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PubMed2003

Design of hard water stable emulsifier systems for petroleum- and bio-based semi-synthetic metalworking fluids.

Metalworking fluids (MWFs) increase productivity and the quality of manufacturing operations by cooling and lubricating during metal forming and cutting processes. Despite their widespread use, they pose significant health and environmental hazards throughout their life cycle. An obvious environmental improvement to MWF technology would be to improve the lifetime of the fluid while utilizing more environmentally friendly and less energy-consuming materials without compromising existing performance levels. This investigation focuses on the design of mixed anionionc:nonionic emulsifier systems for petroleum and bio-based MWFs that improve fluid lifetime by providing emulsion stability under hard water conditions, a common cause of emulsion destabilization leading to MWF disposal. Experimental conditions were designed to evaluate the impact of emulsifier structural characteristics (straight chain, branched tail, branched head) and the molar ratios of anionic to nonionic surfactant and oil to total surfactant. Results from the 2500 formulations generated indicate that the use of a twin-headed anionic surfactant can provide improved hard water stability for both mineral oil- and vegetable oil-based formulations, even in the absence of a chelating agent and a coupler. Results also suggest that an oil:total surfactant molar ratio of 0.5 or less is necessary for particle size stability in hard water conditions for these systems. The newly developed petroleum and bio-based formulations with improved hard water stability are competitive with commercially available MWFs in performance evaluations for tramp oil rejection, contact angle, and tapping torque efficiency. These results can be used to design MWF formulations with fewer components and extended lifetime under hard water conditions, both of which would lead to a reduction in the life cycle environmental impact of MWFs.

Calcium Chloride↗
PubMed2004

Optimizing detection limits for the analysis of petroleum hydrocarbons in complex environmental samples.

To evaluate the sources, transport, bioremediation, fate, and effects of spilled petroleum and petroleum products, environmental studies often measure parent and alkylated polycyclic aromatic hydrocarbons (PAH), alkanes, and chemical biomarkers (e.g., triterpanes). Accurate data for low analyte concentrations are required when environmental samples contain hydrocarbons from multiple sources that need to be resolved and quantified. The accuracy and usefulness of the analyses can be improved by lowering the method detection limits (MDLs) for these compounds. Misidentification of hydrocarbon source can result when the MDLs are too high. Modifications to standard analytical methods (i.e., U.S. Environmental Protection Agency Method 8270) can lower MDLs by factors ranging from 10 to 1000. This reduction has important implications for ecological-risk assessments. Modifications having the greatest impact on the MDL include GCMS analysis in the selected-ion-monitoring mode (SIM), increased sample size, column cleanup of the extract, and decreased preinjection volume (volume of final extract prior to injection into instrument). In one study in which a benthic sediment sample was spiked with low levels of topped (heated to remove more volatile PAH that are naturally enriched in crude oil) Alaska North Slope crude, MDLs for individual PAH analytes and biomarkers were determined to be less than 0.5 ng/g (ppb) dry weight and less than 5 ppb dry weightfor individual alkanes. Similar results were obtained when the sediment was spiked with the 16 EPA priority pollutants. In addition, a method has been developed to estimate MDLs for source-specific alkylated PAH analytes and chemical biomarker compounds for which standards are not commercially available or are prohibitively expensive. These improved analytical techniques have been used to identify and quantify low levels of hydrocarbons, derived from both natural and anthropogenic sources, found in the benthic sediments of Prince William Sound, AK.

Environmental Monitoring↗
PubMed2005

Characterization, weathering, and application of sesquiterpanes to source identification of spilled lighter petroleum products.

