Effect of NOx and SO2 on the photooxidation of methylglyoxal: Implications in secondary aerosol formation

Methylglyoxal(CH_3COCHO,MG),which is one of the most abundant α-dicarbonyl compounds in the atmosphere,has been reported as a major source of secondary organic aerosol(SOA).In this work,the reaction of MG with hydroxyl radicals was studied in a 500 L smog chamber at(293±3) K,atmospheric pressure,(18±2)% relative humidity,and under different NOx and SO_2.Particle size distribution was measured by using a scanning mobility particle sizer(SMPS) and the results showed that the addition of SO_2 can promote SOA formation,while different NOx concentrations have different influences on SOA production.High NOx suppressed the SOA formation,whereas the particle mass concentration,particle number concentration and particle geometric mean diameter increased with the increasing NOx concentration at low NOx concentration in the presence of SO_2.In addition,the products of the OH-initiated oxidation of MG and the functional groups of the particle phase in the MG/OH/SO_2 and MG/OH/NOx/SO_2 reaction systems were detected by gas chromatography mass spectrometry(GC-MS) and attenuated total reflection fourier transformed infrared spectroscopy(ATR-FTIR) analysis.Two products,glyoxylic acid and oxalic acid,were detected by GC-MS.The mechanism of the reaction of MG and OH radicals that follows two main pathways,H atom abstraction and hydration,is proposed.Evidence is provided for the formation of organic nitrates and organic sulfate in particle phase from IR spectra.Incorporation of NOx and SO_2 influence suggested that SOA formation from anthropogenic hydrocarbons may be more efficient in polluted environment.     

Plasmonic silver/silver oxide nanoparticles anchored bismuth vanadate as a novel visible-light ternary photocatalyst for degrading pharmaceutical micropollutants

The degradation of pharmaceutical micropollutants is an intensifying environmental problem and synthesis of efficient photocatalysts for this purpose is one of the foremost challenges worldwide. Therefore, this study was conducted to develop novel plasmonic Ag/Ag₂O/BiVO₄ nanocomposite photocatalysts by simple precipitation and thermal decomposition methods, which could exhibit higher photocatalytic activity for mineralized pharmaceutical micropollutants. Among the different treatments, the best performance was observed for the Ag/Ag₂O/BiVO₄ nanocomposites (5 wt.%; 10 min's visible light irradiation) which exhibited 6.57 times higher photodegradation rate than the pure BiVO₄. Further, the effects of different influencing factors on the photodegradation system of tetracycline hydrochloride (TC-HCl) were investigated and the feasibility for its practical application was explored through the specific light sources, water source and cycle experiments. The mechanistic study demonstrated that the photogenerated holes (h⁺), superoxide radicals (?O₂^?) and hydroxyl radicals (?OH) participated in TC-HCl removal process, which is different from the pure BiVO₄ reaction system. Hence, the present work can provide a new approach for the formation of novel plasmonic photocatalysts with high photoactivity and can act as effective practical application for environmental remediation.     

Algal toxicity induced by effluents from textile-dyeing wastewater treatment plants

This research aimed to evaluate the alga Scenedesmus obliquus toxicity induced by textiledyeing effluents(TDE).The toxicity indicator of TDE in alga at the physiological(algal growyth),biochemical(chlorophyll-a(Chl-a) synthesis and superoxide dismutase(SOD) activity) and structural(cell membrane integrity) level were investigated.Then we further study the relationship among toxicity indicators at physiological and biochemical level,and supplemented by research on algal biomacromolecules.According to the analysis of various endpoints of the alga,the general sensitivity sequence of toxicity endpoints of Scenedesmus obliquus was:SOD activity Chl-a synthesis algal growth.The stimulation rate of SOD activity increased from day 3(57.25%～83.02%) to day 6(57.25%～103.81%),and then decreased on day 15(-4.23%～-32.96%),which indicated that the antioxidant balance system of the algal cells was destroyed.The rate of Chl-a synthesis inhibition increased gradually,reaching19.70%～79.39% on day 15,while the rate of growth inhibition increased from day 3(-12.90%～10.16%) to day 15(-21.27%～72.46%).Moreover,the algal growth inhibition rate was positively correlated with the inhibition rate of SOD activity or Chl-a synthesis,with the correlation coefficients were 0.6713 and 0.5217,respectively.Algal cells would be stimulating to produce excessive reactive oxygen species,which would cause peroxidation in the cells,thereby destroying chloroplasts,inhibiting chlorophyll synthesis and reducing photosynthesis.With increasing exposure time,irreversible damage to algae can lead to death.This study is expected to enhance our understanding of the ecological risks through algal tests caused by TDE.     

