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  • 1
    Publication Date: 2022-05-25
    Description: This paper is not subject to U.S. copyright. The definitive version was published in Marine Chemistry 154 (2013): 55–66, doi:10.1016/j.marchem.2013.05.002.
    Description: Environmental contamination in Castle Harbour, Bermuda, has been linked to the dissolution and leaching of contaminants from the adjacent marine landfill. This study expands the evidence for environmental impact of leachate from the landfill by quantitatively demonstrating elevated metal uptake over the last 30 years in corals growing in Castle Harbour. Coral Pb/Ca, Zn/Ca and Mn/Ca ratios and total Hg concentrations are elevated relative to an adjacent control site in John Smith's Bay. The temporal variability in the Castle Harbour coral records suggests that while the landfill has increased in size over the last 35 years, the dominant input of metals is through periodic leaching of contaminants from the municipal landfill and surrounding sediment. Elevated contaminants in the surrounding sediment suggest that resuspension is an important transport medium for transferring heavy metals to corals. Increased winds, particularly during the 1990s, were accompanied by higher coral metal composition at Castle Harbour. Coupled with wind-induced resuspension, interannual changes in sea level within the Harbour can lead to increased bioavailability of sediment-bound metals and subsequent coral metal assimilation. At John Smith's Bay, large scale convective mixing may be driving interannual metal variability in the coral record rather than impacts from land-based activities. Results from this study provide important insights into the coupling of natural variability and anthropogenic input of contaminants to the nearshore environment.
    Description: This work was supported by a grant from a postdoctoral scholarship to N.G. Prouty from the Woods Hole Oceanographic Institution and grants from the NSF (OCE-0402728; K. Hughen) and the Cove Point Foundation (C. Lamborg).
    Keywords: Bermuda ; Corals ; Landfill ; Trace metals ; Resuspension ; Sediment
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 2
    Publication Date: 2022-05-25
    Description: Author Posting. © The Author(s), 2011. This is the author's version of the work. It is posted here by permission of Elsevier B.V. for personal use, not for redistribution. The definitive version was published in Marine Chemistry 126 (2011): 108-113, doi:10.1016/j.marchem.2011.04.004.
    Description: Photosynthesis by marine phytoplankton requires bioavailable forms of several trace elements that are found in extremely low concentrations in the open ocean. We have compared the concentration, lability and size distribution (〈 1 nm and 〈 10 nm) of a suite of trace elements that are thought to be limiting to primary productivity as well as a toxic element (Pb) in two High Nutrient Low Chlorophyll (HNLC) regions using a new dynamic speciation technique, Diffusive Gradients in Thin-film (DGT). The labile species trapped within the DGT probes have a size that is smaller or similar than the pore size of algal cell walls and thus present a proxy for bioavailable species. Total Dissolvable trace element concentrations (TD concentration) varied between 0.05 nM (Co) and 4.0 nM (Ni) at K2 (Northwest Pacific Ocean) and between 0.026 nM (Co) and 4.7 nM (Ni) in the Southern Ocean. The smallest size fractionated labile concentrations (〈 1 nm) observed at Southern Ocean sampling stations ranged between 0.002 nM (Co) and 2.1 nM (Ni). Moreover, large differences in bioavailable fractions (ratio of labile to TD concentration) were observed between the trace elements. In the Northwest Pacific Ocean Fe, Cu and Mn had lower labile fractions (between 10 and 44%) than Co, Cd, Ni and Pb (between 80 and 100%). In the Southern Ocean a similar trend was observed, and in addition: (1) Co, Cd, Ni and Pb have lower labile fractions in the Southern Ocean than in the Northwest Pacific and (2) the ratios of 〈1nm to dissolvable element concentrations at some Southern Ocean stations were very low and varied between 4 and16 %.
