Ca_5(AsO_4)_3OH的溶解度与稳定性研究

通过在不同pH值,温度等条件下Ca5(AsO4)3OH的溶解,确定其稳定存在的pH值范围,得出它的溶度积和生成的自由能(ΔG0f)。结果表明,Ca5(AsO4)3OH在水中的溶解度和稳定范围与pH和温度有关,在酸性条件下(初始pH=2)它的溶解度较大,而且在水中的溶解度随着温度的升高而降低。利用PHREEQC程序计算确定Ca5(AsO4)3OH的溶度积为10-40.86,生成自由能ΔG0f为-5 063.53 kJ/mol。利用JADE5软件计算得到其晶格参数a=b=9.696,c=6.967和晶胞体积为567.304 3。     

Assessment of pesticide contamination in Akkar groundwater,northern Lebanon

According to its high production and value, Akkar is considered as the second agricultural region in Lebanon. Groundwater constitutes the principal source of water in Akkar including drinking water of local inhabitants in Akkar. As such, the contamination of groundwater by organic pollutants can impact directly the population health. In this study, we evaluated the contamination status of groundwater in this region. Three classes of pesticides including 19 organochlorine (OC) pesticides, 8 organophosphorus (OP) pesticides, and 6 organonitrogen (ON) pesticides were monitored in 15 groundwater samples collected from different villages on the Akkar plain. Samples were extracted by using solid phase extraction (SPE) and analyzed by gas chromatography coupled with mass spectrometry (GC-MS). The results showed high contamination of Akkar groundwater by OCs with levels that can reach 58.9 μg/L. They were detected in the majority of the sample and represent 95–100% of ∑pesticides. Our results showed the recent use of these molecules with an average level of 0.3 and 0.39 μg/L for ∑HCHs and DDTs, respectively. Their concentrations were higher than those observed in the same region in 2014 and other regions elsewhere. OPs were also detected at high levels and among them, methylparathion was the predominant OP detected (44.6 μg/L). For ONs, lower levels were measured in all samples with a mean value of 5.6 μg/L. As a conclusion of this work, groundwater on the plain of Akkar was remarkably contaminated by the studied pesticides; indefinitely, more efforts should be taken to manage the pesticide use in this region, assess, and reduce their effects on human health. In the future, the application of organic farming can be a great solution to the groundwater contamination problem.     

Relationships between lichen community composition and concentrations of NO2 and NH3

The relationship between different features of lichen communities in Quercus robur canopies and environmental variables, including concentrations of NO₂ and NH₃ was investigated. NO₂ concentration was the most significant variable, it was positively correlated with the proportion of lichen cover comprising nitrophytes and negatively correlated with total lichen cover. None of the lichen community features were correlated with NH₃ concentrations, which were relatively low across the site. Since nitrophytes and nitrophobes are likely to react in opposite directions to nitrogenous compounds, total lichen cover is not a suitable indicator for these pollutants. It is, therefore, suggested that the proportion of lichen cover comprising nitrophytes may be a suitable simple indicator of air quality, particularly in locations where the pollution climate is dominated by oxides of nitrogen.     

Toxicity of TiO2, ZrO2, Fe,Fe2O3, and Mn2O3 nanoparticles to the yeast, Saccharomyces cerevisiae

The growing application of engineered nanomaterials is leading to an increased occurrence of nanoparticles (NPs) in the environment. Thus, there is a need to better understand their potential impact on the environment. This study evaluated the toxicity of nanosized TiO₂, ZrO₂, Fe⁰, Fe₂O₃, and Mn₂O₃ towards the yeast Saccharomyces cerevisiae based on O₂ consumption and cell membrane integrity. In addition, the state of dispersion of the nanoparticles in the bioassay medium was characterized.     

Assessment of contribution of SO2 and NO2 from different sources in Jamshedpur region, India

