Chemical characteristics and source apportionment of atmospheric particles during heating period in Harbin, China

Atmospheric particles（total suspended particles（TSPs）; particulate matter（PM） with particle size below 10 μm, PM10; particulate matter with particle size below 2.5 μm, PM2.5）were collected and analyzed during heating and non-heating periods in Harbin. The sources of PM10 and PM2.5were identified by the chemical mass balance（CMB） receptor model.Results indicated that PM2.5/TSP was the most prevalent and PM2.5was the main component of PM210, while the presence of PM10–100was relatively weak. SO-4and NO-3concentrations were more significant than other ions during the heating period. As compared with the non-heating period, Mn, Ni, Pb, S, Si, Ti, Zn, As, Ba, Cd, Cr, Fe and K were relatively higher during the heating period. In particular, Mn, Ni, S, Si, Ti, Zn and As in PM2.5were obviously higher during the heating period. Organic carbon（OC） in the heating period was 2–5 times higher than in the non-heating period. Elemental carbon（EC） did not change much. OC/EC ratios were 8–11 during the heating period, which was much higher than in other Chinese cities（OC/EC： 4–6）. Results from the CMB indicated that 11 pollution sources were identified, of which traffic, coal combustion, secondary sulfate, secondary nitrate, and secondary organic carbon made the greatest contribution. Before the heating period, dust and petrochemical industry made a larger contribution. In the heating period, coal combustion and secondary sulfate were higher. After the heating period, dust and petrochemical industry were higher. Some hazardous components in PM2.5were higher than in PM10, because PM2.5has a higher ability to absorb toxic substances. Thus PM2.5pollution is more significant regarding human health effects in the heating period.     

Particle number concentration, size distribution and chemical composition during haze and photochemical smog episodes in Shanghai

The aerosol number concentration and size distribution as well as size-resolved particle chemical composition were measured during haze and photochemical smog episodes in Shanghai in 2009. The number of haze days accounted for 43%, of which 30% was severe （visibility 〈 2 km） and moderate （2 km 〈 visibility 〈 3 km） haze, mainly distributed in winter and spring. The mean particle number concentration was about 17,000/cm3 in haze, more than 2 times that in clean days. The greatest increase of particle number concentration was in 0.5-1μm and 1-10 μm size fractions during haze events, about 17.78 times and 8.78 times those of clean days. The largest increase of particle number concentration was within 50-100 nm and 100-200 nm fractions during photochemical smog episodes, about 5.89 times and 4.29 times those of clean days. The particle volume concentration and surface concentration in haze, photochemical smog and clean days were 102, 49, 15 μm3/cm3 and 949, 649, 206 μm2/cm3, respectively. As haze events got more severe, the number concentration of particles smaller than 50 nm decreased, but the particles of 50-200 nm and 0.5-1μm increased. The diurnal variation of particle number concentration showed a bimodal pattern in haze days. All soluble ions were increased during haze events, of which NH4, SO24- and NO3 increased great/y, followed by Na＋, IC, Ca2＋ and CI-. These ions were very different in size-resolved particles during haze and photochemical smog episodes.     

Performance and microbial response during the fast reactivation of Anammox system by hydrodynamic stress control

Anaerobic ammonium oxidation （Anammox） has become a promising method for biological nitrogen removal. However, this biotechnology application is always limited due to the low growth rate and biomass yield of Anammox bacteria. This study investigated the process of fast reactivation of an Anammox consortium idled for 2 years uia hydrodynamic stress control. The results showed that the Anammox system was efficiently and quickly reactivated by shortening of the hydraulic retention time （I-IRT） of the reactor from 12 to 6 hr within 68 days of operation. Moreover, at a 4-hr HRT with an influent total nitrogen loading rate of 1.2 kg N/（m3.day）, the reactor maintained high biological performance with an ammonium removal loading rate of 0.52 kg N/（m3.day） and a nitrite removal rate of 0.59 kg N/（m3.day）. In the reactivated Anammox reaction, the stoichiometric coefficients of NH4-N to NOE-N and NH4-N to NO4-N were 1：1.04± 0.08 and 1：0.31 ± 0.03, respectively. The specific Anammox activity and hydrazine oxidoreductase activity, both of which represent the degree of Anammox bacteria present, increased as the hydrodynamic stress increased and were maximally （125.38 ± 3.01 mg N/（g VSS.day） and 339.42 ± 6.83 μmol/（min.g VSS）, respectively） at 4-hr HRT. Microbial response analysis showed that the dominant microbial community was obviously shifted and the dominance of Anammox bacteria was enhanced durinR the hydrodynamic selection.     