    Description: This research was supported by Federal Science Policy Office, Brussels, through contracts EV/03/7A, SD/CA/03A, the Research Foundation Flanders through grant G.0021.04 and Vrije Universiteit Brussel via grant GOA 22, as well as for K2, the VERTIGO program funding primarily by the US National Science Foundation programs in Chemical and Biological Oceanography
    Keywords: Trace elements ; Speciation ; Bioavailability ; Pacific Ocean ; Southern Ocean
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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  • 3
    Publication Date: 2022-05-25
    Description: Author Posting. © The Author(s), 2012. This is the author's version of the work. It is posted here by permission of Elsevier B.V. for personal use, not for redistribution. The definitive version was published in Atmospheric Environment 59 (2012): 509-513, doi:10.1016/j.atmosenv.2012.05.048.
    Description: In this study we used lake sediments, which faithfully record Hg inputs, to derive estimates of net atmospheric Hg deposition to Svalbard, Norwegian Arctic. With the exception of one site affected by local pollution, the study lakes show twofold to fivefold increases in sedimentary Hg accumulation since 1850, likely due to long-range atmospheric transport and deposition of anthropogenic Hg. Sedimentary Hg accumulation in these lakes is a linear function of the ratio of catchment area to lake area, and we used this relationship to model net atmospheric Hg flux: preindustrial and modern estimates are 2.5±3.3 μg/m2/y and 7.0±3.0 μg/m2/y, respectively. The modern estimate, by comparison with data for Hg wet deposition, indicates that atmospheric mercury depletion events (AMDEs) or other dry deposition processes contribute approximately half (range 0-70%) of the net flux. Hg from AMDEs may be moving in significant quantities into aquatic ecosystems, where it is a concern because of contamination of aquatic food webs.
    Description: Funding was provided by an NSERC Discovery Grant (Drevnick) and the Norges forskningsråd (grant number 107745/730).
    Keywords: Mercury ; Atmospheric deposition ; Arctic ; Svalbard ; Lake sediments
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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  • 4
    Publication Date: 2022-05-25
    Description: © The Author(s), 2012. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Atmospheric Chemistry and Physics 12 (2012): 7341-7350, doi:10.5194/acp-12-7341-2012.
    Description: The distribution of gaseous elemental mercury (GEM) was determined in the surface atmosphere of the northern South China Sea (SCS) during 12 SEATS cruises between May 2003 and December 2005. The sampling and analysis of GEM were performed on board ship by using an on-line mercury analyzer (GEMA). Distinct annual patterns were observed for the GEM with a winter maximum of 5.7 ± 0.2 ng m−3 (n = 3) and minimum in summer (2.8 ± 0.2; n = 3), with concentrations elevated 2–3 times global background values. Source tracking through backward air trajectory analysis demonstrated that during the northeast monsoon (winter), air masses came from Eurasia, bringing continental- and industrial-derived GEM to the SCS. In contrast, during summer southwest monsoon and inter-monsoon, air masses were from the Indochina Peninsula and Indian Ocean and west Pacific Ocean. This demonstrates the impact that long-range transport, as controlled by seasonal monsoons, has on the Hg atmospheric distribution and cycling in the SCS.
    Description: Support was provided by the National Science Council (Taiwan, Republic of China) through grant number NSC 97-2745-M-002-001-;98- 2611-M-002-013- and through a thematic research grant titled “Atmospheric Forcing on Ocean Biogeochemistry (AFOBi)” and from the College of Science (COS#1010023540), National Taiwan University (NTU#101R3252) through a grant of the NTU “Aim for Top University Project” under research platform of the “Drunken-Moon Lake” scientific integration.
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 5
    Publication Date: 2022-05-25
    Description: Author Posting. © American Geophysical Union, 2013. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Geophysical Research Letters 40 (2013): 167–172, doi:10.1029/2012GL054457.
