Brentwood, Canada
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Yunker M.B.,7137 Wallace Dr. | Macdonald R.W.,Canadian Department of Fisheries and Oceans | Ross P.S.,Vancouver Aquarium Marine Science Center | Johannessen S.C.,Canadian Department of Fisheries and Oceans | Dangerfield N.,Canadian Department of Fisheries and Oceans
Organic Geochemistry | Year: 2015

Marine coastal areas of British Columbia, Canada are subject to a gradient of increasing anthropogenic sources from pristine areas in the north to the more urbanised areas of the south. Along the gradient, the relative contributions of polycyclic aromatic hydrocarbons (PAHs) from multiple natural and anthropogenic sources are not well understood, but concerns linger about bioavailability and consequent risks to marine biota. Composition patterns and principal components analysis (PCA) models for surface sediment and core samples collected along this transect indicate that samples from the urbanised Vancouver area have the highest proportions of tricyclic terpane, hopane and sterane biomarkers, UCM (unresolved complex mixture), the alkyl fluoranthene/pyrene and benz[a]anthracene/chrysene series and most parent PAHs. Those from Hecate and Queen Charlotte Straits and other locations in the Strait of Georgia have, on the other hand, higher proportions of the resolved alkanes, and petrogenic alkyl naphthalene, fluorene, dibenzothiophene and phenanthrene/anthracene series. PAH ratios clearly indicate a predominance of combustion sources for the four ring and higher parent PAHs for all the sediments. Most samples have values close to the biomass/solid fuel and liquid fuel combustion borderline for ratios of the major PAHs, but liquid fuel combustion input dominates closer to urbanised locations. Ratios also suggest similar pyrogenic and petrogenic inputs between central Hecate Strait and reference sediments from Hecate Strait through to Queen Charlotte Strait, which indicates that biomass combustion and immature coal formations are the major putative respective sources for the reference areas. Alkyl PAH ratios for the C3 and C4 naphthalenes, C2 and C3 phenanthrenes and 3- and 2-methylchrysene, reflecting terrigenous/vascular plant sources and petroleum maturity, exhibit marked differences between Comox bituminous coal and Alberta Sweet Mixed Blend (ASMB) oil and reveal that the petrogenic input in all of the sediments is non-biodegraded. Ratios of these alkyl PAHs with multiple substituents indicate that the sediment samples in the northern Strait of Georgia closest to the Comox coal field receive relatively constant input of eroded coal, while those in the southern Strait of Georgia and Vancouver Harbour show a composition closest to ASMB oil. PAHs associated with liquid fossil fuel combustion and petroleum discharges adjacent to urbanised areas are expected to be fully bioavailable to marine food webs, while the char from biomass combustion and coal from immature deposits in more remote areas would have limited bioavailability. This implies that biota in remote areas of Hecate Strait/Queen Charlotte Sound are likely not adapted to the presence of oil and thus would be more sensitive to exposure to spilled oil than those in the more impacted environments in southern British Columbia. © 2015 Elsevier Ltd.

Feng X.,CAS Institute of Botany | Feng X.,ETH Zurich | Gustafsson O.,University of Stockholm | Holmes R.M.,Woods Hole Oceanographic Institution | And 13 more authors.
Global Biogeochemical Cycles | Year: 2015

Distinguishing the sources, ages, and fate of various terrestrial organic carbon (OC) pools mobilized from heterogeneous Arctic landscapes is key to assessing climatic impacts on the fluvial release of carbon from permafrost. Through molecular 14C measurements, including novel analyses of suberin- and/or cutin-derived diacids (DAs) and hydroxy fatty acids (FAs), we compared the radiocarbon characteristics of a comprehensive suite of terrestrial markers (including plant wax lipids, cutin, suberin, lignin, and hydroxy phenols) in the sedimentary particles from nine major arctic and subarctic rivers in order to establish a benchmark assessment of the mobilization patterns of terrestrial OC pools across the pan-Arctic. Terrestrial lipids, including suberin-derived longer-chain DAs (C24,26,28), plant wax FAs (C24,26,28), and n-alkanes (C27,29,31), incorporated significant inputs of aged carbon, presumably from deeper soil horizons. Mobilization and translocation of these "old" terrestrial carbon components was dependent on nonlinear processes associated with permafrost distributions. By contrast, shorter-chain (C16,18) DAs and lignin phenols (as well as hydroxy phenols in rivers outside eastern Eurasian Arctic) were much more enriched in 14C, suggesting incorporation of relatively young carbon supplied by runoff processes from recent vegetation debris and surface layers. Furthermore, the radiocarbon content of terrestrial markers is heavily influenced by specific OC sources and degradation status. Overall, multitracer molecular 14C analysis sheds new light on the mobilization of terrestrial OC from arctic watersheds. Our findings of distinct ages for various terrestrial carbon components may aid in elucidating fate of different terrestrial OC pools in the face of increasing arctic permafrost thaw. © 2015. American Geophysical Union. All Rights Reserved.