Direct radiative forcing of urban aerosols over Pretoria (25.75°S, 28.28°E) using AERONET Sunphotometer data: First scientific results and environmental impact

The present study uses the data collected from Cimel Sunphotometer of Aerosol Robotic Network（AERONET） for the period from January to December, 2012 over an urban site,Pretoria（PTR; 25.75°S, 28.28°E, 1449 m above sea level）, South Africa. We found that monthly mean aerosol optical depth（AOD, τa） exhibits two maxima that occurred in summer（February） and winter（August） having values of 0.36 ± 0.19 and 0.25 ± 0.14,respectively, high-to-moderate values in spring and thereafter, decreases from autumn with a minima in early winter（June） 0.12 ± 0.07. The Angstrom exponents（α440–870） likewise,have its peak in summer（January） 1.70 ± 0.21 and lowest in early winter（June） 1.38 ± 0.26,while the columnar water vapor（CWV） followed AOD pattern with high values（summer） at the beginning of the year（February, 2.10 ± 0.37 cm） and low values（winter） in the middle of the year（July, 0.66 ± 0.21 cm）. The volume size distribution（VSD） in the fine-mode is higher in the summer and spring seasons, whereas in the coarse mode the VSD is higher in the winter and lower in the summer due to the hygroscopic growth of aerosol particles.The single scattering albedo（SSA） ranged from 0.85 to 0.96 at 440 nm over PTR for the entire study period. The averaged aerosol radiative forcing（ARF） computed using SBDART model at the top of the atmosphere（TOA） was- 8.78 ± 3.1 W/m2, while at the surface it was- 25.69 ± 8.1 W/m2 leading to an atmospheric forcing of ＋ 16.91 ± 6.8 W/m2, indicating significant heating of the atmosphere with a mean of 0.47 K/day.     

PM2.5, PM10 and health risk assessment of heavy metals in a typical printed circuit noards manufacturing workshop

A typical Printed Circuit Board（PCB） manufacturer was chosen as the object of this study.During PCB processing, fine particulate matter and heavy metals（Cu, Zn, Pb, Cr, Cd and Ni）will be released into the air and dust, which then impact workers＇ health and the environment. The concentrations of total suspended particle（TSP）, PM10 and PM2.5in the off-site were 106.3, 90.0 and 50.2 μg/m3, respectively, while the concentrations of TSP, PM10 and PM2.5in the workshops ranged from 36.1 to 365.3, from 27.1 to 289.8 and from 22.1 to212.3 μg/m3, respectively. Almost all six of the heavy metals were detected in all of the particle samples except Cd. For each workshop, it was obvious that Zn was the most enriched metal in TSP, followed by Cu 〉 Pb（Cr） 〉 Ni 〉 Cd, and the same trend was found for PM10 and PM2.5. In the dust samples, Cu（which ranged from 4.02 to 56.31 mg/g） was the most enriched metal, followed by Zn, Cr, Pb, Ni and Cd, and the corresponding concentrations ranged from 0.77 to 4.47, 0.37 to 1.59, 0.26 to 0.84, 0.13 to 0.44 and nd to0.078 mg/g, respectively. The health risk assessment showed that noncancerous effects are unlikely for Zn, Pb, Cr, Cu, Cd and Ni. The carcinogenic risks for Cd and Ni were all lower than 10-6, except for Cr. This result indicates that carcinogenic risks for workers are relatively possible in the workshops. These findings suggest that this technology is advanced from the perspective of environmental protection in the waste PCB＇s recycling industry.     

