川南四座城市PM2.5化学组分污染特征及其源解析

为探究川南地区大气气溶胶中化学组分与来源特征,于2015年9月—2016年8月在四川盆地南部4个典型代表城市(泸州、内江、宜宾、自贡)采集了226个PM_2.5样品,对PM_2.5的质量浓度和主要化学组分(水溶性离子和碳质组分)进行测定,并利用颗粒物源解析受体模型对PM_2.5来源进行解析.结果表明:川南地区PM_2.5日均浓度为46.4—68.0μg·m^-3,均高于国家环境空气质量标准年均PM_2.5限值(35.0μg·m^-3).OC、EC和水溶性二次离子(SO₄^2-、NO₃-和NH₄+)分别占PM_2.5质量的15.7%—22.8%、4.2%—6.4%和28.6%—55.8%.PM_2.5及其主要化学组分浓度有显著的季节变化,即冬季浓度显著高于其他季节,夏季浓度最低.泸州除夏季外,其他季节SO₄2-、NO₃-同源性较好;其他城市在冬季,SO₄2-、NO₃-同源性较好.NH₄+主要存在形式为NH₄NO₃、(NH₄)2SO₄、NH₄HSO₄.OC、EC来源复杂,主要为机动车源、煤燃烧源和生物质燃烧源.川南地区PM_2.5的来源主要受8种因子影响,按总体贡献排序依次为:二次硫酸盐、生物质燃烧、工业源、二次硝酸盐、机动车源、煤燃烧、道路尘埃和建筑尘埃.此外,相比较而言,机动车源贡献在泸州市较凸显,煤燃烧源贡献在宜宾市较凸显.     

Denitrification potential in a Louisiana wetland receiving diverted Mississippi River water

Excess nitrate in Mississippi River water entering offshore areas is reported to contribute to low oxygen (hypoxia) conditions in the Gulf of Mexico. Excessive algal growth driven by the excess nitrogen results in a decrease in dissolved oxygen in bottom water. Reintroduction of Mississippi River waters into a Louisiana coastal wetland has the potential to reduce the amount of nitrate reaching offshore waters. In this study, reduction in the concentration of added NO₃^- was determined in sediment-water-columns collected from a wetland site in Breton Sound estuary receiving nutrient inputs from the Mississippi River. The capacity of a wetland to process nitrate in floodwater was determined in the laboratory. The rates of NO₃^- removal (determined from change in nitrate concentration in the floodwater) averaged 97 mg N m^-2 d^-1 over 16 d for a 1750-mg NO₃-N m^-2 addition, and 170 mg N m^-2 d^-1 over 16 d for a 3500-mg NO₃-N m^-2 addition. The total N₂O-N emissions from the 1750- and 3500-mg NO₃-N m^-2 additions were 19 and 54 mg N m^-2 accounting for 1.1% and 1.5% of the applied NO₃-N, respectively. Using the acetylene-inhibition technique, the average denitrification rate was determined to be 57 and 87 mg N m^-2 d^-1 (21 and 32 g N m^-2 yr^-1) during the most active denitrification period of 5 d after incubation for 1750 and 3500 mg NO₃^--N m^-2 of added nitrate in floodwater, respectively. The total N evolved over 11 d as N₂O + N₂ was equivalent to 436 and 921 mg N m^-2 (24.9% and 26.3%, respectively, of added N). Increasing the amount of NO₃^- applied to the overlying water increased the rate of NO₃^- loss and N₂O emission significantly. The thickness of the oxidized surface sediment layer was also influenced by the NO₃^- application to the floodwater with a significant linear correlation between nitrate addition and thickness of the oxidized layer (r = 0.9998, p = 0.01). This study indicates that wetlands receiving diverted Mississippi River water have the potential to process and remove NO₃^- in the river water, reducing the amount of NO₃^- reaching to offshore areas.     

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.     