Harris K.A.,Canadian Department of Fisheries and Oceans | Harris K.A.,University of Victoria | Yunker M.B.,7137 Wallace Dr. | Dangerfield N.,Canadian Department of Fisheries and Oceans | Ross P.S.,Canadian Department of Fisheries and Oceans
Environmental Pollution | Year: 2011

Sediment-associated hydrocarbons can pose a risk to wildlife that rely on benthic marine food webs. We measured hydrocarbons in sediments from the habitat of protected sea otters in coastal British Columbia, Canada. Alkane concentrations were dominated by higher odd-chain n-alkanes at all sites, indicating terrestrial plant inputs. While remote sites were dominated by petrogenic polycyclic aromatic hydrocarbons (PAHs), small harbour sites within sea otter habitat and sites from an urban reference area reflected weathered petroleum and biomass and fossil fuel combustion. The partitioning of hydrocarbons between sediments and adjacent food webs provides an important exposure route for sea otters, as they consume ∼25% of their body weight per day in benthic invertebrates. Thus, exceedences of PAH sediment quality guidelines designed to protect aquatic biota at 20% of the sites in sea otter habitat suggest that sea otters are vulnerable to hydrocarbon contamination even in the absence of catastrophic oil spills. © 2010 Published by Elsevier Ltd.

Feng X.,CAS Institute of Botany | Feng X.,ETH Zurich | Feng X.,Woods Hole Oceanographic Institution | Gustafsson O.,University of Stockholm | And 13 more authors.
Biogeosciences | Year: 2015

Hydrolyzable organic carbon (OC) comprises a significant component of sedimentary particulate matter transferred from land into oceans via rivers. Its abundance and nature are however not well studied in Arctic river systems, and yet may represent an important pool of carbon whose fate remains unclear in the context of mobilization and related processes associated with a changing climate. Here, we examine the molecular composition and source of hydrolyzable compounds isolated from sedimentary particles derived from nine rivers across the pan-Arctic. Bound fatty acids (b-FAs), hydroxy FAs, n-alkane-α,ω-dioic acids (DAs) and phenols were the major components released upon hydrolysis of these sediments. Among them, b-FAs received considerable inputs from bacterial and/or algal sources, whereas ω-hydroxy FAs, mid-chain substituted acids, DAs, and hydrolyzable phenols were mainly derived from cutin and suberin of higher plants. We further compared the distribution and fate of suberin- and cutin-derived compounds with those of other terrestrial biomarkers (plant wax lipids and lignin phenols) from the same Arctic river sedimentary particles and conducted a benchmark assessment of several biomarker-based indicators of OC source and extent of degradation. While suberin-specific biomarkers were positively correlated with plant-derived high-molecular-weight (HMW) FAs, lignin phenols were correlated with cutin-derived compounds. These correlations suggest that, similar to leaf-derived cutin, lignin was mainly derived from litter and surface soil horizons, whereas suberin and HMW FAs incorporated significant inputs from belowground sources (roots and deeper soil). This conclusion is supported by the negative correlation between lignin phenols and the ratio of suberin-to-cutin biomarkers. Furthermore, the molecular composition of investigated biomarkers differed between Eurasian and North American Arctic rivers: while lignin dominated in the terrestrial OC of Eurasian river sediments, hydrolyzable OC represented a much larger fraction in the sedimentary particles from Colville River. Hence, studies exclusively focusing on either plant wax lipids or lignin phenols will not be able to fully unravel the mobilization and fate of bound OC in Arctic rivers. More comprehensive, multi-molecular investigations are needed to better constrain the land-ocean transfer of carbon in the changing Arctic, including further research on the degradation and transfer of both free and bound components in Arctic river sediments. © Author(s) 2015.

