Marine Chemistry and Geochemistry (MC&G)
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Research in MC&G ranges from the glacial history of the Antarctic ice sheet and the formation of surface films in the upper micron of the ocean to the cycling of carbon through various ocean reservoirs, the history of ocean circulation recorded in the growth bands of coral, and the role of hydrothermal vents and seawater-rock interactions on the composition of the oceans.
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ArticleThe 129-iodine content of subtropical Pacific waters : impact of Fukushima and other anthropogenic 129-iodine sources(Copernicus Publications on behalf of the European Geosciences Union, 2014-09-11) Guilderson, Thomas P. ; Tumey, S. J. ; Brown, T. A. ; Buesseler, Ken O.Results obtained from a dedicated radiochemistry cruise approximately 100 days after the 11 March 2011 Tohoku earthquake and subsequent disaster at the Fukushima Daiichi Nuclear Power Plant show that Fukushima derived radionuclides in the nearby ocean environment had penetrated, on average, to ≤250 m depth (1026.5 kg m3 potential density surface). The excess inventory of Fukushima-derived 129I in the region (∼150 000 km2) sampled during the cruise is estimated to have been between 0.89 and 1.173 billion Bq (∼136 to ∼179 grams) of 129I. Based on a tight tracer–tracer relation with 134Cs (or 137Cs) and estimates that most of the excess cesium is due to direct discharge, we infer that much of the excess 129I is from direct (non-atmospheric deposition) discharge. After taking into account oceanic transport, we estimate the direct discharge, i.e., that directly released into the ocean, off Fukushima to have been ∼1 kg 129I. Although this small pulse is dwarfed by the ~90 kg of weapons-testing-derived 129I that was released into the environment in the late 1950s and early 1960s, it should be possible to use Fukushima-derived 129I and other radionuclides (e.g., 134, 137Cs) to study transport and entrainment processes along and across the Kuroshio Current.
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Preprint14C and 13C characteristics of higher plant biomarkers in Washington margin surface sediments( 2012-11-22) Feng, Xiaojuan ; Benitez-Nelson, Bryan C. ; Montlucon, Daniel B. ; Prahl, Fredrick G. ; McNichol, Ann P. ; Xu, Li ; Repeta, Daniel J. ; Eglinton, Timothy I.Plant wax lipids and lignin phenols are the two most common classes of molecular markers that are used to trace vascular plant-derived OM in the marine environment. However, their 13C and 14C compositions have not been directly compared, which can be used to constrain the flux and attenuation of terrestrial carbon in marine environment. In this study, we describe a revised method of isolating individual lignin phenols from complex sedimentary matrices for 14C analysis using high pressure liquid chromatography (HPLC) and compare this approach to a method utilizing preparative capillary gas chromatography (PCGC). We then examine in detail the 13C and 14C compositions of plant wax lipids and lignin phenols in sediments from the inner and mid shelf of the Washington margin that are influenced by discharge of the Columbia River. Plant wax lipids (including n-alkanes, n-alkanoic (fatty) acids, n-alkanols, and n-aldehydes) displayed significant variability in both δ13C (-28.3 to -37.5 ‰) and ∆14C values (-204 to +2 ‰), suggesting varied inputs and/or continental storage and transport histories. In contrast, lignin phenols exhibited similar δ13C values (between -30 to -34 ‰) and a relatively narrow range of ∆14C values (-45 to -150 ‰; HPLC-based mesurement) that were similar to, or younger than, bulk OM (-195 to -137 ‰). Moreover, lignin phenol 14C age correlated with the degradation characteristics of this terrestrial biopolymer in that vanillyl phenols were on average ~500 years older than syringyl and cinnamyl phenols that degrade faster in soils and sediments. The isotopic characteristics, abundance, and distribution of lignin phenols in sediments suggest that they serve as promising tracers of recently biosynthesized terrestrial OM during supply to, and dispersal within the marine environment. Lignin phenol 14C measurements may also provide useful constraints on the vascular plant end member in isotopic mixing models for carbon source apportionment, and for interpretation of sedimentary records of past vegetation dynamics. Key words: 14C and 13C composition, radiocarbon age, plant wax lipids, lignin phenols, Washington margin, marine carbon cycling, terrestrial organic matter
