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PubMed2006

Modelling of iron cycling and its impact on the electron balance at a petroleum hydrocarbon contaminated site in Hnevice, Czech Republic.

Over a period of several decades multiple leaks of large volumes from storage facilities located near Hnevice (Czech Republic) have caused the underlying Quaternary aquifer to be severely contaminated with nonaqueous phase liquid (NAPL) petroleum hydrocarbons. Beginning in the late 1980's the NAPL plume started to shrink as a consequence of NAPL dissolution exceeding replenishment and due to active remediation. The subsurface was classified geochemically into four different zones, (i) a contaminant-free zone never occupied by NAPL or dissolved contaminants, (ii) a re-oxidation zone formerly occupied by NAPL, (iii) a zone currently occupied by NAPL, and (iv) a lower fringe zone between the overlying NAPL and the deeper underlying contaminant-free zone. The study investigated the spatial and temporal variability of the redox zonation at the Hnevice site and quantified the influence of iron-cycling on the overall electron balance. As a first step inverse geochemical modelling was carried out to identify possible reaction models and mass transfer processes. In a subsequent step, two-dimensional (forward) multi-component reactive transport modelling was performed to evaluate and quantify the major processes that control the geochemical evolution at the site. The study explains the observed enrichment of the lower fringe zone with ferrihydrite as a result of the re-oxidation of ferrous iron. It suggests that once the NAPL zone started to shrink the dissolution of previously formed siderite and FeS by oxygen and nitrate consumed a significant part of the oxidation capacity for a considerable time period and therefore limited the penetration of electron acceptors into the NAPL contaminated zone.

Biodegradation, Environmental↗
PubMed2006

Remediation of saturated soil contaminated with petroleum products using air sparging with thermal enhancement.

Pollutants in the form of non-aqueous phase liquids (NAPLs), such as petroleum products, pose a serious threat to the soil and groundwater. A mathematical model was derived to study the unsteady pollutant concentrations through water saturated contaminated soil under air sparging conditions for different NAPLs and soil properties. The comparison between the numerical model results and the published experimental results showed acceptable agreement. Furthermore, an experimental study was conducted to remove NAPLs from the contaminated soil using the sparging air technique, considering the sparging air velocity, air temperature, soil grain size and different contaminant properties. This study showed that sparging air at ambient temperature through the contaminated soil can remove NAPLs, however, employing hot air sparging can provide higher contaminant removal efficiency, by about 9%. An empirical correlation for the volatilization mass transfer coefficient was developed from the experimental results. The dimensionless numbers used were Sherwood number (Sh), Peclet number (Pe), Schmidt number (Sc) and several physical-chemical properties of VOCs and porous media. Finally, the estimated volatilization mass transfer coefficient was used for calculation of the influence of heated sparging air on the spreading of the NAPL plume through the contaminated soil.

Air↗
PubMed2005

Natural attenuation of MTBE at two petroleum-hydrocarbon spill sites.

Methyl tert-butyl ether (MTBE) has been used as a gasoline additive to improve the combustion efficiency and to replace lead since 1978. Because it is widely used and it has been disposed inappropriately, MTBE has become a prevalent groundwater contaminant worldwide. In this study, two petroleum-hydrocarbon contaminated sites (Sites A and B) were selected to evaluate the occurrence and effectiveness of natural attenuation of MTBE at these two sites. Field investigation results indicate that the natural attenuation mechanisms of MTBE at both sites were occurring with the first-order attenuation rates of 0.0021 and 0.0048 1day(-1) at Sites A and B, respectively. Results also reveal that the intrinsic biodegradation pattern was the most important mechanism among the natural attenuation processes at both sites. Results from BIOSCREEN simulation suggest that biodegradation was responsible for 78 and 59% of MTBE mass reduction at Sites A and B, respectively. Investigation results show that MTBE plume at Site B could be effectively controlled via natural attenuation processes. However, MTBE plume at Site A has migrated to a farther downgradient area and passed the boundary line of the site. Thus, more active groundwater remedial technologies should be applied at Site A to protect the downgradient environment. Results from this study suggest that natural attenuation might be feasible to be used as a remedial option for the remediation of MTBE-contaminated site on the premise that (1) detailed site characterization has been conducted and (2) the occurrence and effectiveness of natural attenuation processes have been confirmed.

