47 results on '"Mike Landriault"'
Search Results
2. Effect of evaporative weathering and oil-sediment interaction on the fate and behavior of diluted bitumen in marine environments. Part 2. The water accommodated and particle-laden hydrocarbon species and toxicity of the aqueous phase
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Chun Yang, Keval Shah, Brian Chan, Yujuan Hua, Mike Landriault, Carl E. Brown, Bruce P. Hollebone, Paula Jackman, Zeyu Yang, and Fatemeh Mirnaghi
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Environmental Engineering ,010504 meteorology & atmospheric sciences ,Health, Toxicology and Mutagenesis ,chemistry.chemical_element ,010501 environmental sciences ,01 natural sciences ,Alberta ,chemistry.chemical_compound ,Settling ,Environmental Chemistry ,Petroleum Pollution ,Polycyclic Aromatic Hydrocarbons ,Weather ,0105 earth and related environmental sciences ,Asphaltene ,chemistry.chemical_classification ,Light crude oil ,Public Health, Environmental and Occupational Health ,Environmental engineering ,Water ,Sediment ,General Medicine ,General Chemistry ,Particulates ,Pollution ,Hydrocarbons ,Lakes ,Petroleum ,Hydrocarbon ,chemistry ,Environmental chemistry ,Oils ,Carbon ,Water Pollutants, Chemical - Abstract
In this study, the water accommodated and particle-laden hydrocarbon species, and the toxicity of the aqueous phase after oil-sediment interactions by varying the weathering states of diluted bitumen (Cold Lake blend (CLB)), oil type from light to heavy, and sediment type. Compared to the original oils, the sediment-laden total petroleum hydrocarbons (TPH) contained fewer hydrocarbons in the carbon range C34 range. Sediment-laden oil amounts generally decreased with an increased viscosity and asphaltene content of the test oils, as well as with increased sediment particle size. The presence of sediments significantly decreased the oil accommodated in water due to the formation of oil particulate aggregates (OPA) after mixing and settling. Less water accommodated TPH and polycyclic aromatic hydrocarbons (PAHs) were observed for weathered CLB products. However, oil and sediment types did not clearly affect the water accommodated TPH and PAHs. Light molecular PAHs and their alkylated congeners accounted for most of the water accommodated PAH congeners. A microtoxicity test demonstrated that with or without sediment, and regardless of sediment type, the toxicity of the water phase did not change significantly. Light oil of Alberta sweet mixed blend (ASMB) had the highest toxicity, followed by fresh CLB, and then all other oils, suggesting that ASMB and fresh CLB had relatively higher levels of light toxic components dissolved in the water phase compared with the other tested oils.
- Published
- 2018
3. Characterization of chemical fingerprints of unconventional Bakken crude oil
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Mike Landriault, Gong Zhang, Patrick Lambert, Chun Yang, Carl E. Brown, Fatemeh Mirnaghi, Ben Fieldhouse, Zeyu Yang, and Bruce P. Hollebone
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Pollution ,010504 meteorology & atmospheric sciences ,Health, Toxicology and Mutagenesis ,media_common.quotation_subject ,010501 environmental sciences ,Toxicology ,Diamondoid ,01 natural sciences ,Gas Chromatography-Mass Spectrometry ,chemistry.chemical_compound ,Petroleum product ,Organic chemistry ,Petroleum Pollution ,Polycyclic Aromatic Hydrocarbons ,0105 earth and related environmental sciences ,media_common ,Naphthalene ,Chemistry ,business.industry ,Tight oil ,General Medicine ,Phenanthrene ,Crude oil ,Petroleum ,Environmental chemistry ,business ,Water Pollutants, Chemical - Abstract
The ability to characterize the composition of emerging unconventional Bakken tight oil is essential to better prepare for potential spills and to assess associated environmental concerns. The present work measured and compared the physical and chemical properties of Bakken crudes with conventional crude oils from various regions and different types of refined petroleum products. The physicochemical properties of Bakken crude are overall similar to those of conventional light crudes. The Bakken crude consists of high concentrations of monoaromatic hydrocarbons and alkylated PAHs with a clear dominance of the alkylated naphthalene homologues followed by the phenanthrene series. Its pyrogenic index (PI) values are considerably lower than typical conventional crude oils. The Bakken crude oils in this study exhibit a low abundance of petroleum biomarker such as terpanes, steranes and diamondoids and bicyclic sesquiterpanes. Since tight oil from the Bakken region is produced from low-permeability formations, variations in abundance and diagnostic ratios of common target petroleum hydrocarbons were found among these oils.
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- 2017
4. Chemical Fate of Photodegraded Diluted Bitumen in Seawater
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Gong Zhang, Zhendi Wang, Keval Shah, Carl E. Brown, Mike Landriault, Bruce P. Hollebone, Zeyu Yang, Patrick Lambert, and Chun Yang
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Waste management ,Chemistry ,Dilbit ,General Engineering ,Chemical fate ,02 engineering and technology ,010501 environmental sciences ,Crude oil ,01 natural sciences ,020401 chemical engineering ,Asphalt ,Environmental chemistry ,Oil sands ,Seawater ,0204 chemical engineering ,0105 earth and related environmental sciences - Abstract
2017-336:Diluted bitumen (dilbit), an oil sands product, may present new response challenges differing from conventional crude oil in terms of its potential environmental impacts. Simple naphthenic acids (NAs), a complex group of monocarboxylic acids, with a general formula CnH2n+zO2, may be present in the source bitumen or may be created by photolytic weathering. Knowing the composition and concentrations of NAs created during the photo-degradation process of dilbit will help understand the fate, behavior and toxicity of dilbit.In the present study, two diluted bitumen products, Cold Lake Blend (CLB) and Access Western Blend (AWB), were mixed with saltwater and irradiated with natural solar light (Ottawa, Canada, 45.4°N) over winter and summer seasons, to assess the impact of sunlight on the chemical fate of the dilbit. For comparison, a light, sweet crude oil was exposed under similar conditions. The samples were analyzed by high performance liquid chromatography-high resolution mass spectrometry to examine the molecular transformation of diluted bitumen by solar irradiation. The abundances of NAs in all three test oils increased significantly after 90 days of solar irradiation, strongly suggesting that polar NAs were formed by photolysis. Further, greater increases in NAs in the light crude were found than in the two dilbits. Similarly, the lighter oil had higher photolytic removal rates of petroleum hydrocarbons than the two dilbits.The concentrations of NAs in oils exposed during the summer were generally higher than those exposed in winter. During summer exposure, the abundance of total NAs increased up to the 30-day’s solar exposure, then fell again, indicating the transient nature of these compounds. However, net increases in polar NA compounds were observed for all the winter exposed samples. Greater increases were observed in the smaller NA compounds (average C-number decreased), also accompanied by an increase in saturation (average z-number decreased).These chemical changes strongly indicate the effect of sunlight on the potential behaviour, fate and effects of spilled oil, with creation of new resin group compounds and reduction of aromatics and saturates. These changes may affect the viscosity of the oil and its ability to uptake water. These chemical compositions also imply significant changes to the ecological effects of the oil following a spill when aged in sunlight.
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- 2017
5. The photolytic behavior of diluted bitumen in simulated seawater by exposed to the natural sunlight
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Keval Shah, Zhendi Wang, Carl E. Brown, Gong Zhang, Mike Landriault, Zeyu Yang, Bruce P. Hollebone, Chun Yang, and Patrick Lambert
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021110 strategic, defence & security studies ,Aqueous solution ,Chemistry ,General Chemical Engineering ,Chemical structure ,Organic Chemistry ,0211 other engineering and technologies ,Energy Engineering and Power Technology ,02 engineering and technology ,010501 environmental sciences ,Alkylation ,01 natural sciences ,chemistry.chemical_compound ,Fuel Technology ,Reaction rate constant ,Asphalt ,Environmental chemistry ,Organic chemistry ,Petroleum ,Seawater ,Chemical fingerprinting ,0105 earth and related environmental sciences - Abstract
Two diluted bitumen, Cold Lake Blend (CLB), Accessed Western Blend (AWB), and Alberta Sweet Mixed Blend #5 crude oil (ASMB#5), were spiked into 3.3% NaCl aqueous solution, then exposed to natural sunlight for 90 days in the winter and summer in the Northern Hemisphere (Ottawa, Canada). The effects of temperature and solar intensity on the photolytic behavior of diluted bitumen were evaluated. Simultaneously, the photolytic similarities and differences between diluted bitumen and crude oil were compared. It was found that, in all test oils, the decrease of all total petroleum hydrocarbons followed a pseudo-first-order reaction kinetic with the exposure time regardless of seasons. Aromatic fractions had the highest apparent rate constants. Similarly, the chemical fingerprinting analysis of test oils demonstrated that polycyclic aromatic hydrocarbons (PAHs) and their alkylated homologues (APAHs) were the most photosensitive compounds among the identified targets, followed by n-alkanes, then terpanes, and steranes. The photolytic efficiencies of the target petroleum hydrocarbons in ASMB#5 were generally higher than the two diluted bitumen. Photolysis of APAHs occurred faster in summer than in winter; however, APAHs with different number of rings and degree of alkylation did not have obvious photolytic differences. These phenomena suggest that the photolytic similarities between dilbits and conventional crude oil depend on their similar chemical structure of petroleum hydrocarbons; their differences depend on the specific oil properties. The accumulated solar irradiation intensity and temperature are the main factors contributing to their photolytic differences for winter and summer exposed oils.
- Published
- 2016
6. Characterization and differentiation of chemical fingerprints of virgin and used lubricating oils for identification of contamination or adulteration sources
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Mike Landriault, Chun Yang, Zhendi Wang, Zeyu Yang, Carl E. Brown, Patrick Lambert, Bruce P. Hollebone, and Gong Zhang
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Biodiesel ,Waste management ,General Chemical Engineering ,010401 analytical chemistry ,Organic Chemistry ,Energy Engineering and Power Technology ,010501 environmental sciences ,Contamination ,01 natural sciences ,0104 chemical sciences ,chemistry.chemical_compound ,Diesel fuel ,Fuel Technology ,chemistry ,Hazardous waste ,Palm oil ,Environmental science ,Petroleum ,Power output ,Total petroleum hydrocarbon ,0105 earth and related environmental sciences - Abstract
Lubricating oil plays a critical role to reduce friction and to ensure the machines are more energy efficient in terms of fuel consumption and power output. The use of unqualified lube oil can result in malfunctions and damage to engines and machinery. Since petroleum-based lube oils are among the most valuable refined products, in some regions, fake, used, or waste lube oils have occasionally been deliberately adulterated into lube oil to extend the volume sold. On the other hand, used or waste lube oil is hazardous material, containing contaminants such as metals and polycyclic aromatic hydrocarbons produced by the engine during use. It becomes an environmental problem when it is purposely disposed of or accidentally spilled into the environment. Some jurisdictions now have relevant regulations to prohibit these illegal activities; therefore, forensic analysis of lube oils is essential to differentiate fake and used lube products from virgin oils, to identify and to track the adulteration source, and to identify the source of spilled oil. This work involved a fingerprinting analysis of a suite of oil samples including a virgin lube oil, used motor oils, a waste lube oil from a motor workshop, a regular diesel oil and a biodiesel blend, etc. The chemical fingerprints such as the abundance and distribution profiles of total petroleum hydrocarbon, polycyclic aromatic hydrocarbons (PAHs), particularly the higher molecular pyrogenic PAHs, and biomarkers indicate that the used and the waste lube oils are mixtures of mainly lube oil and a small amount of diesel type fuel. The presence of C16 to C20 fatty acid methyl esters (FAME) with the dominance of C16:0 and C18:1 isomers suggests that the used and the waste lube oils both contain residual palm oil-based biodiesel.
