ABSTRACT
A series of flume- and laboratory-based experiments defined and quantified the thresholds of sunken oil transport using No.6 heavy fuel oil mixed with kaolinite clay. When the sunken oil became mobile, the current-induced bed shear stress exceeded a threshold value specific to the oil, known as critical shear stress (CSS). The oil's CSS was evaluated as a function of water velocity, water temperature, oil condition, and sediment size. Based on experimental results, the stages of oil transport were defined and empirical relationships using the oil's kinematic viscosity (vo) and sediment size were developed to predict oil CSS at each transport stage. For vo<2 × 104 cSt, multiple thresholds of movement were observed: (1) gravity dispersion, (2) rope formation, (3) ripple formation, and (4) break-apart/resuspension. When vo> 6 × 104 cSt, transport was more likely to occur as a single event with the oil remaining intact, saltating over the bed in the direction of flow.
Subject(s)
Fuel Oils , Water Pollutants, Chemical , Water Pollutants, Chemical/analysis , Fresh Water/chemistry , Petroleum , Viscosity , Stress, MechanicalABSTRACT
The environmental impact of oil spills is a critical concern, particularly pertaining to low sulfur marine diesel (LSMD) and high sulfur fuel oil (HSFO) that are commonly involved in coastal spills. Although transcriptomic biomonitoring of sentinel animals can be a powerful tool for assessing biological effects, conventional methods utilize lethal sampling to examine the liver. As a non-lethal alternative, we have previously shown salmonid caudal fin cyp1a1 is significantly responsive to LSMD-derived toxicants. The present study further investigated the transcriptomic biomonitoring potential of coho salmon smolt caudal fin in comparison to liver tissue in the context of LSMD and HSFO seawater accommodated fraction (seaWAF) exposure in cold-water marine environments. Assessing the toxicity of these seaWAFs involved quantifying polycyclic aromatic hydrocarbon (tPAH50) concentrations and generating gene expression profiles. Initial qPCR analyses revealed significant cyp1a1 response in both liver and caudal fin tissues of both genetic sexes to all seaWAF exposures. RNA-Seq analysis, focusing on the highest LSMD and HSFO seaWAF concentrations (28.4±1.8 and 645.08±146.3⯵g/L tPAH50, respectively), revealed distinct tissue-specific and genetic sex-independent transcriptomic responses with an overall enrichment of oxidative stress, cell adhesion, and morphogenesis-related pathways. Remarkably, the caudal fin tissue exhibited transcriptomic response patterns comparable to liver tissue, particularly consistent differential expression of 33 gene transcripts in the liver (independent of sex and oil type) and 44 in the caudal fin. The present work underscores the viability of using the caudal fin as a non-lethal alternative to liver sampling for assessing and tracking oil spill exposure in marine environments.
Subject(s)
Animal Fins , Cytochrome P-450 CYP1A1 , Fuel Oils , Liver , Petroleum Pollution , Transcriptome , Water Pollutants, Chemical , Animals , Liver/drug effects , Liver/metabolism , Water Pollutants, Chemical/toxicity , Petroleum Pollution/adverse effects , Animal Fins/drug effects , Transcriptome/drug effects , Male , Cytochrome P-450 CYP1A1/genetics , Cytochrome P-450 CYP1A1/metabolism , Fuel Oils/toxicity , Female , Sulfur , Environmental Monitoring/methods , Oncorhynchus kisutch/genetics , Gasoline/toxicity , Polycyclic Aromatic Hydrocarbons/toxicity , Polycyclic Aromatic Hydrocarbons/analysis , Seawater/chemistryABSTRACT
In this study, we focus on the development and validation of a deep learning (long short-term memory, LSTM)-based algorithm to predict the accidental spreading of LSFO (low sulfur fuel oil) on the water surface. The data for the training was obtained by numerical simulations of artificial geometries with different configurations of islands and shorelines and wind speeds (2.0-8.0 m/s). For simulating the spread of oils in O(102) km scales, the volume of fluid and discrete phase models were adopted, and the kinematic variables of particle location, particle velocity, and water velocity were collected as input features for LSTM model. The predicted spreading pattern of LSFO matched well with the simulation (less than 10 % in terms of the mean absolute error for the untrained data). Finally, we applied the model to the Wakashio LSFO spill accident, considering actual geometry and weather information, which confirmed the practical feasibility of the present model.
