的季节规律和PM_2.5的一致.二次离子占水溶性离子的77.12%.湿度和温度与SOR和NOR成正相关.春夏两季水溶性离子主要以Na_...     

天津市夏季PM2.5中碳组分时空变化特征及来源解析

为研究天津市夏季PM_2.5中碳组分的时空变化特征及来源,于2019年7—8月设立2个点位分昼夜采集天津市PM_2.5样品,并测定了其中有机碳(OC)和元素碳(EC)的含量。结果表明,城区PM_2.5、OC和EC浓度日均值分别为(53.4±20.8)μg·m^-3、(8.72±2.56)μg·m^-3和(1.67±0.90)μg·m^-3,郊区PM_2.5、OC和EC浓度日均值分别为(54.2±24.5)μg·m^-3、(7.54±2.50)μg·m^-3和(1.82±1.06)μg·m^-3;白天PM_2.5、OC、EC的平均浓度分别为(47.3±16.1)μg·m^-3、(8.7±2.1)μg·m^-3和(1.5±0.6)μg·m^-3,夜间PM_2.5、OC、EC的平均浓度分别为(60.2±26.2)μg·m^-3、(7.5±2.9)μg·m^-3和(2.0±1.2)μg·m^-3。OC浓度表现为城区高于郊区,白天高于夜间;EC及PM_2.5浓度表现为郊区高于城区,夜间高于白天。OC/EC比值分析得,城区(6.04)高于郊区(5.08);白天(6.58)高于夜间(4.54)。城区OC与EC相关性弱于郊区,白天OC与EC相关性弱于夜间。采用EC示踪法与MRS模型对SOC含量进行估算,得到白天与夜间SOC浓度分别为(5.71±1.35)μg·m^-3和(3.81±1.20)μg·m^-3,白天SOC污染比夜间严重。丰度分析与主成分分析的结果表明,天津市夏季城郊区PM_2.5中碳组分均主要来源于燃煤和机动车尾气排放。     

辽宁西南典型城市冬季大气细颗粒物水溶性无机离子污染特征及来源解析

本研究于2018年12月3日-2019年1月1日在辽宁省西南典型城市葫芦岛市和朝阳市分别布设3个城区采样点,在区域传输点龙屯水库布设1个采样点,采集大气细颗粒物PM2.5样品(n=201).使用离子色谱检测样品中的Na+、Mg2+、Ca2+、K+、NH4+、SO42-、F-、Cl-和NO3-的质量浓度.观测期间PM2....     

青藏高原东缘冬季PM2.5中碳组分特征和来源解析

于2017年冬季12月13—21日在青藏高原东缘理塘地区分昼夜采集PM_2.5样品,并用DRI2001A热光碳分析仪测定了有机碳(OC)和元素碳(EC)的质量浓度,研究青藏高原PM_2.5中碳组分的化学特征及主要来源,以期为理塘地区制定污染排放政策提供参考。结果表明,2017年冬季青藏高原东缘理塘地区PM_2.5平均质量浓度为44.34μg·m^?3,OC和EC的质量浓度为12.72μg·m^?3和3.85μg·m^?3,分别占PM_2.5质量浓度的29.61%和8.96%。通过经验公式,计算得到总碳气溶胶(TCA)质量浓度为24.20μg·m^?3,占PM_2.5的54.84%,说明碳质气溶胶对青藏高原东缘理塘地区PM_2.5有着十分重要的贡献。OC和EC在白天和夜间都有较高的相关性(相关系数分别为0.74和0.91),表明OC和EC的来源基本一致,受燃烧源影响较大。其中白天的相关系数低于夜间,说明青藏高原东缘理塘地区白天碳组分来源相对复杂。昼夜浓度对比显示,青藏高原东缘理塘地区PM_2.5白天和夜间的质量浓度分别为53.88μg·m^?3和33.44μg·m^?3,OC和EC浓度白天高于夜间,表明白天人为排放相对较高。冬季观测期间,PM_2.5中二次有机碳(SOC)昼夜浓度分别为1.11μg·m^?3和3.03μg·m^?3,分别占OC质量浓度的7.09%、26.59%,表明青藏高原东缘理塘城区白天碳组分主要为一次源。利用PMF 5.0软件对理塘城区碳组分进行进一步的解析,结果显示燃煤和生物质燃烧的混合源对总碳(TC)的贡献高达47.84%,占比最高;其次是汽车尾气和柴油车尾气源,贡献率分别为28.62%和23.54%。     

