Photo-oxidation of biodegraded crude oil and toxicity of the photo-oxidized products

We investigated the physicochemical changes resulting from irradiation by sunlight of biodegraded crude oil. An Arabian light crude oil sample was first subjected to microbial degradation. n-Alkanes and aromatic compounds such as naphthalenes, fluorenes, dibenzothiophenes and phenanthrenes possessing short, alkyl side chain(s) were almost completely degraded, while the contents of the saturated and aromatic fractions were reduced by 70% and 40%, respectively. This biodegraded oil was then suspended in seawater and exposed to sunlight irradiation for several weeks. The most remarkable change caused by the irradiation was a substantial decline in the aromatic fraction with a concomitant increase in the resin and asphaltene fractions. A 13C-nuclear magnetic resonance (NMR) spectroscopic analysis showed that the aromaticity of the biodegraded oil was significantly lower in the irradiated sample. A field desorption-mass spectrometric (FD-MS) analysis showed that sunlight irradiation reduced the average molecular weight of the oil components and formed oxygenated compounds. Consistent with this observation is that the oxygen content in the oil increased as the irradiation was prolonged. The bioavailability of the biodegraded oil was increased by the photo-oxidation: the growth of seawater microbes was minimal when the non-irradiated biodegraded oil was used as the source of carbon and energy; however, growth was significant when irradiated biodegraded oil was used. The concentration of dissolved organic carbon (DOC) increased linearly during the sunlight irradiation of the biodegraded oil, and this increase was matched by an increase in ultraviolet-absorptive materials in the seawater. The photochemically formed, water-soluble fraction (WSF) showed acute toxicity against the halophilic crustacean, Artemia.     

Assessment of crude oil biodegradation in arctic seashore sediments: effects of temperature,salinity, and crude oil concentration

The expected increase in offshore oil exploration and production in the Arctic may lead to crude oil spills along arctic shorelines. To evaluate the potential effectiveness of bioremediation to treat such spills, oil spill bioremediation in arctic sediments was simulated in laboratory microcosms containing beach sediments from Barrow (Alaska), spiked with North Slope Crude, and incubated at varying temperatures and salinities. Biodegradation was measured via respiration rates (CO₂ production); volatilization was quantified by gas chromatography/mass spectrophotometry (GC/MS) analysis of hydrocarbons sorbed to activated carbon, and hydrocarbons remaining in the sediment were quantified by GC/flame ionization detector (FID). Higher temperature leads to increased biodegradation by naturally occurring microorganisms, while the release of volatile organic compounds was similar at both temperatures. Increased salinity had a small positive impact on crude oil removal. At higher crude oil dosages, volatilization increased, however CO₂ production did not. While only a small percentage of crude oil was completely biodegraded, a larger percentage was volatilized within 6–9 weeks.     

Characterizing ammonia emissions from swine farms in eastern North Carolina: part 1--conventional lagoon and spray technology for waste treatment

Ammonia (NH3) fluxes from waste treatment lagoons and barns at two conventional swine farms in eastern North Carolina were measured. The waste treatment lagoon data were analyzed to elucidate the temporal (seasonal and diurnal) variability and to derive regression relationships between NH3 flux and lagoon temperature, pH and ammonium content of the lagoon, and the most relevant meteorological parameters. NH3 fluxes were measured at various sampling locations on the lagoons by a flowthrough dynamic chamber system interfaced to an environmentally controlled mobile laboratory. Two sets of open-path Fourier transform infrared (FTIR) spectrometers were also used to measure NH3 concentrations for estimating NH3 emissions from the animal housing units (barns) at the lagoon and spray technology (LST) sites. Two different types of ventilation systems were used at the two farms. Moore farm used fan ventilation, and Stokes farm used natural ventilation. The early fall and winter season intensive measurement campaigns were conducted during September 9 to October 11, 2002 (lagoon temperature ranged from 21.2 to 33.6 degrees C) and January 6 to February 2, 2003 (lagoon temperature ranged from 1.7 to 12 degrees C), respectively. Significant differences in seasonal NH3 fluxes from the waste treatment lagoons were found at both farms. Typical diurnal variation of NH3 flux with its maximum value in the afternoon was observed during both experimental periods. Exponentially increasing flux with increasing surface lagoon temperature was observed, and a linear regression relationship between logarithm of NH3 flux and lagoon surface temperature (T1) was obtained. Correlations between lagoon NH3 flux and chemical parameters, such as pH, total Kjeldahl nitrogen (TKN), and total ammoniacal nitrogen (TAN) were found to be statistically insignificant or weak. In addition to lagoon surface temperature, the difference (D) between air temperature and the lagoon surface temperature was also found to influence the NH3 flux, especially when D > 0 (i.e., air hotter than lagoon). This hot-air effect is included in the statistical-observational model obtained in this study, which was used further in the companion study (Part II), to compare the emissions from potential environmental superior technologies to evaluate the effectiveness of each technology.     