Biomarkers have become increasingly important for identifying the source of spilled oil, due to their specificity and high resistance to biodegradation. The biomarkers most commonly used in forensic investigations are the high molecular weight (MW) tri- and pentacyclic terpanes and steranes. For lighter petroleum products such as jet fuels and diesels, the refining processes remove most high MW biomarkers from the original crude oil feedstock. The smaller bicyclic sesquiterpanes, however, are concentrated in these products. Sesquiterpanes are ubiquitous components of crude oils and ancient sediments. Examination of GC-MS chromatograms of these bicyclic biomarkers using their characteristic fragment ions (m/z 123, 179, 193, and 207) provides a highly diagnostic means for identifying spilled oil, particularly for lighter refined product samples that are difficult to identify by current techniques. In this work, sesquiterpanes in crude oils and petroleum products are identified and characterized, distributions of sesquiterpanes in oils and refined products are compared, the effects of evaporative weathering on sesquiterpane distributions are examined, and a methodology using diagnostic indices of sesquiterpanes is developed for oil correlation and differentiation. Finally, two case studies are presented to illustrate the unique utility of sesquiterpanes for fingerprinting and identifying unknown diesel spills.

Chromatography, Gas↗
PubMed2006

Forensic fingerprinting of diamondoids for correlation and differentiation of spilled oil and petroleum products.

Diamondoids (adamantanes and diamantanes) are rigid, three-dimensionallyfused cyclohexyl-ring alkane compounds that can be found in almost all crude oils and in most petroleum products. Forforensic environmental investigations, the most commonly used biomarkers are high molecular weight (MW) tri- to pentacyclic terpanes and steranes. Most of these high MW biomarkers, however, are removed from the original crude oil feedstocks during the refining processes, while smaller biomarkers including diamondoids are concentrated in petroleum products. Fingerprinting diamondoids could thus provide another diagnostic means for correlation and differentiation of spilled oils and be particularly valuable for light to midrange distillates, such as jet and diesel fuels, the source of which may be difficult to identify using routine biomarker techniques. In this work, a reliable GC-MS analytical method has been developed for characterization and quantitation of diamondoids. The method detection limits for five target diamondoids were determined to be in the range of 0.06-0.14 microg/g oil. Distributions of diamondoids in over 100 different oils and refined products were quantitatively compared. The concentrations of four groups of target biomarkers were found, in general, to decrease in the order of sesquiterpanes > terpanes and steranes > adamantanes > diamantanes in both crude oils and refined products. A number of indices of admantanes and diamantanes have been developed and assessed as source indicators using their diagnostic powers (DP). The effects of evaporative weathering and biodegradation on alteration of diamondoid distributions have been quantitatively investigated. Finally, a spill case study by statistical evaluation of diagnostic ratios using the "two-tailed" Student's tapproach is presented to illustrate the unique utility of diamondoids for correlation and differentiation of unknown spilled diesels.

Adamantane↗
PubMed2004

Potential for aerobic and anaerobic biodegradation of petroleum hydrocarbons in boreal subsurface.

We studied the role of aerobic and anaerobic petroleum hydrocarbon degradation at a boreal, light-weight fuel and lubrication oil contaminated site undergoing natural attenuation. At the site, anoxic conditions prevailed with high concentrations of CH4 (up to 25% v/v) and CO2 (up to 18% v/v) in the soil gas throughout the year. Subsurface samples were obtained mainly from the anoxic parts of the site and they represented both the unsaturated and saturated zone. The samples were incubated in microcosms at near in situ conditions (i.e. in situ temperature 8 degrees C, aerobic and anaerobic conditions, no nutrient amendments) resulting in the removal of mineral oil (as determined by gas chromatography) aerobically as well as anaerobically. In the aerobic microcosms on average 31% and 27% of the initial mineral oil was removed during a 3- and 4-month incubation, respectively. In the anaerobic microcosms, on average 44% and 15% of the initial mineral oil was removed during a 12- and 10-month anaerobic incubation, respectively, and e.g. n-alkanes from C11 to C15 were removed. A methane production rate of up to 2.5 microg CH4 h(-1) g(-1) dwt was recorded in these microcosms. In the aerobic as well as anaerobic microcosms, typically 90% of the mineral oil degraded belonged to the mineral oil fraction that eluted from the gas chromatograph after C10 and before C15, while 10% belonged to the fraction that eluted after C15 and before C40. Our results suggest that anaerobic petroleum hydrocarbon degradation, including n-alkane degradation, under methanogenic conditions plays a significant role in the natural attenuation in boreal conditions.