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Article210Po and 210Pb distributions during a phytoplankton bloom in the North Atlantic: Implications for POC export(Elsevier, 2020-07-07) Horowitz, Evan J. ; Cochran, J. Kirk ; Bacon, Michael P. ; Hirschberg, David J.During the North Atlantic Bloom Experiment (NABE) of the Joint Global Ocean Flux Study (JGOFS), water column sampling for particulate and dissolved 210Po and 210Pb was performed four times (26 April and 4, 20, 30 May 1989) during a month-long Lagrangian time-series occupation of the NABE site, as well as one-time samplings at stations during transit to and from the site. There are few prior studies documenting short-term changes in 210Po and 210Pb profiles over the course of a phytoplankton bloom, and we interpret the profiles in terms of the classical “steady-state” (SS) approach used in most studies, as well as by using a non-steady state approach suggested by the temporal evolution of the profiles. Changes in 210Po profiles during a bloom are expectable as this radionuclide is scavenged and exported. During NABE, 210Pb profiles also displayed non-steady state, with significant increases in upper water column inventory occurring midway through the experiment. Export of 210Po from the upper 150 m using the classic “steady-state” model shows increases from 0.5 ± 8.5 dpm m−2 d−1 to 68.2 ± 4.2 dpm m−2 d−1 over the ~one-month occupation. Application of a non-steady state model, including changes in both 210Pb and 210Po profiles, gives higher 210Po export fluxes. Detailed depth profiles of particulate organic carbon (>0.8 μm) and particulate 210Po (>0.4 μm) are available from the 20 and 30 May samplings and show maxima in POC/Po at ~37 m. Applying the POC/210Po ratios at 150 m to the “steady state” 210Po fluxes yields POC export from the upper 150 m of 8.2 ± 1.5 mmol C m− 2 d−1 on 20 May and 6.0 ± 1.6 mmol C m−2 d−1 on 30 May. The non-steady state model applied to the interval 20 to 30 May yields POC export of 24.3 mmol C m−2 d−1. The non-steady state (NSS) 210Po-derived POC fluxes are comparable to, but somewhat less than, those estimated previously from 234Th/238U disequilibrium for the same time interval (37.3 and 45.0 mmol m−2 d−1, depending on the POC/Th ratio used). In comparison, POC fluxes measured with a floating sediment trap deployed at 150 m from 20 to 30 May were 11.6 mmol m−2 d−1. These results suggest that non-steady state Po-derived POC fluxes during the NABE agree well with those derived from 234Th/238U disequilibrium and agree with sediment trap fluxes within a factor of ~2. However, unlike the 234Th-POC flux proxy, non-steady stage changes in profiles of 210Pb, the precursor of 210Po, must be considered.
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Preprint217 000-year-old DNA sequences of green sulfur bacteria in Mediterranean sapropels and their implications for the reconstruction of the paleoenvironment( 2006-08-08) Coolen, Marco J. L. ; Overmann, JorgDeep-sea sediments of the eastern Mediterranean harbor a series of dark, organic carbon-rich layers, so-called sapropels. Within these layers, the carotenoid isorenieratene was detected. Since it is specific for the obligately anaerobic phototrophic green sulfur bacteria, the presence of isorenieratene may suggest that extended water column anoxia occurred in the ancient Mediterranean Sea during periods of sapropel formation. Only three carotenoids (isorenieratene, β-isorenieratene and chlorobactene) are typical for green sulfur bacteria and thus do not permit to differentiate between the ~80 known phylotypes. In order to reconstruct the paleoecological conditions in more detail, we searched for fossil 16S rRNA gene sequences of green sulfur bacteria employing ancient DNA methodology. 540 bp-long fossil sequences could indeed be amplified from up to 217,000-year-old sapropels. In addition, such sequences were also recovered from carbon-lean intermediate sediment layers deposited during times of an entirely oxic water column. Unexpectedly, however, all the recovered 16S rRNA gene sequences grouped with freshwater or brackish, rather than truly marine, types of green sulfur bacteria. It is therefore feasible that the molecular remains of green sulfur bacteria originated from populations which thrived in adjacent freshwater or estuarine coastal environments rather than from an indigenous pelagic population.
