基于高质量分辨率质谱仪研究上海城区秋季大气亚微米级颗粒物化学特性

利用先进的高分辨飞行时间气溶胶质谱仪(High Resolution Time-of-Flight Aerosol Mass Spectrometer,HR-To F-AMS),于2017年9月8日—2017年10月8日对上海市城区开展了亚微米级颗粒物化学组分、粒径及其污染来源的在线测量.结果表明,观测期间上海城区亚微米颗粒物质量浓度平均为(22.0±17.2)μg·m-3;其中,有机物是PM1的主要贡献者,平均占总颗粒物浓度的49.3%,硫酸根、硝酸根和铵根的占比分别为24.2%、10.5%和9.7%.上海城区亚微米级颗粒物中无机盐组分类(硝酸根,硫酸根和铵根)具有较为一致的粒径分布,峰值粒径主要集中在空气动力学粒径500~600 nm.有机物的粒径分布峰值位于空气动力学粒径400~500 nm,且在小粒径范围内有较高的有机物浓度,表明存在一定程度的一次排放.观测期间有机气溶胶呈现明显的多峰分布,硫酸根、铵根和氯离子呈白天低、夜间高的特点,而硫酸根和黑碳的日变化并不明显.基于高分辨率有机质谱计算得到上海城区有机气溶胶氧碳比(O/C)的平均比值为0.37;有机物与有机碳(OM/OC)的平均比值1.65.利用正矩阵因子解析(PMF)模型对有机气溶胶高质量分辨率质谱进行来源解析,得到4类有机气溶胶:HOA(还原态有机气溶胶)、COA(餐饮源有机气溶胶)、MO-OOA(高氧化性有机气溶胶)和LO-OOA(低氧化性有机气溶胶),分别占有机气溶胶总量的15%、20%、32%和26%,说明观测期间上海城区有机气溶胶主要来自二次气溶胶的贡献.     

Influence of haze pollution on water-soluble chemical species in PM2.5 and size-resolved particles at an urban site during fall

To investigate the influence of haze on the chemical composition and formation processes of ambient aerosol particles,PM_(2.5) and size-segregated aerosol particles were collected daily during fall at an urban site of Gwangju,Korea.During the study period,the total concentration of secondary ionic species(SIS) contributed an average of 43.9% to the PM_(2.5) ,whereas the contribution of SIS to the PM_(2.5) during the haze period was 62.3%.The NO_3 and SO~(2-)_4 concentrations in PM_(2.5) during the haze period were highly elevated,being 13.4 and 5.0 times higher than those during non-haze period,respectively.The PM,NO~-_3,SO~(2-)_4,oxalate,water-soluble organic carbon(WSOC),and humic-like substances(HULIS) had tri-modal size distributions peaks at 0.32,1.0,and 5.2 μm during the non-haze and haze periods.However,during the non-haze period they exhibited dominant size distributions at the condensation mode peaking at 0.32 μm,while on October 21 when the heaviest haze event occurred,they had predominant droplet mode size distributions peaking at 1.00 μm.Moreover,strong correlations of WSOC and HULIS with SO~(2-)_4,oxalate,and K+at particle sizes of 1.8 μm indicate that secondary processes and emissions from biomass burning could be responsible for WSOC and HULIS formations.It was found that the factors affecting haze formation could be the local stable synoptic conditions,including the weak surface winds and high surface pressures,the long-range transportation of haze from eastern China and upwind regions of the Korean peninsula,as well as the locally emitted and produced aerosol particles.     

Characterization of size-resolved effective density of atmospheric particles in an urban atmosphere in Southern China

Effective density (ρ_eff) is one of the most important physical properties of atmospheric particles,providing important references in exploring the emissions and aging processes of fresh particles.In this study,a combined system of differential mobility analyzer,centrifugal particle mass analyzer,and condensation particle counter was used to periodically measure the ρ_eff of atmospheric particles in Shenzhen from Oct.2021 to Jan.2022.Results showed that the ρ_eff of...     