UV/H2O2 oxidation of tri(2-chloroethyl) phosphate: Intermediate products, degradation pathway and toxicity evaluation

Tri(2-chloroethyl) phosphate (TCEP) with the initial concentration of 5 mg/L was degraded by UV/H₂O₂ oxidation process. The removal rate of TCEP in the UV/H₂O₂ system was 89.1% with the production of Cl^? and PO₄^3? of 0.23 and 0.64 mg/L. The removal rate of total organic carbon of the reaction was 48.8% and the pH reached 3.3 after the reaction. The oxidative degradation process of TCEP in the UV/H₂O₂ system obeyed the first order kinetic reaction with the apparent rate constant of 0.0025 min^?1 (R²=0.9788). The intermediate products were isolated and identified by gas chromatography-mass spectrometer. The addition reaction of HO? and H₂O and the oxidation reaction with H₂O₂ were found during the degradation pathway of 5 mg/L TCEP in the UV/H₂O₂ system. For the first time, environment risk was estimated via the “ecological structure activity relationships” program and acute and chronic toxicity changes of intermediate products were pointed out. The luminescence inhibition rate of photobacterium was used to evaluate the acute toxicity of intermediate products. The results showed that the toxicity of the intermediate products increased with the increase of reaction time, which may be due to the production of chlorine compounds. Some measures should be introduced to the UV/H₂O₂ system to remove the highly toxic Cl-containing compounds, such as a nanofiltration or reverse osmosis unit.     

Chemical characteristics of road dust PM2.5 fraction in oasis cities at the margin of Tarim Basin

In order to understand the compositions characteristics of particulate matter with aerodynamic diameter less than 2.5 μm (PM_2.5) fraction in road dust (RD_2.5) of oasis cities on the edge of Tarim Basin, 30 road dust (RD) samples were collected in Kashi, Cele, and Yutian in the spring, 2018, and RD_2.5 was collected using the resuspension approach. Eight water-soluble ions, 39 trace elements and 8 fractions of carbon-containing species in PM_2.5 were analyzed. Ca²⁺ and Ca were the most abundant ions and elements in RD_2.5 (7.1% and 9.5%). Cl^- in RD_2.5 was affected not only by attributed to saline-alkali soils in oasis cities of the Tarim Basin and dust from Taklimakan Desert but also by human activities. Moreover, the organic carbon/elemental carbon (OC/EC) ratio indicated that carbon components in RD_2.5 in Cele town mainly come from fossil fuel combustion, while those in Yutian and Kashi mainly come from biomass combustion. It is noteworthy that high Ca in RD_2.5 was seriously affected by anthropogenic emissions, and high Na and K contents in RD_2.5 could be derived from soil and desert dust. It was estimated that Cd, Tl, Sn and Cr were emitted from anthropogenic emissions using the enrichment factor. The coefficients of divergence (COD) result indicated that the influence of local emission on road dust emission is greater than that of long-distance transmission. This study is the first time to comprehensively analyze the chemical characteristics of road dust in oasis cities, and the results provides the sources of road dust at the margin of Tarim Basin.     

武当山夏季颗粒物数浓度谱分布特征及气团来源影响研究

为研究大气边界层中上层大气颗粒物的数浓度谱分布特征及气团来源的影响,于2018年6月利用3080型SMPS粒径谱仪对武当山14.6~660 nm颗粒物数浓度谱进行观测,分析和探讨了其数浓度谱分布及日变化特征,并结合后向轨迹、潜在源贡献因子法（PSCF）与浓度权重轨迹分析法（CWT）探讨对武当山颗粒物数浓度影响较大的外源输送路径和贡献源区.结果表明:①武当山大气颗粒物主要以爱根模态为主,平均数浓度为2 500个/cm3,积聚模态、核膜态平均数浓度分别为2 265、359个/cm3,3种模态数浓度分别占总数浓度的48.79%、44.21%、7.01%.②在新粒子生成日,核膜态数浓度于10:00开始上升,11:00—17:00的核膜态数浓度相对较高,约2 000个/cm3.新粒子生成日ρ（SO₂）与ρ（O₃）的日变化趋势均与核模态数浓度较为相似,表明SO₂和O₃参与光化学反应后的产物（硫酸及有机物）有利于新粒子的生成与增长.新粒子生成日风速、温度均大于非新粒子生成日,但相对湿度较低.③在东部及局地气团影响下大气颗粒物主要以积聚模态为主,数浓度分别为2 311和2 596个/cm3;核模态、爱根模态数浓度在受西北气团影响时最大,数浓度分别为806和3 078个/cm3.④潜在源区分析表明,影响武当山积聚模态数浓度的主要源区为十堰市本地及襄阳市,二者贡献值在840个/cm3以上.研究显示,武当山颗粒物主要以爱根模态为主,颗粒物数浓度日变化主要受大气边界层发展及山谷风的影响,较高的ρ（SO₂）与ρ（O₃）以及高温、低湿及较大的风速均有利于新粒子的生成,周边城市的区域性传输对武当山颗粒物的影响较大.      