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- 2016
7. Occurrence, source and ecological assessment of petroleum related hydrocarbons in intertidal marine sediments of the Bay of Fundy, New Brunswick, Canada
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Michael Goldthorp, Chun Yang, Mike Landriault, Carl E. Brown, Charlotte Crevier, Patrick Lambert, Keval Shah, Bruce P. Hollebone, Sonia Laforest, and Zeyu Yang
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Geologic Sediments ,010504 meteorology & atmospheric sciences ,Intertidal zone ,010501 environmental sciences ,Aquatic Science ,Oceanography ,complex mixtures ,01 natural sciences ,chemistry.chemical_compound ,Alkanes ,medicine ,Coal ,New Brunswick ,Coal tar ,Coke ,Ecosystem ,0105 earth and related environmental sciences ,business.industry ,Tar ,Pollution ,Hydrocarbons ,Nova Scotia ,Petroleum ,chemistry ,Bays ,Benthic zone ,Environmental chemistry ,Environmental science ,Energy source ,business ,Bay ,Water Pollutants, Chemical ,medicine.drug ,Environmental Monitoring - Abstract
Total petroleum hydrocarbons (TPH), n-alkanes, petroleum-related biomarkers of terpanes and steranes, and polycyclic aromatic hydrocarbons (PAHs) were analyzed in the intertidal sediments in the Bay of Fundy, Nova Scotia/New Brunswick, Canada. Sites close to the harbour and more densely populated areas had higher TPH levels than other pristine areas. n-Alkanes presented a typical single bell-shape in n-C16 to n-C35 range and an obvious odd to even carbon preference. Most sites had trace amounts of petroleum biomarkers. Abundant non-alkylated PAHs and lower amounts of alkylated PAHs represented the major input of the incomplete combustion of solid (e.g., coal, coke, biomass, and coal tar) and liquid fuels. The toxicity estimation for PAHs indicates that they did not have potential toxicity to benthic organisms at most sampling sites. However, possible to probable negative effects from the measured PAH concentrations were found for the two samples from Courtenay Bay and Saint Andrews.
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- 2018
8. Fingerprinting Analysis and Source Differentiation of Petroleum-Contaminated Environmental Samples
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Chun Yang, Gong Zhang, Carl E. Brown, Zeyu Yang, Zhendi Wang, Patrick Lambert, Bruce P. Hollebone, and Mike Landriault
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Diagnostic information ,Chromatography ,Primary (chemistry) ,Chemistry ,02 engineering and technology ,010501 environmental sciences ,Contamination ,Diamondoid ,01 natural sciences ,chemistry.chemical_compound ,020401 chemical engineering ,Environmental chemistry ,Petroleum ,0204 chemical engineering ,Chemical fingerprinting ,0105 earth and related environmental sciences - Abstract
This chapter presents specific cases to describe how to apply forensic chemical fingerprinting to characterize and differentiate biogenic and pyrogenic hydrocarbons from petrogenic hydrocarbons in various petroleum-contaminated environmental samples. The most important criteria from quantitative chromatographic analyses are concentrations, distribution profiles and diagnostic ratios of source-specific petroleum compounds such as normal alkanes and isoprenoids, unsubstituted PAHs (polycyclic aromatic hydrocarbons) and their alkylated series, biomarker terpanes and steranes, bicyclic sesquiterpanes and diamondoids. Chromatographic profiles of gas chromatography–flame ionization detection detectable component and distribution of normal alkanes provide primary diagnostic information for the identification and differentiation of petrogenic and biogenic sources. PAH distributions and associated diagnostic ratios, such as pyrogenic index and perylene index, are very useful tools in distinguishing petrogenic hydrocarbons from both pyrogenic and biogenic hydrocarbons. As petroleum-characteristic alkylated PAH homologues and biomarkers are rarely recognized in biogenic and pyrogenic sources, their co-occurrence can be used as an unambiguous indicator of petrogenic contamination, whereas the absence of petroleum-characteristic component and presence of abundant biogenic compounds such as dominant odd-numbered n-alkanes, sterols, fatty acids and alcohols could serve as strong evidences of a predominance of natural organic compounds in samples.
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- 2018
9. List of Contributors
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Puspa L. Adhikari, Matthew Adkins, Joan Albaigés, Hernando P. Bacosa, Gregory Baker, Fred Baldassare, Josep M. Bayona, C.J. Beegle-Krause, Mark J. Benotti, Detlef A. Birkholz, Cornelia Blaga, Chui-Wei Bong, Samantha H. Bosman, Carl E. Brown, Pamela Brunswick, Jeffrey P. Chanton, Elizabeth Chapman, Mei-Hua Chen, Fanny Chever, Jan H. Christensen, Julie Corley, Deborah Crowley, Laura de la Torre, Olívia M.C. de Oliveira, Antônio F. de Souza Queiroz, Majbrit Dela Cruz, Carmen Domínguez, Gregory S. Douglas, William B. Driskell, Stephen Emsbo-Mattingly, Noemi Esquinas, Meredith M. Evans, Nicolas Fitz, James S. Franks, Deborah P. French-McCay, José Luis R. Gallego, Fabiana D.C. Gallotta, A.J. Gravel, Julien Guyomarch, Jeffery Hardenstine, Joshua A. Harrill, Shijie He, Edward (Ted) Healey, Ching-Jen Ho, Bruce Hollebone, Matthew Horn, Wei-Nung Hung, Katherine Jayko, Ronan Jezequel, Paul G.M. Kienhuis, Marcus Kim, John A. Kind, Kerylynn Krahforst, Mette Kristensen, Michael A. Kruge, Christopher L. Kuhlman, Patrick Lambert, Mike Landriault, Azucena Lara-Gonzalo, Stephen R. Larter, Sandra Layland, Lisa Lefkovitz, Yuanwei Li, Zhengkai Li, Danúsia F. Lima, Eric Litman, Bo Liu, Xiaoxing Liu, Zhanfei Liu, Daniel Mendelsohn, Maria de F.G. Meniconi, Buffy M. Meyer, Martin Scott Miles, Glenn C. Millner, Marc A. Mills, Ícaro T.A. Moreira, Paul A. Nony, Thomas B.P. Oldenburg, Gregory M. Olson, Edward B. Overton, Joseph Papineau, Grace Park, James R. Payne, Leo Peschier, R. Paul Philp, Kristoffer G. Poulsen, Jagoš R. Radović, Claudia Y. Reyes, Kelsey L. Rogers, David Runciman, Dayue Shang, Carine S. Silva, Malcolm L. Spaulding, Scott A. Stout, Gordon Todd, Imma Tolosa, Giorgio Tomasi, Vahab Vaezzadeh, Graham van Aggelen, Angela de L.R. Wagener, Chuanyuan Wang, Qing Wang, Zhendi Wang, Shawn M. Wnek, Wendy Wong, Suh-Huey Wu, Chun Yang, Zeyu Yang, Mohamad P. Zakaria, Gong Zhang, and Haijiang Zhang
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- 2018
10. A preliminary study for the photolysis behavior of biodiesel and its blends with petroleum oil in simulated freshwater
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Chun Yang, Gong Zhang, Bruce P. Hollebone, Zeyu Yang, Mike Landriault, Carl E. Brown, Zhendi Wang, and Xinchao Ruan
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Total organic carbon ,chemistry.chemical_classification ,Biodiesel ,General Chemical Engineering ,Radical ,Organic Chemistry ,food and beverages ,Energy Engineering and Power Technology ,complex mixtures ,Diesel fuel ,chemistry.chemical_compound ,Fuel Technology ,chemistry ,Environmental chemistry ,Oil droplet ,Petroleum ,Organic chemistry ,Humic acid ,Solubility - Abstract
With the increasing use of biodiesel and its blends with petroleum fuel, the corresponding environmental issues also occur during its production, application and transportation. The photolysis behavior for biodiesel and the impacts of biodiesel on the photo-oxidation of petroleum hydrocarbons in simulated freshwater was studied by irradiated with ultra violet (UV) and simulated sunlight in the present study. The results indicated that the photolysis rates of fatty acid methyl esters (FAMEs) were mainly depended on their degree of saturation, slightly on water matrices and the initial concentration of biodiesel, regardless of biodiesel sources. Similar results were observed for total organic carbon (TOC) removal rates; however, TOC removal rates were slightly dependent on the initial concentration of biodiesel. The presence of humic acid and pyrogallic acid or lake water matrices slightly inhibited the removal rates of TOC. The photolysis rates of individual petroleum hydrocarbons with and without the presence of biodiesel followed similar rules. In brief, alkanes with light molecular weights were transformed faster than those with heavy molecules, the removal of polycyclic aromatic hydrocarbons (PAHs) were more significantly than alkanes, and the removal of alkylated PAHs (APAHs) increased concurrently with the alkylation level in each family. The presence of biodiesel only inhibited the photolysis of some heavy alkanes and PAHs, not for all other petroleum hydrocarbons. Biodiesel, as a surfactant-like material, could stabilize small oil droplets initially formed by agitation, therefore, these droplets experience longer lifetimes in the water phase before re-aggregating into larger globules and rising to the surface. The apparent solubility of petroleum hydrocarbons, especially for those with heavier molecular weights, has been enhanced in the presence of FAMEs. In this scenario, light needs to penetrate water phase to degrade these targets compared with diesel alone. The direct contacting opportunities between UV light and targets, and radicals produced to attack targets were reduced, which finally resulted in the inhibited photolysis rates of some heavy molecular weight hydrocarbons.
- Published
- 2015
11. Occurrence, source and ecological assessment of baseline hydrocarbons in the intertidal marine sediments along the shoreline of Douglas Channel to Hecate Strait in British Columbia
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Sonia Laforest, Patrick Lambert, Mike Landriault, Carl E. Brown, Michael Goldthorp, Bruce P. Hollebone, Keval Shah, Chun Yang, and Zeyu Yang
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Pollution ,Geologic Sediments ,010504 meteorology & atmospheric sciences ,media_common.quotation_subject ,Intertidal zone ,010501 environmental sciences ,Aquatic Science ,Oceanography ,complex mixtures ,01 natural sciences ,chemistry.chemical_compound ,Benthos ,Polycyclic Aromatic Hydrocarbons ,0105 earth and related environmental sciences ,media_common ,Islands ,British Columbia ,Ecology ,Sediment ,Ecological assessment ,Hydrocarbons ,Petroleum ,Unresolved complex mixture ,chemistry ,Benthic zone ,Environmental science ,lipids (amino acids, peptides, and proteins) ,Water Pollutants, Chemical ,Environmental Monitoring - Abstract
The occurrence, source and ecological assessment of baseline hydrocarbons in the intertidal zone along the northern British shoreline were evaluated based on analyzing total petroleum hydrocarbons (TPH), n-alkanes, petroleum related biomarkers such as terpanes and steranes, and polycyclic aromatic hydrocarbons (PAHs) including non-alkylated and alkylated homologues (APAHs). The TPH levels, n-alkanes, petroleum biomarkers and PAHs in all the sampling sites, except for Masset Harbor/York Point at Gil Island were low, without obvious unresolved complex mixture (UCM) and petroleum contamination input. Specifically, n-alkanes showed a major terrestrial plants input; PAHs with abundant non-alkylated PAHs but minor APAHs showed a major pyrogenic input. However, obvious petroleum-derived hydrocarbons have impacted Masset Harbor. A historical petroleum input was found in York Point at Gil Island, due to the presence of the low level of petroleum biomarkers. Ecological assessment of 13 non-alkylated PAHs in Masset Harbor indicated no potential toxicity to the benthic organisms.