    Description: A unique seasonal pattern in dissolved elemental mercury (DEM) was observed in the tropical monsoon-dominated South China Sea (SCS). The DEM concentration varied seasonally, with a high in summer of 160 ± 40 fM (net evasion 580 ± 120 pmol m−2 d−1, n = 4) and a low in winter of 60 ± 30 fM (net invasion −180 ± 110, n = 4) and showed a positive correlation with sea surface temperature (SST). The elevated DEM concentration in summer appears mainly abiologically driven. In winter, the SCS acts as a sink of atmosphere Hg0 as a result of low SST and high wind of the year, enhanced vertical mixing, and elevated atmospheric gaseous elemental mercury. Annually, the SCS serves as a source of Hg0 to the atmosphere of 300 ± 50 pmol m−2 d−1 (385 ± 64 kmol Hg yr−1, ~2.6% of global emission in ~1% of global ocean area), suggesting high regional Hg pollution impacts from the surrounding Mainland (mostly China).
    Description: Support was provided by the National Science Council through grants NSC 97-2745-M-002- 001-;98(99,100)-2611-M-002-013(014,004) and from the College of Science, National Taiwan University under the “Drunken Moon Lake Scientific Integrated Scientific Research Platform” grant, NTU 101R3252, as well as through the U.S. National Science Foundation under grant OCE-1132515 and 0928191.
    Description: 2013-07-16
    Keywords: Atmospheric Hg cycling ; Air-sea exchange ; Elemental Hg ; Monsoon cycling ; South China Sea ; Southeast Asian Time-series Study (SEATS)
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 6
    Publication Date: 2022-05-25
    Description: Author Posting. © The Oceanography Society, 2014. This article is posted here by permission of The Oceanography Society for personal use, not for redistribution. The definitive version was published in Oceanography 27, no. 1 (2014): 76–87, doi:10.5670/oceanog.2014.11.
    Description: The toxic metal mercury is present only at trace levels in the ocean, but it accumulates in fish at concentrations high enough to pose a threat to human and environmental health. Human activity has dramatically altered the global mercury cycle, resulting in loadings to the ocean that have increased by at least a factor of three from pre-anthropogenic levels. Loadings are likely to continue to increase as a result of higher atmospheric emissions and other factors related to global environmental change. The impact that these loadings will have on the production of methylated mercury (the form that accumulates in fish) is unclear. In this article, we summarize the biogeochemistry of mercury in the ocean and use this information to examine past impacts that human activity has had on the cycling of this toxic metal. We also highlight ways in which the mercury cycle may continue to be affected and its potential impact on mercury in fish.
    Description: The US GEOTRACES research reported herein was supported by the US National Science Foundation Chemical Oceanography program. National Taiwan University also supported this work through the Drunken Moon Lake Scientific Integrated Scientific Research Platform grant, NTU#102R3252.
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 7
    Publication Date: 2022-05-25
    Description: Author Posting. © Association for the Sciences of Limnology and Oceanography, 2014. This article is posted here by permission of Association for the Sciences of Limnology and Oceanography for personal use, not for redistribution. The definitive version was published in Limnology and Oceanography: Methods 12 (2014): 1-9, doi:10.4319/lom.2014.12.1.
    Description: We developed a technique to measure monomethylmercury (MMHg) concentrations from small volumes (180 mL) of seawater at low femtomolar concentrations using direct ethylation derivitization, decreasing the required volume by 90% from current methods while maintaining a 5 fM detection limit. In this method, addition of ascorbic acid before derivitization of MMHg allows for full recovery of MMHg from the seawater matrix without the need for sample distillation or extraction. The small sample size and relative ease of detection are ideal both for shipboard as well as shore-based measurements of preserved MMHg samples. Combined with shipboard determination of dimethylmercury (DMHg) and elemental mercury (Hg(0)), this method can be used to determine full marine mercury speciation.
    Description: This research was supported by a National Science Foundation grant (OCE-1031271) awarded to C. H. L. and Mak Saito and a Graduate Research Fellowship awarded to K. M. M.