Relations between indoor and outdoor PM2.5 and constituent concentrations

Factors impacting indoor-outdoor relations are introduced. Sulfate seems a fine tracer for other non-volatile species. Particulate nitrate and ammonium desorb during outdoor-to-indoor transport. OC load increases during the transport due to sorption of indoor SVOCs. Outdoor PM_2.5 influences both the concentration and composition of indoor PM_2.5. People spend over 80% of their time indoors. Therefore, to assess possible health effects of PM_2.5 it is important to accurately characterize indoor PM_2.5 concentrations and composition. Controlling indoor PM_2.5 concentration is presently more feasible and economic than decreasing outdoor PM_2.5 concentration. This study reviews modeling and measurements that address relationships between indoor and outdoor PM_2.5 and the corresponding constituent concentrations. The key factors in the models are indoor-outdoor air exchange rate, particle penetration, and deposition. We compiled studies that report I/O ratios of PM_2.5 and typical constituents (sulfate (SO₄^2-), nitrate (NO₃^-), ammonium (NH₄⁺), elemental carbon (EC), and organic carbon (OC), iron (Fe), copper (Cu), and manganese (Mn)). From these studies we conclude that: 1) sulfate might be a reasonable tracer of non-volatile species (EC, Fe, Cu, and Mn) and PM_2.5 itself; 2) particulate nitrate and ammonium generally desorb to gaseous HNO₃ and NH₃ when they enter indoors, unless, as seldom happens, they have strong indoor sources; 3) indoor-originating semi-volatile organic compounds sorb on indoor PM_2.5, thereby increasing the PM_2.5 OC load. We suggest further studies on indoor-outdoor relationships of PM_2.5 and constituents so as to help develop standards for healthy buildings.     

A method for quantifying bias in modeled concentrations and source impacts for secondary particulate matter

A method for quantifying source impacts for secondary PM_2.5 species is derived. The method provides estimates of bias in modeled concentrations. Adjusted concentrations match corresponding observations at monitored locations. Sources impacts on secondary species are estimated over the US for 20 sources. Community Multi-Scale Air Quality (CMAQ) estimates of sulfates, nitrates, ammonium, and organic carbon are highly influenced by uncertainties in modeled secondary formation processes, such as chemical mechanisms, volatilization, and condensation rates. These compounds constitute the majority of PM_2.5 mass, and reducing bias in estimated concentrations has benefits for policy measures and epidemiological studies. In this work, a method for adjusting source impacts on secondary species is developed that provides estimates of source contributions and reduces bias in modeled concentrations compared to observations. The bias correction adjusts concentrations and source impacts based on the difference between modeled concentrations and observations while taking into account uncertainties at the location of interest; and it is applied both spatially and temporally. We apply the method over the US for 2006. The mean bias for initial CMAQ concentrations compared to observations is −0.28 (OC), 0.11 (NO₃), 0.05 (NH₄), and −0.08 (SO₄). The normalized mean bias in modeled concentrations compared to observations was effectively zero for OC, NO₃, NH₄, and SO₄ after applying the secondary bias correction. 10-fold cross-validation was conducted to determine the performance of the spatial application of the bias correction. Cross-validation performance was favorable; correlation coefficients were greater than 0.69 for all species when comparing observations and concentrations based on kriged correction factors. The methods presented here address model uncertainties by improving simulated concentrations and source impacts of secondary particulate matter through data assimilation. Secondary-adjusted concentrations and source impacts from 20 emissions sources are generated for 2006 over continental US.     