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。     

Dilution sampling and analysis of particulate matter in biomass-derived syngas

Thermochemical biomass gasification, followed by conversion of the produced syngas to fuels and electrical power, is a promising energy alternative. Real-world characterization of particulate matter (PM) and other contaminants in the syngas is important to minimize damage and ensure efficient operation of the engines it powers and the fuels created from it. A dilution sampling system is demonstrated to quantify PM in syngas generated from two gasification plants utilizing different biomass feedstocks: a BioMax^?15 Biopower System that uses raw and torrefied woodchips as feedstocks, and an integrated biorefinery (IBR) that uses rice hulls and woodchips as feedstocks. PM_2.5 mass concentrations in syngas from the IBR downstream of the purification system were 12.8–13.7 μg·m^-3, which were significantly lower than the maximum level for catalyst protection (500 μg·m^-3) and were 2–3 orders of magnitude lower than those in BioMax^?15 syngas (2247–4835 μg·m^-3). Ultrafine particle number concentration and PM_2.5 chemical constituents were also much lower in the IBR syngas than in the BioMax^?15. The dilution sampling system enabled reliable measurements over a wide range of concentrations: the use of high sensitivity instruments allowed measurement at very low concentrations (~1 μg·m^-3), while the flexibility of dilution minimized sampling problems that are commonly encountered due to high levels of tars in raw syngas (~1 g·m^-3).     

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。     

Continuous biohydrogen production from diluted molasses in an anaerobic contact reactor

An anaerobic contact reactor (ACR) system comprising a continuous flow stirred tank reactor (CSTR) with settler to decouple the hydraulic retention time (HRT) from solids retention time (SRT) was developed for fermentative hydrogen production from diluted molasses by mixed microbial cultures. The ACR was operated at various volumetric loading rates (VLRs) of 20–44 kgCOD·m^-3·d^-1 with constant HRT of 6 h under mesophilic conditions of 35°C. The SRT was maintained at about 46–50 h in the system. At the initial VLR of 20 kgCOD·m^-3·d^-1, the hydrogen production rate dropped from 22.6 to 1.58 L·d^-1 as the hydrogen was consumed by the hydrogentrophic methanogen. After increasing the VLR to 28 kgCOD·m^-3·d^-1 and discharging the sludge for 6 consecutive times, the hydrogentrophic methanogens were eliminated, and the hydrogen content reached 36.4%. As the VLR was increased to 44 kgCOD·m^-3·d^-1, the hydrogen production rate and hydrogen yield increased to 42.1 L·d^-1 and 1.40 mol H₂·molglucose-consumed^-1, respectively. The results showed that a stable ethanol-type fermentation that favored hydrogen production in the reactor was thus established with the sludge loading rate (SLR) of 2.0–2.5 kgCOD·kgMLVSS^-1·d^-1. It was found that the ethanol increased more than other liquid fermentation products, and the ethanol/acetic acid (mol/mol) ratio increased from 1.27 to 2.45 when the VLR increased from 28 to 44 kgCOD·m^-3·d^-1, whereas the hydrogen composition decreased from 40.4% to 36.4%. The results suggested that the anaerobic contact reactor was a promising bioprocess for fermentative hydrogen production.     

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....     

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.     

Fermentative hydrogen production from beet sugar factory wastewater treatment in a continuous stirred tank reactor using anaerobic mixed consortia

A low pH, ethanol-type fermentation process was evaluated for wastewater treatment and bio-hydrogen production from acidic beet sugar factory wastewater in a continuous stirred tank reactor (CSTR) with an effective volume of 9.6 L by anaerobic mixed cultures in this present study. After inoculating with aerobic activated sludge and operating at organic loading rate (OLR) of 12 kgCOD?m^-3·d^-1, HRT of 8h, and temperature of 35°C for 28 days, the CSTR achieved stable ethanol-type fermentation. When OLR was further increased to 18 kgCOD?m^-3·d^-1 on the 53rd day, ethanol-type fermentation dominant microflora was enhanced. The liquid fermentation products, including volatile fatty acids (VFAs) and ethanol, stabilized at 1493 mg·L^-1 in the bioreactor. Effluent pH, oxidation-reduction potential (ORP), and alkalinity ranged at 4.1–4.5, -250–(-290) mV, and 230–260 mgCaCO₃?L^-1. The specific hydrogen production rate of anaerobic activated sludge was 0.1 L?gMLVSS^-1·d^-1 and the COD removal efficiency was 45%. The experimental results showed that the CSTR system had good operation stability and microbial activity, which led to high substrate conversion rate and hydrogen production ability.     

