Lamborg Carl H.

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Lamborg

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Carl H.

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Thorium speciation in seawater

( 2005-07) Santschi, Peter H. ; Murray, James W. ; Baskaran, Mark ; Benitez-Nelson, Claudia R. ; Guo, L. D. ; Hung, C.-C. ; Lamborg, Carl H. ; Moran, S. Bradley ; Passow, Uta ; Roy-Barman, Matthieu

Since the 1960’s, thorium isotopes occupy a special place in the oceanographer’s toolbox as tracers for determining rates and mechanisms of oceanic scavenging, particle dynamics, and carbon fluxes. Due to their unique and constant production rates from soluble parent nuclides of uranium and radium, their disequilibrium can be used to calculate rates and time scales of sinking particles. In addition, by ratio-ing particulate 234Th (as well, in principle, other Thnuclides) to carbon (and other elements), and linking this ratio to the parent-daughter disequilibrium in the water column, it is possible to calculate fluxes of carbon and other elements. Most of these applications are possible with little knowledge of the dissolved chemical properties of thorium, other than its oxidation state (IV) and tendency to strongly sorb to surfaces, i.e., its “particle- or surface-activity”. However, the use of any tracer is hindered by a lack of knowledge of its chemical properties. Recent observations in the variability of carbon to 234Th ratios in different particle types, as well as of associations of Th(IV) with various marine organic biomolecules has led to the need for a review of current knowledge and what future endeavors should be taken to understand the marine chemistry of thorium.
Environmental assessment of metal exposure to corals living in Castle Harbour, Bermuda

(Elsevier B.V., 2013-05-07) Prouty, Nancy G. ; Goodkin, Nathalie F. ; Jones, R. ; Lamborg, Carl H. ; Storlazzi, Curt D. ; Hughen, Konrad A.

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.
Thaumarchaeal ecotype distributions across the equatorial Pacific Ocean and their potential roles in nitrification and sinking flux attenuation

(John Wiley & Sons, 2017-04-05) Santoro, Alyson E. ; Saito, Mak A. ; Goepfert, Tyler J. ; Lamborg, Carl H. ; Dupont, Christopher L. ; DiTullio, Giacomo R.

Thaumarchaea are among the most abundant microbial groups in the ocean, but controls on their abundance and the distribution and metabolic potential of different subpopulations are poorly constrained. Here, two ecotypes of ammonia-oxidizing thaumarchaea were quantified using ammonia monooxygenase (amoA) genes across the equatorial Pacific Ocean. The shallow, or water column “A” (WCA), ecotype was the most abundant ecotype at the depths of maximum nitrification rates, and its abundance correlated with other biogeochemical indicators of remineralization such as NO3 : Si and total Hg. Metagenomes contained thaumarchaeal genes encoding for the catalytic subunit of the urease enzyme (ureC) at all depths, suggesting that members of both WCA and the deep, water column “B” (WCB) ecotypes may contain ureC. Coupled urea hydrolysis-ammonia oxidation rates were similar to ammonia oxidation rates alone, suggesting that urea could be an important source of ammonia for mesopelagic ammonia oxidizers. Potential inducement of metal limitation of both ammonia oxidation and urea hydrolysis was demonstrated via additions of a strong metal chelator. The water column inventory of WCA was correlated with the depth-integrated abundance of WCB, with both likely controlled by the flux of sinking particulate organic matter, providing strong evidence of vertical connectivity between the ecotypes. Further, depth-integrated amoA gene abundance and nitrification rates were correlated with particulate organic nitrogen flux measured by contemporaneously deployed sediment traps. Together, the results refine our understanding of the controls on thaumarchaeal distributions in the ocean, and provide new insights on the relationship between material flux and microbial communities in the mesopelagic.
Mercury contamination and cycling in the coastal zone

(IAMSLIC, 2004) Balcom, Prentiss ; Fitzgerald, William F. ; Hammerschmidt, Chad R. ; Lamborg, Carl H. ; Visscher, Pieter T.
Size-fractionated labile trace elements in the Northwest Pacific and Southern Oceans

( 2011-04-11) Baeyens, W. ; Bowie, Andrew R. ; Buesseler, Ken O. ; Gao, Y. ; Lamborg, Carl H. ; Remenyi, Tomas A. ; Zhang, H.

