Use of Compound-Specific Stable Isotope Analysis to Source Anthropogenic Natural Gas-Derived Polycyclic Aromatic Hydrocarbons in a Lagoon Sediment (original) (raw)

2000, Environmental Science & Technology

https://doi.org/10.1021/ES0010002

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Abstract

... Carole McRae, † Colin E. Snape,* ‡ Cheng-Gong Sun, † Daniele Fabbri, § Daniele Tartari, § Claudio ... 31 to −62 ‰) is ascribed mainly to biodegradation rather than to major inputs from sources of isotopically heavy PAH, such as the neighboring modern-day carbon black plants. ...

Polycyclic aromatic hydrocarbons in ancient sediments and their relationships to palaeoclimate

Organic Geochemistry, 1998

ÐCombustion-derived and land-plant-derived polycyclic aromatic hydrocarbons (PAHs) have been investigated for an Upper Triassic to Middle Jurassic sedimentary sequence from the Northern Carnarvon Basin, Western Australia. The former included¯uoranthene, pyrene, benzo¯uoranthenes, benzo[e]pyrene and benzo[a]pyrene, and the latter included retene, cadalene and simonellite. Combustion-derived PAHs are most abundant in the Upper Triassic and late Lower Jurassic sediments. The abundances of land-plant-derived markers all maximise in the upper part of the Lower Jurassic section, but vary independently of one another through time. The changes in the relative abundances of these markers have been related to the variation of regional climatic conditions, especially the changes in humidity and seasonality during the Late Triassic to Middle Jurassic times.

Dissolved, particulate and sedimentary naturally derived polycyclic aromatic hydrocarbons in a coastal environment: geochemical significance

Marine Chemistry, 1993

. Dissolved, particulate and sedimentary naturally derived polycyclic aromatic hydrocarbons in a coastal environment: geochemical significance. Mar. Chem.,. Polycyclic aromatic hydrocarbons (PAH) derived from natural precursors have been analysed in superficial sediments and waters in the deltaic area of the Rhrne river. This area is characterized by major water and solid inputs from the Rhrne river into the Mediterranean Sea. Nine superficial sediment samples were collected in , with further separation of particulate and dissolved phases. After extraction of lipids, isolation and fractionation of hydrocarbons by HPLC, PAH were analysed by GC and GC-MS. Retene and tetrahydrochrysenes (THCs) were the major naturally derived PAH detected in the Rhrne delta. They derive from diterpenoid and triterpenoid precursors, which are common constituents of terrestrial plants. In sediments, intermediate products were absent or at trace levels, suggesting that formation of natural PAH occurred mainly before deposition. Concentrations of retene and THCs were in the range 12.92-52.86 ngg-~ and 16.56-162.68 ngg -~ , respectively. Their distributions were different from those of anthropogenic PAH. Despite their common origin, retene and THCs did not show identical distributions and relations to parameters such as total organic carbon and terrestrial n-alkanes; these findings indicate that they follow different transport pathways, as a result of different particle associations. Estimations of retene and THC fluxes and the use of these markers for determining the percentage of 'terrestrial organic carbon' are presented. Analysis of water samples confirmed that naturally derived PAH were mainly formed before deposition, in soils of the drainage basin or during the early stages of riverine transport. The distributions of natural and anthropogenic PAH were different, which suggests that the carrier particles of natural PAH were coarser and settled more rapidly than those carrying anthropogenic PAH. However, retene and THCs did not appear to be associated with the same particle types, shown by distributional differences and by the presence of retene in the dissolved phase in contrast to THCs. Consequently, the distributional trends observed in sediments can be explained by the different aquatic transport of the various PAH classes as demonstrated by the analysis of water samples. Instantaneous fluxes were estimated in three seasons for both dissolved and particulate phases. They again showed decoupling between natural and anthropogenic PAH. Fluxes of natural PAH were strongly dependent on the river flow, whereas those of anthropogenic pAH were more dependent on emission rates. The dissolved phase was a significant factor in the transport of retene and of anthropogenic PAH. Naturally derived PAH, and more specifically THCs, appear to be promising tracers of inputs and dispersal of continental organic matter.