Methane and nitrous oxide fluxes from four tundra ecotopes in Ny-Ålesund of the High Arctic

During the summers of 2008 and 2009, net methane（CH4） and nitrous oxide（N2O） fluxes were investigated from 4 tundra ecotopes： normal lowland tundra（LT）, bird sanctuary tundra（BT）, the tundra in an abandoned coal mine（CT） and the tundra in scientific bases（ST） in Ny-Alesund of the High Arctic. Tundra soils in CT（184.5 ± 40.0 μg CH4/（m2·hr）） and ST（367.6 ± 92.3 μg CH4/（m2·hr）） showed high CH4 emissions due to the effects of human activities, whereas high CH4 uptake or low emission occurred in the soils of LT and BT.The lowland tundra soils（mean,-4.4-4.3 μg N2O/（m2·hr）） were weak N2 O sources and even sinks. Bird activity increased N2 O emissions from BT with the mean flux of7.9 μg N2O/（m2·hr）. The mean N2 O fluxes from CT（45.4 ± 10.2 μg N2O/（m2·hr）） and ST（78.8 ± 18.5 μg N2O/（m2·hr）） were one order of magnitude higher than those from LT and BT, indicating that human activities significantly increased N2 O emissions from tundra soils. Soil total carbon and water regime were important factors affecting CH4 fluxes from tundra soils. The N2 O fluxes showed a significant positive correlation with ammonia nitrogen（NH4＋-N） contents（r = 0.66, p 〈 0.001） at all the observation sites, indicating that ammonia nitrogen（NH4＋-N） content acted as a strong predictor for N2 O emissions from tundra soils. The CH4 and N2O fluxes did not correspond to the temperature variations of soil at 0-15 cm depths.Overall our results implied that human activities might have greater effects on soil CH4 and N2O emissions than current climate warming in Ny-Alesund, High Arctic.     

Chemical characterization of size-resolved aerosols in four seasons and hazy days in the megacity Beijing of China

Size-resolved aerosol samples were collected by MOUDI in four seasons in 2007 in Beijing. The PM₁₀ and PM_1.8 mass concentrations were 166.0 ± 120.5 and 91.6 ± 69.7 μg/m³, respectively, throughout the measurement, with seasonal variation: nearly two times higher in autumn than in summer and spring. Serious fine particle pollution occurred in winter with the PM_1.8/PM₁₀ ratio of 0.63, which was higher than other seasons. The size distribution of PM showed obvious seasonal and diurnal variation, with a smaller fine mode peak in spring and in the daytime. OM (organic matter = 1.6 × OC (organic carbon)) and SIA (secondary inorganic aerosol) were major components of fine particles, while OM, SIA and Ca^2 + were major components in coarse particles. Moreover, secondary components, mainly SOA (secondary organic aerosol) and SIA, accounted for 46%–96% of each size bin in fine particles, which meant that secondary pollution existed all year. Sulfates and nitrates, primarily in the form of (NH₄)₂SO₄, NH₄NO₃, CaSO₄, Na₂SO₄ and K₂SO₄, calculated by the model ISORROPIA II, were major components of the solid phase in fine particles. The PM concentration and size distribution were similar in the four seasons on non-haze days, while large differences occurred on haze days, which indicated seasonal variation of PM concentration and size distribution were dominated by haze days. The SIA concentrations and fractions of nearly all size bins were higher on haze days than on non-haze days, which was attributed to heterogeneous aqueous reactions on haze days in the four seasons.     

Chemical and optical properties of aerosols and their interrelationship in winter in the megacity Shanghai of China

A field campaign on air quality was carried out in Shanghai in winter of 2012. The concentrations of NO, NO₂, NO_x, SO₂, CO, and PM_2.5 increased during haze formation. The average masses of SO₄^2-, NO₃^- and NH₄⁺ were 10.3, 11.7 and 6.7 μg/m³ during the haze episodes, which exceeded the average (9.2, 7.9, and 3.4 μg/m³) of these components in the non-haze days. The mean values for the aerosol scattering coefficient (b_sp), aerosol absorption coefficient (b_ap) and single scattering albedo (SSA) were 288.7, 27.7 and 0.91 Mm^-1, respectively. A bi-peak distribution was observed for the mass concentrations of CO, NO, NO₂, and NO_x. More sulfate was produced during daytime than that in the evening due to photochemical reactions. The mass concentration of NH₄⁺ achieved a small peak at noontime. NO₃^- showed lower concentrations in the afternoon and higher concentrations in the early morning. There were obvious bi-peak diurnal patterns for bsp and bap as well as SSA. bsp and bap showed a positive correlation with PM_2.5 mass concentration. (NH₄)₂SO₄, NH₄NO₃, organic mass, elemental carbon and coarse mass accounted for 21.7%, 19.3%, 31.0%, 9.3% and 12.3% of the total extinction coefficient during non-haze days, and 25.6%, 24.3%, 30.1%, 8.1% and 8.2% during hazy days. Organic matter was the largest contributor to light extinction. The contribution proportions of ammonium sulfate and ammonium nitrate to light extinction were significantly higher during the hazy time than during the non-haze days.     