Subject(s)
Fuel Oils , Sulfur/chemistry , Petroleum Pollution , Water Pollutants, Chemical , Algorithms , Models, Theoretical , Computer SimulationABSTRACT
Developing an optimal environmentally friendly bioremediation strategy for petroleum products is of high interest. This study investigated heavy fuel oil (HFO)-contaminated soil (4 and 6 g kg-1) remediation by individual and combined bioaugmentation-assisted phytoremediation with alfalfa (Medicago sativa L.) and with cold plasma (CP)-treated M. sativa. After 14 weeks of remediation, HFO removal efficiency was in the range between 61 and 80% depending on HFO concentration and remediation technique. Natural attenuation had the lowest HFO removal rate. As demonstrated by growth rate and biomass acquisition, M. sativa showed good tolerance to HFO contamination. Cultivation of M. sativa enhanced HFO degradation and soil quality improvement. Bioaugmentation-assisted phytoremediation was up to 18% more efficient in HFO removal through alleviated HFO stress to plants, stimulated plant growth, and biomass acquisition. Cold plasma seed treatment enhanced HFO removal by M. sativa at low HFO contamination and in combination with bioaugmentation it resulted in up to 14% better HFO removal compared to remediation with CP non-treated and non-bioaugmented M. sativa. Our results show that the combination of different remediation techniques is an effective soil rehabilitation strategy to remove HFO and improve soil quality. CP plant seed treatment could be a promising option in soil clean-up and valorization.
Subject(s)
Biodegradation, Environmental , Medicago sativa , Soil Pollutants , Soil , Medicago sativa/metabolism , Soil Pollutants/metabolism , Soil/chemistry , Fuel Oils , Plasma Gases , Environmental Restoration and Remediation/methodsABSTRACT
The present paper considers the results of long-term (up to 17 years) in situ and laboratory research carried out on oiled French, Spanish, and Russian seacoasts. The objective of this research is to quantify the influence of geographical factors on the rates of natural transformation of the heavy fuel oil stranded ashore and to develop an empirical statistical model in order to evaluate the self-cleansing capacity of the coastal environment. In a number of field campaigns, 363 samples of weathered oil slicks and tar balls have been collected and analysed with the use of thin-layer chromatography combined with optical and gravimetric methods. The results obtained have been subjected to multiple nonlinear regression analyses. It has been shown that heavy fuel oil natural attenuation is more active in continental or estuarine environments influenced by nutrient-rich freshwater runoff and characterised by a higher number of sunny days, solar irradiation, and large temperature fluctuations. On the oceanic coasts, especially in sectors with low hydrodynamic energy, these processes take more time. The resulting model allows for the identification and mapping of the most vulnerable seacoasts, characterised by a low potential to degrade oil pollution. This information may be used in the contingency plans in order to optimise clean-up techniques and associated costs.
Subject(s)
Fuel Oils , Environmental Monitoring , Petroleum Pollution , Water Pollutants, Chemical/analysis , Models, Theoretical , PetroleumABSTRACT
Chemical recycling of complex plastic waste via pyrolysis can reduce fossil resource dependence of the plastics value chain and greenhouse gas emissions. However, economic viability is crucial for its implementation, especially considering challenging waste streams with high shares of engineering plastics that have lower pyrolysis product quality than standard thermoplastics waste. Thus, this study conducts a techno-economic assessment determining the profitability factors of pyrolysis plants for automotive plastic waste in Germany including different plant capacities and calculating cost-covering minimum sales prices for the resulting pyrolysis oil. Main findings are that due to economies of scale, the cost-covering minimum sales prices vary between 1182 /Mg pyrolysis oil (3750 Mg input/year) and 418 /Mg pyrolysis oil (100,000 Mg input/year). The pyrolysis technology employed must be robust and scalable to realize these economies of scale. Large plant capacities face challenges such as feedstock availability at reasonable costs, constant feedstock quality, and pyrolysis oil quality, affecting pyrolysis oil pricing. Due to the limited yield and quality of pyrolysis oil produced from these technically demanding feedstocks, policy implications are that additional revenue streams such as gate fees or subsidies that are essential to ensure a positive business case are necessary. Depending on the assessed plant capacity, additional revenues between 720 and 59 /Mg pyrolysis oil should be realized to be competitive with the price of the reference product heavy fuel oil. Otherwise, the environmental potential of this technology cannot be exploited.