含氮芳香化合物的厌氧生物降解研究回顾

回顾了硝基芳香化合物和偶氮化合物在厌氧条件下的生物脱毒、转化和矿化作用的研究成果。这些研究表明 ,由于硝基和偶氮基具有强烈的吸电子性 ,好氧条件下很难降解。但是 ,硝基和偶氮基芳香化合物在产甲烷菌群作用下较易还原脱毒 ,转化为相应的芳香胺类 ,其毒性要小几个数量级 ,因而有些毒性很高的芳香化合物废水可利用厌氧反应器处理 ,而且反应过程中发现一些芳香胺类化合物可被完全矿化 ,表明一些含氮芳香化合物可作为厌氧菌的碳源和能源 ,在厌氧条件下被完全生物降解。     

Interactive factors leading to dying-off Carex tato in Momoge wetland polluted by crude oil, Western Jilin, China

Momoge wetland is an internationally important wetland not only because it is a habitat for many rare bird species but also because it is an internationally important stopover for some rare global migratory bird species. However the petroleum exploitation in wetland has brought about many environmental problems. One of the most severe problems is crude oil pollution, which has caused the dying-off Carex tato and imposes great threat on survival of rare birds. This work studied the factors that caused the dying off of Carex tato. The results showed that death of Carex tato was the result narcosis toxicity of alcohols, intermediate biodegradation products of crude oil, on the root tissue, and the fragmentization of cuticle of leaves by light components of crude oil volatized from soil surface. However, the mechanism involved was much more complex and three interactive factors including crude oil pollution of soil, long-term drought and poor permeability of soil were responsible for the dying-off of Carex tato grassland. The distribution of crude oil in soil profile was characterized with high concentrations at top silty layer and the layer below root zone and low or no crude oil at root zone layer. This distribution was relative to root system characteristics and rhizospheric biodegradation. In root zone, substantive oxygen could be transported to root zone through dense root system and well developed aerenchyma. The crude oil in root zone was easily biodegraded by aerobic rhizosphere microbes. However, some toxic intermediate products, such as some alcohols, was sealed in root zone due to poor permeability of the top soil layer and the deeper soil layer and they had lethal effects on root tissue. Above ground, low molecular components of crude oil in top soil layer was easily volatized into atmosphere during long-term drought. Some of the volatized components were adsorbed onto leaves. SEM analysis showed that these components destroyed the leaves by fragmentization of cuticle of leave. This study also shows that although wetland has natural attenuation of pollutants, natural attenuation of pollutants by natural wetland should not be overemphasized. This attenuation function may lose under some conditions such as long-term drought and poor soil texture.     

Bages-Sigean and Canet-St Nazaire lagoons (France): physico-chemical characteristics and contaminant concentrations (Cu,Cd, PCBs and PBDEs) as environmental quality of water and sediment

Environmental characteristics in water and sediments of two contrasted coastal Mediterranean lagoons, Bages-Sigean and Canet-St Nazaire, were measured over a three season survey. The urban pollution (treatment plant discharges) is very important in Canet-St Nazaire lagoon reflecting untreated sewages, while in Bages-Sigean, the northern part appears more impacted due to larger anthropogenic inputs. Dissolved Cd concentrations are on the whole similar in both lagoons, whereas Cu concentrations are by far higher in lagoon Canet-St Nazaire. Cu concentrations appear to be highly dependent on dissolved organic carbon whereas salinity seems to control Cd variations. Concerning the sediments, the confined northern part of lagoon Bages-Sigean shows organic carbon and total nitrogen enrichment whereas lipid concentrations are much higher in the Canet-St Nazaire lagoon. Cu complexation seems to be strongly related to organic matter as evidenced by the two significant positive relationships, on one hand between Cu and organic carbon, and on the other hand, between Cu and lipids. On the contrary, Cd concentrations appear to be mainly controlled by carbonates. PCBs and PBDEs were detected only in sediments and show relatively low concentrations compared to similar lagoon environments. Regarding the sediment quality guidelines, Cd, Cu and PCBs in both lagoons did not exceed any Probable Effect Concentration (PEC).     