Biodegradation, Environmental↗
PubMed2006

Treatment of petroleum refinery sourwater by advanced oxidation processes.

The performance of several oxidation processes to remove organic pollutants from sourwater was investigated. Sourwater is a specific stream of petroleum refineries, which contains slowly biodegradable compounds and toxic substances that impair the industrial biological wastewater treatment system. Preliminary experiments were conducted, using the following processes: H2O2, H2O2/UV, UV, photocatalysis, ozonation, Fenton and photo-Fenton. All processes, except Fenton and photo-Fenton, did not lead to satisfactory results, reducing at most 35% of the sourwater dissolved organic carbon (DOC). Thus, further experiments were performed with these two techniques to evaluate process conditions and organic matter removal kinetics. Batch experiments revealed that the Fenton reaction is very fast and reaches, in a few minutes, an ultimate DOC removal of 13-27%, due to the formation of iron complexes. Radiation for an additional period of 60 min can increase DOC removal up to 87%. Experiments were also conducted in a continuous mode, operating one 0.4L Fenton stirred reactor and one 1.6L photo-Fenton reactor in series. DOC removals above 75% were reached, when the reaction system was operated with hydraulic retention times (HRT) higher than 85 min. An empirical mathematical model was proposed to represent the DOC removal kinetics, allowing predicting process performance quite satisfactorily.

Equipment Design↗
PubMed2005

Effect of the tropical grass Brachiaria brizantha (Hochst. ex A. Rich.) Stapf on microbial population and activity in petroleum-contaminated soil.

The effect of the tropical pasture grass Brachiaria brizantha on numbers of bacteria, fungi and degraders of alkanes, aromatics, cycloalkanes and crude oil in petroleum hydrocarbon contaminated and uncontaminated savannah soil was evaluated. Substrate induced soil respiration and soil pH were compared between planted and unplanted soil. B. brizantha had a mostly increasing effect on microbial numbers. As an exception, growth of bacteria was not or negatively affected. Microbial respiration and pH were always lower in planted than in unplanted soil. Low pH may result from enhanced oil degradation in planted soil leading to an accumulation of organic acids. A comparable stimulation of crude oil degraders and fungi in planted soil points to the importance of fungi. Since they tolerate lower pH values than bacteria, they are considered to play a central role in oil degradation. Given that the enhancement of crude oil degradation under the influence of B. brizantha could not clearly be correlated to microbial numbers and activity, other factors like oxygen availability, plant enzymes and synergistic degradation by microbial consortia have to be considered.

Bacteria↗
PubMed2005

The selection of mixed microbial inocula in environmental biotechnology: example using petroleum contaminated tropical soils.

The impact of inorganic N and P additions on a tropical soil contaminated with petroleum hydrocarbons was investigated using molecular and culture techniques. Microcosms were incubated for 42 days and sampled at 0, 1, 7, 28 and 42 days. Changes in bacterial community structure were determined using denaturing gradient gel electrophoresis (DGGE) of the rRNA following reverse transcription PCR using primers specific to the V3 region of the 16S rRNA gene. To identify which components of the microbial community were changing during incubation, PCR amplicons were resolved using DGGE and the banding patterns analyzed using stepwise discriminant function analysis (SDA). SDA showed that the number of bands needed to recover the differences between samples over time could be reduced from the initial 11 bands for the 16S rRNA transcript to 3 bands. Sequences originating from the rRNA gels (16S rRNA transcripts) were recovered in clades containing known cultured isolates of Bacillus marisflavi, Microbacterium oxydans and Pseudomonas oleovorans. Isolation studies on these soils using lubricant oil as a carbon source yielded 317 bacterial isolates, 3 of which showed high sequence similarity (>96%) with the 16S rRNA transcripts identified using SDA as being important in differentiating between bacterial communities over time. These isolates were then tested singly and in combination for their ability to degrade lubricant oil. These analyses demonstrated that the consortium selected using the combined molecular-SDA approach was more effective at degrading the lubricant in both liquid media and in contaminated sand than the single isolates.

Bacteria↗
PubMed2006

Identification and biodegradation potential of a novel strain of Dietzia cinnamea isolated from a petroleum-contaminated tropical soil.