Contribution of pollution from different types of sources in Jamshedpur, the steel city of India, has been estimated in winter 1993 using two approaches in order to delineate and prioritize air quality management strategies for the development of region in an environmental friendly manner. The first approach mainly aims at preparation of a comprehensive emission inventory and estimation of spatial distribution of pollution loads in terms of SO₂ and NO₂ from different types of industrial, domestic and vehicular sources in the region. The results indicate that industrial sources account for 77% and 68% of the total emissions of SO₂ and NO₂, respectively, in the region, whereas vehicular emissions contributed to about 28% of the total NO₂ emissions. In the second approach, contribution of these sources to ambient air quality levels to which the people are exposed to, was assessed through air pollution dispersion modelling. Ambient concentration levels of SO₂ and NO₂ have been predicted in winter season using the ISCST3 model. The analysis indicates that emissions from industrial sources are responsible for more than 50% of the total SO₂ and NO₂ concentration levels. Vehicular activities contributed to about 40% of NO₂ pollution and domestic fuel combustion contributed to about 38% of SO₂ pollution. Predicted 24-h concentrations were compared with measured concentrations at 11 ambient air monitoring stations and good agreement was noted between the two values. In-depth zone-wise analysis of the above indicates that for effective air quality management, industrial source emissions should be given highest priority, followed by vehicular and domestic sources in Jamshedpur region.     

Ce-TiO2催化剂在含SO2气氛下的NH3-SCR中毒机理及其Co3O4改性性能

通过对Ce-TiO₂催化剂在含硫气氛下、不同温度的NH₃-SCR活性演变,结合含硫组分的定量分析、原位红外分析,研究了Ce-TiO₂催化剂在不同温度的SO₂中毒机理。结果表明,在180 ℃下,Ce-TiO₂脱硝活性对硫酸铈的生成极为敏感,0.1 mmol·g⁻¹的硫酸铈生成导致脱硝活性从50.7%降至18.5%,随后硫酸铈持续沉积,低温脱硝活性缓慢下降;在240 ℃下,Ce-TiO₂脱硝活性对硫酸铈的生成敏感性较低,脱硝活性随时间缓慢下降,0.18 mmol·g⁻¹的硫酸铈生成导致脱硝活性从100%降至53.8%,随后硫酸铈持续生成。Co改性活性结果表明：在180 ℃时,脱硝活性从50.7%提升至94.2%,且180 ℃和240 ℃抗硫性能均有所提升。进一步的表征测试表明：Co的掺杂能提升Ce-TiO₂催化剂的氧化还原性能,并抑制SO₂在催化剂表面的吸附,提升催化剂的抗硫性能。原位红外测试结果表明：硫酸化后的Ce-Co-TiO₂催化剂仍能维持了E-R、L-H脱硝反应路径的进行,保证了一定的低温脱硝活性。本研究探索了SCR催化剂的中毒机制,可为其改性与活性提升提供参考。     

六氯苯的O3及UV/O3高级氧化降解试验研究

采用O₃、UV/O₃高级氧化法对水中六氯苯（HCB）的降解效果及机理进行了研究，并对结果进行了比较，结果表明，UV本身对HCB的去除率贡献不大，HCB可被O₃、UV/O₃快速降解，即UV＜O₃＜UV/O₃；O₃、UV/O₃作用时，提高体系的初始pH值不利于HCB的降解，在pH＝3，HCB=0.2 mg/L，反应40 min时，HCB的去除可达50%左右，酸性条件下有利于降解反应的进行；无论是O₃单独作用还是UV/O₃联合作用，HCB的降解基本上满足准一级反应动力学规律，如果体系的pH值基本保持恒定，这种规律就更为明显。根据离子色谱(IC)、GC对六氯苯降解中间产物进行了测定，探讨了O₃、UV/O₃降解六氯苯的途径和机理。     

烟气成分对负载V_2O_5-WO_3/TiO_2聚苯硫醚纤维脱除烟气中Hg~0的影响

通过固定床实验系统模拟烟气脱除Hg0的实验,研究了O2、HCl、NO、SO2、H2O和NH3对滤袋常用的聚苯硫醚(PPS)纤维负载V2O5-WO3/TiO2新型催化剂后脱除烟气中Hg0的影响,并分析其影响机理。结果表明,在温度为200℃、高纯N2气氛下,Hg0的脱除率很低,加入4%O2后,脱除率有所增加;0.05‰HCl条件下Hg0的脱除率仅为5%,而0.01‰HCl与4%O2并存的条件下,脱除率明显提高;NO对Hg0的催化氧化促进作用不是很显著;SO2对Hg0氧化具有毒害作用;H2O和NH3可抑制Hg0的脱除,O2的存在可抵消NH3的部分抑制作用。     

Stomatal uptake of O3 in aspen and aspen-birch forests under free-air CO2 and O3 enrichment