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Article238U-Th-230-Ra-226-Pb-210-Po-210, Th-232-Ra-228, and U-235-Pa-231 constraints on the ages and petrogenesis of Vailulu'u and Malumalu Lavas, Samoa(American Geophysical Union, 2008-04-01) Sims, Kenneth W. W. ; Hart, Stanley R. ; Reagan, Mark K. ; Blusztajn, Jerzy S. ; Staudigel, Hubert ; Sohn, Robert A. ; Layne, Graham D. ; Ball, Lary A. ; Andrews, J. E.We report 238U-230Th-226Ra-210Pb-210Po, 232Th-228Ra and 235U-231Pa measurements for a suite of 14 geologically and geochemically well-characterized basaltic samples from the Samoan volcanoes Vailulu'u, Malumalu, and Savai'i. Maximum eruption ages based on the presence of parent-daughter disequilibria indicate that Vailulu'u is magmatically productive with young lavas (<8 Ka) resurfacing both its summit crater and lower flanks. 210Pb and 210Po measurements indicate that several flows have erupted within its summit crater in the past 100 years, with the newest observed flow being erupted in November of 2004. For lavas which have eruption ages that are demonstrably young, relative to the half-lives of 230Th, 231Pa, and 226Ra, we interpret their 238U -230Th, 235U-231Pa and 230Th - 226Ra disequilibria in terms of the magmatic processes occurring beneath the Samoan Islands. (230Th/238U) > 1 indicates that garnet is required as a residual phase in the magma sources for all these lavas. The large range of (238U/232Th) and (230Th/232Th) is attributed to long-term source variation. The Samoan basalts are all alkaline basalts and show significant 230Th and 231Pa excesses but limited variability, indicating that they have been derived by small but similar extents of melting. Their (230Th/238U), (231Pa/235U) and Sm/Nd fractionation are consistent with correlations among other ocean island basalt suites (particularly Hawaii) which show that (230Th/238U) and (231Pa/235U) of many OIBS can be explained by simple time-independent models. Interpretation of the 226Ra data requires time-dependent melting models. Both chromatographic porous flow and dynamic melting of a garnet peridotite source can adequately explain the combined U-Th-Ra and U-Pa data for these Samoan basalts. Several young samples from the Vailulu'u summit crater also exhibit significant 210Pb deficits that reflect either shallow magmatic processes or continuous magma degassing. In both cases, decadal residence times are inferred from these 210Pb deficits. The young coeval volcanism on Malumalu and Vailulu'u suggests the Samoa hot spot is currently migrating to the northeast due to dynamic interaction with the Tonga slab.
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ArticleThe 3He flux gauge in the Sargasso Sea : a determination of physical nutrient fluxes to the euphotic zone at the Bermuda Atlantic Time-series Site(Copernicus Publications on behalf of the European Geosciences Union, 2015-09-04) Stanley, Rachel H. R. ; Jenkins, William J. ; Doney, Scott C. ; Lott, Dempsey E.Significant rates of primary production occur in the oligotrophic ocean, without any measurable nutrients present in the mixed layer, fueling a scientific paradox that has lasted for decades. Here, we provide a new determination of the annual mean physical supply of nitrate to the euphotic zone in the western subtropical North Atlantic. We combine a 3-year time series of measurements of tritiugenic 3He from 2003 to 2006 in the surface ocean at the Bermuda Atlantic Time-series Study (BATS) site with a sophisticated noble gas calibrated air–sea gas exchange model to constrain the 3He flux across the sea–air interface, which must closely mirror the upward 3He flux into the euphotic zone. The product of the 3He flux and the observed subsurface nitrate–3He relationship provides an estimate of the minimum rate of new production in the BATS region. We also apply the gas model to an earlier time series of 3He measurements at BATS in order to recalculate new production fluxes for the 1985 to 1988 time period. The observations, despite an almost 3-fold difference in the nitrate–3He relationship, yield a roughly consistent estimate of nitrate flux. In particular, the nitrate flux from 2003 to 2006 is estimated to be 0.65 ± 0.14 mol m−2 yr−1, which is ~40 % smaller than the calculated flux for the period from 1985 to 1988. The difference in nitrate flux between the time periods may be signifying a real difference in new production resulting from changes in subtropical mode water formation. Overall, the nitrate flux is larger than most estimates of export fluxes or net community production fluxes made locally for the BATS site, which is likely a reflection of the larger spatial scale covered by the 3He technique and potentially also by the decoupling of 3He and nitrate during the obduction of water masses from the main thermocline into the upper ocean. The upward nitrate flux is certainly large enough to support observed rates of primary production at BATS and more generally in the oligotrophic subtropical ocean.
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ArticleA global ocean dissolved organic phosphorus concentration database (DOPv2021)(Nature Research, 2022-12-16) Liang, Zhou ; McCabe, Kelly ; Fawcett, Sarah E. ; Forrer, Heather J. ; Hashihama, Fuminori ; Jeandel, Catherine ; Marconi, Dario ; Planquette, Hélène ; Saito, Mak A. ; Sohm, Jill A. ; Thomas, Rachel K. ; Letscher, Robert T. ; Knapp, Angela N.Dissolved organic phosphorus (DOP) concentration distributions in the global surface ocean inform our understanding of marine biogeochemical processes such as nitrogen fixation and primary production. The spatial distribution of DOP concentrations in the surface ocean reflect production by primary producers and consumption as an organic nutrient by phytoplankton including diazotrophs and other microbes, as well as other loss processes such as photolysis. Compared to dissolved organic carbon and nitrogen, however, relatively few marine DOP concentration measurements have been made, largely due to the lack of automated analysis techniques. Here we present a database of marine DOP concentration measurements (DOPv2021) that includes new (n = 730) and previously published (n = 3140) observations made over the last ~30 years (1990-2021), including 1751 observations in the upper 50 m. This dataset encompasses observations from all major ocean basins including the poorly represented Indian, South Pacific, and Southern Oceans and provides insight into spatial distributions of DOP in the ocean. It is also valuable for researchers who work on marine primary production and nitrogen fixation.
