The Mercury-Tolerant Microbiota of the Zooplankton Daphnia Aids in Host Survival and Maintains Fecundity under Mercury Stress.

Many aquatic organisms can thrive in polluted environments by having the genetic capability to withstand suboptimal conditions. However, the contributions of microbiomes under these stressful environments are poorly understood. We investigated whether a mercury-tolerant microbiota can extend its phenotype to its host by ameliorating host survival and fecundity under mercury-stress. We isolated microbiota members from various clones of Daphnia magna, screened for the mercury-biotransforming merA gene, and determined their mercury tolerance levels. We then introduced the mercury-tolerant microbiota, Pseudomonas-10, to axenic D. magna and quantified its merA gene expression, mercury reduction capability, and measured its impact on host survival and fecundity. The expression of the merA gene was up-regulated in Pseudomonas-10, both in isolation and in host-association with mercury exposure. Pseudomonas-10 is also capable of significantly reducing mercury concentration in the medium. Notably, mercury-exposed daphnids containing only Pseudomonas-10 exhibited higher survival and fecundity than mercury-exposed daphnids supplemented with parental microbiome. Our study showed that zooplankton, such as Daphnia, naturally harbor microbiome members that are eco-responsive and tolerant to mercury exposure and can aid in host survival and maintain host fecundity in a mercury-contaminated environment. This study further demonstrates that under stressful environmental conditions, the fitness of the host can depend on the genotype and the phenotype of its microbiome

Determination of monomethylmercury from seawater with ascorbic acid-assisted direct ethylation

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.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.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

Dynamic mercury methylation and demethylation in oligotrophic marine water

© The Author(s), 2018. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Biogeosciences 15 (2018): 6451-6460, doi:10.5194/bg-15-6451-2018.Mercury bioaccumulation in open-ocean food webs depends on the net rate of inorganic mercury conversion to monomethylmercury in the water column. We measured significant methylation rates across large gradients in oxygen utilization in the oligotrophic central Pacific Ocean. Overall, methylation rates over 24h incubation periods were comparable to those previously published from Arctic and Mediterranean waters despite differences in productivity between these marine environments. In contrast to previous studies that have attributed Hg methylation to heterotrophic bacteria, we measured higher methylation rates in filtered water compared to unfiltered water. Furthermore, we observed enhanced demethylation of newly produced methylated mercury in incubations of unfiltered water relative to filtered water. The addition of station-specific bulk filtered particulate matter, a source of inorganic mercury substrate and other possibly influential compounds, did not stimulate sustained methylation, although transient enhancement of methylation occurred within 8h of addition. The addition of dissolved inorganic cobalt also produced dramatic, if transient, increases in mercury methylation. Our results suggest important roles for noncellular or extracellular methylation mechanisms and demethylation in determining methylated mercury concentrations in marine oligotrophic waters. Methylation and demethylation occur dynamically in the open-ocean water column, even in regions with low accumulation of methylated mercury.This work was funded by the National Science Foundation in a Chemical Oceanography Program Grant (OCE-1031271) awarded to Carl H. Lamborg and Mak A. Saito and a graduate student fellowship to Kathleen M. Munson

Increase in mercury in Pacific yellowfin tuna

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, one might 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 Hawaii (USA) over the past half century, the authors found that the concentration of mercury in these fish currently is increasing at a rate of at least 3.8% per year. This rate of increase is consistent with a model of anthropogenic forcing on the mercury cycle in the North Pacific Ocean and suggests that fish mercury concentrations are keeping pace with current loading 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. Environ Toxicol Chem 2015;34:931–934. © 2015 SETACPeer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/110840/1/etc2883.pdfhttp://deepblue.lib.umich.edu/bitstream/2027.42/110840/2/etc2883-sup-0001-SuppData-S1.pd

A unique seasonal pattern in dissolved elemental mercury in the South China Sea, a tropical and monsoon-dominated marginal sea

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.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).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 0928191.2013-07-1

An intercomparison of procedures for the determination of total mercury in seawater and recommendations regarding mercury speciation during GEOTRACES cruises

