Water chemistry controlled aggregation and photo-transformation of silver nanoparticles in environmental waters

The inevitable release of engineered silver nanoparticles (AgNPs) into aquatic environments has drawn great concerns about its environmental toxicity and safety. Although aggregation and transformation play crucial roles in the transport and toxicity of AgNPs, how the water chemistry of environmental waters influences the aggregation and transformation of engineered AgNPs is still not well understood. In this study, the aggregation of polyvinylpyrrolidone (PVP) coated AgNPs was investigated in eight typical environmental water samples (with different ionic strengths, hardness, and dissolved organic matter (DOM) concentrations) by using UV–visible spectroscopy and dynamic light scattering. Raman spectroscopy was applied to probe the interaction of DOM with the surface of AgNPs. Further, the photo-transformation and morphology changes of AgNPs in environmental waters were studied by UV–visible spectroscopy, inductively coupled plasma mass spectrometry, and transmission electron microscopy. The results suggested that both electrolytes (especially Ca^2 + and Mg^2 +) and DOM in the surface waters are key parameters for AgNP aggregation, and sunlight could accelerate the morphology change, aggregation, and further sedimentation of AgNPs. This water chemistry controlled aggregation and photo-transformation should have significant environmental impacts on the transport and toxicity of AgNPs in the aquatic environments.     

Remarkable promotion effect of trace sulfation on OMS-2 nanorod catalysts for the catalytic combustion of ethanol

OMS-2 nanorod catalysts were synthesized by a hydrothermal redox reaction method using MnSO₄ (OMS-2-SO₄) and Mn(CH₃COO)₂ (OMS-2-AC) as precursors. SO₄^2 −-doped OMS-2-AC catalysts with different SO₄^2 − concentrations were prepared next by adding (NH₄)₂SO₄ solution into OMS-2-AC samples to investigate the effect of the anion SO₄^2 − on the OMS-2-AC catalyst. All catalysts were then tested for the catalytic oxidation of ethanol. The OMS-2-SO₄ catalyst synthesized demonstrated much better activity than OMS-2-AC. The SO₄^2 − doping greatly influenced the activity of the OMS-2-AC catalyst, with a dramatic promotion of activity for suitable concentration of SO₄^2 − (SO₄/catalyst = 0.5% W/W). The samples were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), inductively coupled plasma optical emission spectroscopy (ICP-OES), NH₃-TPD and H₂-TPR techniques. The results showed that the presence of a suitable amount of SO₄^2 − species in the OMS-2-AC catalyst could decrease the Mn–O bond strength and also enhance the lattice oxygen and acid site concentrations, which then effectively promoted the catalytic activity of OMS-2-AC toward ethanol oxidation. Thus it was confirmed that the better catalytic performance of OMS-2-SO₄ compared to OMS-2-AC is due to the presence of some residual SO₄^2 − species in OMS-2-SO₄ samples.     

Enhanced CO2 adsorptive performance of PEI/SBA-15 adsorbent using phosphate ester based surfactants as additives

In this study,a series of polyetherimide/SBA-15: 2-D hexagonal P6 mm,Santa Barbara USA(PEI/SBA-15) adsorbents modified by phosphoric ester based surfactants(including tri(2-ethylhexyl)phosphate(TEP),bis(2-ethylhexyl) phosphate(BEP) and trimethyl phosphonoacetate(TMPA))were prepared for CO_2 adsorption.Experimental results indicated that the addition of TEP and BEP had positive effects on CO_2 adsorption capacity over PEI/SBA-15.In particular,the CO_2 adsorption amount could be improved by around 20% for 45PEI–5TEP/SBA-15 compared to the additive-free adsorbent.This could be attributed to the decrease of CO_2 diffusion resistance in the PEI bulk network due to the interactions between TEP and loaded PEI molecules,which was further confirmed by adsorption kinetics results.In addition,it was also found that the cyclic performance of the TEP-modified adsorbent was better than the surfactant-free one.This could be due to two main reasons,based on the results of in situ DRIFT and TG-DSC tests.First and more importantly,adsorbed CO_2 species could be desorbed more rapidly over TEP-modified adsorbent during the thermal desorption process.Furthermore,the enhanced thermal stability after TEP addition ensured lower degradation of amine groups during adsorption/desorption cycles.     