Subject(s)
Fuel Oils , Plastics , Pyrolysis , Recycling , TechnologyABSTRACT
Identifying the sources of environmental oil contamination can be challenging, especially for oil in motile organisms such as fish. Lipophilic hydrocarbons from oil can bioaccumulate in fish adipose tissue and potentially provide a forensic "fingerprint" of the original oil. Herein, diamondoid hydrocarbon distributions were employed to provide such fingerprints. Indices produced from diamondoids were used to compare extracts from fish adipose tissues and the crude and fuel oils to which the fish were exposed under laboratory conditions. A suite of 20 diamondoids was found to have bioaccumulated in the dietary-exposed fish. Cross-plots of indices between fish and exposure oils were close to the ideal 1:1 relationship. Comparisons with diamondoid distributions of non-exposure oils produced overall, but not exclusively, weaker correlations. Linear Discriminatory Analysis on a combined set of 15 diamondoid and bicyclane molecular ratios was able to identify the exposure oils, so a use of both compound classes is preferable.
Subject(s)
Fuel Oils , Petroleum , Animals , Oils , Hydrocarbons/analysis , Fuel Oils/analysis , Fishes , Seafood/analysis , Petroleum/analysisABSTRACT
In early 2020, two unique events perturbed ship emissions of pollutants around Southern China, proffering insights into the impacts of ship emissions on regional air quality: the decline of ship activities due to COVID-19 and the global enforcement of low-sulfur (<0.5%) fuel oil for ships. In January and February 2020, estimated ship emissions of NOx, SO2, and primary PM2.5 over Southern China dropped by 19, 71, and 58%, respectively, relative to the same period in 2019. The decline of ship NOx emissions was mostly over the coastal waters and inland waterways of Southern China due to reduced ship activities. The decline of ship SO2 and primary PM2.5 emissions was most pronounced outside the Chinese Domestic Emission Control Area due to the switch to low-sulfur fuel oil there. Ship emission reductions in early 2020 drove 16 to 18% decreases in surface NO2 levels but 3.8 to 4.9% increases in surface ozone over Southern China. We estimated that ship emissions contributed 40% of surface NO2 concentrations over Guangdong in winter. Our results indicated that future abatements of ship emissions should be implemented synergistically with reductions of land-borne anthropogenic emissions of nonmethane volatile organic compounds to effectively alleviate regional ozone pollution.
Subject(s)
Air Pollutants , Air Pollution , Fuel Oils , Ozone , Air Pollutants/analysis , Ships , Vehicle Emissions/analysis , Particulate Matter/analysis , Nitrogen Dioxide , Air Pollution/analysis , China , Ozone/analysis , Sulfur , Environmental Monitoring/methodsABSTRACT
Diesel was accidently released into the shallow subsurface at an industrial site in the province of Québec, Canada, in the late 1980s. Subsequent remediation efforts removed much of the contamination; however, traces of petroleum hydrocarbons continue to impact the local aquifer. In addition to the historical diesel spill, more recent yet unconfirmed accidental releases from ongoing on-site and neighbouring industrial activities may have potentially contributed to elevated levels of polycyclic aromatic compounds (PACs) in groundwater. To identify the main source(s) of contamination, compound-specific stable carbon isotope ratios (δ13C) of PACs in groundwater monitoring wells were compared to those in asphalt produced from a nearby plant and in fuel oil #6 oil being used by local industry. The δ13C values of five individual compounds (biphenyl, C2-naphthalene, C1-fluorene, dibenzothiophene and phenanthrene) and two groups of combined C1-phenanthrenes/anthracenes in all groundwater samples were within analytical uncertainty (±0.5). Moreover, the δ13CPAC values in groundwater samples were distinct from those in asphalt and fuel oil #6, indicating negligible contributions from these sources. The similarity in δ13CPAC values across monitoring wells, including one situated in the former source zone containing a floating hydrocarbon phase, pointed to a common source of subsurface contamination that was attributed to the historical diesel spill. These results thus demonstrate that δ13CPAC values can be used for source apportionment in shallow aquifers decades after the original spill event.