Rising atmospheric carbon dioxide (CO₂) may alleviate the toxicological impacts of concurrently rising tropospheric ozone (O₃) during the present century if higher CO₂ is accompanied by lower stomatal conductance (g_s), as assumed by many models. We investigated how elevated concentrations of CO₂ and O₃, alone and in combination, affected the accumulated stomatal flux of O₃ (AFst) by canopies and sun leaves in closed aspen and aspen-birch forests in the free-air CO₂-O₃ enrichment experiment near Rhinelander, Wisconsin. Stomatal conductance for O₃ was derived from sap flux data and AFst was estimated either neglecting or accounting for the potential influence of non-stomatal leaf surface O₃ deposition. Leaf-level AFst (AFst_l) was not reduced by elevated CO₂. Instead, there was a significant CO₂ × O₃ interaction on AFst_l, as a consequence of lower values of g_s in control plots and the combination treatment than in the two single-gas treatments. In addition, aspen leaves had higher AFst_l than birch leaves, and estimates of AFst_l were not very sensitive to non-stomatal leaf surface O₃ deposition. Our results suggest that model projections of large CO₂-induced reductions in g_s alleviating the adverse effect of rising tropospheric O₃ may not be reasonable for northern hardwood forests.     

Influence of the operation conditions on CO2 capture by CaO-derived sorbents prepared from synthetic CaCO3

In this work, a statistical experimental design is performed in order to prepare CaCO₃ materials for use as CaO-based CO₂ sorbent precursors. The influence of different operational parameters such as synthesis temperature (ST), stirring rate (SR) and surfactant percent (SP) on CO₂ capture is studied by applying Response Surface Methodology (RSM). The samples were characterized using different analytical techniques including X-ray diffraction, N₂ adsorption isotherm analysis and Scanning Electron Microscopy–X-ray Energy Dispersive Spectroscopy (SEM-EDX). CO₂ capture capacity was determined by means of a thermogravimetric analyzer which recorded the mass uptake of the samples when these were exposed to a gas stream containing diluted (15%) CO₂. The statistical approach used in this work provides a rapid way of predicting and optimizing the main preparation variables of CaO-derived sorbents for CO₂ sorption. The results obtained clearly indicate that four parameters statistically influence CO₂ uptake: SR, the square of SR, its interaction with SP and the square of SP.     

负载V2O5-WO3/TiO2掺炭纤维脱除烟气中Hg0

通过固定床实验系统研究烟气脱除零价汞的实验,首先研究了滤袋常用的聚苯硫醚（polyphenylene sulfide,PPS）以及活性炭纤维（activated carbon fiber,ACF）在不同温度、不同气体组分下负载V₂O₅-WO₃/TiO₂催化剂,对模拟燃煤烟气中零价汞（Hg⁰）的脱除效果。然后对比研究了活性炭纤维协同滤袋常用纤维负载催化剂后,对模拟燃煤烟气中Hg⁰的脱除性能。结果表明,在汞蒸气入口浓度为50 μg/m³,纯N₂气氛下,当温度为25℃时,两者脱除率均能达到99%,当温度为200℃,负载催化剂的活性炭纤维脱除率在30%左右,PPS纤维仅为10%左右。在200℃情况下,模拟烟气的组分为N₂+O₂时,2种纤维的Hg⁰脱除率提高了10%~20%,当在混合气体中添加0.01‰后,负载催化剂的PPS纤维Hg⁰脱除率能达到80%,活性炭纤维Hg⁰脱除率能达到98%。当温度为200℃,模拟烟气的组分为N₂+O₂+HCl时,不同性能掺炭纤维负载催化剂后Hg⁰脱除率在69%~95%范围之间变化,其中PPS掺炭纤维对Hg⁰脱除效率最高达到95%,因此,负载V₂O₅-WO₃/TiO₂催化剂的PPS掺炭纤维能在高温烟气中保持较高的Hg⁰脱除率。     