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ArticleA meta-analysis of the stony coral tissue loss disease microbiome finds key bacteria in unaffected and lesion tissue in diseased colonies(Springer, 2023-03-09) Rosales, Stephanie M. ; Huebner, Lindsay K. ; Evans, James S. ; Apprill, Amy ; Baker, Andrew C. ; Becker, Cynthia C. ; Bellantuono, Anthony J. ; Brandt, Marilyn E. ; Clark, Abigail S. ; del Campo, Javier ; Dennison, Caroline E. ; Eaton, Katherine R. ; Huntley, Naomi E. ; Kellogg, Christina A. ; Medina, Mónica ; Meyer, Julie L. ; Muller, Erinn M. ; Rodriguez-Lanetty, Mauricio ; Salerno, Jennifer L. ; Schill, William B. ; Shilling, Erin N. ; Stewart, Julia Marie ; Voss, Joshua D.Stony coral tissue loss disease (SCTLD) has been causing significant whole colony mortality on reefs in Florida and the Caribbean. The cause of SCTLD remains unknown, with the limited concurrence of SCTLD-associated bacteria among studies. We conducted a meta-analysis of 16S ribosomal RNA gene datasets generated by 16 field and laboratory SCTLD studies to find consistent bacteria associated with SCTLD across disease zones (vulnerable, endemic, and epidemic), coral species, coral compartments (mucus, tissue, and skeleton), and colony health states (apparently healthy colony tissue (AH), and unaffected (DU) and lesion (DL) tissue from diseased colonies). We also evaluated bacteria in seawater and sediment, which may be sources of SCTLD transmission. Although AH colonies in endemic and epidemic zones harbor bacteria associated with SCTLD lesions, and aquaria and field samples had distinct microbial compositions, there were still clear differences in the microbial composition among AH, DU, and DL in the combined dataset. Alpha-diversity between AH and DL was not different; however, DU showed increased alpha-diversity compared to AH, indicating that, prior to lesion formation, corals may undergo a disturbance to the microbiome. This disturbance may be driven by Flavobacteriales, which were especially enriched in DU. In DL, Rhodobacterales and Peptostreptococcales–Tissierellales were prominent in structuring microbial interactions. We also predict an enrichment of an alpha-toxin in DL samples which is typically found in Clostridia. We provide a consensus of SCTLD-associated bacteria prior to and during lesion formation and identify how these taxa vary across studies, coral species, coral compartments, seawater, and sediment.
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ArticleA North Pacific meridional section (U.S. GEOTRACES GP15) of helium isotopes and noble gases I: deep water distributions(American Geophysical Union, 2023-04-18) Jenkins, William J. ; Doney, Scott C. ; Seltzer, Alan M. ; German, Christopher R. ; Lott, Dempsey E. ; Cahill, Kevin L.The noble gas signature of incoming Pacific Bottom Water (PBW), when compared to North Atlantic Deep Water, indicates the addition of 450 ± 70 GT a−1 glacial melt water to form AABW and subsequently PBW. The downstream evolution of this signature between the southern (20°S to equator) and northern (25°–45°N) bottom waters indicates a decrease in sea level pressure around Antarctica over the past two millennia. Vertical profiles of noble gases in the deep Pacific show exponential relationships with depth with scale heights identical to temperature and salinity. Unlike the other noble gases, helium isotopes show evidence of mid‐depth injection of non‐atmospheric helium. Using observed deviations from exponential behavior, we quantify its magnitude and isotope ratio. There is a clear latitude trend in the isotope ratio of this added helium that decreases from a high exceeding 9 RA (atmospheric 3He/4He ratio) in the south to around 8 RA near the equator. North of 30–40°N, it systematically decreases northward to a low of ∼2 RA north of 50°N. This decline results from a combination of northward decline in seafloor spreading, release of radiogenic helium from increased sediment thickness, and the possible emission of radiogenic helium through cold seeps along the Alaskan and North American margins. Finally, we derive an improved method of computing the excess helium isotope concentrations and that the distributions of bottom water 3HeXS/4HeXS are consistent with what is known about bottom water flow patterns and the input of low 3He/4He sedimentary helium.