Yunker M.B.,7137 Wallace Dr. | McLaughlin F.A.,Canadian Department of Fisheries and Oceans | Fowler M.G.,Geological Survey of Canada | Fowler B.R.,Axys Analytical Ltd.
Organic Geochemistry | Year: 2014

Significant reserves of oil and gas have been predicted for Hecate Strait, a pristine, semi-enclosed sea on the continental shelf adjacent to British Columbia, on the west coast of Canada. To establish a baseline for the natural background of hydrocarbons in sediment prior to any further offshore oil and gas development or increase in oil tanker traffic in the Hecate Strait region, three sediment box cores were collected along a west to east transect across southern Hecate Strait in September 2003. 210Pb measurements established that the bottom sections date to ~1920, pre-1800 and ~1870, respectively, which predate any significant industrial development on the coast. Alkane and polycyclic aromatic hydrocarbon (PAH) concentrations are low in most sediment samples and both the concentrations and fluxes differ little between surface and bottom core sections. PAH profiles exhibit a dominance of alkyl PAHs for each alkyl PAH homologous series with varying amounts of parent (unsubstituted) PAHs, while alkane chromatograms show no unresolved complex mixture (UCM), and there is little change in composition between present day and pre-1800 sediments for most parameters. Principal components analysis (PCA) models, and PAH and biomarker ratios indicate that composition patterns are consistent with low and varying natural petrogenic and pyrogenic inputs, with little or no anthropogenic input. The most likely primary source of petrogenic PAHs to the sediments is Cenozoic lignites from the Skonun Formation, which outcrops on Haida Gwai and underlies most of Hecate Strait. Two subsurface sections (deposited in ~1990 and ~1930) in the core from Milbanke Sound, on the east side of the transect, have elevated concentrations for the alkyl phenanthrene/anthracenes and dibenzothiophenes with no UCM, and most likely also have a source in immature coal. This study suggests that the Hecate Strait environment has low hydrocarbon concentrations, with an apparent minor role for oil seeps and a likelihood that most of the petrogenic PAH sources are shales or immature coals with limited PAH bioavailability. If these characteristics are representative of Hecate Strait sediments overlying the Queen Charlotte Basin, it may mean that biota are likely unadapted to the presence of oil and thus would be more sensitive to exposure to oil from an oil spill than those in a more impacted environment. © 2014 Elsevier Ltd.

Yunker M.B.,7137 Wallace Dr. | Lachmuth C.L.,Canadian Department of Fisheries and Oceans | Cretney W.J.,13 909 Carolwood Dr. | Fowler B.R.,Axys Analytical Ltd. | And 3 more authors.
Marine Environmental Research | Year: 2011

The question of polycyclic aromatic hydrocarbon (PAH) bioavailability and its relationship to specific PAH sources with different PAH binding characteristics is an important one, because bioavailability drives PAH accumulation in biota and ultimately the biochemical responses to the PAH contaminants. The industrial harbour at Kitimat (British Columbia, Canada) provides an ideal location to study the bioavailability and bioaccumulation of sediment hydrocarbons to low trophic level biota. Samples of soft shell clams (Mya arenaria) and intertidal sediment collected from multiple sites over six years at various distances from an aluminium smelter and a pulp and paper mill were analysed for 106 PAHs, plant diterpenes and other aromatic fraction hydrocarbons. Interpretation using PAH source ratios and multivariate data analysis reveals six principal hydrocarbon sources: PAHs in coke, pitch and emissions from anode combustion from the aluminium smelter, vascular plant terpenes and aromatised terpenes from the pulp and paper mill, petroleum PAHs from shipping and other anthropogenic activities and PAHs from natural plant detritus. Harbour sediments predominantly contain either pitch or pyrogenic PAHs from the smelter, while clams predominantly contain plant derived PAHs and diterpenes from the adjacent pulp mill. PAHs from the smelter have low bioavailability to clams (Biota-Sediment Accumulation Factors; BSAFs <1 for pitch and coke; <10 for anode combustion, decreasing to ~0.1 for the mass 300 and 302 PAHs), possibly due to binding to pitch or soot carbon matrices. Decreases in PAH isomer ratios between sediments and clams likely reflect a combination of variation in uptake kinetics of petroleum PAHs and compound specific metabolism, with the importance of petroleum PAHs decreasing with increasing molecular weight. Plant derived compounds exhibit little natural bioaccumulation at reference sites, but unsaturated and aromatised diterpenes released from resins by industrial pulping processes are readily accumulated by the clams (BSAFs >500). Thus while most of the smelter associated PAHs in sediments may not be bioavailable to benthic organisms, the plant terpenes (including retene, totarol, ferruginol, manool, dehydroabietane and other plant terpenes that form the chemical defence mechanism of conifers) released by pulp mills are bioavailable and possess demonstrated toxic properties. The large scale release of plant terpenes by some of the many pulp mills located in British Columbia and elsewhere represents a largely undocumented risk to aquatic biota. © 2011 Elsevier Ltd.