Subject(s)
Fuel Oils , Groundwater , Polycyclic Aromatic Hydrocarbons , Polycyclic Compounds , Environmental Monitoring/methods , Carbon Isotopes/analysis , Polycyclic Aromatic Hydrocarbons/analysisABSTRACT
Recent restrictions on marine fuel sulfur content and a heightened regulatory focus on maritime decarbonization are driving the deployment of low-carbon and low-sulfur alternative fuels for maritime transport. In this study, we quantified the life-cycle greenhouse gas and sulfur oxide emissions of several novel marine biofuel candidates and benchmarked the results against the emissions reduction targets set by the International Maritime Organization. A total of 11 biofuel pathways via four conversion processes are considered, including (1) biocrudes derived from hydrothermal liquefaction of wastewater sludge and manure, (2) bio-oils from catalytic fast pyrolysis of woody biomass, (3) diesel via Fischer-Tropsch synthesis of landfill gas, and (4) lignin ethanol oil from reductive catalytic fractionation of poplar. Our analysis reveals that marine biofuels' life-cycle greenhouse gas emissions range from -60 to 56 gCO2e MJ-1, representing a 41-163% reduction compared with conventional low-sulfur fuel oil, thus demonstrating a considerable potential for decarbonizing the maritime sector. Due to the net-negative carbon emissions from their life cycles, all waste-based pathways showed over 100% greenhouse gas reduction potential with respect to low-sulfur fuel oil. However, while most biofuel feedstocks have a naturally occurring low-sulfur content, the waste feedstocks considered here have higher sulfur content, requiring hydrotreating prior to use as a marine fuel. Combining the break-even price estimates from a published techno-economic analysis, which was performed concurrently with this study, the marginal greenhouse gas abatement cost was estimated to range from -$120 to $370 tCO2e-1 across the pathways considered. Lower marginal greenhouse gas abatement costs were associated with waste-based pathways, while higher marginal greenhouse gas abatement costs were associated with the other biomass-based pathways. Except for lignin ethanol oil, all candidates show the potential to be competitive with a carbon credit of $200 tCO2e-1 in 2016 dollars, which is within the range of prices recently received in connection with California's low-carbon fuel standard.
Subject(s)
Fuel Oils , Greenhouse Gases , Animals , Biofuels , Lignin , Pyrolysis , Wood , Sulfur , Carbon , Ethanol , Life Cycle StagesABSTRACT
In the present study, through the laboratory-to-field scale experiments and trials, we report the development and evaluation of an integrated oil-spill response system capable of oil collection, recovery (separation), and storage, for a timely and effective response to the initial stage of oil-spill accidents. With the laboratory-scale experiments, first, we evaluate that the water-surface waves tend to abate the oil recovery rate below 80% (it is above 95% for the optimized configuration without the waves), which is overcome by installing the hydrophilic (and oleophobic) porous structures at the inlet and/or near the water outlet of the separator. In the follow-up meso-scale towing tank tests with a scaled-up prototype, (i) we optimize the maneuverability of the assembled system depending on the speed and existence of waves, and (ii) evaluate the oil recovery performance (more than 80% recovery for the olive oil and Bunker A fuel oil). Although more thorough investigations and improvements are needed, a recovery rate of over 50% can be achieved for the newly enforced marine fuel oil (low sulfur fuel oil, LSFO) that was not targeted at the time of development. Finally, we perform a series of field tests with a full-scale system, to evaluate the rapid deployment and operational stability in the real marine environment. The overall floating balance and coordination of each functional part are sustained to be stable during the straight and rotary maneuvers up to the speed of 5 knots. Also, the collection of the floating debris (mimicking the spilled oil) is demonstrated in the field test. The present system is now being tested by the Korea Coast Guard and we believe that it will be very powerful to prevent the environmental damage due to the oil spills.
Subject(s)
Fuel Oils , Petroleum Pollution , Bays , Laboratories , WaterABSTRACT
The continuous expansion of shipping trade has brought about increasingly serious marine pollution problems. In the context of emission reduction in the global shipping industry, this paper focuses on the operation optimization of container ships inside and outside the emission control area (ECA). From the dual perspectives of shipowners and the general public, models in the annual operating cycle are established to study the economic and environmental benefit differences between traditional fuels, i.e., heavy fuel oil (HFO) and low-sulfur fuel oil (LSFO), and alternative fuels, i.e., liquefied natural gas (LNG) and methanol. Sensitivity analysis was carried out for the proportion of ECA and ship speed. The results show that, in the current situation of high natural gas prices, the use of HFO after the installation of scrubbers is still the most cost-effective option in the short term, followed by the use of LSFO and methanol. LNG is no longer an attractive option, while LSFO and methanol are the best options for both cost and the environment. With the tightening of ECA regulations, methanol will become the optimal choice when the ECA ratio is higher than 47%. By reducing the speed of the ship, the pollutant emission can be effectively reduced, but it will also lead to an overall decrease in profits. Considering the future "zero carbon" emission targets, slow streaming is only suitable as a short-term response measure, while switching to green power energy is a choice that is more in line with the long-term development strategy.