Distribution and sources of polycyclic aromatic hydrocarbons in surface sediments from two Brazilian estuarine systems

Journal of the Brazilian Chemical Society, 2010

Este estudo concentra-se nos sistemas estuarinos tropicais de Mundaú-Manguaba (MMELS) e do Rio Paraíba do Sul (PSR), ambos no Brasil e afetados por práticas da monocultura da canade-açúcar e por urbanização. Os níveis de 17 hidrocarbonetos policíclicos aromáticos (HPAs), 16 dos quais são classificados como poluentes prioritários para estudos ambientais pela US-EPA e o perileno (HPA biogênico) foram avaliados nos sedimentos superficiais para identificar fontes da poluição e determinar níveis base como estratégias para gerenciamentos futuros. O Σ16HPAs variou de 2,90 a 231,30 μg kg -1 em MMELS e de 87,10 a 9344,29 μg kg -1 no PSR. As relações entre HPAs isômeros sugeriram principalmente fontes de origem pirogênica. This study focuses on the tropical estuarine systems of Mundaú-Manguaba (MMELS) and Paraíba do Sul River (PSR), Brazil, affected by sugarcane monoculture practices and also urbanization. The levels of 17 polycyclic aromatic hydrocarbons (PAHs), 16 of which are classified as priority pollutants by the US-EPA and perylene (a biogenic PAH) were measured in surface sediments to identify pollution sources and determine baseline data looking for future management strategies. The Σ16PAH ranged from 2.90 to 231.30 μg kg -1 in MMELS and from 87.10 to 9344.29 μg kg -1 in the PSR. PAH isomeric ratios suggested mainly pyrogenic input.

Concentrations and sources of polycyclic aromatic hydrocarbons in surface coastal sediments of the northern Gulf of Mexico

Geochemical Transactions, 2014

Background: Coastal sediments in the northern Gulf of Mexico have a high potential of being contaminated by petroleum hydrocarbons, such as polycyclic aromatic hydrocarbons (PAHs), due to extensive petroleum exploration and transportation activities. In this study we evaluated the spatial distribution and contamination sources of PAHs, as well as the bioavailable fraction in the bulk PAH pool, in surface marsh and shelf sediments (top 5 cm) of the northern Gulf of Mexico. Results: PAH concentrations in this region ranged from 100 to 856 ng g −1 , with the highest concentrations in Mississippi River mouth sediments followed by marsh sediments and then the lowest concentrations in shelf sediments. The PAH concentrations correlated positively with atomic C/N ratios of sedimentary organic matter (OM), suggesting that terrestrial OM preferentially sorbs PAHs relative to marine OM. PAHs with 2 rings were more abundant than those with 5-6 rings in continental shelf sediments, while the opposite was found in marsh sediments. This distribution pattern suggests different contamination sources between shelf and marsh sediments. Based on diagnostic ratios of PAH isomers and principal component analysis, shelf sediment PAHs were petrogenic and those from marsh sediments were pyrogenic. The proportions of bioavailable PAHs in total PAHs were low, ranging from 0.02% to 0.06%, with higher fractions found in marsh than shelf sediments. Conclusion: PAH distribution and composition differences between marsh and shelf sediments were influenced by grain size, contamination sources, and the types of organic matter associated with PAHs. Concentrations of PAHs in the study area were below effects low-range, suggesting a low risk to organisms and limited transfer of PAHs into food web. From the source analysis, PAHs in shelf sediments mainly originated from direct petroleum contamination, while those in marsh sediments were from combustion of fossil fuels.