Reduction and characterization of bioaerosols in a wastewater treatment station via ventilation

Bioaerosols from wastewater treatment processes are a significant subgroup of atmospheric aerosols. In the present study,airborne microorganisms generated from a wastewater treatment station(WWTS) that uses an oxidation ditch process were diminished by ventilation.Conventional sampling and detection methods combined with cloning/sequencing techniques were applied to determine the groups,concentrations,size distributions,and species diversity of airborne microorganisms before and after ventilation. There were 3021 ± 537 CFU/m3 of airborne bacteria and 926 ± 132 CFU/m3 of airborne fungi present in the WWTS bioaerosol.Results showed that the ventilation reduced airborne microorganisms significantly compared to the air in the WWTS. Over 60% of airborne bacteria and airborne fungi could be reduced after4 hr of air exchange. The highest removal(92.1% for airborne bacteria and 89.1% for fungi) was achieved for 0.65–1.1 μm sized particles. The bioaerosol particles over 4.7 μm were also reduced effectively. Large particles tended to be lost by gravitational settling and small particles were generally carried away,which led to the relatively easy reduction of bioaerosol particles0.65–1.1 μm and over 4.7 μm in size. An obvious variation occurred in the structure of the bacterial communities when ventilation was applied to control the airborne microorganisms in enclosed spaces.     

Composition, source, mass closure of PM2:5 aerosols for four forests in eastern China

PM2.5 aerosols were collected in forests along north latitude in boreal-temperate, temperate, subtropical and tropical climatic zones in eastern China, i.e., Changbai Mountain Nature Reserve (CB), Dongping National Forest Park in Chongming Island (CM), Dinghu Mountain Nature Reserve (DH), Jianfengling Nature Reserve in Hainan Island (HN). The mass concentrations of PM2.5, organic carbon (OC), elemental carbon (EC), water soluble organic carbon (WSOC) as well as concentrations of ten inorganic ions (F-, Cl-, NO3-, SO42-, C2O42-, NH4+, Na+, K+, Ca2+, Mg2+) were determined. Aerosol chemical mass closures were achieved. The 24-hr average concentrations of PM2.5 were 38.8, 89.2, 30.4, 18 μg/m3 at CB, CM, DH and HN, respectively. Organic matter and EC accounted for 21%-33% and 1.3%-2.3% of PM2.5 mass, respectively. The sum of three dominant secondary ions (SO42-, NO3-, NH4+) accounted for 44%, 50%, 45% and 16% of local PM2.5 mass at CB, CM, DH and HN, respectively. WSOC comprised 35%-65% of OC. The sources of PM2.5 include especially important regional anthropogenic pollutions at Chinese forest areas.     

上海市夏季颗粒物污染过程数值模拟研究

利用观测资料和嵌套网格空气质量模式(Nested Air Quality Prediction Model System,NAQPMS)模拟研究了2010年7月26日—8月26日上海市及周边城市PM10、PM2.5及其无机盐组分的浓度变化趋势及时空分布特点.结果表明,NAQPMS模式较为合理的重现了上海各方位站点及其周边城市PM10、PM2.5及其硫酸盐、硝酸盐等无机化学组分的浓度水平与变化趋势,相关系数在0.7以上.研究期间造成上海颗粒物污染的主要原因是:弱气旋低压系统控制下,西南或西北气流将内陆污染物输送至上海市,当低压中心移至上海附近时带来的辐合气流使得污染进一步累积上升.长三角地区PM2.5主要无机盐组分分布特征表明,上海市及周边城市的硫酸盐、硝酸盐和铵盐的总和占PM2.5浓度的40%~60%,二次气-粒转化过程贡献明显,且以SO2向SO2-4的氧化转换为主;污染上升过程中NO-3/SO2-4比率增大,说明流动源的贡献有所增加.     