Aerobiosis↗
PubMed2003

Determination of petroleum hydrocarbons and polycyclic aromatic hydrocarbons in sludge from wastewater treatment basins.

Screening by gas chromatography with flame ionization detection and gas chromatography-mass spectrometry has been carried out on sludge extracts of wastewater treatment basins. Soxhlet extraction with trichlorotrifluoroethane was applied. The yields for petroleum hydrocarbons and PAH recovery were high, usually in excess of 90%. The proposed investigations permit a quick assessment of petroleum pollutants in the environment.

Environmental Monitoring↗
PubMed2003

Application of laser-based ion mobility (IM) spectrometry for the analysis of polycyclic aromatic compounds (PAC) and petroleum products in soils.

The capability of laser-based IM spectrometry to detect PAC and petroleum products (oils) in model matrices, laboratory reference (LR) materials and in real-world contaminated soil samples was demonstrated. Quantitative IM investigations of PAC-doped PVC films yielded detection limits in the ppm range for single PAC. The potential of IM spectrometry for in situ analysis was demonstrated by the analysis of PAC-containing certified reference (CR) material, and of petroleum product-containing LR materials and real-world soil samples. The calibration of IM signals obtained from oil-doped LR materials was also possible, and detection of oils with concentrations below 100 mg kg(-1) was achieved. The in situ analysis of real-world contaminated soils with the IM and LIF techniques was in good accordance with ex situ reference investigations.

Lasers↗
PubMed1992

[The accidental aspiration and ingestion of petroleum in a "fire eater"].

A 26-year-old man, practicing for a variety performance as "fire-eater", accidentally inhaled and ingested about 10 ml petroleum. Soon afterwards he developed dyspnoea, an urge to cough, fever up to 39 degrees C and loss of retentiveness. He was treated as an out-patient with doxycycline, 100 mg daily, and aspirin, 500 mg three times daily. While this reduced the dyspnoea, the elevated temperature persisted and he had haemoptysis. Chest x-ray and computed tomography 12 days after the aspiration revealed areas of atelectasis and of liquefaction necroses. Bronchoscopic and cytological examinations showed eosinophilic alveolitis and mucosal necrosis in both main bronchi. The symptoms were improved by two inhalations of beclomethasone four times daily, and systemic treatment with prednisolone, 50 mg daily, together with parenteral antibiotic administration (cefotaxime, 1.0 g twice daily). The focal lung lesions regressed completely within a few weeks. Five months after the aspiration computed tomography merely demonstrated discrete scarring of the previously necrotic lesions. This case illustrates that, even with extensive necrotic lung changes after petroleum aspiration, conservative treatment is justified and likely to be effective.

Adult↗
PubMed2006

The Iranian petroleum crisis and United States national security.

The U.S. case against Iran is based on Iran's deceptions regarding nuclear weapons development. This case is buttressed by assertions that a state so petroleum-rich cannot need nuclear power to preserve exports, as Iran claims. The U.S. infers, therefore, that Iran's entire nuclear technology program must pertain to weapons development. However, some industry analysts project an Irani oil export decline [e.g., Clark JR (2005) Oil Gas J 103(18):34-39]. If such a decline is occurring, Iran's claim to need nuclear power could be genuine. Because Iran's government relies on monopoly proceeds from oil exports for most revenue, it could become politically vulnerable if exports decline. Here, we survey the political economy of Irani petroleum for evidence of this decline. We define Iran's export decline rate (edr) as its summed rates of depletion and domestic demand growth, which we find equals 10-12%. We estimate marginal cost per barrel for additions to Irani production capacity, from which we derive the "standstill" investment required to offset edr. We then compare the standstill investment to actual investment, which has been inadequate to offset edr. Even if a relatively optimistic schedule of future capacity addition is met, the ratio of 2011 to 2006 exports will be only 0.40-0.52. A more probable scenario is that, absent some change in Irani policy, this ratio will be 0.33-0.46 with exports declining to zero by 2014-2015. Energy subsidies, hostility to foreign investment, and inefficiencies of its state-planned economy underlie Iran's problem, which has no relation to "peak oil."