g-C3N4/TiO2复合薄膜光催化降解石油采出水中多环芳烃

针对亟待解决的石油开采废水中的多环芳烃(polycyclic aromatic hydrocarbons, PAHs)污染物的生物毒害性问题,利用紫外光辐照g-C₃N₄/TiO₂复合薄膜光催化剂,对取自内蒙某采油现场的采出水水样进行降解处理,研究多组分PAHs污染物共存条件下的不同环数PAHs发生光催化氧化反应的降解规律及降解动力学。采用扫描电子显微镜(scanning electron microscope, SEM)表征光催化剂表面微观形貌,采用固相微萃取法富集和萃取水样中的PAHs,采用气相色谱-质谱联用法(gas chromatography-mass spectrometry, GC-MS)检测分析PAHs含量。经UV/g-C₃N₄/TiO₂光催化反应处理,采出水中不溶的颗粒态萘优先于溶解态萘被降解去除,经60 min后对萘的总去除率可达61.13%。大于4环不溶性高环PAHs,可被优先光催化降解,从而高毒性的PAHs污染物被逐级转化为相对较低生物毒性的苊烯、蒽、菲、萘等,其中苊烯的含量增长最显著。结论石油采出水的外排处理工艺中增加PAHs光催化脱毒工艺具有一定可行性,对于保障原有水厂中的生化工艺段高效率、稳定运行将极具价值。     

Informal e-waste recycling: environmental risk assessment of heavy metal contamination in Mandoli industrial area,Delhi, India

Nowadays, e-waste is a major source of environmental problems and opportunities due to presence of hazardous elements and precious metals. This study was aimed to evaluate the pollution risk of heavy metal contamination by informal recycling of e-waste. Environmental risk assessment was determined using multivariate statistical analysis, index of geoaccumulation, enrichment factor, contamination factor, degree of contamination and pollution load index by analysing heavy metals in surface soils, plants and groundwater samples collected from and around informal recycling workshops in Mandoli industrial area, Delhi, India. Concentrations of heavy metals like As (17.08 mg/kg), Cd (1.29 mg/kg), Cu (115.50 mg/kg), Pb (2,645.31 mg/kg), Se (12.67 mg/kg) and Zn (776.84 mg/kg) were higher in surface soils of e-waste recycling areas compared to those in reference site. Level exceeded the values suggested by the US Environmental Protection Agency (EPA). High accumulations of heavy metals were also observed in the native plant samples (Cynodon dactylon) of e-waste recycling areas. The groundwater samples collected form recycling area had high heavy metal concentrations as compared to permissible limit of Indian Standards and maximum allowable limit of WHO guidelines for drinking water. Multivariate analysis and risk assessment studies based on total metal content explains the clear-cut differences among sampling sites and a strong evidence of heavy metal pollution because of informal recycling of e-waste. This study put forward that prolonged informal recycling of e-waste may accumulate high concentration of heavy metals in surface soils, plants and groundwater, which will be a matter of concern for both environmental and occupational hazards. This warrants an immediate need of remedial measures to reduce the heavy metal contamination of e-waste recycling sites.     

Fe2O3-Cr2O3/TiO2系列催化剂的结构和脱硝性能

研究以纳米TiO2为载体,浸渍负载过渡金属氧化物,以CO为还原剂的脱硝催化剂的脱硝性能。实验中以计算量的Ni(NO3)2和Fe(NO3)3混合溶液浸渍纳米TiO2粉末,室温下搅拌30 min至混合均匀,放入旋转蒸发器中,70℃下至水分蒸干为止;所得粉末在550℃下、空气气氛中焙烧4 h即得所需催化剂。用以上方法分别制备2%Fe2O3-10%Cr2O3/TiO2、4%Fe2O3-8%Cr2O3/TiO2、6%Fe2O3-6%Cr2O3/TiO2、8%Fe2O3-4%Cr2O3/TiO2与10%Fe2O3-2%Cr2O3/TiO2等5种催化剂样品。实验结果表明,制备的催化剂具有较好的结构,分散较为均匀。对于CO+NO反应,Fe2O3-Cr2O3/TiO2系列催化剂具有较好的催化活性,NO的转化率都达到了100%。其中,10%Fe2O3-2%Cr2O3/TiO2样品具有最好的低温活性,H2-TPR结果表明,这是由于10%Fe2O3-2%Cr2O3/TiO2催化剂更易于被CO预还原。     

H2O2协同O3预处理垃圾填埋场后期渗滤液的研究

应用自制微孔扩散式接触反应器,考察了H2O3/O3在不同摩尔比下对垃圾填埋场后期渗滤液的氧化处理效果.结果表明,H2O3/O3的摩尔比对处理效果有明显的影响.在试验范围内,确定H2O3/O3的最佳摩尔比为0.2:1,最佳处理时间为90 min,经过H2O3/O3处理后,垃圾填埋场后期渗滤液的BOD5/COD可从初始的0.17提高到0.36,改善了废水的可生化性,同时渗滤液的色度、浊度、腐殖酸和SS也有较高的去除率.     