Polycyclic aromatic hydrocarbons pollution in sediments: Distribution and sources in a lagoon system (Orbetello, Central Italy)

1 - The presence, distribution and origin of 16 US EPA polycyclic aromatic hydrocarbons (PAHs) in the surface sediments of Orbetello lagoon (Tuscany, Italy) were investigated by high pressure liquid chromatography (HPLC). 2 - PAH concentrations in the sediments (Σ16PAHs) ranged from 0.92 to 279.38 ng/g of dry matrix, indicating low PAHs pollution. A prevalence of high molecular weight PAHs was observed (>90% of Σ16PAHs) with a considerable predominance of 4-rings PAHs; fluoranthene was the dominant compound. 3 - A comparison with other studies of total PAHs suggests that the levels are within the concentration ranges already reported by the other authors. Total PAH concentrations measured in the studied area indicate a relatively clean environment when compared to values reported by the literature for Mediterranean lagoons. 4 - Molecular ratios were calculated in order to estimate PAH origin and transport from sources. As indicated by the Phen/Ant and Flu/Pyr molar ratio, the mai...

Polycyclic aromatic hydrocarbons in Recent lake sediments—I. Compounds having anthropogenic origins

Geochimica et Cosmochimica Acta, 1980

Polycyclic aromatic hydrocarbons (PAHj in sediment cores from Lake Lucerne, Lake Ziirich. and Greifensee. Switzerland. and Lake Washington. northwest U.S.A.. have been Isolated, identified and quantified by glass capillary gas chromatography and gas chromatography/mass spectrometry. Surface sediment layers are greatly enriched in PAH-up to 40 times--compared to deeper layers. In addition, concentration increases in upper sediments generally correspond to increasing industrialization and urbanization in the catchment basins of the lakes. Few PAH could be detected in pre-industrial revolution sediments. indicating that background levels for most PAH in aquatic sediments are extremely low.

Cited by

Anthropogenic disturbance and spatial heterogeneity of macrobenthic invertebrate assemblages in coastal lagoons: the study case of Pialassa Baiona (northern Adriatic Sea

Helgoland Marine Research, 2011

The distribution patterns of macrobenthic invertebrate assemblages at different spatial scales and in relation to natural and anthropogenic disturbance gradients were investigated in the Pialassa Baiona, a eutrophic and polluted brackish coastal lagoon located along the Italian coast of the northern Adriatic Sea. This coastal lagoon shows a complex physiography with several shallow water ponds and channels separated by discontinuous artificial embankments. Environmental variables and macrobenthic invertebrate assemblages showed higher heterogeneity at small spatial scale (i.e. within channels and ponds). Distinction between channels and ponds is only weakly supported by the distribution patterns of macrobenthic assemblages. Depth was the major factor in structuring benthic communities within ponds, while species distributions along the channels were strongly correlated with the anthropogenic disturbance gradient. Anthropogenic disturbance mainly affected species richness, which was inversely correlated with the organic carbon contents in the sediments and the water surface temperature, which is affected by the input of cooling water from two thermal power plants. Some opportunistic species, like the polychaetes Streblospio shrubsolii and Capitella capitata, were more abundant in the southern polluted areas. In particular, the abundance of S. shrubsolii significantly increased with organic carbon contents in the sediments and water surface temperature, while C. capitata was more abundant in the warmed sites and close to sewages. Conversely, the abundance of the amphipod Corophium insidiosum was inversely related to organic carbon contents.

Carbon Isotope Signatures and Polyarenes in the Pedogenic Material of Ice Wedges of the Batagay Yedoma (Yakutia)

Eurasian Soil Science, 2020

The carbon isotope signatures and the content of polycyclic aromatic hydrocarbons (PAHs) in the pedogenic material of inclusions in ice wedges of the Batagay yedoma (Yakutia) are studied. The mean concentration of 11 PAHs is 170 ppb (minimum, 7 ppb and maximum, 430 ppb) and the mean δ 13 С value in soil lipids is-29‰ (minimum,-31.1‰ and maximum,-26.2‰). The prevalent polyarenes in associations are naphthalene homologs and phenanthrene. Trace amounts of heavy PAHs, including benzo[a]pyrene (an indicator of pyrogenic processes), are also detectable. The PAH contents and δ 13 С values in ice wedges show the trend of a decrease with depth. The δ 13 С values and PAH content suggest a pedogenic origin of the deposit: therefore, PAHs originate from plant residues and wildfires. The observed trend of changes in the concentrations of polyarenes along the ice wedge may be associated with the changes in landscapes in the Late Pleistocene.