杭州市大气气溶胶光学厚度研究

利用2011~2012年杭州国家基准气候站内太阳光度计(CE-318)观测资料,分析杭州市气溶胶光学厚度(AOD)和Angstrom波长指数(α)的变化特征.结果表明,2011~2012年杭州市AOD500nm年平均值为0.86±0.47,α440~870nm年平均值为1.25±0.23.AOD季节变化特征不明显,主要与该地区天气形势以及内外源影响密切相关.α季节变化差异也不大,受北方带来的沙尘气溶胶影响,春季α略偏低.AOD呈现单峰型日变化特征,峰值出现在15:00,谷值出现在06:00,午后AOD明显升高主要与强烈的太阳辐射引起光化学反应产生的二次气溶胶以及近地层气溶胶在湍流输送作用下向城市上空扩散有关.从频率分布来看,AOD和α频率分布均呈现明显的单峰特征,并且较好的符合对数正态分布.α在高值区间1.1~1.7出现频率为77.8%,表明杭州市以平均半径较小的气溶胶粒子为主,属于城市-工业型气溶胶类型.杭州市AOD的高值(>1.0)主要表现为粗模态气溶胶以及细模态气溶胶的吸湿增长.     

微生物燃料电池处理含S2-/NH4+废水的研究

以除硫硝化微生物燃料电池(Microbial Fuel Cell,MFC)处理含S~(2-)/NH_4~+的模拟无机废水,研究了不同进水S~(2-)浓度下MFC的产电性能、污染物去除效果和阳极室硫累积情况.结果表明,除硫硝化MFC可实现同步阳极除硫和阴极硝化,并通过非生物电化学作用和生物电化学作用共同产电.进水S~(2-)浓度为(60.8±2.9)、(131.7±2.4)、(161.7±4.5)和(198.1±3.1)mg·L~(-1)时,最佳阳极碳刷清洗周期分别为3、3、3、4个换水周期,前3个进水浓度下的换水周期可分别缩短为6、8和8 h.MFC阴极硝化完全,不受进水S~(2-)浓度影响,但氧从阴极向阳极的渗漏导致阳极库仑效率较低(40%).适当增加进水S~(2-)浓度可增强MFC的产电性能并提高S~(2-)去除负荷和颗粒硫累积比.除硫硝化MFC适宜的进水S~(2-)浓度为(161.7±4.5)mg·L~(-1),相应的最大功率密度为5.77 W·m~(-3),周期产电量为(141.0±5.2)C,S~(2-)去除负荷为(0.31±0.00)g·L~(-1)·d~(-1),颗粒硫累积比达58%.阳极碳纤维丝上沉积有粒径约100 nm的颗粒硫.阳极悬浮物与沉积物相比,悬浮物中S0含量比例较高,而S6+含量比例较低.     

Hygroscopicity of ambient submicron particles in urban Hangzhou, China

In this study, hygroscopicity of size-segregated ambient submicron particles in urban Hangzhou was studied from 28th December 2009 to 18th January 2010, using a hygroscopicity-tandem differential mobility analyzer (H-TDMA). The submicron particles in Hangzhou showed a minor hygroscopic growth at 73% relative humidity (RH), and then grew significantly between 77% and 82% RH. Monomodal distribution accounted for 90% for 30 nm particles, 17% for 50 nm particles, and less than 7% for particles larger than 50 nm at 82% RH. Deconvolution of the bimodal distribution indicated a less hygroscopic group and a more hygroscopic group, with the fraction of the more hygroscopic group increasing with the initial dry particle size and then remaining almost constant for accumulation mode particles. Our results imply that submicron particles in urban Hangzhou were almost entirely externally mixed, and the hygroscopic properties of ambient particles in urban Hangzhou were mainly a function of their size and chemical composition.     

Temporal variations and source apportionment of volatile organic compounds at an urban site in Shijiazhuang, China

Shijiazhuang, the city with the worst air quality in China, is suffering from severe ozone pollution in summer. As the key precursors of ozone generation, it is necessary to control the Volatile Organic Compounds(VOCs) pollution. To have a better understanding of the pollution status and source contribution, the concentrations of 117 ambient VOCs were analyzed from April to August 2018 in an urban site in Shijiazhuang. Results showed that the monthly average concentration of total VOCs was 66.27...     