- Published
- 2017
12. Development of a methodology for accurate quantitation of alkylated polycyclic aromatic hydrocarbons in petroleum and oil contaminated environmental samples
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Carl E. Brown, Bruce P. Hollebone, Zhendi Wang, Gong Zhang, Mike Landriault, Chun Yang, Keval Shah, and Zeyu Yang
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Chrysene ,business.industry ,General Chemical Engineering ,General Engineering ,Fluorene ,Phenanthrene ,Analytical Chemistry ,chemistry.chemical_compound ,Petroleum product ,chemistry ,Environmental chemistry ,polycyclic compounds ,Petroleum ,Polycyclic Hydrocarbons ,Gas chromatography–mass spectrometry ,business ,Naphthalene - Abstract
Polycyclic aromatic hydrocarbons (PAHs) are compounds of concern because most of these compounds are toxic, carcinogenic, or mutagenic and are relatively persistent in the environment. Reliable quantitative information of PAHs is important to evaluate the acute and chronic harmful effects of PAHs on the ecosystem. Crude oils and refined petroleum products contain many highly abundant PAHs and heterocyclic PAHs, in particular the alkylated homologues of naphthalene, phenanthrene, dibenzothiophene, fluorene and chrysene (APAH). The alkylated PAH homologues usually occur in significantly higher concentrations than their corresponding unsubstituted parent PAHs. Petrogenic alkylated PAHs generally consist of large numbers of isomers. Unlike those individual unsusbstituted PAHs, most of the APAH isomers are not commercially available. Therefore, historically, the target APAHs are generally quantified using the relative response factors (RRFs) obtained from their respective unsubstituted parent PAH compounds, this inevitably results in the quantitative results of APAH being significantly underestimated. In order to improve the accuracy of the measurement of PAHs and their alkylated homologues in oil and oil related samples, this study measured and compared the response factors of a large number of alkylated PAHs relative to the internal standards in gas chromatography-mass spectrometry (GC-MS) analysis, with the goal of developing a more accurate quantitative methodology for the determination of oil APAHs, and eventually leading to a standardized methodology of quantitative APAH analysis. The PAHs in different oils and related environmental samples collected from oil impacted areas were determined using this GC-MS methodology. Furthermore, the influence of the measurement methodology on the diagnostic ratios of target PAHs was also assessed in this work.
- Published
- 2014
13. Forensic source differentiation of petrogenic, pyrogenic, and biogenic hydrocarbons in Canadian oil sands environmental samples
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Gong Zhang, Ben Fieldhouse, Zhendi Wang, Mike Landriault, Joanne L. Parrott, Y. Liu, C. Yang, Richard A. Frank, Carl E. Brown, Zeyu Yang, L. M. Hewitt, and Bruce P. Hollebone
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Geologic Sediments ,Environmental Engineering ,Health, Toxicology and Mutagenesis ,Industrial Waste ,Fresh Water ,Mining ,Alberta ,chemistry.chemical_compound ,Snow ,Environmental Chemistry ,Oil and Gas Fields ,Waste Management and Disposal ,Environmental engineering ,Coke ,Particulates ,Pollution ,Tailings ,Hydrocarbons ,chemistry ,Asphalt ,Environmental chemistry ,Snowmelt ,Petroleum ,Oil sands ,Environmental Pollutants ,Chemical fingerprinting ,Fuel Oils ,Environmental Monitoring - Abstract
To facilitate monitoring efforts, a forensic chemical fingerprinting methodology has been applied to characterize and differentiate pyrogenic (combustion derived) and biogenic (organism derived) hydrocarbons from petrogenic (petroleum derived) hydrocarbons in environmental samples from the Canadian oil sands region. Between 2009 and 2012, hundreds of oil sands environmental samples including water (snowmelt water, river water, and tailings pond water) and sediments (from river beds and tailings ponds) have been analyzed. These samples were taken from sites where assessments of wild fish health, invertebrate communities, toxicology and detailed chemistry are being conducted as part of the Canada-Alberta Joint Oil Sands Monitoring Plan (JOSMP). This study describes the distribution patterns and potential sources of PAHs from these integrated JOSMP study sites, and findings will be linked to responses in laboratory bioassays and in wild organisms collected from these same sites. It was determined that hydrocarbons in Athabasca River sediments and waters were most likely from four sources: (1) petrogenic heavy oil sands bitumen; (2) biogenic compounds; (3) petrogenic hydrocarbons of other lighter fuel oils; and (4) pyrogenic PAHs. PAHs and biomarkers detected in snowmelt water samples collected near mining operations imply that these materials are derived from oil sands particulates (from open pit mines, stacks and coke piles).
- Published
- 2014
14. Storage stability of commercially available biodiesels and their blends under different storage conditions
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Carl E. Brown, Zhendi Wang, Mike Landriault, Bruce P. Hollebone, Chun Yang, and Zeyu Yang
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chemistry.chemical_classification ,Acid value ,Biodiesel ,Chromatography ,Chemistry ,General Chemical Engineering ,Organic Chemistry ,Energy Engineering and Power Technology ,Fatty acid ,chemistry.chemical_element ,Copper ,Diesel fuel ,Fuel Technology ,Impurity ,Degradation (geology) ,Organic chemistry ,Composition (visual arts) - Abstract
The present study investigated the storage stability of two commercially available biodiesels and their blends with diesel spiked with different impurities, which were stored at two different temperatures (15 and 40 °C) with air tight and light screen. These samples were periodically monitored during the whole storage period by measuring a number of properties, such as acid value (AV), induction time (IT) and composition of fatty acid methyl esters (FAMEs). It was found that (1) acid values increased but induction time decreased with the extension of storage for all samples without copper; however, both IT and AV values kept nearly constant for all samples with copper; (2) the presence of water did not contribute significantly to the degradation of all tested samples over time; and (3) higher temperature (40 °C) was favorable to the degradation of unsaturated FAMEs, accompanying with the altered acid values and induction time in comparison with the same samples stored at 15 °C. Faster degradation of FAMEs in blended samples than those in pure biodiesels may be partially due to the diluting effects of antioxidants in biodiesel. However, the presence of any impurities did not affect the degradation rates of FAMEs, which was not in agreement with the above mentioned AV and IT time series. This suggested that the addition of copper affected the measurement of AV and IT. Therefore, for samples with copper, FAME profiles can represent their quality more appropriately than IT or AV.
- Published
- 2014
15. Aromatic Steroids in Crude Oils and Petroleum Products and Their Applications in Forensic Oil Spill Identification
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Gong Zhang, Zhendi Wang, Yingrong Liu, Chun Yang, Songbai Tian, Patrick Lambert, Mike Landriault, Yan Li, Carl E. Brown, Bruce P. Hollebone, Zeyu Yang, Zelong Liu, and Keval Shah
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animal structures ,Chromatography ,Chemistry ,business.industry ,Ms analysis ,Management, Monitoring, Policy and Law ,law.invention ,Petroleum product ,law ,Oil spill ,Gas chromatography–mass spectrometry ,business ,Waste Management and Disposal ,Distillation ,Volume concentration - Abstract
Aromatic steroids including monoaromatic (MAS) and triaromatic steroids (TAS) are a series of naphthenoaromatic hydrocarbons, which consist of mixed structures of aromatic and saturated 6-carbon or 5-carbon rings. Although these aromatic steroids are in relatively low concentration in oils, their specific fingerprints and high weathering resistance make them desirable biomarkers for the characterization, correlation, differentiation, and source identification in environmental forensic investigations of oil spills. This study presents a quantitative GC/MS analysis of these aromatic hydrocarbons in a number of crude oils and refined petroleum products including light and mid-range distillate fuels, heavy fuels, and lubricating oils collected from various sources. TAS-cholestanes (C26), TAS-ergostanes (C27), and TAS-stigmastanes (C28) are the most distinguishable triaromatic steroids in most oil samples. C26 TAS-cholestane (20R) and C27 TAS-ergostane (20S) are coeluted and often present as the highest peak i...
- Published
- 2013
16. Evaluation of Total Petroleum Hydrocarbons (TPH) Measurement Methods for Assessing Oil Contamination in Soil
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Zhendi Wang, Chun Yang, Zeyu Yang, Carl E. Brown, Mike Landriault, and Bruce P. Hollebone
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chemistry.chemical_classification ,endocrine system ,Silica gel ,chemistry.chemical_element ,Management, Monitoring, Policy and Law ,Contamination ,complex mixtures ,Soil contamination ,humanities ,law.invention ,chemistry.chemical_compound ,Hydrocarbon ,chemistry ,law ,Environmental chemistry ,Petroleum ,Flame ionization detector ,Gas chromatography ,Waste Management and Disposal ,Carbon - Abstract
The most commonly used total petroleum hydrocarbons (TPH) analysis method measures petroleum hydrocarbon concentrations in soil by carbon range that can be detected by gas chromatography/flame ionization detection (GC/FID). Different cleanup procedures have been performed for removing some naturally occurring organics from petrogenic hydrocarbons prior to GC/FID analysis. To evaluate the different pre-treatment methods, more than 60 samples (including background soil and plant samples, as well as oil contaminated soil samples) were sampled from 2008 to 2010 in Canada. TPH values without cleanup (TPH-T), with column cleanup (TPH-F 3) and with in-situ cleanup (TPH-F) were compared to evaluate the effects of different pre-treatment methods on the TPH analysis values. Different total solvent extractable materials (TSEM) loading amounts were applied for in-situ silica gel cleanup method to evaluate the effect of the TSEM loading amount on the measured TPH-F values. The column cleanup method was evaluated by co...
- Published
- 2013
17. Forensic identification of spilled biodiesel and its blends with petroleum oil based on fingerprinting information
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Carl E. Brown, Mike Landriault, Zhendi Wang, Bruce P. Hollebone, Chun Yang, and Zeyu Yang
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chemistry.chemical_classification ,Biodiesel ,Chromatography ,Glyceride ,Fatty acid ,Filtration and Separation ,complex mixtures ,Analytical Chemistry ,chemistry.chemical_compound ,Vegetable oil ,chemistry ,Petroleum ,Organic chemistry ,Polycyclic Hydrocarbons ,Chemical fingerprinting ,Fatty acid methyl ester - Abstract
A case study is presented for the forensic identification of several spilled biodiesels and its blends with petroleum oil using integrated forensic oil fingerprinting techniques. The integrated fingerprinting techniques combined SPE with GC/MS for obtaining individual petroleum hydrocarbons (aliphatic hydrocarbons, polyaromatic hydrocarbons and their alkylated derivatives and biomarkers), and biodiesel hydrocarbons (fatty acid methyl esters, free fatty acids, glycerol, monoacylglycerides, and free sterols). HPLC equipped with evaporative scattering laser detector was also used for identifying the compounds that conventional GC/MS could not finish. The three environmental samples (E1, E2, and E3) and one suspected source sample (S2) were dominant with vegetable oil with high acid values and low concentration of fatty acid methyl ester. The suspected source sample S2 was responsible for the three spilled samples although E1 was slightly contaminated by petroleum oil with light hydrocarbons. The suspected source sample S1 exhibited with the high content of glycerol, low content of glycerides, and high polarity, indicating its difference from the other samples. These samples may be the separated byproducts in producing biodiesel. Canola oil source is the most possible feedstock for the three environmental samples and the suspected source sample S2.