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ArticleA response to community questions on the marine20 radiocarbon age calibration curve: marine reservior ages and the calibration of 14 C samples from the oceans(Cambridge University Press, 2022-11-02) Heaton, Timothy J. ; Bard, Edouard ; Bronk Ramsey, Christopher ; Butzin, Martin ; Hatté, Christine ; Hughen, Konrad A. ; Köhler, Peter ; Reimer, Paula J.Radiocarbon (14C) concentrations in the oceans are different from those in the atmosphere. Understanding these ocean-atmospheric 14C differences is important both to estimate the calendar ages of samples which obtained their 14C in the marine environment, and to investigate the carbon cycle. The Marine20 radiocarbon age calibration curve is created to address these dual aims by providing a global-scale surface ocean record of radiocarbon from 55,000–0 cal yr BP that accounts for the smoothed response of the ocean to variations in atmospheric 14C production rates and factors out the effect of known changes in global-scale palaeoclimatic variables. The curve also serves as a baseline to study regional oceanic 14C variation. Marine20 offers substantial improvements over the previous Marine13 curve. In response to community questions, we provide a short intuitive guide, intended for the lay-reader, on the construction and use of the Marine20 calibration curve. We describe the choices behind the making of Marine20, as well as the similarities and differences compared with the earlier Marine calibration curves. We also describe how to use the Marine20 curve for calibration and how to estimate ΔR—the localized variation in the oceanic 14C levels due to regional factors which are not incorporated in the global-scale Marine20 curve. To aid understanding, illustrative worked examples are provided.
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ArticleA synthesis of monsoon exploration in the Asian marginal seas(Copernicus Publications, 2022-10-28) Clift, Peter D ; Betzler, Christian ; Clemens, Steven C ; Christensen, Beth ; Eberli, Gregor P ; France-Lanord, Christian ; Gallagher, Stephen J. ; Holbourn, Ann ; Kuhnt, Wolfgang ; Murray, Richard W ; Rosenthal, Yair ; Tada, Ryuji ; Wan, ShimingThe International Ocean Discovery Program (IODP) conducted a series of expeditions between 2013 and 2016 that were designed to address the development of monsoon climate systems in Asia and Australia. Significant progress was made in recovering Neogene sections spanning the region from the Arabian Sea to the Sea of Japan and southward to western Australia. High recovery by advanced piston corer (APC) has provided a host of semi-continuous sections that have been used to examine monsoonal evolution. Use of the half-length APC was successful in sampling sand-rich sediment in Indian Ocean submarine fans. The records show that humidity and seasonality developed diachronously across the region, although most regions show drying since the middle Miocene and especially since ∼ 4 Ma, likely linked to global cooling. A transition from C3 to C4 vegetation often accompanied the drying but may be more linked to global cooling. Western Australia and possibly southern China diverge from the general trend in becoming wetter during the late Miocene, with the Australian monsoon being more affected by the Indonesian Throughflow, while the Asian monsoon is tied more to the rising Himalaya in South Asia and to the Tibetan Plateau in East Asia. The monsoon shows sensitivity to orbital forcing, with many regions having a weaker summer monsoon during times of northern hemispheric Glaciation. Stronger monsoons are associated with faster continental erosion but not weathering intensity, which either shows no trend or a decreasing strength since the middle Miocene in Asia. Marine productivity proxies and terrestrial chemical weathering, erosion, and vegetation proxiesare often seen to diverge. Future work on the almost unknown Paleogene is needed, as well as the potential of carbonate platforms as archives of paleoceanographic conditions.
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ArticleAbiotic methane synthesis and serpentinization in olivine-hosted fluid inclusions(National Academy of Sciences, 2019-09-03) Klein, Frieder ; Grozeva, Niya G. ; Seewald, Jeffrey S.The conditions of methane (CH4) formation in olivine-hosted secondary fluid inclusions and their prevalence in peridotite and gabbroic rocks from a wide range of geological settings were assessed using confocal Raman spectroscopy, optical and scanning electron microscopy, electron microprobe analysis, and thermodynamic modeling. Detailed examination of 160 samples from ultraslow- to fast-spreading midocean ridges, subduction zones, and ophiolites revealed that hydrogen (H2) and CH4 formation linked to serpentinization within olivine-hosted secondary fluid inclusions is a widespread process. Fluid inclusion contents are dominated by serpentine, brucite, and magnetite, as well as CH4(g) and H2(g) in varying proportions, consistent with serpentinization under strongly reducing, closed-system conditions. Thermodynamic constraints indicate that aqueous fluids entering the upper mantle or lower oceanic crust are trapped in olivine as secondary fluid inclusions at temperatures higher than ∼400 °C. When temperatures decrease below ∼340 °C, serpentinization of olivine lining the walls of the fluid inclusions leads to a near-quantitative consumption of trapped liquid H2O. The generation of molecular H2 through precipitation of Fe(III)-rich daughter minerals results in conditions that are conducive to the reduction of inorganic carbon and the formation of CH4. Once formed, CH4(g) and H2(g) can be stored over geological timescales until extracted by dissolution or fracturing of the olivine host. Fluid inclusions represent a widespread and significant source of abiotic CH4 and H2 in submarine and subaerial vent systems on Earth, and possibly elsewhere in the solar system.