聚苯硫醚滤料协同飞灰-CaCO_3配方型吸附剂脱除烟气中Hg~0的实验研究

通过固定床实验系统模拟烟气脱除Hg0的实验,研究了布袋常用的聚苯硫醚(polyphenylene sulfide,PPS)滤料协同飞灰-CaCO3配方型吸附剂对模拟烟气中Hg0的脱除效率,以及不同温度、气体成分对Hg0氧化及吸附的影响,分析了其影响机理。结果表明,在温度为120℃,N2+4%O2的条件下,质量比为3∶1的飞灰-CaCO3配方型吸附剂对Hg0的脱除效率最高,虽低于纯飞灰条件下的28%,但其吸附催化寿命较长;温度越高,Hg0的脱除效率越低,PPS滤料协同飞灰-CaCO3配方型吸附剂对Hg0的吸附主要表现为物理吸附;HCl对脱除Hg0的促进作用较为明显;SO2条件下其附加产物对Hg0的脱除表现出一定的抑制作用;NO对Hg0的脱除具有一定的促进作用,但与HCl相比,其促进效果较弱。     

纳米Bi2O3/TiO2复合光催化剂的制备及性能研究

以光催化效果为评价标准,采用超声波作用下水解法制备Bi₂O₃/TiO₂复合光催化剂,考察了水解条件和Bi₂O₃掺入量等制备条件对复合光催化剂性能的影响。结果表明,与传统制备方法相比,该方法操作简单、快速;当水和乙醇的比例为4∶1时所得样品的光催化活性最好;Bi₂O₃的掺入拓宽了TiO₂对光的吸收范围,提高了TiO₂的光催化活性,掺入量(Bi₂O₃)为0.25%复合光催化剂催化活性最高;复合光催化剂对多种水溶性染料均具有较好的处理效果。     

飞灰对氨法烟气脱硫中硫酸铵结晶的影响机制

燃烧后烟气中飞灰的存在,对氨法烟气脱硫中硫酸铵((NH₄)₂SO₄)结晶的影响至关重要。系统研究了飞灰固体质量浓度、粒径及含碳量对(NH₄)₂SO₄结晶晶形、粒径大小和均匀性的影响,并分析了其影响机制。结果表明,当(NH₄)₂SO₄溶液中飞灰固体质量浓度为1 200 mg·L⁻¹时,(NH₄)₂SO₄晶体的晶形最规则,晶体的平均粒径最大(320 µm),均匀性最高（0.40）;飞灰粒径的增大对 (NH₄)₂SO₄晶体的晶形规则性、平均粒径和均匀性的提高均有一定作用,飞灰中不含碳或含有高于4 %的碳,均有利于(NH₄)₂SO₄晶体的晶形规则性、平均粒径的提高,但均匀性会略有下降。飞灰对(NH₄)₂SO₄结晶的影响机制为：飞灰晶核影响(NH₄)₂SO₄晶核的形成和生长,进而影响(NH₄)₂SO₄晶面生长,从而影响(NH₄)₂SO₄晶体的尺寸和均匀性。本研究可为氨法烟气脱硫中(NH₄)₂SO₄结晶的有效调控提供参考。     

Toxicity of nanoparticulate and bulk ZnO, Al2O3 and TiO2 to the nematode Caenorhabditis elegans

Limited information is available on the environmental behavior and associated potential risk of manufactured oxide nanoparticles (NPs). In this research, toxicity of nanoparticulate and bulk ZnO, Al₂O₃ and TiO₂ were examined to the nematode Caenorhabditis elegans with Escherichia coli as a food source. Parallel experiments with dissolved metal ions from NPs were also conducted. The 24-h median lethal concentration (LC₅₀) and sublethal endpoints were assessed. Both NPs and their bulk counterparts were toxic, inhibiting growth and especially the reproductive capability of the nematode. The 24-h LC₅₀ for ZnO NPs (2.3 mg L⁻¹) and bulk ZnO was not significantly different, but significantly different between Al₂O₃ NPs (82 mg L⁻¹) and bulk Al₂O₃ (153 mg L⁻¹), and between TiO₂ NPs (80 mg L⁻¹) and bulk TiO₂ (136 mg L⁻¹). Oxide solubility influenced the toxicity of ZnO and Al₂O₃ NPs, but nanoparticle-dependent toxicity was indeed observed for the investigated NPs.