Subject(s)
Air Pollutants , Fuel Oils , Natural Gas , Vehicle Emissions/analysis , Methanol , Ships , Air Pollutants/analysisABSTRACT
In this work, we present hardware and firmware design and preliminary testing results for a noninvasive device for measuring fuel oil consumption in fuel oil vented heaters. Fuel oil vented heaters are a popular space heating method in northern climates. Monitoring fuel consumption is useful to understanding residential daily and seasonal heating patterns and understanding the thermal characteristics of buildings. The device is a pump monitoring apparatus (PuMA) that employs a magnetoresistive sensor to monitor the activity of solenoid driven positive displacement pumps, which are commonly used in fuel oil vented heaters. PuMA accuracy for calculating fuel oil consumption was evaluated in a lab setting and found to vary up to 7% from the measured consumption value during testing. This variance will be explored more in field testing.
Subject(s)
Fuel Oils , Household Articles , Puma , Animals , Heating , ClimateABSTRACT
Given the urgent need for continuous and diverse research on marine fuel oils, this study investigated the effects of the properties of fuel oil on its adsorption to adsorbent materials. Very low-sulfur fuel oil (VLSFO), which is increasingly being utilized in vessels, was tested to simulate adsorption from seawater at temperatures of 1, 15, and 25 °C. Temperature minimally affected the adsorbed amount of low-viscosity VLSFOs and high-sulfur fuel oils. Conversely, the amount of high-viscosity VLSFO adsorbed decreased sharply at 1 and 15 °C. The viscosity, pour point, aromatics, asphaltenes, and wax contents of fuel oils determined the amounts adsorbed on an adsorbent. Therefore, at low sea surface temperatures associated with VLSFO spills, adsorption may be challenging. These findings highlight the need to improve fuel oil quality to accommodate spills in the marine environment.
Subject(s)
Fuel Oils , Petroleum Pollution , Water Pollutants, Chemical , Petroleum Pollution/analysis , Adsorption , Water Pollutants, Chemical/analysis , TemperatureABSTRACT
The present work aimed to study, predict and understand benzene migration that occurred during an industrial spill using numerical simulation by computational fluid dynamics. Advection, diffusion and adsorption were the main mechanisms considered that governed the spill incident. The incident occurred due to a fracture under a fuel oil storage tank. The tank was located on a hill 18 m high, and the initial value of benzene concentration (soil saturation) was 60 ppm. When the spill was discovered, samples in the affected zone were taken using an experimental design. Many samples showed a greater concentration of benzene than allowed by Mexican Official Standards (MOSs) (15 ppm). The concentrations found 100 m away from the spill were around 60 to 15 ppm. Due to the spill being under the tank, it was difficult to discover. The numerical simulation provided an estimate that the spill started around 2 years ago. The type of soil in the afflicted zone is rocky, and, consequently, it is difficult to estimate how long it will take to reach the concentration allowed by the MOSs, but the numerical simulation predicts that this concentration will be reached in 14 years. Experimental values of the spill contaminant concentration were statistically similar to the CFD estimated data (p < 0.05).