- Published
- 2013
18. Factors affecting oxidation stability of commercially available biodiesel products
- Author
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Bruce P. Hollebone, Chun Yang, Zeyu Yang, Mike Landriault, and Zhendi Wang
- Subjects
Acid value ,General Chemical Engineering ,Induction period ,Energy Engineering and Power Technology ,chemistry.chemical_element ,Copper ,chemistry.chemical_compound ,Fuel Technology ,chemistry ,Pyrogallol ,Acetone ,Organic chemistry ,Methanol ,Butylated hydroxyanisole ,Propyl gallate ,Nuclear chemistry - Abstract
Factors affecting oxidation stability for several commercially available biodiesels were primarily investigated by acid value (AV) and induction period (IP) evaluations in this study. It was found that the measured IP at different storage time points were somewhat dependent on the saturated degree of fatty acid methyl esters (FAMEs), the corresponding measured AV scattered randomly. Generally, AV increased and IP decreased after one year of storing in a dark cold room in an air‐tight tank. Solvents (methanol, acetone and water) did not show a contribution to altering IP. Metals (copper and lead) showed the strongest detrimental effects to oxidative stability although somewhat depending on the particle size and oxide coating thickness, however, aluminum alloy and steel were not the case. Among the antioxidants, pyrogallol (PY) was the best in enhancing IP with a concentration of less than 3000 ppm, however, tert-butylhydroquinone (TBHQ) was the best after 3000 ppm, followed by propyl gallate (PG), butylated hydroxyanisole (BHA), 3,5-di-tert-butyl-4-hydroxyltoluene (BHT), and α-tocopherol. The appropriate dosage of PY was also evaluated to achieve the specified IP regulated by EN-14112 for samples with copper or lead contamination.
- Published
- 2013
19. Effect of storage period on the dominant weathering processes of biodiesel and its blends with diesel in ambient conditions
- Author
-
Zhendi Wang, Chun Yang, Zeyu Yang, Mike Landriault, and Bruce P. Hollebone
- Subjects
Biodiesel ,food.ingredient ,General Chemical Engineering ,Organic Chemistry ,technology, industry, and agriculture ,food and beverages ,Energy Engineering and Power Technology ,complex mixtures ,chemistry.chemical_compound ,Diesel fuel ,Boiling point ,Fuel Technology ,food ,chemistry ,Volume (thermodynamics) ,Environmental chemistry ,Petroleum ,Organic chemistry ,Canola ,Chemical composition ,Chemical decomposition - Abstract
The weathering of petroleum has attracted many researchers’ interest, but the dominant weathering process and storage stability of biodiesel and its blends with diesel under an open air and ambient temperature conditions, and the effect of biodiesel on the evaporation rate of petroleum hydrocarbons were seldom concerned. The present study reported the mass and chemical composition changes in neat biodiesel samples sourced from soybean and canola oil, diesel, and blended with diesel (5% and 20%, volume/volume), at ambient temperature with air exposure lasting for 190 days. The mass-loss curves indicated losses for both the pure diesel and the blends of biodiesel and diesel, but negligible changes in mass for pure biodiesel. The chemical composition of the diesel petroleum hydrocarbons followed the expected evaporative-loss profile, however, fatty acid methyl esters did not show significant loss even after 190 days exposure. The rate of evaporation of fatty acid methyl esters for pure biodiesel or blends is significantly lower than conventional diesel because of the higher boiling point of the biodiesel component compared with some petroleum hydrocarbons. Additionally, losses due to microbial activity and chemical degradation were negligible as the chemical composition of fatty acid methyl esters did not have significant variation from the starting materials even after 190 days exposure to air.
- Published
- 2013
20. Application of Light Petroleum Biomarkers for Forensic Characterization and Source Identification of Spilled Light Refined Oils
- Author
-
Bruce P. Hollebone, Zeyu Yang, Chun Yang, Carl E. Brown, Ben Fieldhouse, Zhendi Wang, and Mike Landriault
- Subjects
chemistry.chemical_classification ,business.industry ,Chemistry ,Polycyclic aromatic hydrocarbon ,Management, Monitoring, Policy and Law ,Diamondoid ,complex mixtures ,Diesel fuel ,chemistry.chemical_compound ,Petroleum product ,Environmental chemistry ,Petroleum ,Polycyclic Hydrocarbons ,Gas chromatography ,Gasoline ,business ,Waste Management and Disposal - Abstract
Light petroleum biomarkers such as bicyclic sesquiterpanes and diamondoids are ubiquitous components of crude oils and ancient sediments, and are also widely found in intermediate petroleum distillates and many finished petroleum products. These compounds are relatively resistant to biodegradation and light-to-medium evaporation weathering, thus particularly useful in oil-source correlation and differentiation for those cases where the traditional tri- to pentacyclic biomarkers are absent. This work utilized sesquiterpanes and diamondoids for fingerprinting and identification of light oils spilled on water. The gas chromatography/flame ionization detection (GC/FID) analysis and distribution profiles of polycyclic aromatic hydrocarbon (PAHs) and conventional biomarkers suggest that the spilled oils are mixtures of mainly gasoline and light diesel type fuel. Since potential source oil candidates were not available, and a large part of the hydrocarbons in gasoline and diesel co-eluted in chromatographic anal...
- Published
- 2012
21. Fingerprinting Analysis and Characterization of Hydrocarbons in Sediment Cores from the Pearl River Estuary, China
- Author
-
Zeyu Yang, Chun Yang, Xianzhi Peng, Mike Landriault, Carl E. Brown, Zhendi Wang, and Bruce P. Hollebone
- Subjects
chemistry.chemical_classification ,geography ,geography.geographical_feature_category ,Sediment ,Estuary ,Management, Monitoring, Policy and Law ,engineering.material ,Contamination ,Diamondoid ,Hydrocarbon ,Dry weight ,chemistry ,Southern china ,Environmental chemistry ,engineering ,Environmental science ,Waste Management and Disposal ,Pearl - Abstract
The Pearl River Delta (PRD) in southern China has undergone rapid urbanization and industrialization over the past few decades, leading to a substantial accumulation of hazardous organic compounds and a significant environmental impact. Forensic analysis of estuarine sediments is critical in order to uncover the contamination history and evaluate the level of contamination of the aquatic system and its ambient regions. A number of hydrocarbons and hydrocarbon groups including polycyclic aromatic hydrocarbons (PAHs), biomarkers, and diamondoids were found in representative sediment cores collected in the Pearl River Estuary (PRE) with average values determined to be 1,300, 288, and 5.85 ng/g dry weight in core #1 (inner shelf) and 283, 26.8, and 2.06 ng/g dry weight in core #2 (outer shelf), respectively. The results clearly suggest that the contamination in PRE sediment was derived from various inputs including petrogenic, biogenic, and pyrogenic sources. Because diamondoids are naturally absent from mode...
- Published
- 2011
22. Determination of polar impurities in biodiesels using solid-phase extraction and gas chromatography-mass spectrometry
- Author
-
Zeyu Yang, Bruce P. Hollebone, Zhendi Wang, Mike Landriault, and Chun Yang
- Subjects
Acid value ,Biodiesel ,food.ingredient ,Chromatography ,Chemistry ,Glyceride ,food and beverages ,Filtration and Separation ,Brassicasterol ,complex mixtures ,Soybean oil ,Analytical Chemistry ,chemistry.chemical_compound ,Vegetable oil ,food ,lipids (amino acids, peptides, and proteins) ,Solid phase extraction ,Gas chromatography–mass spectrometry - Abstract
This paper reports on a method for development and validation for simultaneous characterization and determination of oxygenated polar impurities – free fatty carboxylic acids (FFAs), partial glycerides (monoacylglycerides, MGs), residual glycerol and free sterols – in various biodiesels based on the combination of solid-phase extraction (SPE), silylation and GC/MS technologies. The effects of various SPE and silylation conditions on the method recoveries were evaluated. Using this integrated SPE-GC/MS method, 38 target polar compounds (13 FFAs, 17 glycerides and 8 sterols) in 9 biodiesels derived from 4 different feedstocks were successfully separated and quantified. It was found that the carbon chain length of FFAs was ranged from C6 to C24, with C16 and C18 being the most abundant in all biodiesels. The total FFAs concentration was consistent with the acid values (AVs) measured by standard method ASTM D974-04. MG congeners with carbon number of 18 (mono-C18) were most abundant in the biodiesel samples, followed by mono-C16 and free glycerol. β-Sitosterol and campesterol were found to be the prevailing phytosterols in all pure vegetable oil-based biodiesels, while brassicasterol and stigmasterol was only significant in the biodiesel from canola oil and soybean oil, respectively, and abundant cholesterol was only detected in animal fat-based biodiesels.
- Published
- 2011
23. Forensic differentiation of biogenic organic compounds from petroleum hydrocarbons in biogenic and petrogenic compounds cross-contaminated soils and sediments
- Author
-
Zeyu Yang, Carl E. Brown, J. Sun, C. Yang, Xianzhi Peng, Bruce P. Hollebone, Mike Landriault, F. Kelly-Hooper, and Zhendi Wang
- Subjects
Models, Molecular ,Geologic Sediments ,Environmental remediation ,Carboxylic Acids ,Sensitivity and Specificity ,Biochemistry ,Gas Chromatography-Mass Spectrometry ,Analytical Chemistry ,Petroleum product ,Alkanes ,Soil Pollutants ,Flame Ionization ,chemistry.chemical_classification ,Wax ,Chromatography ,Chemistry ,business.industry ,Fatty Acids ,Organic Chemistry ,Reproducibility of Results ,Soil classification ,General Medicine ,Soil contamination ,Hydrocarbons ,Sterols ,Petroleum ,Hydrocarbon ,visual_art ,Environmental chemistry ,Calibration ,Soil water ,visual_art.visual_art_medium ,Fatty Alcohols ,business - Abstract
"Total petroleum hydrocarbons" (TPHs) or "petroleum hydrocarbons" (PHCs) are one of the most widespread soil pollutants in Canada, North America, and worldwide. Clean-up of PHC-contaminated soils and sediments costs the Canadian economy hundreds of million of dollars annually. Much of this activity is driven by the need to meet regulated levels of PHC in soil. These PHC values are legally required to be assessed using standard methods. The method most commonly used in Canada, specified by the Canadian Council of Ministers of the Environment (CCME), measures the total hydrocarbon concentrations in a soil by carbon range (Fraction 1: C(6)-C(10); Fraction 2: C(10)-C(16), Fraction 3: C(16)-C(34): and Fraction 4: C(34)+). Using the CCME method, all of the materials extractible by a mixture of 1:1 hexane:acetone are considered to be petroleum hydrocarbon contaminants. Many hydrocarbon compounds and other extractible materials in soil, however, may originate from non-petroleum sources. Biogenic organic compounds (BOCs) is a general term used to describe a mixture of organic compounds, including alkanes, sterols and sterones, fatty acids and fatty alcohols, and waxes and wax esters, biosynthesized by living organisms. BOCs are also produced during the early stages of diagenesis in recent aquatic sediments. BOC sources could include vascular plants, algae, bacteria and animals. Plants and algae produce BOCs as protective wax coating that are released back into the sediment at the end of their life cycle. BOCs are natural components of thriving plant communities. Many solvent-extraction methods for assessing soil hydrocarbons, however, such as the CCME method, do not differentiate PHCs from BOCs. The naturally occurring organics present in soils and wet sediments can be easily misidentified and quantified as regulated PHCs during analysis using such methods. In some cases, biogenic interferences can exceed regulatory levels, resulting in remediation of petroleum impacts that are not actually present. Consequently, reliance on these methods can trigger unnecessary and costly remediation, while also wasting valuable landfill space. Therefore, it is critically important to develop new protocols to characterize and differentiate PHCs and BOCs in contaminated sediments. In this study, a new reliable gas chromatography-mass spectrometry (GC-MS) method, in combination with a derivatization technique, for characterization of various biogenic compounds (including biogenic alkanes, sterols, fatty acids and fatty alcohols) and PHCs in the same sample has been developed. A multi-criteria approach has been developed to positively identify the presence of biogenic compounds in soil and sediment samples. More than thirty sediment samples were collected from city stormwater management (SWM) ponds and wetlands across Canada. In these wet sediment samples, abundant biogenic n-alkanes, thirteen biogenic sterols, nineteen fatty carboxylic acids, and fourteen fatty alcohols in a wide carbon range have been positively identified. Both PHCs and BOCs in these samples were quantitatively determined. The quantitation data will be used for assessment of the contamination sites and toxicity risks associated with the CCME Fraction 3 hydrocarbons.
