黄淮平原农田土壤中多环芳烃的分布、风险及来源

对227个黄淮平原农田表层土壤样品中16种多环芳烃(PAHs)含量进行了调查,并对其致癌风险和来源等进行了分析.结果表明,有15种PAHs被普遍检出,各单体检出率在23.3%~100%之间(苊烯未检出).土壤中PAHs总量(∑PAHs15)为33.44~1246μg/kg,平均值为152.4±166.2μg/kg,且以4环及4环以上PAHs为主,其中16.7%的样品中PAHs含量达到了污染水平(>200μg/kg),与国内外其他地区相比,黄淮平原农田土壤中PAHs含量处于相对较低水平.黄淮平原农田土壤7种致癌性PAHs毒性当量浓度(TEQBap)占总毒性当量浓度的98.27%,其中苯并(a)芘(Bap)潜在致癌风险最大.同分异构体比值法和主成分分析结果表明黄淮平原农田土壤中PAHs的主要来源是汽油、柴油高温燃烧、以及煤和秸秆燃烧.相关性分析表明有机质含量与∑PAHs15及PAHs单体含量具有显著相关性,表明有机质是影响PAHs在土壤中含量、空间分布及归趋的一个重要因素.     

垃圾填埋场渗滤液溶解性有机质特性及其去除技术综述

垃圾填埋场渗滤液所含物质种类繁多,理化特性复杂,且随填埋时间等条件而变化.本文综合分析了垃圾渗滤液溶解性有机质的组成特征、结构特征及随年代变化特征.针对垃圾渗滤液难降解有机质的特性而研发的处理技术包括物化法、高级氧化法和微电解法等,并在实际工程中得到应用.随着越来越严格的渗滤液排放要求,溶解性有机质的去除应充分考虑投资的经济、运行的稳定性和可靠性.     

我国四个大气背景点颗粒物浓度及其元素分布特征

选择全国由南至北的4个大气背景站(广东南岭、湖北神农架、山西庞泉沟和吉林长白山),于2013年分4个季度同步采集环境空气颗粒物PM10和PM2.5样品,采用微波消解电感耦合等离子体质谱法测定滤膜样品中60余种元素.结果表明,4个背景点PM2.5日均质量浓度平均值为17μg·m-3,PM10为29μg·m-3,低于《环境空气质量标准》(GB 3095—2012)规定的一级浓度限值.第一季度的PM10和PM2.5最高,除长白山第三季度高于第四季度之外,其他3个点位均呈现第二季度第四季度第三季度的趋势.PM2.5和PM10二者呈线性正相关,4个季度的PM2.5/PM10比值均小于0.5,第二、第三季度较高,而第一、第四季度较低.PM10和PM2.5中元素随季节变化不大,PM2.5含量在同一水平上低于PM10.Na、Mg、Al、S、K、Ca、Fe、Zn质量浓度在0.1—10μg·m-3之间,P、Ti、Mn、Ni、Cu、Ba、Pb质量浓度在10—100 ng·m-3之间,Cd、Co、Ge、Ga、Zr、Sr、V等质量浓度在0.01—10 ng·m-3之间.K、Al、Ca含量大于10%,S、Mg、Na、Fe、Zn、Pb、Mn含量大于1%,Cu、P、Ba、Ti量介于0.5%—1%,其他痕量元素含量所占比例小于0.5%.     