Yunker M.B.,7137 Wallace Dr. | Macdonald R.W.,Canadian Department of Fisheries and Oceans | Snowdon L.R.,Snowdon Research | Fowler B.R.,Axys Analytical Ltd.
Organic Geochemistry | Year: 2011

We present the first sedimentary biomarker study encompassing the entire Arctic Ocean. A large data set of organic markers for terrigenous, petroleum and combustion inputs [alkanes, hopanes and steranes, parent and alkyl polycyclic aromatic hydrocarbons (PAHs)] is examined for patterns in space and time using principal components analysis (PCA) and partial least squares (PLS). Biomarker patterns reveal the central Arctic Ocean basin sediments to be compositionally distinct from those of the Mackenzie River/Beaufort Sea and Barents Sea, but similar to those of the Laptev Sea. PAH distributions reflected in PAH ratios and PCA projections demonstrate that Arctic Ocean sediment is dominated by natural inputs to the extent that anthropogenic combustion PAHs are not significant. We find only modest changes between the glacial and post-glacial sediments for atmospherically transported hydrocarbon biomarkers, while particle associated biomarkers were captured strongly at basin edges during the glacial period, and much more evenly transported across basins during the post-glacial period. The orders of magnitude decreases in particle associated petrogenic alkanes and PAHs in central basins during glacial times, coupled with the uniformity of most petrogenic biomarker parameters for most basin and shelf locations, reflect a massive reduction in ice transport that makes the margins the most likely source of petrogenic material for the Pleistocene/Holocene central Arctic basins. The proximity of large coal deposits of various maturity levels along the Lena River, the overlap in PAH and biomarker composition of the Laptev Sea and surficial sediments from the central Arctic Ocean and the location of the Laptev Sea at the origin of the main Transpolar Drift all point to eroded coals from the Lena River/Laptev Sea as the likely source of petrogenic hydrocarbons to the central Arctic Ocean. The ubiquitous presence of allochthonous coal in Arctic Ocean surface sediments provides a major constraint on the use of petrogenic biomarkers to infer the presence of subsurface petroleum reserves. © 2011 Elsevier Ltd.

Yunker M.B.,7137 Wallace Dr. | Perreault A.,Capital Regional District | Lowe C.J.,Capital Regional District
Organic Geochemistry | Year: 2012

Previous studies have suggested that coal from the 1891 shipwreck of a collier off Victoria, BC, Canada is responsible for elevated parent (unsubstituted) PAH concentrations in sediments near deep marine outfalls from Esquimalt and Victoria in the Strait of Juan de Fuca. To resolve this question, we analysed a comprehensive suite of resolved and unresolved complex mixture (UCM) alkanes, tricyclic terpane, hopane and sterane biomarkers, and parent and alkyl polycyclic aromatic hydrocarbons (PAHs) in samples of coal, wastewater and sediments. Composition patterns, principal components analysis (PCA) models and PAH and biomarker ratios all indicate that coal from the collier does not make a dominant contribution to any sediment sample. Mass balance calculations based on the n-C 24 content and 24/4 tetracyclic terpane to 26/3R tricyclic terpane ratio in coal provide a particularly good match between predicted and observed alkyl PAH concentrations for sediments with high alkyl naphthalenes and phenanthrene/anthracenes and low UCM, but the predicted coal contribution substantially underestimates the measured parent PAHs for all sediment samples. Methylbenz[a]anthracene/chrysene profiles for sediments with a dominance of parent PAHs are very close to coal tar, with a marked predominance of methylbenz[a]anthracenes and the possible 10-methylbenz[a]anthracene as a major constituent, while the methylchrysenes predominate in coal. Hence, coal from the collier could account for most alkyl PAHs in the sediments, but dredged sediment containing pyrolised coal waste from a former coal gas plant in Victoria Harbour is a more likely source for the samples with elevated parent PAHs. PAH ratios indicate that these sources are superimposed on combustion PAHs introduced by a combination of atmospheric deposition and delivery via stormwater and the outfalls. Parent PAH distributions also suggest that PAHs in wastewater that originate from oils and soot in liquid fossil fuel combustion are dispersed and degraded, while the larger wood char particles (containing PAHs more protected from degradation) settle closer to the outfalls. Overall, results suggest that PAHs have predominant sources in wood combustion, coal and possibly coke, with a likelihood of much lower bioavailability than would be expected from wastewater dominated by oils and soot from vehicle combustion. © 2012 Elsevier Ltd.

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