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Geology topics

Thomas M. Holsen

Publications and source records attributed to Thomas M. Holsen.

6 recordsLinked to original sources

Bioaccumulation of perfluoroalkyl substances in a Lake Ontario food web

Per- and polyfluoroalkyl substances (PFAS) are a group of synthetic chemicals detected throughout the environment. To better understand the distribution of PFAS in an aquatic system (the Laurentian Great Lakes), stable isotope enrichment (δ13C and δ15N), fatty acid (FA) profiles, and PFAS were measured in various species from the Lake Ontario (LO) aquatic food web. Sampled organisms included top predator fish, prey fish, and benthic and pelagic macroinvertebrates. The trophic level of each species in the LO food web was determined using δ15N, and FA concentrations (range: <1–139 mg/g wet weight (ww)). The individual PFAS concentrations in the LO food web were ~1.5 to 5 times lower than previously reported. The highest PFAS concentrations were observed in deepwater sculpin (Myoxocephalus thompsonii, 150 ± 35.7 ng/g ww) suggesting a potential source of PFAS from the offshore benthic zone or sediment. The concentration of PFOS and long chain (C9-C14) perfluoroalkyl carboxylic acids (PFCAs) were significantly higher than short chain PFAS indicating the significant impact of hydrophobicity on the bioaccumulation of PFAS in organisms from the food web. However, high molecular weight PFCAs (>C8) did not exhibit increasing biomagnification factors (BMFs) and trophic magnification factors (TMFs) with log Kow, suggesting hydrophobicity does not govern the movement of PFAS from low to high trophic levels in the LO food web.

Lake Ontario

Characterization of halogenated organic compounds in pelagic sharks and sea turtles using a nontargeted approach

Halogenated organic compounds (HOCs) in marine species collected from the Atlantic Ocean [3 shortfin mako ( Isurus oxyrinchus ) and 1 porbeagle ( Lamna nasus )], and 12 sea turtles collected from the Pacific Ocean [3 loggerhead ( Caretta caretta ), 3 green ( Chelonia mydas ), 3 olive ridley ( Lepidochelys olivacea ), and 3 hawksbill ( Eretmochelys imbricata )] were analyzed with a nontargeted analytical method using two-dimensional gas chromatography coupled to high-resolution time-of-flight mass spectrometry. Sharks and sea turtles had distinct HOC profiles. Halogenated methoxyphenols (halo-MeOPs) were the most abundant compound class identified in sea turtle livers, while polychlorinated biphenyls (PCBs) were the most abundant in shark livers. In addition to legacy contaminants and halo-MeOPs, a total of 110 nontargeted/novel HOCs (NHOCs) were observed in the shark livers. Shortfin mako collected from the northern Gulf of Mexico contained the largest number (89) and most diverse structural classes of NHOCs. Among all NHOCs, a group of compounds with the elemental composition C 14 H 12– n Cl n ( n = 5–8) exhibited the highest concentrations, followed by chlorocarbazoles and tris(chlorophenyl) methanes (TCPMs). Using nontargeted workflows, a variety of known and unknown HOCs were observed, which demonstrate the need to develop more complete chemical profiles in the marine environment.

Environmental Science & Technology

Legacy contaminant-stable isotope-age relationships in Lake Ontario year-class Alewife (Alosa pseudoharengus)

Alewife ( Alosa pseudoharengus ) are the preferred prey species of the top piscivore predators in the Lake Ontario food web and are an essential constituent in the bioaccumulation of persistent organic contaminants. Year-class samples collected in 2016 represent the alewife age ranges of 2015 (Age-01) sequentially dating back to 2008 (Age-08). The most abundant contaminant measured in Lake Ontario alewife (151.5 ng/g) were total polychlorinated biphenyls (PCBs), increasing at a rate of 11.8 ng/g per year on an age-averaged concentration basis. Total mercury demonstrated the largest percent increase (240%) accumulated over alewife ages of 1–8 years. Average total concentrations of the most abundant polychlorinated dibenzo-p-dioxin isomer (2378-tetrachlorinated dibenzo-p-dioxin (TCDD), 1.3 pg/g) and polychlorinated dibenzofuran isomer (2378-tetrachlorinated dibenzofuran (2378-TCDF), 6.6 pg/g) comprised most of the overall total dioxin (2.5 pg/g) and total furan concentrations (8.7 pg/g). The vast majority (69%) of alewife total toxic equivalence (TEQ) was comprised of the non-ortho coplanar PCBs. Both mammal and avian wildlife protection values based on total TEQ were uniformly exceeded for the dioxin-like compounds measured in Lake Ontario alewife. Ontogenetic dietary influences expressed a significant impact on Age-01 alewife age-contaminant relationships and age-stable isotope concentrations and trends for legacy contaminants. Total Hg and all dioxin-like contaminants did not demonstrate the Age-01 ontogenetic dietary effects found in legacy contaminants. A prominent polychlorinated naphthalene (PCN) concentration peak measured in year-class Age-04 alewife was followed by a corresponding lake trout peak 3–4 years later illustrating a unique example of trophic-level contaminant uptake and concomitant integration delay.