Subject(s)
Fuel Oils , Petroleum Pollution , Benzene/analysis , Hydrodynamics , Hydrocarbons , Computer Simulation , Petroleum Pollution/analysisABSTRACT
The transformation of waste plastics into fuels via energy-efficient and low-cost pyrolysis could incentivize better waste plastic management. Here, we report pressure-induced phase transitions in polyethylene, which continue to heat up without additional heat sources, prompting the thermal cracking of plastics into premium fuel products. When the nitrogen initial pressure is increased from 2 to 21 bar, a monotonically increasing peak temperature is observed (from 428.1 °C to 476.7 °C). At 21 bar pressure under different atmosphere conditions, the temperature change driven by high-pressure helium is lower than that driven by nitrogen or argon, indicating that phase transition is related to the interaction between long-chain hydrocarbons and intercalated high-pressure medium layers. In view of the high cost of high-pressure inert gases, the promotion or inhibition effect of low-boiling hydrocarbons (transitioning into the gaseous state with increasing temperature) on phase transition is explored, and a series of light components are used as phase transition initiators to replace high-pressure inert gases to experiment. The reason that the quantitative conversion of polyethylene to high-quality fuel products is realized through the addition of 1-hexene at a set temperature of 340 °C and the initial atmospheric pressure. This discovery provides a method for recycling plastics by low energy pyrolysis. In addition, we envisage recovering some of the light components after plastic pyrolysis as phase change initiators for the next batch of the process. This method is able to reduce the cost of light hydrocarbons or high-pressure gas insertion, reduce heat input, and improve material and energy utilization.
Subject(s)
Fuel Oils , Polyethylene , Refuse Disposal , Atmospheric Pressure , Hydrocarbons , Nitrogen , Plastics , Temperature , Refuse Disposal/methods , Recycling/methodsABSTRACT
The Western Pacific Ocean (the WPO), as one of the busiest shipping areas in the world, holds a complex water traffic network. In 2020, the International Maritime Organization (IMO) low-sulfur fuel regulations were implemented globally, while the COVID-19 outbreak influenced shipping activities together. This study aimed to assess the combined impact of epidemics and low-sulfur fuel policies on ship emissions, as well as their environmental effects on the WPO. The ship emission model based on the Automatic Identification System (AIS) data was applied to analyze the monthly emission variations during 2018-2020. It was found that the epidemic had obvious diverse influences on the coastal ports in the WPO. Overall, shipping emissions declined by 15 %-30 % in the first half of 2020 compared with those in 2019 due to the COVID-19 lockdown, whereas they rebounded in the second half as a result of trade recovery. The pollutants discharged per unit of cargo by ships rose after the large-range lockdown. China's multiphase domestic emission control areas (DECAs) and the IMO global low-sulfur fuel regulation have greatly reduced SO2 emissions from ships and caused them to "bypass and come back" to save fuel costs around emission control areas from 2018 to 2020. Based on satellite data and land-based measurements, it was found that the air quality over sea water and coastal cities has shown a positive response to changes in ship-emitted NOx and SO2. Our results reveal that changes in shipping emissions during typical periods, depending on their niches in the complex port traffic network, call for further efforts for cleaner fuel oils, optimized ECA and ship lane coordination in the future. Shipping related air pollutions during the later economic recovery also needs to be addressed after international scale standing-by events.
Subject(s)
Air Pollutants , Air Pollution , COVID-19 , Epidemics , Fuel Oils , Humans , Air Pollutants/analysis , Ships , COVID-19/epidemiology , Communicable Disease Control , Air Pollution/analysis , Sulfur , Vehicle Emissions/analysis , Particulate Matter/analysisABSTRACT
Special Antarctic Blend (SAB) diesel is the main fuel used on Macquarie Island and has been identified as the primary contaminant in several past spill events. This study evaluates the environmental impact of petroleum spills at high latitudes, in the soils of subantarctic Macquarie Island. Soil samples were collected from seven locations, including the "fuel farm" and main powerhouse that have been contaminated by petroleum in the past, and five reference locations, away from station infrastructure and from any obvious signs of contamination. Soils were solvent extracted and analysed using gas chromatography-mass spectrometry. The results show that both contaminated and uncontaminated sites contained a suite of different chain-length hydrocarbons. The more contaminated samples from the fuel farm and main powerhouse contained higher concentrations and a greater range of hydrocarbons that typically indicate numerous spills of varying ages. The hydrocarbon signature of samples collected near the fuel farm and at some of the main powerhouse sites was typical of SAB diesel. However, the hydrocarbon signature at other main powerhouse sites suggest contamination with a heavier fuel with different characteristics, including lower pristane/phytane ratios. Traces of C21-C35 cyclic biomarkers in the spill sites may be derived from additional heavier fuels, and include a signature characteristic of crude oil derived from marine carbonate source rocks. Reference samples had lower concentrations of hydrocarbons, and these were dominated by high molecular weight n-alkanes with an odd-carbon-number predominance, typical of higher-plant derived lipids. Some reference samples also contained geochemical signatures that suggest that they too were contaminated by fuel oil. Variable levels of biodegradation of fuels in soils are consistent with a heterogenous site and a relatively slow rate of biodegradation. The occurrence of fresh spilled fuel overprinting biodegraded fuel from earlier spills is compelling evidence of multiple spills and complex mixing in the environment.