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%。     

Sediment nutrient flux in a coastal lake impacted by diverted Mississippi River water

The internal nutrient load from bottom sediment to the water column of a Louisiana Barataria Basin lake (Lake Cataouatche) receiving diverted Mississippi River water was determined. Dissolved reactive phosphorus (DRP), ammonium (NH₄-N) and nitrate (NO₃-N) flux from sediment to water column were measured. The DRP flux averaged-0.22 mg m^-2 d^-1 under aerobic water column conditions, as compared with that 3.29 mg m^-2 d^-1 under anaerobic conditions. The average NH₄-N released under anaerobic conditions (1.42 mg m^-2 d^-1) was significantly greater than rates under aerobic conditions (-0.02 mg m^-2 d^-1), indicating a strong relationship between nutrient flux and oxygen availability in the water column. The average NO₃-N flux was 2.13 mg m^-2 d^-1 under aerobic conditions as compared with-0.24 mg m^-2 d^-1 under anaerobic conditions in the sediment-water column. When the water column maintained under anaerobic conditions was switched to aerobic conditions, the DRP, NH₄-N, and NO₃-N concentrations in overlying water decreased rapidly over a short period of time. The mean annual internal DRP and NH₄-N load from the sediment to the overlying water was estimated to be 69.26 and 29.9 tonnes (Mg) yr^-1 respectively, which represents a significant portion of the total nutrient load to the Lake. Results demonstrate that the internal flux of nutrients from sediments can contribute a significant portion of the total nutrient load to the water column and should be considered in decisions on impact of nutrient in diverted Mississippi River on water quality of Barataria Basin.     

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.     

Mass concentrations and temporal profiles of PM10, PM2.5 and PM1 near major urban roads in Beijing

Mass concentrations of PM₁₀, PM_2.5 and PM₁ were measured near major roads in Beijing during six periods: summer and winter of 2001, winter of 2007, and periods before, during and after the 2008 Beijing Olympic Games. Since the control efforts for motor vehicles helped offset the increase of emissions from the rapid growth of vehicles, the averaged PM_2.5 concentrations at roadsides during the sampling period between 2001 and 2008 fluctuated over a relatively small range. With the implementation of temporary traffic control measures during the Olympics, a clear “V” shaped curve showing the concentrations of particulate matter and other gaseous air pollutants at roadsides over time was identified. The average concentrations of PM₁₀, PM_2.5, CO and NO decreased by 31.2%, 46.3%, 32.3% and 35.4%, respectively, from June to August; this was followed by a rebound of all air pollutants in December 2008. Daily PM₁₀ concentrations near major roads exceeded the National Ambient Air Quality Standard (Grade II) for 61.2% of the days in the non-Olympic periods, while only for 12.5% during the Olympics. The mean ratio of PM_2.5/PM₁₀ near major roads remained relatively stable at 0.55 (±0.108) on non-Olympic days. The ratio decreased to 0.48 (±0.099) during the Olympics due to a greater decline in fine particles than in coarse-mode PM. The ratios PM₁/PM_2.5 fluctuated over a wide range and were statistically different from each other during the sampling periods. The average ratios of PM₁/PM_2.5 on non-Olympic days were 0.71.     

Electrocatalytic reduction of nitrate using Pd-Cu modified carbon nanotube membranes

● Pd-Cu modified CNT membranes were prepared successfully by electrodeposition method. ● The deposition voltage and deposition time were optimized for Pd-Cu co-deposition. ● NO₃⁻-N was removed efficiently from water by Pd-Cu modified CNT membranes. ● The presence of dissolved oxygen did not affect the nitrate reduction performance. ● Mass transfer rate was promoted significantly with the increase in membrane flux. Excessive nitrate in water is harmful to the ecological environment and human health. Electrocatalytic reduction is a promising technology for nitrate removal. Herein, a Pd-Cu modified carbon nanotube membrane was fabricated with an electrodeposition method and used to reduce nitrate in a flow-through electrochemical reactor. The optimal potential and duration for codeposition of Pd and Cu were −0.7 V and 5 min, respectively, according to linear scan voltammetry results. The membrane obtained with a Pd:Cu ratio of 1:1 exhibited a relatively high nitrate removal efficiency and N₂ selectivity. Nitrate was almost completely reduced (~99 %) by the membrane at potentials lower than −1.2 V. However, −0.8 V was the optimal potential for nitrate reduction in terms of both nitrate removal efficiency and product selectivity. The nitrate removal efficiency was 56.2 %, and the N₂ selectivity was 23.8 % for the Pd:Cu=1:1 membrane operated at −0.8 V. Nitrate removal was enhanced under acidic conditions, while N₂ selectivity was decreased. The concentrations of Cl⁻ ions and dissolved oxygen showed little effect on nitrate reduction. The mass transfer rate constant was greatly improved by 6.6 times from 1.14 × 10⁻³ m/h at a membrane flux of 1 L/(m²·h) to 8.71 × 10⁻³ m/h at a membrane flux of 15 L/(m²·h), which resulted in a significant increase in the nitrate removal rate from 13.6 to 133.5 mg/(m²·h). These findings show that the Pd-Cu modified CNT membrane is an efficient material for nitrate reduction.     