- Published
- 2009
24. EFFECTS OF CHEMICAL DISPERSANT ON OIL SEDIMENTATION DUE TO OIL-SPM FLOCCULATION: EXPERIMENTS WITH THE NIST STANDARD REFERENCE MATERIAL 1941?
- Author
-
Chun Yang, Ali Khelifa, Zhendi Wang, Merv Fingas, Carl E. Brown, Ben Fieldhouse, and Mike Landriault
- Subjects
Flocculation ,Materials science ,Environmental chemistry ,Oil droplet ,Environmental engineering ,Sedimentation ,Particulates ,Sediment concentration ,Dispersant ,Corexit - Abstract
As it is well established that application of chemical dispersant to oil slicks enhances the concentration of oil droplets and reduces their size, chemical dispersants are expected to enhance oil sedimentation if applied in coastal waters rich in suspended particulate matter (SPM) and if flocculation between chemically dispersed oil and SPM, which leads to formation of oil-SPM aggregates (OSAs), occurs readily. New laboratory experiments were conducted to establish a quantitative understanding of the process and to verify this hypothesis. This paper presents findings from experiments conducted using Standard Reference Material 1941b prepared by the National Institute of Standards and Technology, Arabian Medium, Alaska North Slope and South Louisiana crude oils, and Corexit 9500 and Corexit 9527 chemical dispersants. Results showed that OSAs do form with chemically dispersed oil. Oil sedimentation increases with sediment concentration and reach a maximum at a sediment-to-oil ratio of approximately 2:1 for most of the oils used. No obvious effect of chemical dispersant on oil sedimentation was measured for sediment concentration of 100 mg/L and higher. However, measured oil sedimentation was 3 to 5 times higher with chemical dispersant than with physically dispersed oil at low sediment concentration of 25 and 50 mg/L. UV epi-fluorescence microscopy showed that OSAs formed with chemically dispersed oil contain many oil droplets that are smaller than those trapped in OSAs formed with physically dispersed oil.
- Published
- 2008
25. APPLICATION OF STATISTICAL ANALYSIS IN THE SELECTION OF DIAGNOSTIC RATIOS FOR FORENSIC IDENTIFICATION OF AN OIL SPILL SOURCE
- Author
-
Chun Yang, Zhendi Wang, Mike Landriault, Bruce P. Hollebone, and Carl E. Brown
- Subjects
Forensic identification ,Chromatography ,Chemistry ,Oil spill ,Analytical chemistry ,Statistical analysis ,Gas chromatography ,Diamondoid - Abstract
In this work, 14 fresh crude oils of different types and origins were analyzed by gas chromatography with mass-selective detection, and over 80 potentially diagnostic ratios were calculated based on the quantitation of isoprenoids, polycyclic aromatic hydrocarbons (PAHs), biomarkers, diamondoids, bicyclic sesquiterpanes and aromatic steranes, etc. Diagnostic power (DP) was calculated for the selection of the candidate source-sensitive diagnostic ratios and used to determine which ratios were most diagnostic among the crude oils studied. In order to investigate the effect of evaporative and biodegradative weathering on diagnostic ratios and thereby to differentiate weathering-resistant ratios from weathering-sensitive ratios, triplicate analyses were performed for two suites of reference oils, laboratory-evaporated Prudhoe Bay crude oils and laboratory-biodegraded Alberta Sweet Mixed Blend (ASMB) crude oils, respectively. Student'S t-test was used to statistically evaluate whether diagnostic ratios were significantly affected by weathering and to ensure that the observed change is not due to analytical variance. It was found that, diagnostic ratios generally remained consistent for oils with slight to medium evaporative weathering, only the ratios of those compounds with lower boiling points such as adamantanes changed greatly. For biodegraded oils, most of diagnostic ratios remained constant for lightly to moderately biodegraded oils; while most of diagnostic ratios with exception of certain triaromatic steranes and high-molecular-weight terpane and sterane biomarkers demonstrated significant changes for heavily biodegraded oils.
- Published
- 2008
26. AQUEOUS SOLUBILITY, DISPERSIBILITY AND TOXICITY OF BIODIESELS
- Author
-
Paula Jackman, Ben Fieldhouse, K. Doe, Mike Landriault, and Bruce P. Hollebone
- Subjects
Diesel fuel ,Biodiesel ,chemistry.chemical_compound ,Aqueous solution ,Materials science ,Waste management ,chemistry ,Tallow ,Biofuel ,Aquatic ecosystem ,Environmental chemistry ,Aqueous two-phase system ,Petroleum - Abstract
With increasing interest in the use of plant and animal oils as potential petroleum fuel replacements, there is the potential for accidental release of these biodiesels to the environment. While the behaviours and effects of petroleum diesels have been extensively studied, little is known about either the fate of biofuels in water or their potential effects on aquatic ecosystems. The most important mechanism for exposure of aquatic ecosystems to biodiesels and petroleum diesels is the transfer of material from the non-aqueous phase liquid (NAPL) into the aqueous phase, as both soluble and dispersed components. The equilibrium levels of fuel components in the water, the water-accommodated fractions (WAF) have been measured in fresh water for biodiesels from feedstocks of soy oil, canola oil, waste fry tallow and fish wastes. Biodiesel and petroleum diesels blends of 5% (B5) and 20% (B20) are also measured. Aqueous toxicities are also reported for pure biodiesels and petroleum diesel. Acute toxicities were assessed by 96-hour LC5os of Daphnia magna and rainbow trout and by IC5os of bioluminescent bacteria. The correlations between acute toxicity, WAF concentrations and fuel property data are examined. Natural and chemically-enhanced dispersion of biodiesel is examined in both low- and high-energy conditions. Biodiesels are found to have significant differences with petroleum diesels in water chemistries and in potential ecological impacts. All organisms tested show that biodiesels have less acute toxicity than petroleum diesels. Biodiesels and biodiesel-rich blends were found to be very much more dispersible in high-energy conditions than petroleum diesel.
- Published
- 2008
27. SOURCE IDENTIFICATION OF SPILLED DIESEL USING DIAGNOSTIC SESQUITERPANES AND DIAMONDOIDS
- Author
-
Bruce P. Hollebone, Carl E. Brown, Mike Landriault, Zhendi Wang, and C. Yang
- Subjects
Diesel fuel ,Biomarker (petroleum) ,Petroleum engineering ,Chemistry ,Oil spill ,Diamondoid - Abstract
Examination of GC-MS chromatograms of bicyclic biomarker sesquiterpanes and diamondoids using their characteristic fragment ions provides another highly diagnostic means for correlation and differentiation of unknown spilled oil samples that are difficult to identify by current fingerprinting techniques. In this work, GC-FID and GC-MS fingerprinting analysis in conjunction with statistical data analysis of target oil hydrocarbons including sesquiterpanes and diamondoids was performed for identification of an unknown oil spill incident occurred in a harbor of the Netherlands in 2004. Forensic investigation included the: (1) identification and characterization of numerous sesquiterpanes and diamondoids; (2) comparison of the distribution of sesquiterpanes and diamondoids; (3) development of a series of diagnostic indices for correlation and differentiation of spilled fuel samples; and (4) use of “Two-tailed” unpaired Student'S t-test to statistically evaluate the imperceptible differences between the selected diagnostic ratios of target compounds in the spill fuel and the suspected source fuel samples. At a 95% confidence interval, 33 of all 38 diagnostic indices (among them, 20 are diagnostic indices of sesquiterpanes and diamondoids) show positive matches between spill sample and suspected source fuel sample 1. In comparison, only 5 of 38 diagnostic indices indicate positive matches between spill sample and suspected source sample 3. These evidences demonstrate that the bunker ship has the responsibility for this oil spill incident.
- Published
- 2008
28. A CASE STUDY: DISTINGUISHING PYROGENIC HYDROCARBONS FROM PETROGENIC HYDROCARBONS
- Author
-
Mike Landriault, Carl E. Brown, Zhendi Wang, Bruce P. Hollebone, and C. Yang
- Subjects
Chrysene ,Fluoranthene ,Anthracene ,chemistry.chemical_compound ,chemistry ,Environmental chemistry ,Organic chemistry ,Pyrene ,Phenanthrene - Abstract
A new diagnostic parameter of “Pyrogenic Index (PI),” defined as(other 3–6 ring EPA priority PAHs)/N(5 alkylated PAHs), has been proposed as a quantitative indicator for identification of pyrogenic PAHs and for differentiating pyrogenic from petrogenic PAHs. It has been well understood that petrogenic and pyrogenic PAHs are characterized by dominance of five alkylated PAH homologues and by dominance of unsubstituted high molecular weight PAHs, respectively. In comparison with traditional diagnostic ratios such as phenanthrene/anthracene (Ph/An), benz[a]anthracene/chrysene (BaA/Ch), and fluoranthene/pyrene (Fl/Py), the PI Index more truly reflects the difference in the PAH distribution between these two sets of PAHs. The PI Index has been successfully used as an effective criterion to unambiguously differentiate pyrogenic and petrogenic PAHs. In this paper a case study is presented to illustrate the utility of the PI index to distinguish the pyrogenic PAHs generated by burning from the petrogenic PAHs. On October of 2004, a fire accident happened in the HMCE Chicoutimi submarine at sea off the west coast of Ireland as the submarine was making its way to Halifax, Canada. In order to determine effects of the fire accident on the health of crew members, a number of fire samples were collected and sent to the ESTD for characterization. Sample characterization results clearly revealed that the distribution profiles of PAHs in the samples are combined signatures from both pyrogenic and petrogenic PAHs. The pyrogenic PAHs were generated from the fire accident, while the petrogenic PAHs came from contamination of petroleum products used by the submarine. The presence of petroleum hydrocarbons is further confirmed by the discovery of oil-characteristic n-alkanes and biomarker compounds in the fire samples.