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 %.
The spatial and temporal variability of Mn speciation in the coastal Northwest Atlantic Ocean

(American Geophysical Union, 2019-12-20) Oldham, Véronique E. ; Lamborg, Carl H. ; Hansel, Colleen M.

Manganese (Mn) is distributed widely throughout the global ocean, where it cycles between three oxidation states that each play important biogeochemical roles. The speciation of Mn in seawater was previously operationally defined on filtration, with soluble Mn presumed to be Mn(II) and solid‐phase Mn as Mn(III/IV) oxides. Recent findings of abundant soluble Mn(III) complexes (Mn(III)‐L) highlights the need to reexamine the redox cycling of Mn, as these complexes can donate or accept electrons. To better understand the complex cycling of Mn in coastal waters, the distribution of Mn species at four Northwest Atlantic sites with different characteristics was examined. Diurnal influences on Mn speciation were investigated within a productive site. At all sites, Mn(III)‐L complexes dominated, particularly in surface waters, and Mn oxides were low in abundance in surface waters but high in bottom waters. Despite intrasite similarities, Mn speciation was highly variable between our stations, emphasizing the diverse processes that impact Mn redox. Diel Mn measurements revealed that the cycling of Mn is also highly variable over time, even on time scales as short as hours. We observed a change of over 100 nM total Mn over 17 hrs and find that speciation changed drastically. These changes could include contributions from biological, light‐mediated, and/or abiotic mechanisms but more likely point to the importance of lateral mixing at coastal sites. This exploration demonstrates the spatial and temporal variability of the Mn redox cycle and indicates that single timepoint vertical profiling is not sufficient when describing the geochemistry of dynamic coastal systems.
Aqueous phase methylation as a potential source of methylmercury in wet deposition

( 2006-10-17) Hammerschmidt, Chad R. ; Lamborg, Carl H. ; Fitzgerald, William F.

The source of monomethylmercury (MMHg) in wet deposition is unknown. Volatilization of gaseous MMHg, evasion and demethylation of dimethylmercury, and methylation of Hg0 have been either proposed or tested unsuccessfully as potential sources. Here, we show that MMHg in precipitation, sampled across a wide geographical range in North America, is related positively to an operationally defined and measured reactive Hg species (HgR), but connected weakly to total Hg. The mean molar ratio of MMHg:HgR measured in continental precipitation (0.025 ± 0.006) is comparable to the MMHg:Hg(II) ratio estimated from first-order rate constants for acetate-mediated Hg methylation and MMHg photolysis (0.025 ± 0.002). This suggests MMHg may be formed in the atmosphere through a reaction between labile Hg(II) complexes and an unknown methylating agent(s), potentially acetate or similar molecules. Availability of Hg(II) appears to limit the reaction, and accordingly, increased atmospheric loadings of Hg could lead to enhanced MMHg in precipitation.
Mercury and monomethylmercury in fluids from Sea Cliff submarine hydrothermal field, Gorda Ridge

(American Geophysical Union, 2006-09-09) Lamborg, Carl H. ; Von Damm, Karen L. ; Fitzgerald, William F. ; Hammerschmidt, Chad R. ; Zierenberg, Robert

Submarine hydrothermal systems are hypothesized to be a potentially important source of monomethylmercury (MMHg) to the ocean, yet the amount of MMHg in vent fluids is unknown. Here, we report total Hg and MMHg concentrations in hydrothermal vent fluids sampled from the Sea Cliff site on the Gorda Ridge. MMHg is the dominant Hg species, and levels of total Hg are enhanced slightly compared to seawater. Hg is enriched in deposits surrounding the site, suggesting near-field deposition from fluid plumes, with rapid MMHg demethylation and scavenging of Hg(II) complexes. Assuming the flux of MMHg from Sea Cliff is representative of global submarine hydrothermal inputs, we estimate a flux of 0.1–0.4 Mmoles y−1, which may be attenuated by scavenging near the vents. However, deep waters are not typically known to be elevated in Hg, and thus we suggest that hydrothermal systems are not significant sources of MMHg to commercial fisheries.
Basin-scale inputs of cobalt, iron, and manganese from the Benguela-Angola front to the South Atlantic Ocean

(Association for the Sciences of Limnology and Oceanography, 2012-07) Noble, Abigail E. ; Lamborg, Carl H. ; Ohnemus, Daniel C. ; Lam, Phoebe J. ; Goepfert, Tyler J. ; Measures, Christopher I. ; Frame, Caitlin H. ; Casciotti, Karen L. ; DiTullio, Giacomo R. ; Jennings, Joe C. ; Saito, Mak A.