A bacterial strain, named P4, isolated previously from microcosms containing oil-contaminated soil collected from an environmentally protected area of a tropical Atlantic forest (Biological Reserve of Poço das Antas) located in Brazil was identified as Dietzia cinnamea by morphological, biochemical and genotypic tests. Arabian Light and Marlin oils were both degraded when strain P4 was tested for oil degradation ability in microplates. Total Petroleum Hydrocarbons (TPH) analysis, determined by gas chromatography, showed that strain P4 degraded a wide range of n-alkanes, and also pristane and phytane. Furthermore, this strain was also able to grow in mineral liquid media amended with carbazole, quinoline, naphthalene, toluene, gasoline and diesel as the sole carbon sources. The species D. cinnamea has been previously described with only one representative strain isolated from a perianal swab of a patient with a bone marrow transplant. With the results presented here this species is implicated not only as a human pathogen but also as a potential strain for further studies concerning its role for bioremediation of oil contaminated soil.

Actinomycetales↗
PubMed2006

The interpretation of occupational epidemiologic data in regulation and litigation: studies of auto mechanics and petroleum workers.

Epidemiologic data often serve as scientific basis for policies in regulation and opinions in litigation. The interpretation of epidemiologic data in both regulation and litigation is often challenged and debated. In this commentary, a wide range of issues concerning the interpretation of epidemiologic data in regulation and litigation are discussed. These issues include: case reports, study design, specificity of exposure, interview or recall bias, misclassification of occupation or exposure, confounding multiple exposures, confidence intervals and statistical power, selection of relevant studies, consistency of study results, study cohort definition, cohort membership misclassification, dilution effect, and subcohort or stratified analysis. Epidemiologic studies of auto mechanics and petroleum workers are used as examples to illustrate the importance of relying on sound epidemiologic principles in study interpretation. If these principles are not followed, the interpretation of epidemiologic studies will likely be erroneous and not useful to regulatory policy-makers or to those involved in litigation.

Automobiles↗
PubMed2002

Isolation and characterization of Sphingomonas sp. GTIN11 capable of carbazole metabolism in petroleum.

A bacterial culture was isolated from a manufactured gas plant (MGP) soil based on its ability to metabolize the nitrogen-containing heterocycle carbazole. The culture was identified as a Sphingomonas sp. and was given the designation GTIN11. A cloned 4.2kb DNA fragment was confirmed to contain genes responsible for carbazole degradation. DNA sequence analysis revealed that the fragment contained five open reading frames (ORFs) with the deduced amino acid sequence showing homology to; carbazole terminal dioxygenase (ORF1), 2,3-dihydroxybiphenyl dioxygenase subunits (ORF2 and ORF3), meta-cleavage compound hydrolases (ORF4), and ferrodoxin component of bacterial multicomponent dioxygenases (ORF5). The percent similarity was 61% of these proteins or less to known proteins. The specific activity of Sphingomonas sp. GTIN11 for the degradation of carbazole at 37 degrees C was determined to be 8.0 micromol carbazole degraded/min/g dry cell. This strain is unique in expressing the carbazole degradation trait constitutively. Resting cells of Sphingomonas sp. GTIN11 removed 95% of carbazole and 50% of C1-carbazoles from petroleum in a 16-h treatment time.

Biodegradation, Environmental↗
PubMed1986

Pulmonary fibrosis in cable plant workers exposed to mist and vapor of petroleum distillates.

Twenty-five cable plant workers exposed to mists and vapors of mineral oils and kerosene for 5-35 years have been investigated in a cross-sectional, matched pairs study. The exposed cohort and the referents were examined by radiology, pulmonary function measurements, and a questionnaire for symptoms of respiratory disease. Lung tissue from a deceased worker with 35 years of exposure was investigated by histopathologic methods and by scanning electron microscopy. Exposure measurements were performed by personal sampling. Previous employment and smoking habits were recorded for all subjects. An increased prevalence of slight basal lung fibrosis was found in chest films of the exposed workers. Pulmonary fibrosis was confirmed histopathologically. A moderately decreased vital capacity (VC) and forced expiratory volume (FEV1) was found. Oil mist was measured to time-weighted average levels of 0.15-0.30 mg/m3 with short-term vapor exposure of up to 4000 mg/m3. It is concluded that mists and vapors from petroleum distillates are the most probable causes of the findings.

Adult↗
PubMed1981

Microextraction and gas chromatographic analysis of selected petroleum hydrocarbons in water and fish tissue.