- Published
- 2008
29. Chromatographic Fingerprinting Analysis of Crude Oils and Petroleum Products
- Author
-
Zhendi Wang, Bruce P. Hollebone, Carl E. Brown, Chun Yang, Zeyu Yang, and Mike Landriault
- Subjects
chemistry.chemical_compound ,Biomarker (petroleum) ,Petroleum product ,Chromatography ,chemistry ,business.industry ,Oil spill ,Petroleum ,Gas chromatography–mass spectrometry ,business ,Diamondoid - Published
- 2015
30. GC/MS Quantitation of Diamondoid Compounds in Crude Oils and Petroleum Products
- Author
-
Mike Landriault, Bruce P. Hollebone, Xianzhi Peng, Zhendi Wang, Mervin F. Fingas, and C. Yang
- Subjects
Chromatography ,business.industry ,Management, Monitoring, Policy and Law ,Diamondoid ,Mass spectrometry ,law.invention ,chemistry.chemical_compound ,Diesel fuel ,Petroleum product ,chemistry ,law ,Gas chromatography ,Gas chromatography–mass spectrometry ,business ,Waste Management and Disposal ,Diamantane ,Distillation - Abstract
This study presents a quantitative gas chromotography/mass spectrometry (GC/MS) method for the analysis of adamantane, diamantane, and their alkylated homologues in 14 crude oils and 22 petroleum products including light and mid-range distillate fuels, residual fuels, and lubricating oils collected from various sources. The method detection limits for five target diamondoids were in the range of 0.06 to 0.14 μ g/g oil. The total concentration of adamantane and its 16 alkylated homologues commonly range from approximately 40 to 500 μ g/g in most crude oils and from 0.6 to 1,300 μ g/g in refined products, but reaching values of up to 2,000 μ g/g for the south Louisiana crude oil and the Jet A fuel. Diamantanes occur in all crude oils and lighter to middle distillates, and their total concentration was in a range of 5 to 200 μ g/g and with maximum values near 600 μ g/g in weathered diesel fuel, but they were not detected in very light distillates and most lubricating oils. Laboratory distillation of crude oi...
- Published
- 2006
31. OIL COMPOSITION AND PROPERTY DATABASE FOR OIL SPILL MODELING
- Author
-
L. Gamble, Chun Yang, Xianzhi Peng, Mike Landriault, Zhendi Wang, Ben Fieldhouse, Bruce P. Hollebone, Mervin F. Fingas, and J. Weaver
- Subjects
Engineering ,Database ,Petroleum engineering ,Property (programming) ,business.industry ,Oil spill ,Multiple component ,Fractionation ,computer.software_genre ,business ,computer - Abstract
At the request of the US EPA Oil Program Center, the National Exposure Research Laboratory's Ecosystems Research Division (ERD) in Athens is developing an oil spill model that focuses on fate and transport of oil components under various response scenarios. A database of prototype oils for use in models is necessary. This multiple component composition data, however, is not typically available because of complexity of oil composition and the impossibility of immediate characterization in the event of a spill. Thus the creation of a database containing both physical property and chemical composition data for a number of common oils at various weathering percentages is highly desirable. The data set must be based upon fractionation of the oils into groups of compounds with similar structures and properties and further must reflect the changes to the oil over the course of the spill. Since 1984, the Emergencies Science and Technology Division (ESTD) of Environment Canada (EC) has developed a database on various physical and chemical properties of crude oils and petroleum products. Through many years endeavour, the database now contains information of hundreds of oils from all over the world. In 2002, funded by the US EPA and EC, the ESTD and ERD completed the cooperative project “Development of a Composition Database for Selected Multicomponent Oils,” to characterize ten prototype crude oils and refined petroleum products. The present work, Oil Composition and Property Database for Oil Spill Modeling, is a logical extension of the 2002 project. Nine new crude oils in common use and with potential to be spilled in the US waters were selected for inclusion in the model database. Comprehensive physical property measurement and chemical composition characterization have been performed for these oils at four weathered stages of each oil. This project provides the most complete and comprehensive database for the selected oils to date. The new composition data has been integrated into the existing US EPA and EC oil properties database. The results are made available to the public on the world wide web.
- Published
- 2005
32. SOURCE IDENTIFICATION OF AN UNKNOWN SPILL (2002) FROM QUEBEC BY THE MULTI-CRITERION ANALYTICAL APPROACH AND LAB SIMULATION OF THE SPILL SAMPLE
- Author
-
C. Yang, Mike Landriault, Bruce P. Hollebone, Zhendi Wang, and Mervin F. Fingas
- Subjects
Engineering ,Identification (information) ,Petroleum engineering ,business.industry ,Oil spill ,Sample (statistics) ,business - Abstract
This paper describes a case study of an oil spill into Canal Ste-Anne-de-Bellevue, Quebec in 2002. In response to this specific oil identification need, a lab spill simulation was designed to obtain simulated spill samples from the suspected source samples. The integrated multi-criterion approach using GC/MS and GC/FID was then applied for fingerprinting and identifying the spill oil samples. The distribution patterns of hydrocarbons in the spill and suspected source samples were recognized and compared. Analysis of oil-characteristic biomarkers and the extended suite of parent and alkylated polycyclic aromatic hydrocarbons (PAH) were performed. A variety of diagnostic ratios of “source-specific marker” compounds for interpreting chemical fingerprinting data were determined and analyzed. Finally, the major components in suspected source samples were identified. The detailed chemical characterization data highlight that: (1) the spilled oil 264 is diesel fuel, while the suspected source sample 265 is an emulsified Bunker C type fuel; (2) another suspected source sample 266 is a de greaser-type “pine oil” product; (3) the synthetic spill sample from 265 and 266 has a completely different GC profile and chemical composition from the spill sample 264. No component of sample 266 was found and recognized in sample 264.
- Published
- 2005
33. THE DYNAMICS OF ORIMULSION IN WATER WITH VARYING ENERGY, SALINITY AND TEMPERATURE
- Author
-
Zhendi Wang, Mike Landriault, Ben Fieldhouse, and Merv Fingas
- Subjects
Orimulsion ,geography ,Buoyancy ,geography.geographical_feature_category ,Brackish water ,Chemistry ,Environmental engineering ,Soil science ,engineering.material ,Sink (geography) ,Salinity ,Thermal ,Emulsion ,Particle-size distribution ,engineering - Abstract
Orimulsion is an oil-in-water emulsion of Venezuelan bitumen. Orimulsion was found to behave predictably in salt (33°/oo NaCl) and fresh water, driven by buoyancy to rise in salt water and sink in fresh water; but behaviour in brackish water (20°/oo NaCl) was difficult to predict. Temperature has also been indicated as having an influence on Orimulsion behaviour. The current study extended experimentation down to lower temperatures, and a variety of mixing energies. This study resulted in new information on the behaviour of Orimulsion spills in salt, fresh, and brackish water with salinity values of 20 and 33 degrees at temperatures of 5 and 15 degrees Celsius. Energy was varied by adjusting the applied rotational field and measurement with thermal probes. Depletion rates and characteristics were determined by adding Orimulsion to a 300-L tank of water, taking a time series of samples, and determining the concentration of bitumen and the particle size distribution. Changes in bitumen concentration and particle size distribution as a function of time were also measured. Using these data, simple equations were developed to describe and predict the concentration of bitumen in the water column as a function of time. Similarly nomograms showing the amount of oil on the bottom and on the water surface are presented.
- Published
- 2005
34. Development of a Composition Database for Selected Multicomponent Oils
- Author
-
Jordan Noonan, Bruce P. Hollebone, G. Thouin, Mike Landriault, L. Sigouin, Zhendi Wang, Ben Fieldhouse, J. Weaver, and Merv Fingas
- Subjects
chemistry.chemical_classification ,Petroleum engineering ,Database ,business.industry ,Pour point ,computer.software_genre ,API gravity ,Boiling point ,Hydrocarbon ,Petroleum product ,chemistry ,Flash point ,business ,Water content ,computer ,Chemical composition - Abstract
Multicomponent composition and corresponding physical properties data of crude oils and petroleum products are needed as input to environmental fate simulations. Complete sets of such data, however, are not available in the literature due to the complexity and expense of making the measurements. Environment Canada has previously developed a database of various physical and chemical properties of crude oils and petroleum products. In this cooperative project, ten “typical” crude oils and refined products in common use or transport were identified for subsequent characterization. Measured oil physical properties include API gravity, density, sulphur content, water content, flash point, pour point, viscosity, surface and interfacial tension, adhesion, the equation for predicting evaporation, emulsion formation, and simulated boiling point distribution. The chemical composition of the oils are quantified for hydrocarbon groups, volatile organic compounds, n-alkane distribution, distribution of alkylated polyaromatic hydrocarbon (PAH) homologues and other EPA priority PAHs, and biomarker concentrations. This project will provide the most complete and comprehensive database for the selected oils to date. The new composition data will be integrated into the existing Environment Canada oil properties database. The results will be made available to the public both on the world wide web and as a database on disc.
- Published
- 2003
35. The Effect of Varying Salinity and Temperature on the Dynamics of Orimulsion in Water
- Author
-
Merv Fingas, Ron MacKay, Jordan Noonan, Zhendi Wang, and Mike Landriault
- Subjects
Orimulsion ,Salinity ,Hydrology ,geography ,geography.geographical_feature_category ,Buoyancy ,Brackish water ,Chemistry ,Environmental chemistry ,Particle-size distribution ,engineering ,engineering.material ,Sink (geography) - Abstract
Studies have shown that Orimulsion behaves somewhat predictably in saltwater (33 ppt NaCl) and freshwater, driven by buoyancy to rise in saltwater and sink in freshwater, but behaviour in brackish water (20 ppt NaCl) is difficult to predict. Temperature has also been indicated as having an influence on Orimulsion behaviour. The current study extended experimentation to lower temperatures and a large number of salinity values, ranging from fresh to saltwater. This study resulted in information on the behaviour of Orimulsion spills in salt, fresh, and brackish water with salinity values ranging from 0.1 to 33 °/oo at temperatures of 5 and 15 °C. Depletion rates and characteristics were determined by adding Orimulsion to a 300-L tank of water, taking a time series of samples, and determining the concentration of bitumen and the particle size distribution. Changes in bitumen concentration and particle size distribution as a function of time were also measured. Resurfaced bitumen was scraped from the top of the tank and weighed to determine the amount rising. Using these data, simple equations were developed to describe and predict the concentration of bitumen in the water column as a function of time. Similarly, nomograms showing the amount of oil on the bottom and on the water surface are presented.
- Published
- 2003
36. Development In Fingerprinting Analysis of Petroleum Hydrocarbons
- Author
-
Mervin F. Fingas, L. Sigouin, Mike Landriault, Zhendi Wang, David Hostetter, and Bill Castle
- Subjects
chemistry.chemical_compound ,Petroleum product ,Petroleum engineering ,chemistry ,Waste management ,business.industry ,Petroleum ,business - Abstract
Major advances have been made on analyses of petroleum hydrocarbons in oils, petroleum products and complex oil-spill-related environmental samples. This paper briefly describes how the advanced chemical fingerprinting and data interpretation techniques are used to identify the source(s) of tarballs from the coast of Vancouver Island and Northern California. Characterization of the unknown oil was achieved by not only a variety of “standard” analyses including distribution analyses of aliphatic, aromatic and biomarker hydrocarbons, but also analyses of diagnostic ratios of “source-specific marker” compounds, in particular the alkylated series of polycyclic aromatic hydrocarbons within the same alkylation isomeric groups. Results of the analysis revealed that (1) California/Oregon and British Columbia/Washington tarball samples were chemically similar, but were identified to be from two different types of bunker fuel; (2) the source of the tarball samples was neither Alaska North Slope oil nor California Monterrey Miocene oil; and (3) the spilled oil samples have been highly weathered since release, and the California samples were more heavily weathered than the British Columbia samples.