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.
VERTIGO project Sediment Trap Fluxes of mass, elements and phytoplankton pigments data from KM0414 and RR_K2 cruises

(Biological and Chemical Oceanography Data Management Office (BCO-DMO). Contact: bco-dmo-data@whoi.edu, 2010-12-01) Lamborg, Carl H. ; Buesseler, Ken O.

The main goal of VERTIGO is the investigation of the mechanisms that control the efficiency of particle transport through the mesopelagic portion of the water column. Question: What controls the efficiency of particle transport between the surface and deep ocean? More specifically, what is the fate of sinking particles leaving the upper ocean and what factors influence remineralization length scales for different sinking particle classes? VERTIGO researchers have set out to test two basic hypotheses regarding remineralization control, namely: 1. particle source characteristics are the dominant control on the efficiency of particle transport; and/or that 2. mid-water processing, either by zooplankton or bacteria, controls transport efficiency. To test their hypotheses, they will conduct process studies in the field focused on particle flux and composition changes in the upper 500-1000m of the ocean. The basic approach is to examine changes in particle composition and flux with depth within a given source region using a combination of approaches, many of which are new to the field. These include neutrally buoyant sediment traps, particle pumps, settling columns and respiration chambers, along with the development of new biological and geochemical tools for an integrated biogeochemical assessment of the biological pump. Three week process study cruises have been planned at two sites - the Hawaii Ocean Time-series site (HOT) and a new moored time-series site in the subarctic NW Pacific (Japanese site K2; 47°N 160°E) - where there are strong contrasts in rates of production, export, particle composition and expected remineralization length scales. Evidence for variability in the flux vs. depth relationship of sinking particles is not in dispute but the controls on particle transport efficiency through the twilight zone remain poorly understood. A lack of reliable flux and particle characterization data within the twilight zone has hampered our ability to make progress in this area, and no single approach is likely to resolve these issues. The proposed study will apply quantitative modeling to determine the net effects of the individual particle processes on the effective transport of carbon and other elements, and to place the shipboard observations in the context of spatial and temporal variations in these processes. For rapid progress in this area, we have organized this effort as a group proposal taking advantage of expertise in the US and international community. The efficiency of particle transport is important for an accurate assessment of the ocean C sink. Globally, the magnitude and efficiency of the biological pump will in part modulate levels of atmospheric CO2. We maintain that to understand present day ocean C sequestration and to evaluate potential strategies for enhancing sequestration, we need to assess possible changes in the efficiency of particle transport due to climate variability or via purposeful manipulations of C uptake, such as via iron fertilization.
Large subglacial source of mercury from the southwestern margin of the Greenland Ice Sheet

(Nature Research, 2021-05-24) Hawkings, Jon ; Linhoff, Benjamin S. ; Wadham, Jemma L. ; Stibal, Marek ; Lamborg, Carl H. ; Carling, Gregory T. ; Lamarche-Gagnon, Guillaume ; Kohler, Tyler J. ; Ward, Rachael ; Hendry, Katharine R. ; Falteisek, Lukáš ; Kellerman, Anne M. ; Cameron, Karen A. ; Hatton, Jade E. ; Tingey, Sarah ; Holt, Amy D. ; Vinšová, Petra ; Hofer, Stefan ; Bulínová, Marie ; Větrovský, Tomáš ; Meire, Lorenz ; Spencer, Robert G. M.

