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.     

基于TMVOC的地下水位波动带苯系物迁移转化模拟

为探究水位波动情况下苯系物的迁移转化规律,提高石油污染场地地下水污染治理精度,以西北某傍河石化场地为研究对象,基于TMVOC模型对特征污染物苯系物开展泄漏模拟,通过情景模拟比较水位波动对苯系物迁移转化的影响,并从污染分布、相间转化等方面,解析地下水位稳定和波动状态下苯系物迁移转化过程差异.结果表明:①TMVOC模型较好地模拟了水位波动状态下苯系物迁移转化过程.②相较于水位稳定状态下,水位波动作用下苯系物污染深度增加0.5 m,污染面积增加25%,总质量增加12 kg.③水位稳定和波动状态下苯系物"气-液-NAPL（Non-Aqueous Phase Liquids）相"占比分别为0.17%、2.03%、97.8%和0.04%、3.69%、96.27%.④NAPL相苯系物饱和度分布与苯系物质量分布呈正相关,水位波动造成NAPL相初始饱和度降低,且初始水位面以下NAPL相饱和度升高.⑤对于苯而言,水位波动状态下非饱和带中苯在液相中的质量是水位稳定状态下的1.11倍,饱和带为10.15倍.研究显示,水位波动显著地影响了苯系物的迁移转化过程,促进了苯系物的溶解,并使更多的苯系物残留在地下介质中.      

长沙市近郊莲花镇土壤重金属生态风险评价

选择长沙市近郊的莲花镇作为研究对象,采集了镇域范围内54个土壤样品,运用综合的生态风险评价方法对Hg、Cd、As、Pb、Cr 5种土壤重金属元素污染程度及对人体的健康危害程度进行评价。结果表明:1)5种重金属元素的污染程度排序为Cd > Hg > Pb > As > Cr,Cd呈现重度污染;Cd和Pb空间变异显著,其来源受人为干扰程度高。2)5种重金属元素的潜在生态危害排序为Cd > Hg > As > Pb > Cr,Cd和Hg处于强生态危害程度,是研究区域土壤重金属污染的主要因子;研究区域综合潜在生态风险达到强生态危害等级。3)"手-口"摄入是土壤重金属暴露的主要途径,儿童的非致癌暴露剂量远大于成人。5种重金属对儿童和成人所产生的非致癌风险商和非致癌风险指数均<1,不存在非致癌健康风险。4)Cr的致癌风险指数>10-4,具有极高的致癌风险;Cd和As的致癌风险指数为10-6~10-4,处于可以接受的风险范围。Cr、As的污染有不断加剧的趋势,成为影响人体健康的主要因子,应引起关注。     

含油污泥处理技术进展

石油工业生产的特征固体废物——含油污泥,是一种由石油烃、水、固体颗粒物和其他物质（如重金属）组成的固态/半固态复合物,因毒性和易燃性被归入危险废物管理。我国含油污泥年产量高达500万t,其中含有15%~50%的石油烃。含油污泥的处理要兼顾无害化和资源化。基于其组成、性质和危害,介绍了含油污泥的油品资源化分离法（离心、溶剂萃取、热解）和无害化剩余含油残渣处理法（焚烧、固化、生物处理）等国内外常用的处理方法。大体上,含油污泥的处理思路为,首先预处理降低含水率、提高含油率,再经油品分离法回收含油污泥中的石油烃,最后无害化处理剩余含油残渣。讨论了各方法的特点以及国内外研究进展,提出了含油污泥处理技术的发展建议。     

特殊区域地表水环境背景值表征技术方法研究与应用

选取黑龙江省源头水保护区作为研究对象,根据DEM数据对保护区内随机布设的水质监测点控制单元进行划分并提取单元内的相关指标建立监测点背景特性量化模型,基于量化结果提出地表水环境背景值监测方案,建立背景值数据库.选取研究区自然属性指标与空间属性指标,以空间叠置技术与聚类分析方法对研究区地表水进行背景值分区,最终将黑龙江省分为六大地表水水质背景值地理分区,并计算了各分区地表水环境背景值表征范围.表征范围显示：依据现行标准进行水质评价,保护区内水质背景值已超出Ⅱ类水质标准限值.因此,基于水质背景值研究成果提出了考虑背景值影响下的水环境质量评价方法,并将方法应用于研究区,结果表明方法切实可行且优于单因子评价法.研究成果可为区域制定背景值影响下的水环境评价方法提供科学的数据支撑与理论依据.     

CeO2形貌结构对催化湿式空气氧化苯酚性能的影响

采用水热法、沉淀法和溶胶凝胶法制备了3种不同形貌的CeO₂催化材料,并将其用于湿式空气氧化苯酚水溶液过程中,探讨了CeO₂形貌结构对催化湿式氧化苯酚水溶液性能的影响.采用扫描电子显微镜（SEM）、透射电子显微镜（TEM）、X射线衍射（XRD）、程序升温还原（TPR）等手段对CeO₂催化材料进行了表征.结果表明,水热法制备的CeO₂催化材料表现出较好催化性能,主要原因是水热法合成的CeO₂呈现交错的纳米棒状结构,主要暴露（220）晶面,且沿着（220）晶向生长.在反应温度为200℃、空气压力为2MPa、苯酚初始浓度500mg/L的条件下,最终（240min）COD的去除率为95.5%.