Effects of a diesel oxidation catalyst on gaseous pollutants and fine particles from an engine operating on diesel and biodiesel

The effects of a diesel oxidation catalytic (DOC) converter on diesel engine emissions were investigated on a diesel bench at various loads for two steady-state speeds using diesel fuel and B20. The DOC was very effective in hydrocarbon (HC) and CO oxidation. Approximately 90%–95% reduction in CO and 36%–70% reduction in HC were realized using the DOC. Special attention was focused on the effects of the DOC on elemental carbon (EC) and organic carbon (OC) fractions in fine particles (PM_2.5) emitted from the diesel engine. The carbonaceous compositions of PM_2.5 were analyzed by the method of thermal/optical reflectance (TOR). The results showed that total carbon (TC), OC and EC emissions for PM_2.5 from diesel fuel were generally reduced by the DOC. For diesel fuel, TC emissions decreased 22%–32% after the DOC depending on operating modes. The decrease in TC was attributed to 35%–97% decrease in OC and 3%–65% decrease in EC emissions. At low load, a significant increase in the OC/EC ratio of PM_2.5 was observed after the DOC. The effect of the DOC on the carbonaceous compositions in PM_2.5 from B20 showed different trends compared to diesel fuel. At low load, a slight increase in EC emissions and a significant decrease in OC/EC ratio of PM_2.5 after DOC were observed for B20.     

天津市采暖季PM2.5组分消光特性及来源分析

为了解天津市采暖季细颗粒物组分对能见度的影响、明确消光组分来源,对天津市2017年采暖季大气PM_2.5样品进行了为期一月的连续采集,并测定水溶性离子、有机碳和元素碳的含量,通过修正IMPROVE方程研究了细颗粒物消光特性,并采用主成分分析—多元线性回归模型(PCA-MLR)对其来源进行解析,同时应用潜在源贡献因子(PSCF)和浓度权重轨迹(CWT)明确PM_2.5质量浓度的潜在污染源区域。结果表明,OC、EC以及SNA(NO3^?、NH₄⁺、SO₄^2?)的生成和积累对于能见度的下降具有重要影响,且能见度随SOR和NOR二次转化程度的升高而下降;2017年天津市采暖季日均消光系数为(294.56±262.89)Mm^?1,其中OM(34.86%)、硝酸盐(22.84%)、硫酸盐(11.59%)和EC(11.54%)为主要消光组分,硝酸盐和硫酸盐的增加对于能见度的下降起主要影响作用;根据PCA分析结果可知,天津市采暖季PM_2.5中的碳组分和水溶性离子主要来源于燃煤、生物质燃烧(68%),受扬尘(22%)和海盐(8%)的影响较小;区域传输分析结果表明天津市采暖季PM_2.5污染源潜在区域主要分布在河北中西部、河南北部、山西北部和内蒙古中部、西部。     

New insights into the formation of ammonium nitrate from a physical and chemical level perspective

● Factor analysis of ammonium nitrate formation based on thermodynamic theory. ● Aerosol liquid water content has important role on the ammonium nitrate formation. ● Contribution of coal combustion and vehicle exhaust is significant in haze periods. High levels of fine particulate matter (PM_2.5) is linked to poor air quality and premature deaths, so haze pollution deserves the attention of the world. As abundant inorganic components in PM_2.5, ammonium nitrate (NH₄NO₃) formation includes two processes, the diffusion process (molecule of ammonia and nitric acid move from gas phase to liquid phase) and the ionization process (subsequent dissociation to form ions). In this study, we discuss the impact of meteorological factors, emission sources, and gaseous precursors on NH₄NO₃ formation based on thermodynamic theory, and identify the dominant factors during clean periods and haze periods. Results show that aerosol liquid water content has a more significant effect on ammonium nitrate formation regardless of the severity of pollution. The dust source is dominant emission source in clean periods; while a combination of coal combustion and vehicle exhaust sources is more important in haze periods. And the control of ammonia emission is more effective in reducing the formation of ammonium nitrate. The findings of this work inform the design of effective strategies to control particulate matter pollution.