- Published
- 1999
37. PAH Distribution in the 1994 and 1997 Mobile Burn Products and Determination of the Diesel PAH Destruction Efficiencies
- Author
-
Patrick Lambert, Rod Turpin, L. Sigouin, Zhendi Wang, Mervin F. Fingas, Joseph V. Mullin, Mike Landriault, and Phil Campagna
- Subjects
Diesel fuel ,Waste management ,Chemistry ,Environmental engineering ,complex mixtures - Abstract
In 1994 and 1997, several U.S. and Canadian government agencies jointly conducted a series of mesoscale burns in Mobile Bay, Alabama, to study various aspects of in situ diesel fuel burning. Samples were taken from the oil, residue and the smoke plume during each burn and analysed by capillary gas Chromatograph/mass spectrometry (GC/MS). Analysis results reveal that the PAH distribution patterns in the diesel, residue, and soot samples are significantly different from each other. A simple model based on mass balance of individual petroleum ?AHs pre- and post-burn is proposed to estimate the destruction efficiencies of the total petroleum PAHs. The average destruction efficiency of the total diesel PAHs from three 1994 Mobile burns was estimated to be greater than 99%. The high molecular weight PAHs with five or more rings were found to be largely generated by combustion. These studies demonstrated that under certain circumstances, in situ burning is an effective measure to minimise the impact of an oil spill on the environment and to reduce the damage of an oil spill to the ecological system.
- Published
- 1999
38. Comparison of oil composition changes due to biodegradation and physical weathering in different oils
- Author
-
Julia M. Foght, Sandra Blenkinsopp, Gary A. Sergy, Merv Fingas, Mike Landriault, Kathleen M. Semple, Donald W. S. Westlake, L. Sigouin, and Zhendi Wang
- Subjects
Canada ,Chromatography, Gas ,Chemical Phenomena ,Environmental pollution ,Weathering ,Biochemistry ,Gas Chromatography-Mass Spectrometry ,Analytical Chemistry ,chemistry.chemical_compound ,Petroleum product ,Polycyclic Aromatic Hydrocarbons ,Chemical composition ,chemistry.chemical_classification ,Chromatography ,Bacteria ,Chemistry, Physical ,Chemistry ,business.industry ,Organic Chemistry ,Water ,General Medicine ,Biodegradation ,Hydrocarbons ,Biodegradation, Environmental ,Petroleum ,Biomarker (petroleum) ,Hydrocarbon ,Environmental chemistry ,Environmental Pollution ,business - Abstract
The well-characterized Alberta Sweet Mixed Blend oil and several other oils which are commonly transported in Canada were physically weathered and then incubated with a defined microbial inoculum. The purpose was to produce quantitative data on oil components and component groups which are more susceptible or resistant to biodegradation, and to determine how oils rank in relation to each other in terms of biodegradation potential. The biodegraded oils were characterized by quantitative determination of changes in important hydrocarbon groups including the total petroleum hydrocarbons, total saturates and aromatics, and also by quantitation of more than 100 individual target aliphatic, aromatic and biomarker components. The study reveals a pattern of distinct oil composition changes due to biodegradation, which is significantly different from the pattern due to physical or short-term weathering. It is important to be able to distinguish between these two forms of loss, so that loss due to weathering is not interpreted as loss due to biodegradation in the laboratory or in the field. Based on these findings, the oil composition changes due to biodegradation can be readily differentiated from those due to physical weathering. To rank the tested oils with respect to biodegradability, losses in total petroleum hydrocarbons and aromatics were used to calculate biodegradation potential indices, employing equations proposed by Environment Canada and the US National Oceanic and Atmospheric Administration. The different methods produced very similar biodegradation trends, confirming that patterns of oil biodegradability do exist.
- Published
- 1998
39. Method development for forensic identification of biodiesel based on chemical fingerprints and corresponding diagnostic ratios
- Author
-
Zeyu Yang, Carl E. Brown, Chun Yang, Zhendi Wang, Mike Landriault, and Bruce P. Hollebone
- Subjects
chemistry.chemical_classification ,Biodiesel ,Chromatography ,Stigmasterol ,Chemistry ,Campesterol ,Fatty acid ,Brassicasterol ,Sterol ,Pathology and Forensic Medicine ,chemistry.chemical_compound ,Glycerol ,Organic chemistry ,Law ,Chemical fingerprinting - Abstract
A forensic identification method based on the chemical fingerprinting of the first generation of biodiesel (fatty acid alkyl esters as effective components), and several corresponding diagnostic ratios was developed and validated. The distribution of major fatty acid methyl esters (FAMEs) and polar compounds (free fatty acids, glycerol, monoacylglycerides, and free sterols) in several representative above biodiesel products commercially available in Canada were positively quantified and compared, a number of cross-plots of diagnostic ratios of target FAMEs and sterols were developed for biofuel correlation and differentiation. It was found that the cross-plots of FAME ratios, for example, the sum of the di-unsaturated relative to saturated homologues of FAMEs (D/S) versus the sum of the mono-saturated to saturated FAMEs (M/S), and the sum of di-unsaturated to mono-saturated FAMEs (D/M) versus the sum of the mono-saturated to saturated FAMEs (M/S), could cluster samples clearly into their individual feedstock. The cross-plots of diagnostic ratios of individual major sterols (cholesterol, brassicasterol, campesterol, β-stiosterol and stigmasterol) to the total sterols were also developed and proved to be effective in identifying biodiesel sources due to their self-normalizing effect on sterol data. The case study of a mystery biodiesel spill using this method showed that the two real samples can be tightly clustered into biodiesel from animal fat (Ban) group. However, the significant discrepancy of free fatty acids, glycerol, monoacylglycerides and sterol concentrations between the two real samples indicated their different producing batches.
- Published
- 2013
40. Forensic identification of spilled biodiesel and its blends with petroleum oil based on fingerprinting information
- Author
-
Zeyu, Yang, Bruce P, Hollebone, Zhendi, Wang, Chun, Yang, Carl, Brown, and Mike, Landriault
- Subjects
Quality Control ,Petroleum ,Biofuels ,Forensic Sciences ,Gas Chromatography-Mass Spectrometry ,Hydrocarbons - Abstract
A case study is presented for the forensic identification of several spilled biodiesels and its blends with petroleum oil using integrated forensic oil fingerprinting techniques. The integrated fingerprinting techniques combined SPE with GC/MS for obtaining individual petroleum hydrocarbons (aliphatic hydrocarbons, polyaromatic hydrocarbons and their alkylated derivatives and biomarkers), and biodiesel hydrocarbons (fatty acid methyl esters, free fatty acids, glycerol, monoacylglycerides, and free sterols). HPLC equipped with evaporative scattering laser detector was also used for identifying the compounds that conventional GC/MS could not finish. The three environmental samples (E1, E2, and E3) and one suspected source sample (S2) were dominant with vegetable oil with high acid values and low concentration of fatty acid methyl ester. The suspected source sample S2 was responsible for the three spilled samples although E1 was slightly contaminated by petroleum oil with light hydrocarbons. The suspected source sample S1 exhibited with the high content of glycerol, low content of glycerides, and high polarity, indicating its difference from the other samples. These samples may be the separated byproducts in producing biodiesel. Canola oil source is the most possible feedstock for the three environmental samples and the suspected source sample S2.
- Published
- 2013
41. Forensic fingerprinting and source identification of the 2009 Sarnia (Ontario) oil spill
- Author
-
J. Sun, Zhendi Wang, Zeyu Yang, Mike Landriault, C. Yang, Carl E. Brown, and Bruce P. Hollebone
- Subjects
chemistry.chemical_classification ,Ontario ,Waste management ,Sample (material) ,Public Health, Environmental and Occupational Health ,Polycyclic aromatic hydrocarbon ,General Medicine ,Management, Monitoring, Policy and Law ,Mass spectrometry ,Gas Chromatography-Mass Spectrometry ,Diesel fuel ,Hydrocarbon ,chemistry ,Environmental chemistry ,Environmental science ,Petroleum Pollution ,Bilge ,Polycyclic Aromatic Hydrocarbons ,Bilge pump ,Chemical fingerprinting ,Fuel Oils ,Gasoline ,Environmental Monitoring - Abstract
This paper presents a case study in which integrated forensic oil fingerprinting and data interpretation techniques were used to characterize the chemical compositions and determine the source of the 2009 Sarnia (Ontario) oil spill incident. The diagnostic fingerprinting techniques include determination of hydrocarbon groups and semi-quantitative product-type screening via gas chromatography (GC), analysis of oil-characteristic biomarkers and the extended suite of parent and alkylated PAH (polycyclic aromatic hydrocarbon) homologous series via gas chromatography-mass spectrometry (GC-MS), determination and comparison of a variety of diagnostic ratios of "source-specific marker" compounds, and determination of the weathering degree of the spilled oil, and whether the spilled oil hydrocarbons have been mixed with any other "background" chemicals (biogenic and/or pyrogenic hydrocarbons). The detailed chemical fingerprinting data and results reveal the following: (1) all four samples are mixtures of diesel and lubricating oil with varying percentages of diesel to lube oil. Both samples 1460 and 1462 are majority diesel-range oil mixed with a smaller portion of lube oil. Sample 1461 contains slightly less diesel-range oil. Sample 1463 is majority lubricating-range oil. (2) The diesel in the four diesel/lube oil mixture samples was most likely the same diesel and from the same source. (3) The spill sample 1460 and the suspected-source sample 1462 have nearly identical concentrations and distribution patterns of target analytes including TPHs, n-alkane, PAHs and biomarker compounds; and have nearly identical diagnostic ratios of target compounds as well. Furthermore, a perfect "positive match" correlation line (with all normalized ratio data points falling into the straight correlation line) is clearly demonstrated. It is concluded that the spill oil water sample 1460 (#1, from the water around the vessel enclosed by a boom) matches with the suspected source sample 1462 (#3, from the vessel engine room bilge pump). (4) From the n-alkane and PAH analysis, it appears that the oil in the spill sample 1460 is slightly more weathered in comparison with sample 1462. The minor differences in fingerprints of two samples were most likely caused by weathering effects. (5) Sample 1461 (#2, from the vessel engine room bilge) and sample 1463 (#4, from the vessel bilge waste collection tank) demonstrated significantly different fingerprints and diagnostic ratios of target compounds from that of spill sample 1460. This was caused most likely by percentages of diesel to lube oil in these two samples different from that in spill sample 1460.