Field measurements of dissociation of ammonium nitrate at a Beijing site

The atmospheric nitric acid, ammonia and ammonium nitrate aerosol was determined simultaneously in a Beijing site to teste quilibrium. Rather good agreement between measurements and theory was found at ambient temperature above 9oC at relative humidity below 70%. Below 9oC the kinetic constraints preventing rapid attainment equilibrium were observed. A procedure for calculation of dependence of NH4NO3 aerosol dissociation constants on temperature and relative humidity was given. The seasonal variation of concentration of NH3, total NH4+ and HNO3 was observed.The seasonal variation of concentration of HNO3 was caused by dissociation of aerosol of NH4NO3. The concentrations of NH3 were 1-2 order higher than those of HNO3. For formation of NH4NO3 aerosol the HNO3 was the control reagent. Any increase of HNO3 to formed from NOx would react with NH3 form NH4NO3 aerosol in Beijing area except for someday in summer time.     

Abundance and sources of particulate polycyclic aromatic hydrocarbons and aromatic acids at an urban site in central China

We conducted a simultaneous field study of PM_2.5-bound particulate polycyclic aromatic hydrocarbons (PAHs) and aromatic acids (AAs) in a polluted city Zhengzhou to explore the concentration,sources and potential conversion pathways between PAHs and AAs in different seasons.The average concentrations of PM_2.5,28PAHs and 8AAs during the sampling period were 77μg/m³,75 ng/m³,and 283 ng/m³,respectively.The concentration of both28PAHs and 8AAs we...     

New approaches to characterizing urban air particles in central London

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重庆市主城区大气细颗粒物污染特征与来源解析

重庆市主城区大气细颗粒物(PM_(2.5))浓度从1990s的100μg·m~(-3)下降至当前的约70μg·m~(-3),但仍高于环境标准限值.为探讨重庆市主城区PM_(2.5)化学组成与来源特征,于2012—2013年在渝北区大气超级站利用四通道采样仪连续采集了颗粒物样品,分析了其中水溶性离子、碳质组分和无机元素含量.采样期间,重庆市主城区大气PM_(10)和PM_(2.5)的年日均浓度分别为103.9和75.3μg·m~(-3),扩散条件不利的冬季,细颗粒物污染较为严重.受静稳天气影响的1月和2月,受沙尘影响的3月,及二次转化显著的6月是重庆市细颗粒物污染较重的月份.重庆市PM_(2.5)组成以有机物(OM,30.8%)为主,其次为硫酸盐(SO_4~(2-),23.0%)、硝酸盐(NO_3~-,11.7%)、铵盐(NH_4~+,10.9%)、地壳物质(Soil,8.2%)、元素碳(EC,5.2%)、K~+(1.1%)、Cl~-(1.0%)和微量元素(Trace,0.6%).较高的SO_4~(2-)浓度和逐步上升的[NO_3~-]/[SO_4~(2-)]比值反映了重庆市燃煤污染较重,同时机动车污染比例逐步增加.采用主因子分析/绝对主因子得分法解析了重庆城区细颗粒物5类主要来源是:二次粒子(41.7%)、燃煤(15.6%)、建筑/道路尘(12.4%)、土壤尘(11.0%)和工业尘(10.4%),通过各污染源季节变化及与其他结果对比,该源解析结果能够较可靠反映重庆市细颗粒物的来源信息.     

Secondary organic aerosols in Jinan, an urban site in North China: Significant anthropogenic contributions to heavy pollution