Commerce↗
PubMed2002

The evolution of multicomponent systems at high pressures: VI. The thermodynamic stability of the hydrogen-carbon system: the genesis of hydrocarbons and the origin of petroleum.

The spontaneous genesis of hydrocarbons that comprise natural petroleum have been analyzed by chemical thermodynamic-stability theory. The constraints imposed on chemical evolution by the second law of thermodynamics are briefly reviewed, and the effective prohibition of transformation, in the regime of temperatures and pressures characteristic of the near-surface crust of the Earth, of biological molecules into hydrocarbon molecules heavier than methane is recognized. For the theoretical analysis of this phenomenon, a general, first-principles equation of state has been developed by extending scaled particle theory and by using the technique of the factored partition function of the simplified perturbed hard-chain theory. The chemical potentials and the respective thermodynamic Affinity have been calculated for typical components of the H-C system over a range of pressures between 1 and 100 kbar (1 kbar = 100 MPa) and at temperatures consistent with those of the depths of the Earth at such pressures. The theoretical analyses establish that the normal alkanes, the homologous hydrocarbon group of lowest chemical potential, evolve only at pressures greater than approximately 30 kbar, excepting only the lightest, methane. The pressure of 30 kbar corresponds to depths of approximately 100 km. For experimental verification of the predictions of the theoretical analysis, a special high-pressure apparatus has been designed that permits investigations at pressures to 50 kbar and temperatures to 1,500 degrees C and also allows rapid cooling while maintaining high pressures. The high-pressure genesis of petroleum hydrocarbons has been demonstrated using only the reagents solid iron oxide, FeO, and marble, CaCO3, 99.9% pure and wet with triple-distilled water.

Carbon↗
PubMed2001

Evaluation of myelotoxicity in cotton rats (Sigmodon hispidus) exposed to environmental contaminants. II. Myelotoxicity associated with petroleum industrial wastes.

Various chemical mixtures exist in soil contaminated with petrochemical wastes, yet no comprehensive assessment of their impact on terrestrial ecosystems has been conducted. The purpose of this study was to evaluate hematotoxicity risks to wild populations of cotton rats (Sigmodon hispidus) residing in habitats previously contaminated by petroleum industrial wastes. Resident cotton rats were monitored on nine contaminated sites and nine ecologically matched reference sites in Oklahoma. The possible toxicological interactions of petrochemical wastes on bone marrow was investigated by using the assay of colony formation of granulocyte-macrophage progenitor cells. There was a consistent significant 21 to 39% decrease in the number of colony-forming units of granulocyte-macrophage (CFU-GM) in cotton rats from petrochemical-contaminated sites compared to matched reference sites, with no marked changes in hematological or histopathological parameters. These results suggest that bone-marrow progenitor cell culture is a sensitive indicator for the assessment of ecotoxicity risks associated with petrochemical wastes that are generated by the oil refining industry. Long-term exposure to hazardous wastes associated with the petroleum industry may represent a subtle risk to the hematopoietic system in humans.

Animals↗
PubMed2006

Occupational exposure to carbon/coke fibers in plants that produce green or calcined petroleum coke and potential health effects: 1. Fiber characteristics.