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ArticleAbiotic redox reactions in hydrothermal mixing zones: decreased energy availability for the subsurface biosphere(National Academy of Sciences, 2020-08-12) McDermott, Jill M. ; Sylva, Sean P. ; Ono, Shuhei ; German, Christopher R. ; Seewald, Jeffrey S.Subseafloor mixing of high-temperature hot-spring fluids with cold seawater creates intermediate-temperature diffuse fluids that are replete with potential chemical energy. This energy can be harnessed by a chemosynthetic biosphere that permeates hydrothermal regions on Earth. Shifts in the abundance of redox-reactive species in diffuse fluids are often interpreted to reflect the direct influence of subseafloor microbial activity on fluid geochemical budgets. Here, we examine hydrothermal fluids venting at 44 to 149 °C at the Piccard hydrothermal field that span the canonical 122 °C limit to life, and thus provide a rare opportunity to study the transition between habitable and uninhabitable environments. In contrast with previous studies, we show that hydrocarbons are contributed by biomass pyrolysis, while abiotic sulfate (SO42−) reduction produces large depletions in H2. The latter process consumes energy that could otherwise support key metabolic strategies employed by the subseafloor biosphere. Available Gibbs free energy is reduced by 71 to 86% across the habitable temperature range for both hydrogenotrophic SO42− reduction to hydrogen sulfide (H2S) and carbon dioxide (CO2) reduction to methane (CH4). The abiotic H2 sink we identify has implications for the productivity of subseafloor microbial ecosystems and is an important process to consider within models of H2 production and consumption in young oceanic crust.
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PreprintAbundance and diversity of archaeal ammonia oxidizers in a coastal groundwater system( 2010-10-12) Rogers, Daniel R. ; Casciotti, Karen L.Nitrification, the microbially-catalyzed oxidation of ammonia to nitrate, is a key process in the nitrogen cycle. Archaea have been implicated in the first part of the nitrification pathway (oxidation of ammonia to nitrite), but the ecology and physiology of these organisms remain largely unknown. This work describes two different populations of sediment-associated ammonia-oxidizing archaea (AOA) in a coastal groundwater system on Cape Cod, Massachusetts. Sequence analysis of the ammonia monooxygenase subunit A gene (amoA) shows that one population of putative AOA inhabits the upper meter of the sediment where they may experience frequent ventilation with tidally-driven overtopping and infiltration of bay water supplying dissolved oxygen, ammonium and perhaps organic carbon. A genetically distinct population occurs deeper in the sediment, in a mixing zone between a nitrate- and oxygen-rich freshwater zone and a reduced, ammonium-bearing salt water wedge. Both of these AOA populations are coincident with increases in the abundance of Group I crenarchaeota 16S rRNA gene copies.
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ArticleAccelerating global ocean observing: monitoring the coastal ocean through broadly accessible, low-cost sensor networks(Marine Technology Society, 2021-05-01) Wang, Zhaohui Aleck ; Michel, Anna P. M. ; Mooney, T. AranThe global coastal ocean provides food and other critical resources to human societies. Yet this habitat, for which many depend, has experienced severe degradation from human activities. The rates of human-induced changes along the coast demand significantly improved coverage of ocean observations in order to support science-based decision making and policy formation tailored to specific regions. Our proposal envisions developing a global network of low-cost, easily produced and readily deployed oceanographic sensors for use on a wide variety of platforms in the coastal ocean. A substantially large number of these sensors can thus be installed on existing infrastructure, ships of opportunity, and fishing fleets, or even individually along the coast, particularly in vulnerable and disadvantaged regions. This would vastly increase the spatiotemporal resolution of the current data coverage along the coast, allowing greater equitable access. It would also offer significant opportunities for partnership with communities, NGOs, governments, and other stakeholders, as well as a wide range of commercial and industrial sectors to develop and deploy sensors in scalable networks transmitting data in near-real time. Finally, it presents a vastly lowered bar for participation by citizen scientists and other engaged members of the public to address location-specific coastal problems anywhere in the world.