Secondary organic aerosols(SOAs) are an important component of particulates, but whether biogenic SOAs(BSOAs) or anthropogenic SOAs(ASOAs) are the dominant contributors to haze pollution remains poorly characterized. In this study, particulate samples were collected from September 2014 to August 2015 at an urban site in Jinan, which is the capital of Shandong Province and a typical city in the North China Plain. The PM2.5 samples were analyzed for BSOA(isoprene(SOAI) and monoterpenes(SOAM)) and ASOA(aromatic(SOAA)) tracers. The concentrations of the SOAAtracer(1.1 ± 1.0 ng/m3) were lowest, and those of SOAItracers(41.8 ± 86.2 ng/m3) were highest, with the concentrations of SOAMtracers(19.4 ± 9.9 ng/m3) being intermediate. The SOAItracers were more abundant in the summer and less abundant in the winter. Both SOAIand SOAMincreased with increasing ozone level but decreased with increasing NOx level. Correlation analysis revealed a good correlation between 2,3-dihydroxy-4-oxopentanoic acid and levoglucosan levels in three seasons. These results suggested that biomass burning activities occurring in the NCP can enhance the emissions of aromatics and should be controlled, especially in the autumn and winter. SOA tracers were classified according to pollution degree, and the results showed that as pollution increases, the contributions of SOAAincrease. These results indicate that reducing anthropogenic emissions is necessary to prevent SOA pollution, especially during heavy pollution episodes.     

Study of aerosol characteristics and sources using MAX-DOAS measurement during haze at an urban site in the Fenwei Plain

Atmospheric aerosols have effects on atmospheric radiation assessments, global climate change, local air quality and visibility. In particular, aerosols are more likely transformed and accumulated in winter. In this paper, we used the Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument to study the characteristics of aerosol type and contributions of PM_2.5 chemical components to aerosol extinction (AE), vertical distribution of aerosols, and source. From December 30, 2018 to January 27, 2019, we conducted MAX-DOAS observations on Sanmenxia. The proportion of PM_2.5 to PM₁₀ was 69.48%–95.39%, indicating that the aerosol particles were mainly fine particles. By analyzing the ion data and modifying Interagency Monitoring of Protected Visual Environments (IMPROVE) method, we found that nitrate was the largest contributor to AE, accounting for 31.51%, 28.98%, and 27.95% of AE on heavily polluted, polluted, and clean days, respectively. NH₄⁺, OC, and SO₄^2? were also major contributors to AE. The near-surface aerosol extinction retrieved from MAX-DOAS measurement the PM_2.5 and PM₁₀ concentrations measured by an Unmanned Aerial Vehicle (UAV) have the same trend in vertical distribution. AE increased about 3 times from surface to 500 m. With the backward trajectory of the air mass during the haze, we also found that the continuous heavy pollution was mainly caused by transport of polluted air from the northeast, then followed by local industrial emissions and other sources of emissions under continuous and steady weather conditions.     

Characteristics of one-year observation of VOCs, NOx, and O3 at an urban site in Wuhan, China

A continuous online observation of ozone and its precursors(NOx, VOCs) was carried out in central urban Wuhan from September 2016 to August 2017. The concentration levels of ozone,NOx, VOCs and their variations in urban Wuhan were analyzed, as well as effects of VOCs on ozone photochemical generation and the main controlling factors for ozone production. During the observation period, the average concentrations of ozone and NOx in Wuhan was 22.63 and30.14 ppbv, respectively, and the average concentration of VOCs was 32.61 ppbv(42.3% alkanes,13.0% alkenes, 10.0% aromatics, 7.3% acetylene, 9.9% OVOCs, and 10.5% halohydrocarbons).Ozone concentration was higher in spring and summer as compared with autumn and winter,wheras VOCs and NOx concentratios were lower in spring and summer but higher in autumn and winter. Aromatics and alkenes, two of VOCs species, showed the highest contributions to ozone formation potential in Wuhan(35.7% alkenes, 35.4 aromatics, 17.5% alkanes, 8.6% OVOCs,1.6% halogenated hydrocarbons, and 1.4% acetylene). Among all VOCs species, those with the highest contribution were ethylene, m-xylene, toluene, propylene and o-xylene. The contribution of these five compounds to the total ozone formation potential concentration was 43.90%.Ozone-controlling factors in Wuhan changed within one day; during the early morning hours(6:00–9:00), VOCs/NOx was low, and ozone generation followed a VOCs-limited regime.However, during the peak time of ozone concentration(12:00–16:00), the ratio of VOCs/NOx was relatively high, suggesting that ozone generation followed a NOx-limited regime.     