The most effective water to solvent ratio is determined for the analyses of aromatic hydrocarbons in water using hexane. The recoveries of these hydrocarbons formed in the water soluble fraction of crude oils and petroleum products are measured using a microextraction procedure. Recoveries were in the 30-40% range but are consistent for each compound. Fish muscle samples are fortified with the standards and the recoveries measured with a modified extraction procedure using dichloromethane as the primary extracting solvent. This is dispersed in water using acetone and finally extracted with hexane. Recoveries range from 90-113% with a mean value of 98%.

Animals↗
PubMed2002

Nordic laboratory intercomparison of supercritical fluid extraction for the determination of total petroleum hydrocarbon, polychlorinated biphenyls and polycyclic aromatic hydrocarbons in soil.

Two developed supercritical fluid extraction (SFE) methods [one for the determination of total petroleum hydrocarbon (TPH) and polychlorinated biphenyls (PCBs), and one for polycyclic aromatic hydrocarbons (PAHs) and creosote components in soil] were evaluated in a Nordic laboratory intercomparison study with 11 participating laboratories. The interlaboratory comparison showed that excellent recoveries can be obtained with SFE for PAHs and PCBs compared to the solvent extraction. For the TPH, the recoveries were significantly higher than those achieved with solvent extraction. The accuracy, expressed as the relative standard deviation, was higher than expected (generally 8-25% for PAHs, 6-20% for PCBs and less than 18% for TPH with a few very high values, especially for PCBs), but not different from the other intercomparison studies. Difference between liquid- and solid-phase collection in SFE was found to be significant only for more volatile PAH components such as naphthalene and fluorene. For PCBs and TPH, there were some variation in the results obtained with the two trapping methods.

Chromatography, Supercritical Fluid↗
PubMed2003

Determination of total petroleum hydrocarbons in soil by dynamic on-line supercritical fluid extraction with infrared photometric detection.

Total petroleum hydrocarbons (TPHs) in soil are determined by on-line dynamic supercritical fluid extraction (SFE) using infrared filter photometry detection. The filter photometer was constructed in the laboratory using a tungsten lamp, an optical notch filter that selects the C-H stretching vibration of the extracted organics, an optical chopper with demodulation electronics, and a PbSe detector. A modified high-pressure fiber optic flow cell was used to couple the SFE system to the photometer. Quantitation of TPHs was accomplished through the construction of calibration curves of integrated absorbance of C-H stretching (over time) versus concentration. Our studies show that the sensitivity of this system is affected by both the optical path length in the high-pressure cell and the SFE fluid flow-rate, and detection limits for TPHs are in the mid part-per-million range. The results of the application of this on-line SFE-IR instrument to the determination of TPHs in real-world samples show good agreement with those obtained from standard Soxhlet extraction-IR methods.

Calibration↗
PubMed2002

Evaluation of two direct immunoassays for rapid detection of petroleum products on marine birds.

To reduce rehabilitation time and improve survival, a practical, objective test is needed to determine if marine birds are contaminated with oil before they enter captivity. The RaPID Assays and EnviroGard immunoassays for detection of polycyclic aromatic hydrocarbons (PAHs) in soil were evaluated for their ability to detect petroleum on feather samples from 30 intermediate fuel oil contaminated and 30 uncontaminated common murres (Uria aalge). Sensitivity, specificity, positive and negative predictive value, precision, and time required to run each assay were determined. The RaPID Assays was 96.7% sensitive and specific, while the EnviroGard assay was 93.3% sensitive, and 90.0% specific. Sensitivity decreased at higher dilutions for both assays. Intra-replicate variation was less than 20%. Our evaluation showed that these immunoassays are rapid and cost-effective methods for detecting oil-contamination on the plumage of seabirds, with the EnviroGard assay being more practical in most oil spill response situations due to ease of use and rapidity of results.

Animals↗
PubMed2002

Improved approaches to ecotoxicity testing of petroleum products.