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ArticleThe acceleration of dissolved cobalt's ecological stoichiometry due to biological uptake, remineralization, and scavenging in the Atlantic Ocean(Copernicus Publications on behalf of the European Geosciences Union, 2017-10-20) Saito, Mak A. ; Noble, Abigail E. ; Hawco, Nicholas J. ; Twining, Benjamin S. ; Ohnemus, Daniel C. ; John, Seth G. ; Lam, Phoebe J. ; Conway, Tim M. ; Johnson, Rod ; Moran, Dawn M. ; McIlvin, Matthew R.The stoichiometry of biological components and their influence on dissolved distributions have long been of interest in the study of the oceans. Cobalt has the smallest oceanic inventory of inorganic micronutrients and hence is particularly vulnerable to influence by internal oceanic processes including euphotic zone uptake, remineralization, and scavenging. Here we observe not only large variations in dCo : P stoichiometry but also the acceleration of those dCo : P ratios in the upper water column in response to several environmental processes. The ecological stoichiometry of total dissolved cobalt (dCo) was examined using data from a US North Atlantic GEOTRACES transect and from a zonal South Atlantic GEOTRACES-compliant transect (GA03/3_e and GAc01) by Redfieldian analysis of its statistical relationships with the macronutrient phosphate. Trends in the dissolved cobalt to phosphate (dCo : P) stoichiometric relationships were evident in the basin-scale vertical structure of cobalt, with positive dCo : P slopes in the euphotic zone and negative slopes found in the ocean interior and in coastal environments. The euphotic positive slopes were often found to accelerate towards the surface and this was interpreted as being due to the combined influence of depleted phosphate, phosphorus-sparing (conserving) mechanisms, increased alkaline phosphatase metalloenzyme production (a zinc or perhaps cobalt enzyme), and biochemical substitution of Co for depleted Zn. Consistent with this, dissolved Zn (dZn) was found to be drawn down to only 2-fold more than dCo, despite being more than 18-fold more abundant in the ocean interior. Particulate cobalt concentrations increased in abundance from the base of the euphotic zone to become ∼ 10 % of the overall cobalt inventory in the upper euphotic zone with high stoichiometric values of ∼ 400 µmol Co mol−1 P. Metaproteomic results from the Bermuda Atlantic Time-series Study (BATS) station found cyanobacterial isoforms of the alkaline phosphatase enzyme to be prevalent in the upper water column, as well as a sulfolipid biosynthesis protein indicative of P sparing. The negative dCo : P relationships in the ocean interior became increasingly vertical with depth, and were consistent with the sum of scavenging and remineralization processes (as shown by their dCo : P vector sums). Attenuation of the remineralization with depth resulted in the increasingly vertical dCo : P relationships. Analysis of particulate Co with particulate Mn and particulate phosphate also showed positive linear relationships below the euphotic zone, consistent with the presence and increased relative influence of Mn oxide particles involved in scavenging. Visualization of dCo : P slopes across an ocean section revealed hotspots of scavenging and remineralization, such as at the hydrothermal vents and below the oxygen minimum zone (OMZ) region, respectively, while that of an estimate of Co* illustrated stoichiometrically depleted values in the mesopelagic and deep ocean due to scavenging. This study provides insights into the coupling between the dissolved and particulate phase that ultimately creates Redfield stoichiometric ratios, demonstrating that the coupling is not an instantaneous process and is influenced by the element inventory and rate of exchange between phases. Cobalt's small water column inventory and the influence of external factors on its biotic stoichiometry can erode its limited inertia and result in an acceleration of the dissolved stoichiometry towards that of the particulate phase in the upper euphotic zone. As human use of cobalt grows exponentially with widespread adoption of lithium ion batteries, there is a potential to affect the limited biogeochemical inertia of cobalt and its resultant ecology in the oceanic euphotic zone.
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PreprintAccessing monomers, surfactants, and the queen bee substance by acrylate cross-metathesis of long-chain alkenones( 2017-05) O’Neil, Gregory W. ; Williams, John R. ; Craig, Alexander M. ; Nelson, Robert K. ; Gosselin, Kelsey M. ; Reddy, Christopher M.Polyunsaturated long-chain alkenones are a unique class of lipids biosynthesized in significant quantities (up to 20% of cell carbon) by several algae including the industrially grown marine microalgae Isochrysis. Alkenone structures are characterized by a long linear carbon-chain (35-40 carbons) with one to four trans-double bonds and terminating in a methyl or ethyl ketone. Alkenones were extracted and isolated from commercially obtained Isochrysis biomass and then subjected to cross-metathesis (CM) with methyl acrylate or acrylic acid using the Hoveyda-Grubbs metathesis initiator. Within 1 h at room temperature alkenones were consumed, however complete fragmentation (i.e. conversion to the smallest subunits by double bond cleavage) required up to 16 h. Analysis of the reaction mixture by gas chromatography and comprehensive two-dimensional gas chromatography revealed a predictable product mixture consisting primarily of long-chain (mostly C17) acids (or methyl esters from CM with methyl acrylate) and diacids (or diesters), along with smaller amounts (~5%) of the honey bee “queen substance” (E)-9-oxo-decenoic acid. Together, these compounds comprise a diverse mixture of valuable chemicals that includes surfactants, monomers, and an agriculturally relevant bee pheromone.