杭州市区大气气溶胶吸收系数观测研究

利用2011年6~8月和2011年12月~2012年2月杭州国家基准气候站内黑碳及气象观测资料,分析了杭州市区气溶胶吸收系数的变化特征.结果表明,杭州市区气溶胶吸收系数冬季[(42.3±17.7)Mm-1]要高于夏季[(35.8±10.5)Mm-1],且冬季气溶胶吸收系数变化较为剧烈.在边界层变化以及人类活动的共同影响下,气溶胶吸收系数呈现明显的双峰型日变化特征,峰值出现在07:00~09:00,谷值出现在14:00,次峰值出现在19:00~20:00.通过拟合小时平均值最大出现频率得出该地区气溶胶吸收系数本底值为24.7Mm-1.霾时气溶胶吸收系数要高于非霾时,随着霾污染的加重,气溶胶吸收系数呈现阶梯上升趋势.霾期间气溶胶吸收系数的增加是造成能见度下降的重要原因之一.     

Gravimetric analysis for PM2.5 mass concentration based on year-round monitoring at an urban site in Beijing

Daily PM_(2.5)(particulate matter with an aerodynamic diameter of below 2.5 μm) mass concentrations were measured by gravimetric analysis in Chinese Research Academy of Environmental Sciences(CRAES), in the northern part of the Beijing urban area, from December 2013 to April 2015. Two pairs of Teflon(T1/T2) and Quartz(Q1/Q2) samples were obtained, for a total number of 1352 valid filters. Results showed elevated pollution in Beijing,with an annual mean PM_(2.5)mass concentration of 102 μg/m~3. According to the calculated PM_(2.5)mass concentration, 50% of our sampling days were acceptable(PM_(2.5) 75 μg/m~3), 30% had slight/medium pollution(75–150 μg/m~3), and 7% had severe pollution( 250 μg/m~3). Sampling interruption occurred frequently for the Teflon filter group(75%) in severe pollution periods,resulting in important data being missing. Further analysis showed that high PM_(2.5)combined with high relative humidity(RH) gave rise to the interruptions. The seasonal variation of PM_(2.5)was presented, with higher monthly average mass concentrations in winter(peak value in February, 422 μg/m~3), and lower in summer(7 μg/m~3 in June). From May to August, the typical summer period, least severe pollution events were observed, with high precipitation levels accelerating the process of wet deposition to remove PM_(2.5). The case of February presented the most serious pollution, with monthly averaged PM_(2.5)of 181 μg/m~3 and 32% of days with severe pollution. The abundance of PM_(2.5)in winter could be related to increased coal consumption for heating needs.     

德国城镇水事管理法律的发展——供水保障和污水处理

关于饮用水供应和污水处理的法律规范,属于市政水管理的核心领域,是水管理法的重要组成部分。特别在国际和欧盟层面,以长期保障饮用水供应为核心内容的“涉水人权”成为关注热点。首先对德国水事管理法律的发展做一概览,《水法》确保一种公法上的监管秩序。尽管受到欧盟《水框架指令》影响,德国水事管理在向水环境质量达标转型,但饮用水供应与污水处理仍是《水法》的核心内容。在欧盟层面上,除了《水框架指令》外,《市政污水指令》和《饮用水指令》分别对供水保障和污水处理2个领域做了具体规定。在德国法律层面上,首先对供水保障和污水处理领域的组织体系,从集中式和分散式的发展趋势以及保障效率的私营化趋势加以评析;其次对《水法》在联邦制改革下的发展和作为水事监管核心的许可制度进行介绍;然后在污水监管领域,分别就污水排放许可的先进技术水准、直接与间接排放、污水收费和污泥处理进行分析;最后就饮用水供应领域,从水源地保护和饮用水供应2个方面加以介绍,指出了德国在水事监管领域的挑战。     

Physicochemical characteristics of ambient particles settling upon leaf surfaces of urban plants in Beijing