The Greenland Ice Sheet is currently not accounted for in Arctic mercury budgets, despite large and increasing annual runoff to the ocean and the socio-economic concerns of high mercury levels in Arctic organisms. Here we present concentrations of mercury in meltwaters from three glacial catchments on the southwestern margin of the Greenland Ice Sheet and evaluate the export of mercury to downstream fjords based on samples collected during summer ablation seasons. We show that concentrations of dissolved mercury are among the highest recorded in natural waters and mercury yields from these glacial catchments (521–3,300 mmol km−2 year−1) are two orders of magnitude higher than from Arctic rivers (4–20 mmol km−2 year−1). Fluxes of dissolved mercury from the southwestern region of Greenland are estimated to be globally significant (15.4–212 kmol year−1), accounting for about 10% of the estimated global riverine flux, and include export of bioaccumulating methylmercury (0.31–1.97 kmol year−1). High dissolved mercury concentrations (~20 pM inorganic mercury and ~2 pM methylmercury) were found to persist across salinity gradients of fjords. Mean particulate mercury concentrations were among the highest recorded in the literature (~51,000 pM), and dissolved mercury concentrations in runoff exceed reported surface snow and ice values. These results suggest a geological source of mercury at the ice sheet bed. The high concentrations of mercury and its large export to the downstream fjords have important implications for Arctic ecosystems, highlighting an urgent need to better understand mercury dynamics in ice sheet runoff under global warming.
Increased accumulation of sulfur in lake sediments of the high Arctic

( 2010-08-31) Drevnick, Paul E. ; Muir, Derek C. G. ; Lamborg, Carl H. ; Horgan, Martin J. ; Canfield, Donald E. ; Boyle, John F. ; Rose, Neil L.

We report a synchronous increase in accumulation of reduced inorganic sulfur since c. 1980 in sediment cores from eight of nine lakes studied in the Canadian Arctic and Svalbard (Norway). Sediment incubations and detailed analyses of sediment profiles from two of the lakes indicate that increases in sulfur accumulation may be due ultimately to a changing climate. Warming-induced lengthening of the ice-free season is resulting in well-documented increases in algal production and sedimentation of the resulting detrital matter. Algal detritus is a rich source of labile carbon, which in these sediments stimulates dissimilatory sulfate reduction. The sulfide produced is stored in sediment (as acid volatile sulfide), converted to other forms of sulfur, or reoxidized to sulfate and lost to the water column. An acceleration of the sulfur cycle in Arctic lakes could have profound effects on important biogeochemical processes, such as carbon burial and mercury methylation.
Dark reduction drives evasion of mercury from the ocean

(Frontiers Media, 2021-04-27) Lamborg, Carl H. ; Hansel, Colleen M. ; Bowman, Katlin ; Voelker, Bettina M. ; Marsico, Ryan M. ; Oldham, Véronique E. ; Swarr, Gretchen J. ; Zhang, Tong ; Ganguli, Priya M.

Much of the surface water of the ocean is supersaturated in elemental mercury (Hg0) with respect to the atmosphere, leading to sea-to-air transfer or evasion. This flux is large, and nearly balances inputs from the atmosphere, rivers and hydrothermal vents. While the photochemical production of Hg0 from ionic and methylated mercury is reasonably well-studied and can produce Hg0 at fairly high rates, there is also abundant Hg0 in aphotic waters, indicating that other important formation pathways exist. Here, we present results of gross reduction rate measurements, depth profiles and diel cycling studies to argue that dark reduction of Hg2+ is also capable of sustaining Hg0 concentrations in the open ocean mixed layer. In locations where vertical mixing is deep enough relative to the vertical penetration of UV-B and photosynthetically active radiation (the principal forms of light involved in abiotic and biotic Hg photoreduction), dark reduction will contribute the majority of Hg0 produced in the surface ocean mixed layer. Our measurements and modeling suggest that these conditions are met nearly everywhere except at high latitudes during local summer. Furthermore, the residence time of Hg0 in the mixed layer with respect to evasion is longer than that of redox, a situation that allows dark reduction-oxidation to effectively set the steady-state ratio of Hg0 to Hg2+ in surface waters. The nature of these dark redox reactions in the ocean was not resolved by this study, but our experiments suggest a likely mechanism or mechanisms involving enzymes and/or important redox agents such as reactive oxygen species and manganese (III).
A unique seasonal pattern in dissolved elemental mercury in the South China Sea, a tropical and monsoon-dominated marginal sea

(John Wiley & Sons, 2013-01-16) Tseng, Chun-Mao ; Lamborg, Carl H. ; Hsu, Shih-Chieh

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).
Correction to “Mercury and monomethylmercury in fluids from Sea Cliff submarine hydrothermal field, Gorda Ridge”

(American Geophysical Union, 2007-01-18) Lamborg, Carl H. ; Von Damm, Karen L. ; Fitzgerald, William F. ; Hammerschmidt, Chad R. ; Zierenberg, Robert
Increase in mercury in Pacific yellowfin tuna

( 2015-01) Drevnick, Paul E. ; Lamborg, Carl H. ; Horgan, Martin J.