闽江河口养虾塘养殖期和非养殖期CO2通量变化特征

为揭示河口区陆基养虾塘从养殖期到非养殖期一年间的CO₂通量变化,以福建省闽江河口鳝鱼滩陆基养虾塘为研究对象,于2016年5月-2017年3月采用悬浮箱/静态箱-气相色谱法对养虾塘养殖期水-大气界面和非养殖期沉积物-大气界面白天CO₂垂直通量进行原位观测.结果表明:①养虾塘在整个研究期间CO₂通量变化范围为-62.87~162.81 mg/（m2·h）,平均值为（42.66±18.12）mg/（m2·h）,总体上表现为大气CO₂的释放源,且呈非养殖期CO₂通量平均值[（78.51±16.61）mg/（m2·h）]显著高于养殖期[（17.98±18.26）mg/（m2·h）]的特征.②养殖期间,养虾塘CO₂通量呈"排放-吸收"交替变化的特征,而非养殖期养虾塘一直是大气CO₂的净排放源.③养虾塘养殖期CO₂通量时间变化特征主要受到ρ（DOC）（DOC为总溶解有机碳）、ρ（SO₄2-）、ρ（Cl-）、盐度、pH、ρ（Chla）（Chla为叶绿素a）的影响,其中,pH和ρ（SO₄2-）是其主要影响因子,而ρ（TDN）（TDN为总溶解氮）、ρ（TDP）（TDP为总溶解磷）、ρ（SO₄2-）对非养殖期CO₂通量时间变化影响较大.研究显示,滨海陆基养殖塘是大气CO₂的重要来源,其排放通量多低于河流、水库等水生生态系统,但高于湖泊生态系统;养殖塘CO₂通量受人为影响明显,其较高的变异性与养殖生物、饲料投放以及浮游藻类有关.      

达里诺尔湖水体DOM荧光特征及其来源解析

达里诺尔湖（简称“达里湖”）是内蒙古自治区高原地区重要的生态屏障,探究达里湖水质状况及污染来源,对加强流域水环境治理、改善水环境质量具有十分重要的意义.于2018年9月及2019年6月对湖水进行采样,并通过三维荧光光谱结合PARAFAC（平行因子分析）模型,探究达里湖水体DOM（溶解性有机质）来源及其与水质的关系.结果表明:①达里湖水体中pH较高,ρ（DOC）（DOC为溶解性有机碳）、ρ（NH₄+-N）、ρ（TP）相对较高,均超过GB 3838—2002《地表水环境质量标准》Ⅴ类水质标准限值.②水体中DOM含4种荧光组分.夏季水体DOM主要分布于河流入湖口附近,其中,类腐殖质荧光组分（紫外区类富里酸和可见区类富里酸）占总组分的62.93%,类蛋白类荧光组分（类色氨酸和类酪氨酸）占总组分的36.07%;秋季水体DOM主要分布于东南侧,其中,类腐殖质荧光组分占总组分的40.52%,类蛋白类荧光组分占总组分的59.48%.③达里湖采样点荧光参数表明,达里湖DOM自生源特征较强,腐殖化程度较低.类腐殖质荧光组分与ρ（DOC）、ρ（Chla）均呈正相关,类色氨酸荧光组分与pH呈正相关,类络氨酸与ρ（DTN）、ρ（NH4+-N）、ρ（DTP）均呈正相关.研究显示,达里湖DOM具有陆源与生物源双重特性,DOM的形成与微生物、细菌、浮游生物的生命活动密切相关.      

洱海北部入湖河流水质特征及其对北部湖区的影响

基于2016—2018年罗时江、弥苴河、永安江及洱海北部湖区监测数据分析,探讨洱海北部入湖河流污染变化特征及对北部湖区的影响。结果表明:1）"北三江"监测断面总磷、COD、氨氮浓度整体稳定在GB 3838—2002《地表水环境质量标准》Ⅱ—Ⅲ类标准限值内,年内污染物浓度变化表现出典型的农业面源污染特征,且受流域内产业模式等的综合影响;2）研究期间,河流首要污染物为TN,旱季次要污染物为COD,雨季为TP。雨季入湖负荷高于旱季,弥苴河污染负荷大于罗时江、永安江。"北三江"入湖TN和TP污染负荷分别占洱海允许负荷的50.1%和59.7%;3）入湖河流的磷元素输入是洱海北部湖区磷污染的重要来源。北部湖区污染物浓度对氮、磷入湖污染负荷相关性次月强于当月,响应存在延迟。筛选环境友好型种植模式,控制"北三江"氮磷入湖负荷,有利于保护洱海水环境。     

应用改良型水质综合指数法评价饮用水水质

应用1套改良型水质综合指数法对3种不同类型的饮用水水质进行评价。将选取的26项检测指标按照卫生学意义分为5大类,并对各分类指标赋权。选用内梅罗法和最差因子判别法与五色等级分级法结合对2017年4—8月的3种类型饮用水进行水质评价。除7月和8月的管网水水质为2级（水质综合指数>0.5,蓝色）以外,其余月份的出水水质均达到1级（绿色）评价标准。不同类型饮用水中对水质综合指数影响最大的水质分类指标均是有机污染指标。2种不同类型的净水机出水水质均优于管网末梢水,但需注意个别指标的污染。