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 8
    Publication Date: 2022-05-25
    Description: Author Posting. © Association for the Sciences of Limnology and Oceanography, 2012. This article is posted here by permission of Association for the Sciences of Limnology and Oceanography for personal use, not for redistribution. The definitive version was published in Limnology and Oceanography 57 (2012): 989-1010, doi:10.4319/lo.2012.57.4.0989.
    Description: We present full-depth zonal sections of total dissolved cobalt, iron, manganese, and labile cobalt from the South Atlantic Ocean. A basin-scale plume from the African coast appeared to be a major source of dissolved metals to this region, with high cobalt concentrations in the oxygen minimum zone of the Angola Dome and extending 2500 km into the subtropical gyre. Metal concentrations were elevated along the coastal shelf, likely due to reductive dissolution and resuspension of particulate matter. Linear relationships between cobalt, N2O, and O2, as well as low surface aluminum supported a coastal rather than atmospheric cobalt source. Lateral advection coupled with upwelling, biological uptake, and remineralization delivered these metals to the basin, as evident in two zonal transects with distinct physical processes that exhibited different metal distributions. Scavenging rates within the coastal plume differed for the three metals; iron was removed fastest, manganese removal was 2.5 times slower, and cobalt scavenging could not be discerned from water mass mixing. Because scavenging, biological utilization, and export constantly deplete the oceanic inventories of these three hybrid-type metals, point sources of the scale observed here likely serve as vital drivers of their oceanic cycles. Manganese concentrations were elevated in surface waters across the basin, likely due to coupled redox processes acting to concentrate the dissolved species there. These observations of basin-scale hybrid metal plumes combined with the recent projections of expanding oxygen minimum zones suggest a potential mechanism for effects on ocean primary production and nitrogen fixation via increases in trace metal source inputs.
    Description: This research was supported US National Science Foundation Chemical Oceanography (Division of Ocean Sciences OCE-0452883, OCE-0752291, OCE-0928414, OCE-1031271), the Center for Microbial Research and Education, the Gordon and Betty Moore Foundation, the WHOI Coastal Ocean Institute, and the WHOI Ocean Life Institute.
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 9
    Publication Date: 2017-01-04
    Description: Citation only. Published in Science 316: 567-570, doi: 10.1126/science.1137959
    Description: Funding was obtained primarily through the NSF, Ocean Sciences Programs in Chemical and Biological Oceanography, with additional support from the U.S. Department of Energy, Office of Science, Biological and Environmental Research Program, and other national programs, including the Australian Cooperative Research Centre program and Australian Antarctic Division.
    Keywords: Carbon flux ; Carbon sequestration ; Biological pump
    Repository Name: Woods Hole Open Access Server
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  • 10
    Publication Date: 2022-05-26
    Description: Author Posting. © Association for the Sciences of Limnology and Oceanography, 2012. This article is posted here by permission of Association for the Sciences of Limnology and Oceanography for personal use, not for redistribution. The definitive version was published in Limnology and Oceanography: Methods 10 (2012): 90-100, doi:10.4319/lom.2012.10.90.
    Description: We conducted a laboratory intercomparison of total mercury (Hg) determination in seawater collected during U.S. GEOTRACES Intercalibration cruises in 2008 and 2009 to the NW Atlantic and NE Pacific Oceans. Results indicated substantial disagreement between the participating laboratories, which appeared to be affected most strongly by bottle cleanliness and preservation procedures. In addition, we examined the effectiveness of various collection and sample preparation procedures that may be used on future GEOTRACES cruises. The type of sampling system and filtration medium appeared to make little difference to results. Finally, and in light of results from experiments that considered sample bottle material effect and the development of new methods for CH3Hg+ extraction from seawater, we propose a recommended procedure for determining all four of the major Hg species in seawater (elemental, dimethyl-, monomethyl-, and total Hg).
    Description: This work was supported by the National Science Foundation program in Chemical Oceanography under grants OCE–0825157, –0825108, –0825583 and –0825068.
    Repository Name: Woods Hole Open Access Server
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