- Published
- 2011
42. Method development for fingerprinting of biodiesel blends by solid-phase extraction and gas chromatography-mass spectrometry
- Author
-
Zeyu, Yang, Bruce P, Hollebone, Zhendi, Wang, Chun, Yang, and Mike, Landriault
- Subjects
Biofuels ,Solid Phase Extraction ,Gas Chromatography-Mass Spectrometry ,Gasoline ,Hydrocarbons - Abstract
A method based on the combination of solid-phase extraction (SPE) with gas chromatography-mass spectrometry (GC/MS) for detailed chemical fingerprinting of biodiesel/petrodiesel blends was developed in the present study. Forensic identification, commonly referred to as chemical fingerprinting, is based on the relative distributions of individual aliphatic hydrocarbons, aromatic hydrocarbons, fatty acid alkyl esters, and free sterols. Fractionation of fuel samples is optimized for the separation of fatty acid esters and free sterols from petroleum hydrocarbons into four fractions: aliphatic, aromatic, fatty acid ester, and polar components. The final recoveries of aliphatic and aromatic hydrocarbons were determined to be in the range of 65-103%, 73-105% for FAMEs, and 78-103% for free sterols in the polar fraction. Excellent separation with negligible crossover of components with different polarities between fractions was observed. Quantitative analysis of blend levels and individual chemical distribution were achieved. The method has great potential for the identification of biodiesel in diesel fuel blends and could form the basis of a method for characterization of biodiesel-contaminated environmental samples.
- Published
- 2011
43. Determination of polar impurities in biodiesels using solid-phase extraction and gas chromatography-mass spectrometry
- Author
-
Zeyu, Yang, Bruce P, Hollebone, Zhendi, Wang, Chun, Yang, and Mike, Landriault
- Subjects
Sterols ,Biofuels ,Solid Phase Extraction ,Carboxylic Acids ,Gas Chromatography-Mass Spectrometry ,Glycerides - Abstract
This paper reports on a method for development and validation for simultaneous characterization and determination of oxygenated polar impurities--free fatty carboxylic acids (FFAs), partial glycerides (monoacylglycerides, MGs), residual glycerol and free sterols--in various biodiesels based on the combination of solid-phase extraction (SPE), silylation and GC/MS technologies. The effects of various SPE and silylation conditions on the method recoveries were evaluated. Using this integrated SPE-GC/MS method, 38 target polar compounds (13 FFAs, 17 glycerides and 8 sterols) in 9 biodiesels derived from 4 different feedstocks were successfully separated and quantified. It was found that the carbon chain length of FFAs was ranged from C(6) to C(24), with C(16) and C(18) being the most abundant in all biodiesels. The total FFAs concentration was consistent with the acid values (AVs) measured by standard method ASTM D974-04. MG congeners with carbon number of 18 (mono-C18) were most abundant in the biodiesel samples, followed by mono-C(16) and free glycerol. β-Sitosterol and campesterol were found to be the prevailing phytosterols in all pure vegetable oil-based biodiesels, while brassicasterol and stigmasterol was only significant in the biodiesel from canola oil and soybean oil, respectively, and abundant cholesterol was only detected in animal fat-based biodiesels.
- Published
- 2010
44. Characteristics of bicyclic sesquiterpanes in crude oils and petroleum products
- Author
-
Chun Yang, Bruce P. Hollebone, Carl E. Brown, Zhendi Wang, and Mike Landriault
- Subjects
chemistry.chemical_classification ,Kerosene ,Chromatography ,business.industry ,Organic Chemistry ,Fraction (chemistry) ,General Medicine ,Fuel oil ,Biochemistry ,Gas Chromatography-Mass Spectrometry ,Analytical Chemistry ,law.invention ,Diesel fuel ,Hydrocarbon ,Petroleum product ,Petroleum ,chemistry ,law ,Gasoline ,business ,Distillation - Abstract
This study presents a quantitative gas chromatography-mass spectrometry analysis of bicyclic sesquiterpanes (BSs) in numerous crude oils and refined petroleum products including light and mid-range distillate fuels, residual fuels, and lubricating oils collected from various sources. Ten commonly recognized bicyclic sesquiterpanes were determined in all the studied crude oils and diesel range fuels with principal dominance of BS3 (C(15)H(28)), BS5 (C(15)H(28)) and BS10 (C(16)H(30)), while they were generally not detected or in trace in light fuel oils like gasoline and kerosene and most lubricating oils. Laboratory distillation of crude oils demonstrated that sesquiterpanes were highly enriched in the medium distillation fractions of approximately 180 to 481 degrees C and were generally absent or very low in the light distillation fraction (boiling point to approximately 180 degrees C) and the heavy residual fraction (481 degrees C). The effect of evaporative weathering on a series of diagnostic ratios of sesquiterpanes, n-alkanes, and biomarkers was evaluated with two suites of weathered oil samples. The change of abundance of sesquiterpanes was used to determine the extent of weathering of artificially evaporated crude oils and diesel. In addition to the pentacyclic biomarker C(29) and C(30) alphabeta-hopane, C(15) and C(16) sesquiterpanes might be alternative internal marker compounds to provide a direct way to estimate the depletion of oils, particularly diesels, in oil spill investigations. These findings may offer potential applications for both oil identification and oil-source correlation in cases where the tri- to pentacyclic biomarkers are absent due to refining or environmental weathering of oils.
- Published
- 2009
45. Fingerprinting of petroleum hydrocarbons (PHC) and other biogenic organic compounds (BOC) in oil-contaminated and background soil samples
- Author
-
J. Sun, Mike Landriault, Carl E. Brown, D. G. Dixon, Zhendi Wang, Bruce P. Hollebone, C. Yang, F. Kelly-Hooper, Stephen M. Mudge, and Zeyu Yang
- Subjects
Soil test ,business.industry ,Environmental remediation ,Chemistry ,Public Health, Environmental and Occupational Health ,Fraction (chemistry) ,General Medicine ,Management, Monitoring, Policy and Law ,Contamination ,complex mixtures ,Soil quality ,Hydrocarbons ,Soil ,chemistry.chemical_compound ,Petroleum ,Petroleum product ,Environmental chemistry ,Soil water ,Soil Pollutants ,Petroleum Pollution ,Polycyclic Aromatic Hydrocarbons ,business ,Environmental Monitoring - Abstract
Total petroleum hydrocarbons (TPH) or petroleum hydrocarbons (PHC) are one of the most widespread soil contaminants in Canada, the United States and many other countries worldwide. Clean-up of PHC-contaminated soils costs the Canadian economy hundreds of millions of dollars annually. In Canada, most PHC-contaminated site evaluations are based on the methods developed by the Canadian Council of the Ministers of the Environment (CCME). However, the CCME method does not differentiate PHC from BOC (the naturally occurring biogenic organic compounds), which are co-extracted with petroleum hydrocarbons in soil samples. Consequently, this could lead to overestimation of PHC levels in soil samples. In some cases, biogenic interferences can even exceed regulatory levels (300 μg g(-1) for coarse soils and 1300 μg g(-1) for fine soils for Fraction 3, C(16)-C(34) range, in the CCME Soil Quality Level). Resulting false exceedances can trigger unnecessary and costly cleanup or remediation measures. Therefore, it is critically important to develop new protocols to characterize and quantitatively differentiate PHC and BOC in contaminated soils. The ultimate objective of this PERD (Program of Energy Research and Development) project is to correct the misconception that all detectable hydrocarbons should be regulated as toxic petroleum hydrocarbons. During 2009-2010, soil and plant samples were collected from over forty oil-contaminated and paired background sites in various provinces. The silica gel column cleanup procedure was applied to effectively remove all target BOC from the oil-contaminated sample extracts. Furthermore, a reliable GC-MS method in combination with the derivatization technique, developed in this laboratory, was used for identification and characterization of various biogenic sterols and other major biogenic compounds in these oil-contaminated samples. Both PHC and BOC in these samples were quantitatively determined. This paper reports the characterization results of this set of 21 samples. In general, the presence of petroleum-characteristic alkylated PAH homologues and biomarkers can be used as unambiguous indicators of the contamination of oil and petroleum product hydrocarbons; while the absence of petroleum-characteristic alkylated PAH homologues and biomarkers and the presence of abundant BOC can be used as unambiguous indicators of the predominance of natural organic compounds in soil samples.
- Published
- 2012
46. Characterization of Biodegraded Wabamun Spill Oil Samples Incubated with Lake Fresh Sediment or Enrichment Culture
- Author
-
C. Yang, Z. Yang, Zhendi Wang, Mike Landriault, Carl E. Brown, Bruce P. Hollebone, and J. Sun
- Subjects
Hydrology ,Residual oil ,Environmental engineering ,Environmental science ,Sediment ,Fuel oil ,Enrichment culture ,Lake water - Abstract
On August 3, 2005, a Canadian National Railway train derailed within the Whitewood Sands community of the Wabamun Lake area. The derailment resulted in the release of 712,500 liters of Bunker C oil and 88,000 liters of pole treating oil from the rail cars into the adjacent Wabamun Lake water. To estimate the hydrocarbon-degrading capabilities of microbes naturally present in oil-contaminated Lake Wabamun sediment, laboratory tests were conducted at the University of Alberta under two incubation conditions. The tests incubated spilled Bunker C oil recovered from the lake and the reference oil, Alberta Sweet Mix Blend (ASMB), at 22°C for 4 weeks or at 4°C for 8 weeks. Residual oil was recovered and quantitatively characterized at the Oil Research Laboratory of Emergencies Science and Technology Section, Environment Canada. Biodegradation results demonstrated that Lake Wabamun sediment microbes were capable of degrading a significant proportion of the ASMB reference oil at both incubation temperatur...
- Published
- 2011
47. Oil fingerprinting analysis using commercial solid phase extraction (SPE) cartridge and gas chromatography-mass spectrometry (GC-MS)
- Author
-
Chun Yang, Mike Landriault, Zeyu Yang, Zhendi Wang, Carl E. Brown, and Bruce P. Hollebone
- Subjects
Chromatography ,business.industry ,Silica gel ,General Chemical Engineering ,General Engineering ,Fractionation ,Analytical Chemistry ,Clean-up ,Hexane ,chemistry.chemical_compound ,Cartridge ,Petroleum product ,chemistry ,Solid phase extraction ,Gas chromatography–mass spectrometry ,business - Abstract
This study used solid phase extraction (SPE) cartridges for rapid cleanup and fractionation of oil samples in oil fingerprinting analysis. A series of commercially available florisil cartridges, normal phase SPE cartridges, and silica gel/cyanopropyl (SiO2/C3-CN) SPE cartridges was selected for the fractionation of oil into aliphatic and aromatic hydrocarbons. The florisil cartridges and normal phase SPE cartridges can clean up the oil samples but are unable to separate them into two fractions. The SiO2/C3-CN (1 g/0.5 g) SPE cartridge successfully separated oil samples into aliphatic and aromatic fractions by eluting with 4 mL of hexane and 4 mL of dichloromethylene (DCM)/hexane (3 : 1, v:v), respectively. No cross-elution was observed between aliphatic and aromatic fractions when oil loading mass was less than 40 mg on the SiO2/C3-CN SPE cartridge. The relative standard deviation (RSD) of five replicates of SPE-GC-MS analysis of 5 mg of reference oil is 2.8%, 1.2%, and 6.9% for total n-alkanes, polycyclic aromatic hydrocarbons (PAHs), and biomarkers, respectively. The recoveries of six spiked deuterated surrogates were all above 95%. This SPE-GC-MS method was used for the fingerprinting analysis of various crude oils, refined petroleum products, and environmental sediment samples. The characterized target hydrocarbons included n-alkanes, unsubstituted priority PAHs and alkylated homologues, and biomarker terpanes and steranes. The concentration profiles and diagnostic ratios of target compounds are both comparable to those obtained by the conventional silica gel column-GC-MS method.
- Published
- 2011
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