Degradation of bisphenol A by microorganisms immobilized on polyvinyl alcohol microspheres

In this study, microorganisms （named B111） were immobilized on polyvinyl alcohol microspheres prepared by the inverse suspension crosslinked method. The biodegradation of bisphenol A （BPA） and 4-hydro- xybenzaldehyde, a degradation product of BPA, by free and immobilized B lll was investigated. The BPA degradation studies were carried out at initial BPA concentrations ranging from 25 to 150 mg·L^-1. The affinity constant Ks and maximum degradation rate Rmax were 98.3 mg·L^-1 and 19.7mg·mg^-1VSS·d^-1 for free B111, as well as 87.2mg·L^-1 and 21.1mg·mg^-1VSS·d^-1 for immobilized B 111, respectively. 16S rDNA gene sequence analyses confirmed that the dominant genera were Pseudomonas and Brevundimonas for BPA biodegradation in microorganisms B 111.     

南京秋季大气PM2.5中类腐殖质的光学性质与来源分析

类腐殖质(humic-like substances, HULIS)是水溶性有机碳(WSOC)中具有吸光特性的重要组分,对空气质量、气候变化和人体健康均有重要影响.尽管目前对HULIS的研究很多,但不同方法分离机理不同,对于HULIS的分离与测定仍然缺乏统一的标准,针对HULIS分离方法的研究很少.固相萃取法(solid phase extraction, SPE)因其操作简单、分离效果较好而被广泛应用,但对于低浓度样品仍存在检出限较高、回收率较低的问题,且很少有人关注提纯过程中流程空白所包含的含碳组分及其吸光能力.本研究通过调整活化溶液(0.01 mol·L^-1 HCl溶液+甲醇+2%NH₃H₂O/MeOH)与洗脱溶液(2%NH₃H₂O/MeOH)用量的比例对提纯方法进行优化.结果表明,应用优化后的方法对流程空白进行测量时,检出限(MDL)降低到0.035 mg·L^-1以下,精密度RSD <5.41%(n=20),标准品回收率达到95%,在保证回收率的情况下减少了流程空白,提高了样品的精密度,使测定浓度较低的HULIS含量成为可能.为了探究生物质燃烧期间含碳组分的光学特性和来源特征,本研究对2017年10月6日至11月9日南京北郊秋季大气气溶胶样品进行采集.采样期间PM_2.5的浓度为(87.9±43.7)μg·m^-3,WSOC和类腐殖质碳(HULIS-C)的浓度分别为(4.2±2.3)μg·m^-3和(3.6±2.0)μg·m^-3,HULIS-C占WSOC的比例为47.3%,是WSOC中的重要组成部分.本研究还对HULIS在330—400 nm波段的吸光进行测定,使用Angstrom指数(absorption angstrom exponent,AAE)进行表征,得到采样期间AAE的值为2—7,说明HULIS污染主要来自二次转化.后向轨迹结果表明,重污染期间污染物来源为本地生物质燃烧和区域或者长距离气团的输送.     