Removal of selected natural and synthetic estrogenic compounds in a Canadian full-scale municipal wastewater treatment plant.

The effect of a full-scale municipal wastewater treatment plant (WWTP) and each of the treatment units within the stream on the removal of endocrine-disrupting compounds was evaluated by tracking 17-beta-estradiol (E2), estrone (E1), and 17-alpha-ethinylestradiol (EE2). The overall performance of the WWTP compared well with other plants, as 90.5% removal of E1+E2 and 74.9% removal of EE2 were observed. A larger fraction of EE2 entered the plant in particulate form than E1 and E2, while a lower fraction of EE2 left the plant in particulate form than soluble form. The activated sludge units reduced the concentration of E1+E2 and EE2 in the liquid phase by 88.2% and 44.6%, respectively. The UV treatment process did not reduce the amount of estrogens. The aqueous phase of the tertiary lagoon solids contained higher levels of estrogens compared with the lagoon influent.     

酯类化合物对四膜虫毒性的拓扑研究

提出了拓扑方法,即考虑分子图顶点的性质,直接用酯类化合物的分子碎片的特征值为主元来构建邻接矩阵。定义并计算了酯类化合物的修正的氢连接性指数^mHA及其倒指数^mHB,分析了30个酯化合物对四膜虫的毒性与分子结构之间的关系,结果表明由酯化合物对四膜虫毒性与^mH的回归方程得出的估算值与实验测定值之间能较好地吻合,平均误差为0．22。     

膜生物反应器中生物膜的生长特性

实验采用经甲苯培养驯化而成的单一假单胞菌菌种,通过分析平板式生物膜反应器内,不同阶段假单胞细菌生物膜干重、厚度、活性生物量和生物种群分布的变化,研究生物膜特性与降解效率之间的关系。实验结果表明,在挂膜初期生物膜迅速生长,生物量以及生物膜干重增长很快,有利于甲苯及营养物质的传输,降解效率也快速提升。随着生物膜的生长,生物量及干重也逐步增加,厚度逐渐增加使传质阻力不断增大,生物膜上层微生物的有机底物供应不足,使生物膜上层结构稀疏,最终维持一个甲苯的总传输量与生化降解量的平衡,生物量的生长与衰亡也达到动态平衡,形成了一个较高且稳定的降解效率。     

Effectiveness of porous covers for control of ammonia, reduced sulfur compounds, total hydrocarbons, selected volatile organic compounds, and odor from hog manure storage lagoons

Anaerobic lagoons are a major source of odor at concentrated animal feeding operations. Seven different kinds of artificial (geotextile and polyethylene foam) and natural (straw and redwood) permeable lagoon covers were evaluated for their potential to reduce odorous emissions generated by anaerobic waste lagoons. A novel floating sampling raft was constructed and used to simultaneously evaluate the effectiveness of lagoon covers on an operating swine waste lagoon. The air collected from the raft was evaluated for odor, total reduced sulfur (TRS) compounds, ammonia, total hydrocarbons, dimethyldisulfide, and trimethylamine. The emission rates from the lagoon were highly variable both temporally and spatially. All of the lagoon covers substantially reduced TRS emissions and odor. Geotextile fabric and a recycled foam cover exhibited the greatest reduction in total hydrocarbon emissions; natural covers were less effective. Because of consistently low emission rates of ammonia, no statistically significant reduction of ammonia emissions were observed from any of the lagoon covers.     