Subject(s)
Fuel Oils , Petroleum , Soil/chemistry , Hydrocarbons/metabolism , Biodegradation, EnvironmentalABSTRACT
Polycyclic aromatic compounds (PACs) are important hazardous air pollutants in China due to the country's coal-dominant energy structure. In order to reveal the pollution characteristics, sources, toxicity, and pollution historical trends of PACs in the atmosphere of the middle reach of the Huaihe River (MRHR), a large-scale coal-fired power base of China, tree barks and tree cores were collected and employed as passive air samplers and historical trend recorders, and 76 PACs were identified for the first time. ΣPACs in tree barks ranged from 170 to 3800 ng g-1 (mean = 700 ± 720 ng g-1), with the high concentrations observed mainly in the coal-mining and coal-bearing area. 16 priority PAHs (PriPAHs) were the predominant substances and accounted for 59 ± 8.3 % of ΣPACs. The combustion of coal and fuel oil was the most significant source of PACs, accounting for 43 % of ΣPACs, followed by the combustion of biomass (30 %) and non-combustion sources (27 %). Based on a bark-air partitioning model, volumetric air concentrations for ΣPACs were calculated to be 450-11,000 ng m-3 (mean = 1600 ± 2000 ng m-3). The BaP-toxic equivalent concentrations (TEQBaP) of ΣPACs (mean = 9.7 ± 15 ng m-3) were significantly higher than the Chinese guideline (1 ng m-3) and were mostly caused by coal & fuel oil combustion (55 ± 13 %). High molecular weight PACs were detected in lower percentages in tree cores than in tree barks, indicating that PACs in the particle phase were difficult to enter the tree core. Major PACs decreased in tree core samples between 2000 and 2020 as pollution control efforts improved, however, some PACs showed different trends when influenced by point sources.
Subject(s)
Air Pollutants , Fuel Oils , Polycyclic Aromatic Hydrocarbons , Polycyclic Compounds , Polycyclic Compounds/analysis , Coal/analysis , Plant Bark/chemistry , Trees , Air Pollutants/analysis , Polycyclic Aromatic Hydrocarbons/analysis , China , Environmental MonitoringABSTRACT
Ship emissions contribute substantial air pollutants when at berth. However, the complexity and diversity of the marine fuels utilized hinder our understanding and mapping of the characteristics of ship emissions. Herein, we applied GC × GC-MS to analyze the components of marine fuel oils. Owing to the high separation capacity of GC × GC-MS, 11 classes of organic compounds, including b-alkanes, alkenes, and cyclo-alkanes, which can hardly be resolved by traditional one-dimensional GC-MS, were detected. Significant differences are observed between light (-10# and 0#) and heavy (120# and 180#) fuels. Notably, -10# and 0# diesel fuels are more abundant in b-alkanes (44~49%), while in 120# and 180#, heavy fuels b-alkanes only account for 8%. Significant enhancement of naphthalene proportions is observed in heavy fuels (20%) compared to diesel fuels (2~3%). Hopanes are detected in all marine fuels and are especially abundant in heavy marine fuels. The volatility bins, one-dimensional volatility-based set (VBS), and two-dimensional VBS (volatility-polarity distributions) of marine fuel oils are investigated. Although IVOCs still take dominance (62-66%), the proportion of SVOCs in heavy marine fuels is largely enhanced, accounting for ~30% compared to 6~12% in diesel fuels. Furthermore, the SVOC/IVOC ratio could be applied to distinguish light and heavy marine fuel oils. The SVOC/IVOC ratios for -10# diesel fuel, 0# diesel fuel, 120# heavy marine fuel, and 180# heavy marine fuel are 0.085 ± 0.046, 0.168 ± 0.159, 0.504, and 0.439 ± 0.021, respectively. Our work provides detailed information on marine fuel compositions and could be further implemented in estimating organic emissions and secondary organic aerosol (SOA) formation from marine fuel storage and evaporation processes.