Seasonal variation and source apportionment of organic and inorganic compounds in PM2.5 and PM10 particulates in Beijing, China

The distribution and source of the solvent-extractable organic and inorganic components in PM 2.5(aerodynamics equivalent diameter below 2.5 microns),and PM 10(aerodynamics equivalent diameter below 10 microns) fractions of airborne particles were studied weekly from September 2006 to August 2007 in Beijing.The extracted organic and inorganic compounds identified in both particle size ranges consisted of n-alkanes,PAHs(polycyclic aromatic hydrocarbons),fatty acids and water soluble ions.The potential emission sources of these organic compounds were reconciled by combining the values of n-alkane carbon preference index(CPI),%waxC n,selected diagnostic ratios of PAHs and principal component analysis in both size ranges.The mean cumulative concentrations of n-alkanes reached 1128.65ng/m3 in Beijing,74% of which(i.e.,831.7ng/m3) was in the PM 2.5 fraction,PAHs reached 136.45ng/m3(113.44ng/m3 or 83% in PM 2.5),and fatty acids reached 436.99ng/m3(324.41ng/m3 or 74% in PM 2.5),which resulted in overall enrichment in the fine particles.The average concentrations of SO42-,NO3-,and NH4+ were 21.3±15.2,6.1±1.8,12.5±6.1μg/m3 in PM 2.5,and 25.8±15.5,8.9±2.6,16.9±9.5μg/m3 in PM 10,respectively.These three secondary ions primarily existed as ammonium sulfate((NH4)2SO4),ammonium bisulfate(NH4HSO4) and ammonium nitrate(NH4NO3).The characteristic ratios of PAHs revealed that the primary sources of PAHs were coal combustion,followed by gasoline combustion.The ratios of stearic/palmitic acid indicated the major contribution of vehicle emissions to fatty acids in airborne particles.The major alkane sources were biogenic sources and fossil fuel combustion.The major sources of PAHs were vehicular emission and coal combustion.     

Progressively narrow the gap of PM2.5 pollution characteristics at urban and suburban sites in a megacity of Sichuan Basin, China

Nowadays, the fine particle pollution is still severe in some megacities of China, especially in the Sichuan Basin, southwestern China. In order to understand the causes, sources, and impacts of fine particles, we collected PM_2.5 samples and analyzed their chemical composition in typical months from July 2018 to May 2019 at an urban and a suburban (background) site of Chengdu, a megacity in this region. The daily average concentrations of PM_2.5 ranged from 5.6-102.3 µg/m³ and 4.3-110.4 µg/m³ at each site. Secondary inorganics and organic matters were the major components in PM_2.5 at both sites. The proportion of nitrate in PM_2.5 has exceeded sulfate and become the primary inorganic component. SO₂ was easier to transform into sulfate in urban areas because of Mn-catalytic heterogeneous reactions. In contrast, NO₂ was easily converted in suburbs with high aerosol water content. Furthermore, organic carbon in urban was much greater than that in rural, other than elemental carbon. Element Cr and As were the key cancer risk drivers. The main sources of PM_2.5 in urban and suburban areas were all secondary aerosols (42.9%, 32.1%), combustion (16.0%, 25.2%) and vehicle emission (15.2%, 19.2%). From clean period to pollution period, the contributions from combustion and secondary aerosols increased markedly. In addition to tightening vehicle controls, urban areas need to restrict emissions from steel smelters, and suburbs need to minimize coal and biomass combustion in autumn and winter.     

城区与县区不同空气质量下碳组分污染特征对比分析

为对比城区与相邻县区不同空气质量下的碳组分污染特征,分别在成都市和仁寿县采集霾期及非霾期PM_2.5有效样品共计88个,确定其相应质量和各碳组分浓度[有机碳(OC)、元素碳(EC)和二次有机碳(SOC)等],并进行各碳组分之间的相关性及主成分分析.结果表明,不同空气质量下的城区污染物浓度均高于县区.OC和EC密切相关,非霾期的相关性系数较霾期大.与城区相比,霾期县区的SOC/PM_2.5较大,说明其受二次有机物污染更为明显;但城区非霾期二次气溶胶占比明显高于霾期,表明霾期的一次排放是城区大气污染的主要原因.燃煤、机动车排放和生物质燃烧均是两个区域PM_2.5的主要来源.     