Carbon/coke fibers are found in bulk samples of calcined petroleum coke. Carbon/coke and other fibers, including calcium silicate, cellulose, gypsum, and iron silicate, have been found in exposure monitoring of workers who make or handle green or calcined petroleum coke. Carbon/coke fibers are not classified or regulated as carcinogens by any agency, and the available literature (summarized in this article) has not reported significant adverse health effects associated with exposure to these fibers or dusts containing these fibers. However, available epidemiological and toxicological studies have limitations that prevent a definitive assessment of carbon/coke fiber toxicity. Therefore, it is prudent to monitor and control workplace concentrations. Analyses by transmission electron microscopy (TEM) indicate that the carbon/coke fibers are amorphous, irregularly shaped, and generally rather short (94% less than 20 microm long). Nearly all carbon/ coke fibers satisfying NIOSH 7400 B counting criteria are detectable by phase-contrast optical microscopy (PCOM), which permits the use of a highly efficient sequential sampling strategy for analysis. Data are presented on the distribution of carbon/coke structure and fiber lengths and diameters. Bootstrap resampling results are presented to determine confidence intervals for structure/fiber length and diameter. Data on time-weighted average concentrations are given in a companion article, but nearly all time-weighted average carbon/coke fiber concentrations were beneath 0.1 fibers per milliliter.

Calcium Compounds↗
PubMed2006

Occupational exposure to carbon/coke fibers in plants that produce green or calcined petroleum coke and potential health effects: 2. Fiber concentrations.

We monitored exposure to various fibers among workers in eight plants operated by ConocoPhillips that produce green or calcined petroleum coke. Carbon/coke and other fibers, including calcium silicate, cellulose, gypsum, and iron silicate, were found in occupational samples. Carbon/coke fibers were found in bulk samples of calcined petroleum coke, the probable source of these fibers in occupational samples. Time-weighted average (TWA) total fiber concentrations were approximately lognormally distributed; 90% were < or = 0.1 f/ml. Although consistently low, TWA total fiber concentrations varied with plant, job (tasks), and type of coke. This was expected given the substantial differences in plant configuration, technology, and workplace practices among refineries and carbon plants. Carbon/coke fibers (identified and measured using transmission electron microscopy [TEM]) were found at all plants producing all types of calcined coke and not detected at any plant producing only green coke. Approximately 98% of all carbon/coke TWAs were < or = 0.1 f/ml. Analysis of task length average (TLA) data by various statistical techniques indicates that the average carbon/coke TLA is certainly < or = 0.05 f/ml and probably < 0.03 f/ml.

Calcium Compounds↗
PubMed2005

Respirometry for assessing the biodegradation of petroleum hydrocarbons.

The respiration method using the Micro-Oxymax respirometer was applied to evaluate the bioremediation potential of hydrocarbon-contaminated soils in two biopiles at the oil refinery in Czechowice-Dziedzice, Poland. In biopiles 1 and 2, two different technologies, i.e., enhanced (engineered) bioremediation and monitored natural attenuation (MNA) were used, respectively. In biopiles 1 and 2, the bioremediation process lasted 6 years and 8 months, respectively. The biodegradation of petroleum hydrocarbons was evaluated on the basis of CO2 production and O2 uptake. The CO2 production and O2 consumption rates during hydrocarbon biodegradation were calculated from the slopes of cumulative curve linear regressions. The results confirmed the hydrocarbon biodegradation process in both biopiles. However, in biopile 2 the process was more effective compared to biopile 1. In biopile 2, the O2 consumption and CO2 production means were 3.37 and 2.4 milliliters per kilogram of soil (dry weight) per minute, respectively. Whereas, in biopile 1, the O2 consumption and CO2 production means were 1.52 and 1.07 milliliters per kilogram of soil (dry weight) per minute, respectively. The mean biodegradation rate for biopile 2 was two times higher--67 mg hydrocarbons kg d.w.(-1)day(-1) compared with biopile 1, where the mean was 30 mg hydrocarbons kg d.w.(-1)day(-l). The results were correlated with petroleum hydrocarbon concentrations and microbial activity measured by dehydrogenase assay.