Oxidation of Cr(III) on birnessite surfaces: The effect of goethite and kaolinite

Oxidation of Cr(III) by manganese oxides may pose a potential threat to environments due to the formation of toxic Cr(VI) species. At present, it was still unclear whether the extent of Cr(III) oxidation and fate of Cr(VI) would be changed when manganese oxides co-exist with other minerals, the case commonly occurring in soils. This study investigated the influence of goethite and kaolinite on Cr(III) oxidation by birnessite under acidic pH condition (pH 3.5) and background electrolyte of 0.01 mol/L NaCl. Goethite was found not to affect Cr(III) oxidation, which was interpreted as the result of overwhelming adsorption of cationic Cr(III) onto the negatively-charged birnessite (point of zero charge (PZC) < 3.0) rather than the positively-charged goethite (PZC = 8.8). However, more Cr(VI) would be retained by the surface with the increase in addition of goethite because of its strong ability on adsorption of Cr(VI) at low pH. Moreover, either Cr(III) oxidation or distribution of the generated Cr(VI) between the solid and solution phases was not affected by kaolinite (PZC < 3.0), indicating its low affinity for Cr species. Reactions occurring in the present mixed systems were suggested, which could be partly representative of those in the soils and further indicates that the mobility and risk of Cr(VI) would be decreased if goethite was present.     

Responses of soil ammonia oxidizers to a short-term severe mercury stress

The responses of soil ammonia-oxidizing archaea(AOA) and ammonia-oxidizing bacteria(AOB) to mercury(Hg) stress were investigated through a short-term incubation experiment.Treated with four different concentrations of Hg(CK,Hg25,Hg50,and Hg100,denoting 0,25,50,and 100 mg Hg/kg dry soil,respectively),samples were harvested after 3,7,and 28 day incubation.Results showed that the soil potential nitrification rate(PNR) was significantly inhibited by Hg stress during the incubation.However,lower abundances of AOA(the highest in CK: 9.20 × 10~7 copies/g dry soil; the lowest in Hg50: 2.68 × 10~7 copies/g dry soil) and AOB(the highest in CK: 2.68 × 10~7 copies/g dry soil; the lowest in Hg50:7.49 × 10~6 copies/g dry soil) were observed only at day 28 of incubation(P 0.05).Moreover,only the community structure of soil AOB obviously shifted under Hg stress as seen through DGGE profiles,which revealed that 2–3 distinct AOB bands emerged in the Hg treatments at day 28.In summary,soil PNR might be a very useful parameter to assess acute Hg stress on soil ecosystems,and the community structure of soil AOB might be a realistic biological indicator for the assessment of heavy metal stress on soil ecosystems in the future.     

珠三角表层沉积物的有机碳及其与卤系阻燃剂的关系

测定了珠江三角洲130个表层沉积物中总有机碳(TOC)和10类卤系阻燃剂(HFRs)的含量,并探讨了TOC与HFRs之间的关系.结果表明:珠三角表层沉积物TOC范围为0.16％～5.76％,平均值为1.25％,呈现明显的空间变化.在工业化程度较高的东莞和广州,沉积物中HFRs与TOC有显著的相关性,而西江和珠江口沉积物中HFRs与TOC的相关性较差,可能与珠江三角洲水动力过程、电子垃圾拆解活动和HFRs不同的来源有关.     

桂林市公共场所空气污染的检测与分析

采用甲醛检测仪、有机气体检测仪等测试分析了桂林市宾馆、商场、候车室、家具城、文化娱乐场等公共场所的甲醛和TVOC浓度。结果显示:候车室和文化娱乐场所的甲醛、TVOC合格率均为100%;宾馆、商场、家具城的TVOC合格率分别为98.7%、98.9%、95.0%,甲醛合格率分别为78.8%、91.1%、85.0%;皮革制品、家具板材等为主要的甲醛和TVOC污染源。     