Crude oils produced in the North West shelf of Western Australia are highly volatile, a characteristic not shared by most of the Northern Hemisphere crude oils on which internationally accepted toxicity test protocols were developed. Because of this volatility and some other factors, the LC50 and EC50 values obtained from acute toxicity tests will be significantly affected by the changes of toxicant concentration in test solutions during the period of exposure. To address these issues all steps of a standard protocol for crude oil toxicity testing have been revised. A systematic study has been performed on factors which affect petroleum hydrocarbon solubilisation in aqueous systems during test solution preparations. The influence of mixing time, agitation energy and volume/ interface ratio on a hydrocarbon concentration in a water-soluble fraction (WSF) was studied for heavy, medium and light crude oils. A study of the sensitivity of marine unicellular algae to WSF of crude oils was conducted with Isochrysis sp., Nannochloropsis-like sp. and Nitzchia closterium. Total concentrations of hydrocarbons dissolved in test solutions were estimated by UV-spectrometry and GC/FID chemical analyses. When the toxicant concentration decreased during the exposure period, the EC50 values derived from initial or final concentrations either underestimate or overestimate toxicity, respectively. Therefore, weighted average concentrations (WAC) calculated for the whole test period were recommended for expressing hydrocarbon concentrations in test solutions of crude oils. Toxicity indices calculated from WAC of total hydrocarbons for different crude oils can be compared regardless of the rates of hydrocarbon loss.

Eukaryota↗
PubMed1997

Correlation of mutagenic potencies of various petroleum oils and oil coal tar mixtures with DNA adduct levels in vitro.

An in vitro system was utilized to measure DNA adduct-forming ability of petroleum oils and oil coal tar mixtures to define correlations between DNA adduct levels and their mutagenic potencies. The system consisted of reaction of dimethyl sulfoxide extracts of oils with calf thymus DNA in the presence of Aroclor-induced hamster liver microsomes for 30 min. Following DNA extraction, DNA adducts were measured by the nuclease P1-enhanced postlabeling assay coupled with two-dimensional polyethyleneimine (PEI)-cellulose TLC. Thin layer plates showed putative aromatic DNA adducts, with levels ranging from 60 to 1400 adducts per 10(9) DNA nucleotides. TLC mobilities suggested adducts to be aromatic compounds containing 4 or more rings. A good correlation (coefficient of correlation = 0.91) was observed between DNA adduct levels and Salmonella mutagenicity for 19 oils. All 19 samples tested produced DNA adducts. To expedite the TLC procedure, adducts were resolved by one-dimensional TLC and the radioactivity measured using a mechanical scanner. Results were comparable to those obtained by two-dimensional TLC and quantification after scraping. Our data show that the in vitro incubation system coupled with the postlabeling adduct assay is a useful screening method to identify mutagenic and potentially carcinogenic oils.

Animals↗
PubMed2002

An application of permeable reactive barrier technology to petroleum hydrocarbon contaminated groundwater.

A funnel and gate permeable reactive barrier was designed and built to treat groundwater contaminated with dissolved phase toluene. ethyl benzene. and xylene and n-alkanes in the C6-C36 fraction range. Removal efficienicies for the funnel and gate system varied from 63% to 96% for the monocyclic aromatic hydrocarbons. Average removal efficiencies for C6-C9, C10-C14, and C15-C28 fraction ranges were 69.2%, 77.6% and 79.5%. respectively. The lowest average removal efficiencies were 54% for the C29-C36 n-alkane fraction. The overall average removal efficiency for the funnel and gate system towards petroleum hydrocarbons present in the groundwater was 72% during the 10 month period over which the data were collected, and has allowed relevant water quality objectives to be met.

Equipment Design↗
PubMed2002

Enhanced photo-degradation of contaminants in petroleum refinery wastewater.

In order to rise efficiency of the wastewater treatment in a refinery plant, several oxidation experiments were done, testing their applicability as an additional pretreatment method. The influence of treatment with low concentrations of H2O2 combined with stirring and UV light on degradation of organic compounds present in the refinery wastewater was studied. Oxidation of the total petroleum hydrocarbons occurs at relatively low concentrations of H2O2, additional UV irradiation slightly accelerates the process due to the increased formation of hydroxyl radicals. 1,2-dichloroethane and t-butyl methyl ether degrade in the similar manner and except for the lowest H2O2 concentration used (1.17 mM), the reduction after 24 h is total. The degradation rate for dichloromethane is the lowest one, depending both on hydrogen peroxide concentration and the presence of UV. Its maximum reduction of 83% was obtained using the highest applied peroxide concentration of 11.76 mM.

Hydrocarbons, Chlorinated↗