Sources of polycyclic aromatic hydrocarbons to the Guaratuba Bay, Brazil

The coasts of Bohai Sea (BS) and Yellow Sea (YS) in China support almost one-quarter of its population and provide more than one-third of the national GDP. BS and YS are downwind of the Asian continental outflow in spring and winter as influenced by the East Asian monsoon. This makes the two seas important sinks of land-based pollutants associated with the Asian continental outflow. The sixteen U.S. EPA proposed priority polycyclic aromatic hydrocarbons (PAHs) in 130 surface sediment samples collected from BS and YS were measured. Combined with our previous PAH data of 90 PM 2.5 samples from the upwind areas, the sources of the PAHs in BS and YS were apportioned using positive matrix factorization (PMF) modeling. Four sources were identified: petroleum residue, vehicular emissions, coal combustion and biomass burning. Petroleum residue was the dominant contributor of PAHs in the coast of the Bohai Bay probably due to Haihe River runoff, oil leakage from ships and offshore oil fields. The contribution of vehicular emissions in BS was higher than that in YS, and the reverse was true for coal combustion and biomass burning. This difference in the source patterns in the sediments of the two seas could be attributed to the different PAH emission features of the upwind area related to demographic and economic conditions, as well as the marine geography. The ratios of selected 4-6 ring PAHs in the sediments compared well with those of the PM 2.5 of the upwind areas, implicating that the particle phase PAHs in the atmosphere play an important role in the source to sink process of the pyrogenic PAHs in the region.

Distribution and sources of polycyclic aromatic hydrocarbons (PAHs) in laminated Santa Barbara Basin sediments

Organic Geochemistry, 2017

After the impoundment of the Three Gorges Reservoir (TGR), the hydrological situation of the 21 reservoir has changed greatly. The concentration and distribution of typical persistent organic 22 pollutants in water and sediment have also changed accordingly. In this study, the 23 concentration, distribution and potential sources of 16 polycyclic aromatic hydrocarbons 24 (PAHs) and 6 phthalic acid esters (PAEs) during the water drawdown and impoundment 25 periods were investigated in water and sediment from the TGR. According to our results, PAHs 26 and PAEs showed temporal and spatial variations. The mean ΣPAH and ΣPAE concentrations 27 in water and sediment were both higher during the water impoundment period than during 28 the water drawdown period. The water samples from the main stream showed larger ΣPAH 29 concentration fluctuations than those from tributaries. Both the PAH and PAE concentrations 30 meet the Chinese national water environmental quality standard (GB 3838-2002). PAH 31 monomers with 2-3 rings and 4 rings were dominant in water, and 4-ring and 5-6-ring PAHs 32 were dominant in sediment. Din -butyl phthalate (DBP) and di-2-ethylhexyl phthalate (DEHP) 33 were the dominant PAE pollutants in the TGR. DBP and DEHP had the highest concentrations 34 in water and sediment, respectively. The main source of PAHs in water from the TGR was 35 petroleum and emissions from coal and biomass combustion, whereas the main sources of 36 PAHs in sediments included coal and biomass combustion, petroleum, and petroleum 37 combustion. The main source of PAEs in water was domestic waste, and the plastics and heavy 38 chemical industries were the main sources of PAEs in sediment Q5 .

Sedimentary record of anthropogenic and biogenic polycyclic aromatic hydrocarbons in San Francisco Bay, California