含油污泥焦化液相油收率影响因素研究

油田产生的高含油污泥,采用催化焦化的方法进行处理,回收其中的原油,分析了影响含油污泥焦化液相油收率的主要因素,采用正交和单因素实验方法对各因素进行考察,确定了高液相油收率的含油污泥焦化操作条件;处理后的焦化固体产物能够达到农用污泥标准。     

Effectiveness of Porous Covers for Control of Ammonia,Reduced Sulfur Compounds,Total Hydrocarbons,Selected Volatile Organic Compounds,and Odor from Hog Manure Storage Lagoons

Abstract

Anaerobic lagoons are a major source of odor at concentrated animal feeding operations. Seven different kinds of artificial (geotextile and polyethylene foam) and natural (straw and redwood) permeable lagoon covers were evaluated for their potential to reduce odorous emissions generated by anaerobic waste lagoons. A novel floating sampling raft was constructed and used to simultaneously evaluate the effectiveness of lagoon covers on an operating swine waste lagoon. The air collected from the raft was evaluated for odor, total reduced sulfur (TRS) compounds, ammonia, total hydrocarbons, dimethyldisulfide, and trimethylamine. The emission rates from the lagoon were highly variable both temporally and spatially. All of the lagoon covers substantially reduced TRS emissions and odor. Geotextile fabric and a recycled foam cover exhibited the greatest reduction in total hydrocarbon emissions; natural covers were less effective. Because of consistently low emission rates of ammonia, no statistically significant reduction of ammonia emissions were observed from any of the lagoon covers.     

Microbial degradation of dissolved organic matter (DOM) and its influence on phenanthrene-DOM interactions

Microbial degradation-induced changes in the characteristics of dissolved organic matter (DOM), and the subsequent effects on phenanthrene-DOM interactions were investigated based on the microbial incubation of DOM collected from four different sources for 28 d. Partially biodegraded DOM presented higher specific UV absorbance (SUVA), lower protein-like fluorescence, higher humic-like fluorescence, lower aliphatic carbon fraction, and higher hydrophobic neutral fractions compared to the original DOM. Microbial changes in DOM led to an increase in the isotherm nonlinearity as well as the extent of phenanthrene binding. A negative relationship between SUVA and the Freundlich n values was established for the original and the biodegraded DOM, suggesting that aromatic condensed structures may play important roles in providing nonlinear strong binding sites irrespective of microbial degradation. In contrast, there were two separate slopes of the correlations between the percentage of hydrophobic acid (HoA) fraction and the n values for the original and the biodegraded DOM with a higher slope exhibited for the latter, implying that the microbial utilization of oxygen-containing structures in the HoA fractions may contribute to enhancing the associated isotherm nonlinearity.     

Detailed characterization of polar compounds of residual oil in contaminated soil revealed by Fourier transform ion cyclotron resonance mass spectrometry

Effects of remediation technologies on polar compounds of crude oil in contaminated soils have not been well understood when compared to hydrocarbons. In this study, ultrahigh resolution Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) was used to characterize the changes in NSO polar compounds of crude oil and residual oil after long-term natural attenuation, biostimulation and subsequent ozonation following biostimulation of contaminated soils. N₁ and O₁ species, which were abundant in the crude oil, were selectively biodegraded, and species with higher double bond equivalent values and smaller carbon numbers appeared to be more resistant to microbial alteration. O₂-O₆ species were enriched by biodegradation and contained a large number of compounds with a high degree of unsaturation. Ozone could react with a variety of polar compounds in residual oil after biodegradation and showed high reactivity with polar species containing aromatic or multi-aliphatic rings, including the residual N₁ and O₁ species, naphthenic acids and unsaturated O₃-O₆ compounds. Fatty acids and O₃-O₈ species dominated by saturated alkyl compounds were resistant to ozonation or the primarily incomplete ozonation products. Principal component analysis of identified peaks in the FT-ICR MS spectra provided a comprehensive overview of the complex samples at the molecular level and the results were consistent with the detailed analysis. Taken together, these results showed the high complexity of polar compounds in residual oils after biodegradation or ozonation in contaminated soil and would contribute to a better understanding of bioremediation and ozonation processes.     

人工神经网络在强化一级处理系统过程模拟与优化中的应用

针对化学强化一级处理系统(CEPT)处理废水时影响因素多,难以进行适当的控制和处理效果的预测等问题,建立起基于BP人工神经网络的CEPT法处理猪场稳定塘废水预测模型,并应用该模型对烧杯试验进行了模拟.结果表明,预测值和实测值吻合较好,模型对COD、总磷、浊度去除率预测的平均相对误差分别为7.5%、4.8%和4.9%.通过对pH值和絮凝剂投药量等可控参数进行优化计算,得到CEPT系统的最佳操作条件和最合理操作条件.该模型的建立为CEPT法处理废水工艺系统实现自动化控制提供了一条简便实用的途径.     