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PreprintActinium and radium fluxes from the seabed in the northeast Pacific Basin(Elsevier, 2022-10-22) Kemnitz, Nathaniel ; Hammond, Douglas E. ; Henderson, Paul ; Le Roy, Emilie ; Charette, Matthew ; Moore, Willard ; Anderson, Robert F. ; Fleisher, Martin Q. ; Leal, Anne ; Black, Erin ; Hayes, Christopher T. ; Adkins, Jess ; Berelson, William ; Bian, XiaopengFive sediment cores were collected along a cruise tract from Hawaii to Alaska in August 2017 (C-Disk-IV cruise) with the objective of characterizing the behavior of 227Ac, 228Ra, and 226Ra and their fluxes into the overlying water column, information that is essential to the interpretation of the distribution of these tracers in the ocean, for example, as measured on GEOTRACES cruises. Solid phase profiles of these isotopes were measured, and reaction-transport models were applied that incorporated molecular diffusion, bioturbation, sedimentation, distribution coefficients (kd), and the fraction of each isotope released to pore water by parent decay (called F). Fits to these profiles used kd values determined in lab experiments for C-Disk-IV sediments. Ra kd values (1000–3000 mL g−1) agreed with previous estimates for deep-sea sediments, and Ac kd values (3500–22,000 mL g−1) correlated with those for Ra but were about 7 times greater. Two independent approaches were used to quantify the benthic fluxes of 227Ac and 228Ra in the Northeast Pacific: (1) use of solid phase profiles with a reaction-transport model, as well as integrated downcore daughter-parent deficiency; and (2) direct measurement of fluxes based on core incubation. The two independent methods agreed within uncertainty, and the average 227Ac and 228Ra sediment fluxes for the Northeast Pacific are 90 ± 20 and 600 ± 200 dpm m−2-yr−1, respectively. The 226Ra sediment flux was only determined by the former approach, and the flux calculated in this study is similar to previous work in the North Pacific, averaging 1300 ± 200 dpm m−2-yr−1. This is over 2× higher than the water column inventory of 226Ra in this region (600 dpm m−2-yr−1), and indicates the importance of lateral 226Ra export from the N. Pacific. The largest 227Ac and Ra isotope fluxes in the study area are near the center of the Northeast Pacific (∼37°N). Smaller 227Ac, 228Ra and 226Ra fluxes occur north of 40°N, primarily due to dilution of their Pa and Th ancestors by higher sediment accumulation rates.
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ArticleActive subseafloor microbial communities from Mariana back-arc venting fluids share metabolic strategies across different thermal niches and taxa(Springer Nature, 2019-05-09) Trembath-Reichert, Elizabeth ; Butterfield, David A. ; Huber, Julie A.There are many unknowns regarding the distribution, activity, community composition, and metabolic repertoire of microbial communities in the subseafloor of deep-sea hydrothermal vents. Here we provide the first characterization of subseafloor microbial communities from venting fluids along the central Mariana back-arc basin (15.5–18°N), where the slow-spreading rate, depth, and variable geochemistry along the back-arc distinguish it from other spreading centers. Results indicated that diverse Epsilonbacteraeota were abundant across all sites, with a population of high temperature Aquificae restricted to the northern segment. This suggests that differences in subseafloor populations along the back-arc are associated with local geologic setting and resultant geochemistry. Metatranscriptomics coupled to stable isotope probing revealed bacterial carbon fixation linked to hydrogen oxidation, denitrification, and sulfide or thiosulfate oxidation at all sites, regardless of community composition. NanoSIMS (nanoscale secondary ion mass spectrometry) incubations at 80 °C show only a small portion of the microbial community took up bicarbonate, but those autotrophs had the highest overall rates of activity detected across all experiments. By comparison, acetate was more universally utilized to sustain growth, but within a smaller range of activity. Together, results indicate that microbial communities in venting fluids from the Mariana back-arc contain active subseafloor communities reflective of their local conditions with metabolisms commonly shared across geologically disparate spreading centers throughout the ocean.
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ArticleAdaptive responses of marine diatoms to zinc scarcity and ecological implications(Nature Research, 2022-04-14) Kellogg, Riss ; Moosburner, Mark A. ; Cohen, Natalie R. ; Hawco, Nicholas J. ; McIlvin, Matthew R. ; Moran, Dawn M. ; DiTullio, Giacomo R. ; Subhas, Adam V. ; Saito, Mak A.Scarce dissolved surface ocean concentrations of the essential algal micronutrient zinc suggest that Zn may influence the growth of phytoplankton such as diatoms, which are major contributors to marine primary productivity. However, the specific mechanisms by which diatoms acclimate to Zn deficiency are poorly understood. Using global proteomic analysis, we identified two proteins (ZCRP-A/B, Zn/Co Responsive Protein A/B) among four diatom species that became abundant under Zn/Co limitation. Characterization using reverse genetic techniques and homology data suggests putative Zn/Co chaperone and membrane-bound transport complex component roles for ZCRP-A (a COG0523 domain protein) and ZCRP-B, respectively. Metaproteomic detection of ZCRPs along a Pacific Ocean transect revealed increased abundances at the surface (<200 m) where dZn and dCo were scarcest, implying Zn nutritional stress in marine algae is more prevalent than previously recognized. These results demonstrate multiple adaptive responses to Zn scarcity in marine diatoms that are deployed in low Zn regions of the Pacific Ocean.