Mercury is a toxic trace metal that can accumulate to levels that threaten human and environmental health. Models and empirical data suggest that humans are responsible for a great deal of the mercury actively cycling in the environment at present. Thus, we would predict that the concentration of mercury in fish should have increased dramatically since the Industrial Revolution. Evidence in support of this hypothesis has been hard to find, however, and some studies have suggested that analyses of fish show no change in mercury concentration. By compiling and re-analyzing published reports on yellowfin tuna (Thunnus albacares) caught near Hawai’i over the past half century, we find that the concentration of mercury in these fish is currently increasing at a rate ≥ 3.8 % per year. This rate of increase is consistent with a model of anthropogenic forcing on the mercury cycle in the North Pacific, and suggests fish mercury concentrations are keeping pace with current loadings increases to the ocean. Future increases in mercury in yellowfin tuna and other fishes can be avoided by reductions in atmospheric mercury emissions from point sources.
An intercomparison of procedures for the determination of total mercury in seawater and recommendations regarding mercury speciation during GEOTRACES cruises

(Association for the Sciences of Limnology and Oceanography, 2012-02) Lamborg, Carl H. ; Hammerschmidt, Chad R. ; Gill, Gary A. ; Mason, Robert P. ; Gichuki, Susan

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).
Net atmospheric mercury deposition to Svalbard : estimates from lacustrine sediments

( 2012-05) Drevnick, Paul E. ; Yang, Handong ; Lamborg, Carl H. ; Rose, Neil L.

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.
Microbial- and thiosulfate-mediated dissolution of mercury sulfide minerals and transformation to gaseous mercury

(Frontiers Media, 2015-06-23) Vazquez-Rodriguez, Adiari I. ; Hansel, Colleen M. ; Zhang, Tong ; Lamborg, Carl H. ; Santelli, Cara M. ; Webb, Samuel M. ; Brooks, Scott C.

Mercury (Hg) is a toxic heavy metal that poses significant environmental and human health risks. Soils and sediments, where Hg can exist as the Hg sulfide mineral metacinnabar (β-HgS), represent major Hg reservoirs in aquatic environments. Metacinnabar has historically been considered a sink for Hg in all but severely acidic environments, and thus disregarded as a potential source of Hg back to aqueous or gaseous pools. Here, we conducted a combination of field and laboratory incubations to identify the potential for metacinnabar as a source of dissolved Hg within near neutral pH environments and the underpinning (a)biotic mechanisms at play. We show that the abundant and widespread sulfur-oxidizing bacteria of the genus Thiobacillus extensively colonized metacinnabar chips incubated within aerobic, near neutral pH creek sediments. Laboratory incubations of axenic Thiobacillus thioparus cultures led to the release of metacinnabar-hosted Hg(II) and subsequent volatilization to Hg(0). This dissolution and volatilization was greatly enhanced in the presence of thiosulfate, which served a dual role by enhancing HgS dissolution through Hg complexation and providing an additional metabolic substrate for Thiobacillus. These findings reveal a new coupled abiotic-biotic pathway for the transformation of metacinnabar-bound Hg(II) to Hg(0), while expanding the sulfide substrates available for neutrophilic chemosynthetic bacteria to Hg-laden sulfides. They also point to mineral-hosted Hg as an underappreciated source of gaseous elemental Hg to the environment.
Determination of monomethylmercury from seawater with ascorbic acid-assisted direct ethylation

(Association for the Sciences of Limnology and Oceanography, 2014-01) Munson, Kathleen M. ; Babi, Diana ; Lamborg, Carl H.

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.

Lamborg Carl H.

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