人工神经网络在强化一级处理系统过程模拟与优化中的应用

针对化学强化一级处理系统（CEPT）处理废水时影响因素多，难以进行适当的控制和处理效果的预测等问题，建立起基于BP人工神经网络的CEPT法处理猪场稳定塘废水预测模型，并应用该模型对烧杯试验进行了模拟。结果表明，预测值和实测值吻合较好，模型对COD、总磷、浊度去除率预测的平均相对误差分别为7．5％、4．8％和4．9％。通过对pH值和絮凝剂投药量等可控参数进行优化计算，得到CEPT系统的最佳操作条件和最合理操作条件。该模型的建立为CEPT法处理废水工艺系统实现自动化控制提供了一条简便实用的途径。     

The anaerobic degradation of endosulfan by indigenous microorganisms from low-oxygen soils and sediments

Indigenous mixed populations of anaerobic microorganisms from an irrigation tailwater drain and submerged agricultural chemical waste pit readily biodegraded the major isomer of endosulfan (endosulfan I). Endosulfan I was biodegraded to endosulfan diol, a low toxicity degradation product, in the presence of organic carbon sources under anaerobic, methanogenic conditions. While there was extensive degradation (>85%) over the 30 days, there was no significant enhancement of degradation from enriched inocula. This study demonstrates that endosulfan I has the potential to be biodegraded in sediments, in the absence of enriched microorganisms. This is of particular importance since such sediments are prevalent in cotton-growing areas and are typically contaminated with endosulfan residues. The importance of minimizing non-biological losses has also been highlighted as a critical issue in determining anaerobic biodegradation potential. Seals for such incubation vessels must be both oxygen and pollutant impermeable. Teflon-lined butyl rubber provides such a seal because of its resistance to the absorption of volatiles and in preventing volatilization. Moreover, including a 100 mM phosphate buffer in the anaerobic media has reduced non-biological losses from chemical hydrolysis, allowing biodegradation to be assessed.     

Revegetation of lagoon ash using the legume species Acacia auriculiformis and Leucaena leucocephala

A greenhouse study was conducted to evaluate the potential use of two legume species, Acacia auriculiformis and Leucaena leucocephala for growth on ameliorated lagoon ash with or without nitrogen (N(2))-fixing bacteria inoculation. Even though amendments of 30% (w/w) vermiculite or with sewage sludge compost were added to improve the chemical and physical limitations of lagoon ash, significant suppressions in biomass and plant nutrient content were found with ameliorated lagoon ash in comparison to an agricultural soil. The high proportion of clay-sized (<53 microm) ash particles limited root growth. In addition, heavy metal toxicity was a possible factor contributing to poor seedling growth. Higher plant productivity resulted from the sewage sludge compost-amended lagoon ash than with vermiculite due to a greater contribution of plant nutrients in the compost. Nodulation was inhibited in ameliorated lagoon ash but not in agricultural soil. High pH and electrical conductivity and elevated toxic metals may be important parameters that limit bacterial activity. Both species showed potential to establish on amended lagoon ash, with Acacia auriculiformis being the best adapted.     

Occurrence and sources of selected phenolic endocrine disruptors in Ria de Aveiro,Portugal

Background, aim and scope  

Ria de Aveiro (Portugal) is a shallow coastal lagoon of high economic and ecological importance. Hardly any data on its chemical pollution by polar organic pollutants are available in literature. This study focused on the presence and sources of a series of phenolic endocrine-disrupting compounds (EDCs) in this area, including parabens, alkylphenolic compounds and bisphenol-A (BPA). A number of possible sources of pollution are present in the area, including the large harbours present in the lagoon, the city of Aveiro and the rivers discharging into the area. A recently constructed submarine wastewater outfall, located a few kilometres from the lagoon inlet has also been suggested as a possible source of pollution to Ria de Aveiro in several publications. The aim of the current field study was to investigate the occurrence and main sources of phenolic endocrine disruptors in Ria de Aveiro.