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.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).This work was supported by the National Science Foundation program in Chemical Oceanography under grants OCE–0825157, –0825108, –0825583 and –0825068

Mercury species concentrations and fluxes in the Central Tropical Pacific Ocean

Author Posting. © American Geophysical Union, 2015. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Global Biogeochemical Cycles 29 (2015): 656–676, doi:10.1002/2015GB005120.The formation of the toxic and bioaccumulating monomethylmercury (MMHg) in marine systems is poorly understood, due in part to sparse data from many ocean regions. We present dissolved mercury (Hg) speciation data from 10 stations in the North and South Equatorial Pacific spanning large water mass differences and gradients in oxygen utilization. We also compare the mercury content in suspended particles from six stations and sinking particles from three stations to constrain local Hg sources and sinks. Concentrations of total Hg (THg) and methylated Hg in the surface and intermediate waters of the Equatorial and South Pacific suggest Hg cycling distinct from that of the North Pacific gyre. Maximum concentrations of 180 fM for both MMHg and dimethylmercury (DMHg) are observed in the Equatorial Pacific. South of the equator, concentrations of MMHg and DMHg are less than 100 fM. Sinking fluxes of particulate THg can reasonably explain the shape of dissolved THg profiles, but those of MMHg are too low to account for dissolved MMHg profiles. However, methylated Hg species are lower than predicted from remineralization rates based on North Pacific data, consistent with limitation of methylation in Equatorial and South Pacific waters. Full water column depth profiles were also measured for the first time in these regions. Concentrations of THg are elevated in deep waters of the North Pacific, compared to those in the intermediate and surface waters, and taper off in the South Pacific. Comparisons with previous measurements from nearby regions suggest little enrichment of THg or MMHg over the past 20 years.Financial support for this study was provided by the National Science Foundation in a grant from the Chemical Oceanography Program (OCE-1031271) to C.H. Lamborg and M.A. Saito and a Graduate Student Fellowship to K.M. Munson.2015-11-2

Environmental assessment of metal exposure to corals living in Castle Harbour, Bermuda

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.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.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)

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

© The Author(s), 2017. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Limnology and Oceanography 62 (2017): 1984–2003, doi:10.1002/lno.10547.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.United States National Science Foundation (NSF) Grant Numbers: OCE-1260006, OCE-1031271, OCE-1337780, OCE-1259994; University of Maryland Center for Environmental Science (UMCES); JGI Community Sequencing Project 133

Lignin biomarkers as tracers of mercury sources in lakes water column

This study presents the role of specific terrigenous organic compounds as important vectors of mercury (Hg) transported from watersheds to lakes of the Canadian boreal forest. In order to differentiate the autochthonous from the allochthonous organic matter (OM), lignin derived biomarker signatures [Lambda, S/V, C/V, P/(V ? S), 3,5-Bd/V and (Ad/Al)v] were used. Since lignin is exclusively produced by terrigenous plants, this approach can give a non equivocal picture of the watershed inputs to the lakes. Moreover, it allows a characterization of the source of OM and its state of degradation. The water column of six lakes from the Canadian Shield was sampled monthly between June and September 2005. Lake total dissolved Hg concentrations and Lambda were positively correlated, meaning that Hg and ligneous inputs are linked (dissolved OM r2 = 0.62, p\0.0001; particulate OM r2 = 0.76, p\0.0001). Ratios of P/(V ? S) and 3,5-Bd/V from both dissolved OM and particulate OM of the water column suggest an inverse relationship between the progressive state of pedogenesis and maturation of the OM in soil before entering the lake, and the Hg concentrations in the water column. No relation was found between Hg levels in the lakes and the watershed flora composition—angiosperm versus gymnosperm or woody versus non-woody compounds. This study has significant implications for watershed management of ecosystems since limiting fresh terrestrial OM inputs should reduce Hg inputs to the aquatic systems. This is particularly the case for largescale land-use impacts, such as deforestation, agriculture and urbanization, associated to large quantities of soil OM being transferred to aquatic systems