鄱阳湖典型湿地沉水植物的分布格局及其水环境影响因子

沉水植物是湖泊湿地生态系统中关键组分,调查研究沉水植物分布格局及其水环境影响因子,对于沉水植被的恢复与重建具有重要的指导意义。2013年5月初期分别对鄱阳湖典型湿地区域中有沉水植物的25个样地进行群落结构调查,采用系统取样方法对沉水植物进行调查采样并监测水环境因子,在野外调查的基础上运用GIS软件制作鄱阳湖典型区域沉水植物的生物量分布图,并采用主成分分析(PCA)和典范对应分析(CCA)方法分析其主要影响因子。结果表明:鄱阳湖湿地沉水植物以苦草(Vallisneria natans)为广布种,其中蚌湖及白沙湖以黑藻(Hydrilla verticillata)为优势种,白沙洲及乐安河龙口段以苦草为优势种,伴生种主要有金鱼藻(Ceratophyllum demersum)、马来眼子菜(Potamogeton malaianus)、菹草(P.crispus)、小茨藻(Najas minor)、大茨藻(N.marina)、刺苦草(V.spinulosa)和水车前(Ottelia alismoides)等。采用双向指示种分析法将研究区沉水植物分为6个群落;5月初大部分沉水植物尚处于生长季初期,生物量相对较低,仅菹草的生物量较大;沉水植物与浮叶植物共存现象明显。主成分分析(PCA)结果显示,第一主成分中水深、总磷和溶解氧等因子的系数值较大,第二主成分中pH值、化学需氧量和水体透明度等因子的系数值较大,是影响沉水植物分布的关键因子;典范对应分析(CCA)结果显示,水深、总磷和总氮对苦草和黑藻的影响显著,水体透明度是马来眼子菜的主要影响因子。     

高效液相色谱-电感耦合等离子体质谱联用测定生物样品中的有机汞

建立了酸提取-高效液相色谱-电感耦合等离子体质谱联用技术(HPLC-ICP-MS)测定生物样品中甲基汞、乙基汞、苯基汞等3种有机汞的分析方法。鱼肉和贝类样品经盐酸消解,苯萃取,硫代硫酸钠溶液反萃取后,采用醋酸铵/L-半胱氨酸缓冲盐及甲醇体系组成的流动相按一定比例进行梯度洗脱,经前处理的生物样品在液相色谱中经C18柱分离后,进入电感耦合等离子体质谱检测其甲基汞、乙基汞和苯基汞的浓度。3种有机汞化合物均在0.50~50.0μg/L范围内呈现良好的线性关系,线性相关系数(r)均大于0.9998。方法检出限为0.010~0.038mg/kg;3种有机汞样品加标的RSD均小于12.2%;两个水平的加标回收率在50.8~129%。     

混凝-超滤处理径流雨水效果——以华南地区为例

采用超滤膜(UF)为核心,以混凝作为预处理措施,对混凝-超滤工艺处理径流雨水的特性和膜通量变化与污染现象进行了研究,并对聚合硫酸铁(PFS)单独混凝、UF、PFS-UF组合工艺进行了对比;在优化混凝基础上,考察了混凝-UF对常规水质指标及总磷、生物可同化有机碳(AOC)、可生物降解溶解性有机碳(BDOC)等生物稳定性指标的去除效果.结果表明,混凝可有效去除TOC、UV254和总磷,混凝剂投加量与污染物去除近似呈线性关系.各混凝剂除浊效能均良好.综合考虑混凝处理效率与经济性,实验采用混凝方案为10 mg·L-1的PFS.PFS、UF、PFS-UF工艺除浊率均在95%以上,PFS和UF对TOC和UV254的去除较为接近,采用PFS-UF可提高去除率13%—15%;PFS-UF处理后雨水的AOC、BDOC分别降低至61.8μg·L-1、0.19 mg·L-1,残余总磷可降至3.8μg·L-1,雨水生物稳定性明显提高.PFS、UF和PFS-UF对颗粒物的去除率分别达80.5%、99.6%和99.9%.膜通量的变化和SEM图分析表明,混凝在一定程度上减轻了UF膜污染;形成的凝胶层具有一定整体强度,水力清洗时易于清除,膜通量恢复较好;但同时凝胶层的产生也增大了透膜阻力,PFS-UF工艺的周期内膜通量衰减有增加的趋势.