Ru(III) catalyzed permanganate oxidation of aniline at environmentally relevant pH

Ru（Ⅲ） was employed as catalyst for aniline oxidation by permanganate at environmentally relevant pH for the first time. Ru（Ⅲ） could significantly improve the oxidation rate of aniline by 5-24 times with its concentration increasing from 2.5 to 15 μmol/L. The reaction of Ru（Ⅲ） catalyzed permanganate oxidation of aniline was first-order with respect to aniline, permanganate and Ru（Ⅲ）, respectively. Thus the oxidation kinetics can be described by a third-order rate law. Aniline degradation by Ru（Ⅲ） catalyzed permanganate oxidation was markedly influenced by pH, and the second-order rate constant （ktapp） decreased from 643.20 to 2.67 （mol/L）^-1 sec^-1 with increasing pH from 4.0 to 9.0, which was possibly due to the decrease of permanganate oxidation potential with increasing pH. In both the uncatalytic and catalytic permanganate oxidation, six byproducts of aniline were identified in UPLC-MS/MS analysis. Ru（Ⅲ）, as an electron shuttle, was oxidized by permanganate to Ru（Ⅵ） and Ru（Ⅶ）, which acted the co-oxidants for decomposition of aniline. Although Ru（Ⅲ） could catalyze permanganate oxidation of aniline effectively, dosing homogeneous Ru（Ⅲ） into water would lead to a second pollution. Therefore, efforts would be made to investigate the catalytic performance of supported Ru（Ⅲ） toward permanganate oxidation in our future study.     

广州PM2.5化学组分特征及其与气象因子的关系

于2012年12月—2013年12月在广州城区(市站)和东部郊区(九龙)开展为期一年的PM2.5样品采集,并同步收集气象因子和气态污染物质量浓度等数据.结果表明,PM2.5中主要化学组分为有机质(OM)和硫酸盐(SO2-4),分别占市站和九龙PM2.5质量浓度的49.4%和15.2%及57.0%和17.3%.碳质气溶胶(OM和EC)贡献接近50%,二次无机气溶胶(SO2-4、NO-3和NH+4总和,SIA)贡献超过30%.由于以机动车尾气为代表的移动污染源在城市区域贡献较大,市站[NO-3]/[SO2-4]比值显著高于九龙.两个站点[NH+4]/[SO2-4]摩尔质量比均高于1.5,表明观测期间广州市干季大气处于富铵状态.市站和九龙站硫氧化率(SOR)和氮氧化率(NOR)的时空变化趋势与O3类似,表明大气光化学过程是影响广州市SOR和NOR的重要因素.相对湿度低于65%时,SOR和NOR均较高;温度对SOR和NOR的影响有显著的城郊差异.降雨对PM2.5及各化学组分浓度有显著去除作用.     

Chemical composition, mass closure and sources of atmospheric PM10 from industrial sites in Shenzhen, China

Concentrations of atmospheric PM10 and chemical components (including twenty-one elements, nine ions, organic carbon (OC) and elemental carbon (EC)) were measured at five sites in a heavily industrial region of Shenzhen, China in 2005. Results showed that PM10 concentrations exhibited the highest values at 264 μg/m3 at the site near a harbor with the influence of harbor activities. Sulfur exhibited the highest concentrations (from 2419 to 3995 ng/m3) of all the studied elements, which may be related to the influence of coal used as fuel in this area for industrial plants. This was verified by the high mass percentages of SO42-, which accounted for 34.3%-39.7% of the total ions. NO3-/SO42- ratios varied from 0.64-0.71, which implies coal combustion was predominant compared with vehicle emission. The anion/cation ratios range was close to 0.95, indicating anion deficiency in this region. The harbor site showed the highest OC and EC concentrations, with the influence of emission from vessels. Secondary organic carbon accounted for about 22.6%-38.7% of OC, with the highest percentage occurring at the site adjacent to a coal-fired power plant and wood plant. The mass closure model performed well in this heavily industrial region, with significant correlation obtained between chemically determined and gravimetrically measured PM10 mass. The main constituents of PM10 were found to be organic materials (30.9%-69.5%), followed by secondary inorganic aerosol (7.9%-25.0%), crustal materials (6.7%-13.8%), elemental carbon (3.5%-10.8%), sea salt (2.4%-6.2%) and trace elements (2.0%-4.9%) in this heavily industrialized region. Principal component analysis indicated that the main sources for particulate matter in this industrial region were crustal materials and coal/wood combustion, oil combustion, secondary aerosols, industrial processes and vehicle emission.     