New York, Ohio

Factors affecting mercury stable isotopic distribution in piscivorous fish of the Laurentian Great Lakes

Identifying the sources of methylmercury (MeHg) and tracing the transformations of mercury (Hg) in the aquatic food web are important components of effective strategies for managing current and legacy Hg sources. In our previous work, we measured stable isotopes of Hg (δ 202 Hg, Δ 199 Hg, and Δ 200 Hg) in the Laurentian Great Lakes and estimated source contributions of Hg to bottom sediment. Here, we identify isotopically distinct Hg signatures for Great Lakes trout ( Salvelinus namaycush ) and walleye ( Sander vitreus ), driven by both food-web and water-quality characteristics. Fish contain high values for odd-isotope mass independent fractionation (MIF) with averages ranging from 2.50 (western Lake Erie) to 6.18‰ (Lake Superior) in Δ 199 Hg. The large range in odd-MIF reflects variability in the depth of the euphotic zone, where Hg is most likely incorporated into the food web. Even-isotope MIF (Δ 200 Hg), a potential tracer for Hg from precipitation, appears both disconnected from lake sedimentary sources and comparable in fish among the five lakes. We suggest that similar to the open ocean, water-column methylation also occurs in the Great Lakes, possibly transforming recently deposited atmospheric Hg deposition. We conclude that the degree of photochemical processing of Hg is controlled by phytoplankton uptake rather than by dissolved organic carbon quantity among lakes.

Environmental Science & Technology

The estimated six-year mercury dry deposition across North America

Dry deposition of atmospheric mercury (Hg) to various land covers surrounding 24 sites in North America was estimated for the years 2009 to 2014. Depending on location, multiyear mean annual Hg dry deposition was estimated to range from 5.1 to 23.8 μg m –2 yr –1 to forested canopies, 2.6 to 20.8 μg m –2 yr –1 to nonforest vegetated canopies, 2.4 to 11.2 μg m –2 yr –1 to urban and built up land covers, and 1.0 to 3.2 μg m –2 yr –1 to water surfaces. In the rural or remote environment in North America, annual Hg dry deposition to vegetated surfaces is dominated by leaf uptake of gaseous elemental mercury (GEM), contrary to what was commonly assumed in earlier studies which frequently omitted GEM dry deposition as an important process. Dry deposition exceeded wet deposition by a large margin in all of the seasons except in the summer at the majority of the sites. GEM dry deposition over vegetated surfaces will not decrease at the same pace, and sometimes may even increase with decreasing anthropogenic emissions, suggesting that Hg emission reductions should be a long-term policy sustained by global cooperation.

Environmental Science & Technology

Use of stable isotope signatures to determine mercury sources in the Great Lakes

Sources of mercury (Hg) in Great Lakes sediments were assessed with stable Hg isotope ratios using multicollector inductively coupled plasma mass spectrometry. An isotopic mixing model based on mass-dependent (MDF) and mass-independent fractionation (MIF) (&delta; 202 Hg and &Delta; 199 Hg) identified three primary Hg sources for sediments: atmospheric, industrial, and watershed-derived. Results indicate atmospheric sources dominate in Lakes Huron, Superior, and Michigan sediments while watershed-derived and industrial sources dominate in Lakes Erie and Ontario sediments. Anomalous &Delta; 200 Hg signatures, also apparent in sediments, provided independent validation of the model. Comparison of &Delta; 200 Hg signatures in predatory fish from three lakes reveals that bioaccumulated Hg is more isotopically similar to atmospherically derived Hg than a lake&rsquo;s sediment. Previous research suggests &Delta; 200 Hg is conserved during biogeochemical processing and odd mass-independent fractionation (MIF) is conserved during metabolic processing, so it is suspected even is similarly conserved. Given these assumptions, our data suggest that in some cases, atmospherically derived Hg may be a more important source of MeHg to higher trophic levels than legacy sediments in the Great Lakes.

Lake Erie, Lake Huron, Lake Michigan, Lake Ontario