Particulate pollution is a serious health problem throughout the world, exacerbating a wide range of respiratory and vascular illnesses in urban areas. Urban plants play an important role in reducing particulate pollution. Physicochemical characteristics of ambient particles settling upon leaf surfaces of eleven roadside plants at four sites of Beijing were studies. Results showed that density of particles on the leaf surfaces greatly varied with plant species and traffic condition. Fraxinus chiuensis, Sophora japonica Ailanthus altissima, Syringa oblata and Prunus persica, had larger densities of particles among the tall species. Due to resuspension of road dust, the densities of particles of Euonymus japonicns and Parthenocissus quinquefolia with low sampling height were 2-35 times to other taller tree species. For test plant species, micro-roughness of leaf surfaces and density of particles showed a close correlation. In general, the larger micro-roughness of leaf surfaces is, the larger density of particles is. Particles settling upon leaf surfaces were dominantly PM30 （particulate matter less than 10 μm in aerodynamic diameter; 98.4%） and PM2.5 （particulate matter less than 2.5 μm in aerodynamic diameter; 64.2%） which were closely relative to human health. Constant elements of particles were C, O, K, Ca, Si, Al, Mg, Na, Fe, S, Cl and minerals with higher content were SiO2, CaCO3, CaMg（CO3）2, NaCI and 2CASO4. H2O, SiO2. CaCO3 and CaMg（CO3）2 mainly came from resuspension of road dust. 2CaSO4. H2O was produced by the reaction between CaCO3 derived from earth dust or industrial emission and SO2, H2SO4 or sulfate. NaCl was derived from sea salt.     

Chemical formation and source apportionment of PM2.5 at an urban site at the southern foot of the Taihang mountains

The region along the Taihang Mountains in the North China Plain (NCP) is characterized by serious fine particle pollution. To clarify the formation mechanism and controlling factors, an observational study was conducted to investigate the physical and chemical properties of the fine particulate matter in Jiaozuo city, China. Mass concentrations of the water-soluble ions (WSIs) in PM_2.5 and gaseous pollutant precursors were measured on an hourly basis from December 1, 2017, to February 27, 2018. The positive matrix factorization (PMF) method and the FLEXible PARTicle (FLEXPART) model were employed to identify the sources of PM_2.5. The results showed that the average mass concentration of PM_2.5 was 111 μg/m³ during the observation period. Among the major WSIs, sulfate, nitrate, and ammonium (SNA) constituted 62% of the total PM_2.5 mass, and NO₃^? ranked the highest with an average contribution of 24.6%. NH₄⁺ was abundant in most cases in Jiaozuo. According to chemical balance analysis, SO₄^2?, NO₃^?, and Cl^? might be present in the form of (NH₄)₂SO₄, NH₄NO₃, NH₄Cl, and KCl. The liquid-phase oxidation of SO₂ and NO₂ was severe during the haze period. The relative humidity and pH were the key factors influencing SO₄^2- formation. We found that NO₃^? mainly stemmed from homogeneous gas-phase reactions in the daytime and originated from the hydrolysis of N₂O₅ in the nighttime, which was inconsistent with previous studies. The PMF model identified five sources of PM_2.5: secondary origin (37.8%), vehicular emissions (34.7%), biomass burning (11.5%), coal combustion (9.4%), and crustal dust (6.6%).     

高氨氮废水短程硝化过程中N2O释放试验研究

试验采用序批式反应器(SBR)处理高氨氮废水,逐步提高废水氨氮(NH+4-N)浓度到800 mg·L-1,通过控制曝气量实现了短程硝化.SBR周期试验表明,在低溶解氧和高游离氨等共同作用下,氨氧化菌(AOB)活性较低,导致AOB以亚硝酸盐氮(NO_2~--N)作为电子受体进行好氧反硝化,氧化亚氮(N_2O)释放因子为9.8%.静态试验控制初始NH_4~+-N为100 mg·L-1且改变曝气量(0.22~0.88 L·min~(-1))条件下,溶解氧浓度的增加能够提高硝化菌活性,N2O释放因子为0.51%~0.85%.当初始NH_4~+-N浓度为100 mg·L~(-1)且曝气量控制在0.66 L·min-1时,初始NO-2-N浓度为0~100 mg·L~(-1)对硝化菌活性影响较小,N2O释放因子为0.50%~0.71%.当溶解氧和游离氨浓度控制在适宜范围内,可维持AOB较高活性,抑制AOB发生好氧反硝化作用,降低N2O释放率.