Biodegradation, Environmental↗
PubMed1997

Toxicity and mutagenicity of component classes of oils isolated from soils at petroleum- and creosote-contaminated sites.

Microtox and Ames bioassays were employed to assess acute toxicity and mutagenicity of water soluble components of class-fractionated oils extracted from one creosote- and four petroleum-contaminated soils. Microtox results revealed that potential acute toxicity resides mainly in the polar class fractions at three sites and indicated potential synergistic and antagonistic effects between compounds in the total extracts at two sites. Ames Salmonella/microsome testing indicated that the polyaromatic fractions at two sites exhibit weak mutagenicity with enzymatic activation, while the polar fractions at two sites are weakly mutagenic without enzyme activation. Further chemical characterization of the polar and polyaromatic fractions is required to fully assess the potential of health and ecological risks at the creosote-and petroleum-contaminated sites exhibiting these toxic responses.

Animals↗
PubMed2005

Pollution prevention and control procedure case study: an application for petroleum refineries.

There is global environmental concern about the pollution from industries and other organizations that should not only be controlled but also prevented. Many alternatives are available to those in charge of environmental protection, but they should be able to draw on a systematic procedure to help implement prevention and control measures. At present, there are three immediate tasks: defining the objective of any environmental study, identifying the potential pollution sources, and selecting alternatives to these sources. However, it is necessary to evaluate these alternatives by using as large a number of criteria as possible and making them cumulative so as to enable the classification and selection of the best available techniques for each pollution source. The petroleum refining industry plays an important role in the developed economies and also has a potential for pollution generation that must be controlled. The best solution for all (i.e., petroleum companies, the public, and the environment) is pollution prevention, because this option will protect all of them and will also reduce costs in terms of lower raw materials consumption as well as reducing potential fines. The procedure we have presented in this article has been applied successfully.

Chemical Industry↗
PubMed2006

Solar-chemical treatment of groundwater contaminated with petroleum at gas station sites: ex situ remediation using solar/TiO(2) photocatalysis and Solar Photo-Fenton.

Groundwater samples contaminated by BTEX (benzene, toluene, ethylbenzene, xylene isomers and TPHs (total petroleum hydrocarbons) were treated with advanced oxidation processes (AOPs), such as TiO(2) photocatalysis and Fe(2+)/H(2)O(2) exposed to solar light (37 degrees N and 128 degrees E) with an average intensity of 1.7 mW/cm(2) at 365 nm. These AOP processes showed feasibility in the treatment of groundwater contaminated with BTEX, TPH and TOC (Total Organic Carbon). Outdoor field tests showed that the degradation efficiency of each contaminant was higher in the Fe(2+)/H(2)O(2) system without solar light compared to the TiO(2)/solar light and H(2)O(2)/solar light systems. However, the TiO(2)/solar light and the Fe(2+)/H(2)O(2)/solar light systems showed significantly enhanced efficiencies in the degradation of BTEX, TPH and TOC with the additional use of H(2)O(2). Near complete degradation of BTEX and TPH was observed within 2 and 4 hrs, respectively, however, that of TOC was slower. Without pretreatment of the groundwater, fouling of the TiO(2), due to the ionic species present, was observed within 1 hr of operation, which resulted in the inhibition of further BTEX, TPH and TOC destruction. The degradation rate of n-alkanes with carbon numbers ranging from C10 to C15 was relatively greater than that of n-alknaes with carbon numbers ranging from C16 to C20. From this work, the AOP process (Fe(2+)/H(2)O(2)/solar light and TiO(2)/H(2)O(2)/solar light) illuminated with solar light was identified as an effective ex situ technique in the remediation of groundwater contaminated with petroleum.

Carbon↗