Seasonal variations of transport pathways and potential sources of PM2.5 in Chengdu,China (2012–2013)

PM_2.5 in Chengdu showed clear seasonal and diurnal variation. 5, 5, 5 and 3 mean clusters are generated in spring, summer, autumn, and winter. Short-distance air masses are important pathways in Chengdu. Emissions within the Sichuan Basin contribute significantly to PM_2.5 pollution. Long-range transport from Southern Xinjiang is a dust invasion path to Chengdu. Seasonal pattern of transport pathways and potential sources of PM_2.5 in Chengdu during 2012–2013 were investigated based on hourly PM_2.5 data, backward trajectories, clustering analysis, potential source contribution function (PSCF), and concentration-weighted trajectory (CWT) method. The annual hourly mean PM_2.5 concentration in Chengdu was 97.4 mg·m^–3. 5, 5, 5 and 3 mean clusters were generated in four seasons, respectively. Short-distance air masses, which travelled within the Sichuan Basin with no specific source direction and relatively high PM_2.5 loadings (>80 mg·m^–3) appeared as important pathways in all seasons. These short pathways indicated that emissions from both local and surrounding regions of Chengdu contributed significantly to PM_2.5 pollution. The cities in southern Chengdu were major potential sources with PSCF>0.6 and CWT>90 mg·m^–3. The northeastern pathway prevailed throughout the year with higher frequency in autumn and winter and lower frequency in spring and summer. In spring, long-range transport from southern Xinjiang was a representative dust invasion path to Chengdu, and the CWT values along the path were 30-60 mg·m^–3. Long-range transport was also observed in autumn from southeastern Xinjiang along a northwesterly pathway, and in winter from the Tibetan Plateau along a westerly pathway. In summer, the potential source regions of Chengdu were smaller than those in other seasons, and no long-range transport pathway was observed. Results of PSCF and CWT indicated that regions in Qinghai and Tibet contributed to PM_2.5 pollution in Chengdu as well, and their CWT values increased to above 30 mg·m^-3 in winter.     

Characterization of submicron aerosols in the urban outflow of the central Pearl River Delta region of China

Submicron aerosol particles (with aerodynamic diameters less than 1 μm, PM₁) were sampled and measured in Heshan, an urban outflow site of Guangzhou megacity in Pearl River Delta in South China, using an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) in November 2010 during 2010 Guangzhou Asian Games. The mean PM₁ mass concentration measured was 47.9±17.0 μg·m^-3 during the campaign, with organic aerosol (OA) and sulfate being the two dominant species, accounting for 36.3% and 20.9% of the total mass, respectively, followed by black carbon (17.1%, measured by an aethalometer), nitrate (12.9%), ammonium (9.6%) and chloride (3.1%). The average size distributions of the species (except black carbon) were dominated by an accumulation mode peaking at ~550 nm. Calculations based on high-resolution organic mass spectrum showed that, C, H, O and N on average contributed 58.1%, 7.3%, 30.7%, and 3.9% to the total organic mass, respectively. The average ratio of organic mass over organic carbon mass (OM/OC) was 1.73±0.08. Four components of OA were identified by the Positive Matrix Factorization (PMF) analysis, including a hydrocarbon-like (HOA), a biomass burning (BBOA) and two oxygenated (SV-OOA and LV-OOA) organic aerosol components, which on average accounted for 18.0%, 14.3%, 28.8% and 38.9% of the total organic mass, respectively.     

Inertial oscillations and particle flux interactions in a marine protected area in Gulf of Naples

The area between the island of Capri and Punta Campanella was investigated from June to November 2003. Punta Campanella separates the Gulf of Naples from the Gulf of Salerno and has been declared a marine protected area in 1997. The study area has a particular interesting topography, due to the presence of a sill situated at a depth of 80 m. Samples were collected by instruments carried on a mooring array (sediment trap, current meters, and temperature sensors) and by CTD cast (along transects perpendicular to the coast). We observed most important fluctuations in the temperature spectra (corresponding to the inertial oscillations period), in August. The total mass flux was 585.67 mg m^-2 d^-1 in the summer, while in early autumn the flux exhibited values one order of magnitude higher than in summer (1539.97 mg m^-2 d^-1). The main focus of this study was to understand the influence of the internal waves on the particle flux. During the autumn, in the particle flux collected, there is a strong resuspension component, and the observation that the enhanced inertial oscillations and increased sedimentation occur at the same time allows us to presume that the inertial oscillations could be one of the reasons for the resuspension process during the sampling period.