南淝河不同排口表层沉积物DOM光谱特征

在南淝河15个排口采集了表层沉积物样品,在测定了其中溶解性有机碳(SDOC)含量的同时,采用紫外-可见吸收光谱和三维荧光光谱分析方法,并结合PARAFAC模型对沉积物中溶解性有机质(DOM)的荧光组分和来源进行了解析.结果表明:南淝河不同排口表层沉积物SDOC的含量在0.28~0.95g/kg之间,平均为0.63g/kg;老城区采样点沉积物SDOC明显高于其他河段,特别是靠近污水厂尾水排放口沉积物SDOC明显高于其他采样点.南淝河沉积物紫外-可见光吸收系数aλ可以很好表征沉积物DOM含量相对大小,而光谱斜率S275-295和光谱斜率比SR反映出各采样点沉积物DOM中自生源组分的差异;利用PARAFAC模型解析出DOM四种荧光组分,其中较老的自生源腐殖质C2和新近类蛋白C4所占比例高.南淝河不同排口沉积物DOM自生源组分比例存在显著差异,其中老城区排口沉积物DOM以自生源组分为主,而上游排口沉积物DOM陆源组分所占比例较高,雨污排口和污水厂尾水排口虽以自生源为主,但陆源的贡献不可忽略.结果表明,光谱分析方法能够有效表征城市河道不同排口污染源强.     

A comparative study of particle size distribution from two oxygenated fuels and diesel fuel

Oxygenated fuels are known to reduce particulate matter (PM) emissions from diesel engines. In this study, 100% soy methyl ester (SME) biodiesel fuel (B100) and a blend of 10% acetal denoted by A-diesel with diesel fuel were tested as oxygenated fuels. Particle size and number distributions from a diesel engine fueled with oxygenated fuels and base diesel fuel were measured using an Electrical Low Pressure Impactor (ELPI). Measurements were made at ten steady-state operational modes of various loads at two engine speeds. It was found that the geometric mean diameters of particles from SME and Adiesel were lower than that from base diesel fuel. Compared to diesel fuel, SME emitted more ultra-fine particles at rated speed while emitting less ultra-fine particles at maximum speed. Ultra-fine particle number concentrations of A-diesel were much higher than those of base diesel fuel at most test modes.     

Photodegradation of chromophoric dissolved organic matters in the water of Lake Dianchi,China

Water samples were taken from Lake Dianchi, on the Yungui Plateau of southwest China, and experiments were conducted to simulate the photochemical degradation characteristic of chromophoric dissolved organic matter (CDOM) in the lake water. Three groups of experiments under different light conditions: ultraviolet (UV) light, visible light, and dark, were done and variations of fluorescence properties, UV absorbance, and dissolved organic carbon (DOC) concentrations during the experiments were analyzed to study the photodegradation process of CDOM with time. The result showed that light irradiation led to significant photochemical degradation of CDOM, resulting in changes in florescent properties, absorbance losses, decreases in aromaticity and average molecular weight, as well as decline in DOC concentration in the water. It was also observed that UV irradiation had greater effect than visible light did. However, various fluorophores had different sensitivities to the same irradiation condition, that is, protein-like fluorophore at the low excitation wavelengths is more sensitive to UV irradiation than the other fluorophores, and is more readily to undergo photo-degradation. In addition, visible light irradiation did not have significant impact on DOC in the water, with DOC concentration decrease by 5.57% –59.9% during the experiment time. These results may provide new knowledge on the environment behavior of CDOM in the water of Lake Dianchi.     

Dibutyl phthalate adsorption characteristics using three common substrates in aqueous solutions

• DBP adsorption was tested using three kinds of substrates in constructed wetlands. • The DBP adsorption capacity followed the order: steel slag>gravel>shell sand. • High temperatures increased the DBP adsorption capacity in the substrates. • DOM consistently inhibited the DBP adsorption onto steel slag and gravel. In recent years, the presence and adverse impacts of phthalic acid esters in aquatic environments have gained increasing attention. This work investigated the adsorption behavior of a typical phthalic acid ester, dibutyl phthalate (DBP), onto steel slag, gravel, and shell sand (substrates commonly used in constructed wetlands). The influence of dissolved organic matter (DOM) on DBP adsorption was investigated using humic acid as a proxy for DOM. The results demonstrated that the adsorption of DBP to three substrates reached equilibrium within 96 h, and the adsorption kinetics were well fitted by a pseudo-second-order model. The DBP adsorption isotherms were best fitted by the Langmuir adsorption model. The DBP adsorption capacity decreased in the order of steel slag>gravel>shell sand, with values of 656 mg/kg, 598 mg/kg, and 6.62 mg/kg at 25°C, respectively. DBP adsorbed to the surface of all substrates in a monolayer via an endothermic process. The DBP adsorption capacities of steel slag and gravel decreased as the DOM content increased. The DBP adsorption mechanisms to steel slag and gravel mainly involved the surface coordination of DBP with –OH or –COOH groups and electrostatic interactions. The results of this work suggest that steel slag and gravel may be ideal substrates for use in constructed wetlands to treat wastewater polluted with DBP.     