上海市浦东城区二次气溶胶生成的估算

利用2010年5～10月不同日最高O3小时浓度(O3,max)下PM10浓度变化评估不同O3浓度水平下二次气溶胶生成量.CO作为一次颗粒物的标志物,O3作为光化学反应水平的指示物种.结果表明不同光化学水平条件下,PM10中一次与二次气溶胶浓度及比例存在较大差异.随着光化学水平的增加,PM10中一次气溶胶排放浓度增长不大(0.036～0.044 mg.m-3),二次气溶胶的生成量却呈数倍增长(0.018～0.055 mg.m-3);二次与一次气溶胶浓度的比例也从49.8%增加到124.5%.O3,max出现的时间也随着光化学水平的增强由13:00推迟到14:00,二次气溶胶生成的主要时段也从11:00～20:00增加到09:00～20:00;此外,PM2.5中主要组分SO24-、NO3-、OC等比例随着光化学水平(即O3,max浓度)的不同而存在一定差异,当O3,max<0.10 mg.m-3时,PM2.5主要由12.0%有机碳(OC)、18.7%硫酸盐、13.1%硝酸盐和4.5%元素碳(EC)组成,而O3,max>0.20mg.m-3时,PM2.5主要由20.0%有机碳(OC)、22.9%硫酸盐、23.1%硝酸盐和4.7%元素碳(EC)组成.说明SO24-、NO3-、OC受光化学水平影响较大.     

机动车源和民用燃料源颗粒物中有机碳和元素碳的排放特征

为了获取机动车源尾气和主要民用燃料源燃烧过程排放的颗粒物中含碳气溶胶的排放特征,使用多功能便携式稀释通道采样器和Model 5L-NDIR型OC/EC分析仪,采集分析了典型机动车源(汽油车、轻柴油车、重柴油车)、民用煤(块煤和型煤)和生物质燃料(麦秆、木板、葡萄树树枝)的PM₁₀和PM_2.5样品中的有机碳(OC)和元素碳(EC).结果表明,不同排放源释放的PM₁₀和PM_2.5中含碳气溶胶的质量分数存在显著差异.总碳(TC)在不同源PM₁₀和PM_2.5中的质量分数范围分别为40.8%～68.5%和30.5%～70.9%,OC/EC范围分别为1.49～31.56和1.90～87.57.不同源产生的含碳气溶胶均以OC为主,OC在PM₁₀和PM_2.5中的质量分数范围分别为56.3%～97.0%和65.0%～98.7%.在PM₁₀和PM_2.5的含碳气溶胶中OC质量分数按照从高到低...     

上海城区二次气溶胶的形成:光化学氧化与液相反应对二次气溶胶形成的影响

二次组分是大气细颗粒物中最重要的组成部分之一.本研究旨在探究上海城区大气气溶胶颗粒物中二次组分的贡献及其形成的主要影响因素.利用高分辨率飞行时间气溶胶质谱仪(HR-TOF-AMS)对上海城区春季及夏季的亚微米颗粒物(PM_1)进行实时的在线表征,发现有机物是PM_1中最主要的组成部分,占比为55%;其次是硫酸盐(24%)与硝酸盐(10%).进一步结合正交矩阵因子解析模型(PMF)对有机组分进行了来源解析.结果表明,一次有机气溶胶(POA)与二次有机气溶胶(SOA)分别占总有机物浓度的34%与66%; POA主要来自机动车源与餐饮源的贡献,且在春季和夏季对有机物的贡献趋于稳定.观测期间共观察到3个二次气溶胶显著生成的过程:其中,春季二次组分的显著增长过程以硫酸盐和老化的有机气溶胶在正午时段上升显著为主要特征,主要受光化学氧化过程的促进;夏季二次组分的显著生成过程主要是液相反应与光化学氧化共同促进的结果,如液相反应过程中,硝酸盐浓度与颗粒相水含量有较好的相关性(R~2=0. 72),而光化学氧化期间SOA浓度与大气氧化性(O_x)有较好的相关性.总体而言,二次组分是上海城市大气气溶胶颗粒物中最重要的组成部分,二次有机与无机组分在PM_1颗粒物中占比分别为35. 5%和43%,光化学氧化与液相反应对二次组分的形成有显著的促进作用.