Marine Chemistry, 1999

Dated sediment cores collected from Richardson and San Pablo Bays in San Francisco Bay were used to reconstruct a Ž . history of polycyclic aromatic hydrocarbon PAH contamination. The sedimentary record of PAHs in Richardson Bay shows that anthropogenic inputs have increased since the turn of the century, presumably as a result of increasing urbanization and industrialization around the Bay Area. Concentrations range from about 0.04-6.3 mg g y1 . The dominant origin of the PAHs contributing to this modern contamination is from combustion processes. Depth profiles in San Pablo Bay indicate higher concentrations of PAHs since the 1950s than during the late 1800s, also presumably resulting from an increase in urbanization and industrialization. Total PAHs in San Pablo Bay range from about 0.04-1.3 mg g y1 . The ratios Ž . of methylphenanthrenesrphenanthrene and methylfluoranthenesq methylpyrenes rfluoranthene were sensitive indicators of anthropogenic influences in the estuary. Variations in the ratio of 1,7-dimethylphenanthrener2,6-dimethylphenanthrene indicate a gradual replacement of wood by fossil-fuel as the main combustion source of PAHs in San Francisco Bay sediments. The profile of perylene may be an indicator of eroding peat from marshlands. q 1999 Elsevier Science B.V. All rights reserved.

Open Access Origin and Distribution of Polycyclic Aromatic Hydrocarbons in Lagoon

2016

3Laboratoire de Physico- et Toxico-Chimie de l’Environnement (LPTC) Université de Bordeaux 1, France Abstract: Polycyclic Aromatic Hydrocarbons (PAHs) were determined in sediments and bivalves by the Gas chromatography coupled to Mass spectrometer (GC/MS). PAHs concentrations in sediments of My Bousselham and Khnifiss, Atlantics lagoons, (expressed as ∑PAH) ranged from 31 to 82 ng/g of dry weight and from 6.6 to 34 ng/g of dry weight, respectively. Concerning organisms, PAHs levels contamination ranged from 28 to 117 ng/g of dry weight for My Bousselham (Ruditapes Decussates) and from 7 to 18.5 ng/g of dry weight for Khnifiss Lagoon Oyster (Crassostrea gigas). In the Med Lag (Nador), the results obtained showed a range varying from 6 to 126 ng/g of dry weight for sediments and from 24 to 32 ng/g of dry weight for organisms (Mytilus Galoprovincialis). The origin investigation of PAHs in sediment revealed, that the process of combustion was the main source in these Lagoons, while the ...

Determination of parent and alkylated polycyclic aromatic hydrocarbons (PAHs) in biota and sediment

2009

This series presents detailed descriptions of methods and procedures relating to chemical and biological measurements in the marine environment. Most techniques described have been selected for documentation based on performance in ICES or other intercalibration or intercomparison exercises: they have been carefully evaluated and shown to yield good results when correctly applied. They have also been subject to review by relevant ICES working groups, but this is not to be construed as constituting official recommendation by the Council.

Resolving coal and petroleum-derived polycyclic aromatic hydrocarbons (PAHs) in some contaminated land samples using compound-specific stable carbon isotope …

Fuel, 2003

4684] that, for thermal conversion regimes where volatiles survive to a significant degree (e.g. low and high temperature carbonisation, domestic combustion), the stable carbon isotopic signatures of polycyclic aromatic hydrocarbons (PAHs) are similar to those of the parent coals (ca. 225‰, cf. 2 23.5‰ for the coals). This information has been used to unambiguously identify coal-derived PAHs in contaminated land sites. Aromatic hydrocarbons in a number of samples analysed from a former foundry site at Mansfield displayed variable compositions with those containing predominately alkylated benzenes and naphthalenes having carbon stable isotopic ratios in the range of 2 28 to 2 30‰, typical of transport fuels. The aliphatic hydrocarbon distributions confirmed the petroleum origin and indicated that the oil had also been biodegraded. Less negative (enriched in 13 C, 225 to 2 26‰) isotopic profiles were obtained for the fractions rich in 3 -6 ring parent PAHs, indicating a significant input from coal utilisation. Separating the aromatic by ring size enabled the coal-derived 3 -6 ring PAHs to be identified in samples where petroleum-derived alkylated benzenes and naphthalenes dominated. A similar situation to this with only a small input from coal-derived PAHs was found for a soil heavily contaminated with diesel fuel from the Motherwell area. Carbon stable isotopic data taken in conjunction with PAH distributions indicate that the coal tar contaminating an area of Glasgow Green, which was believed to be dumped during the Second World War and was unearthed recently, probably originated from a high temperature coking plant as opposed to a gas works, as indicated by the isotopic signatures of the distributions of PAHs. q

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