Diphenylarsinic acid sorption mechanisms in soils using batch experiments and EXAFS spectroscopy

• DPAA sorption data was found to fit the Freundlich equation. • K_f was significantly positive correlated with oxalate-extractable Fe₂O₃. • Ligand exchange was the main mechanism for DPAA sorption on soils. • Bidentate binuclear and monodentate mononuclear DPAA bonds were identified. Diphenylarsinic acid (DPAA) is a phenyl arsenic compound derived from chemical warfare weapons. Macroscopic and microscopic work on DPAA sorption will provide useful information in predicting the partitioning and mobility of DPAA in the soil-water environment. Here, batch experiments and extended X-ray absorption fine structure (EXAFS) spectroscopy were used to investigate the sorption mechanisms of DPAA. The DPAA sorption data from 11 soil types was found to fit the Freundlich equation, and the sorption capacity, K_f, was significantly and positively correlated with oxalate-extractable Fe₂O₃. The K_f values of eight of the 11 untreated soils (1.51–113.04) significantly decreased upon removal of amorphous metal (hydr)oxides (0.51–13.37). When both amorphous and crystalline metal (hydr)oxides were removed from the untreated soils, the K_f values either decreased or slightly increased (0.65–3.09). Subsequent removal of soil organic matter from these amorphous and crystalline metal (hydr)oxide-depleted samples led to further decreases in K_f to 0.02–1.38, with only one exception (Sulfic Aquic-Orthic Halosols). These findings strongly suggest that ligand exchange reactions with amorphous metal (hydr)oxides contribute most to DPAA sorption on soils. EXAFS data provide further evidence that DPAA primarily formed bidentate binuclear (²C) and monodentate mononuclear (¹V) coring-sharing complexes with As-Fe distances of 3.34 and 3.66 Å, respectively, on Fe (hydr)oxides. Comparison of these results with earlier studies suggests that ²C and ¹V complexes of DPAA may be favored under low and high surface coverages, respectively, with the formation of ¹V bonds possibly conserving the sorption sites or decreasing the steric hindrance derived from phenyl substituents.     

雌二醇在土壤/沉积物中的吸附特征及猪粪DOM对吸附的影响

天然类固醇雌激素如17β-雌二醇(E2)在极低质量浓度下(ng.L-1)即可干扰水生生物的生殖功能.为准确预测E2向水体迁移,通过摇床实验研究了E2在中国北方3种不同土壤/沉积物表面的吸附特征,同时探讨了猪粪及其堆肥可溶态有机质(DOM)对E2吸附的影响.结果发现,E2在土壤/沉积物表面吸附符合Freundlich等温吸附方程(R2>0.76),E2在河流沉积物、潮土、黑土皆表现为非线性,其中黑土吸附的非线性最强(n=0.74);吸附系数Kf介于26.2～57.5,并与有机质含量呈显著正相关(P<0.05).猪粪及其堆肥DOM显著抑制E2在土壤/沉积物表面的吸附,其中堆肥DOM的影响尤为显著.研究认为,有机质是土壤/沉积物中吸附E2的主要组分,共存猪粪DOM在较低浓度下可提高E2迁移性,增加E2向地表和地下水的迁移风险.