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  • American Association for the Advancement of Science
  • American Chemical Society
  • Essen : Verl. Glückauf
  • Hindawi
  • Krefeld : Geologischer Dienst Nordhein-Westfalen
  • 2020-2023  (36)
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  • 1
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    Archean cratonic mantle recycled at a mid-ocean ridge (2022)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-09-13
    Description: © The Author(s), 2022. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Liu, C.-Z., Dick, H. J. B., Mitchell, R. N., Wei, W., Zhang, Z.-Y., Hofmann, A. W., Yang, J.-F., & Li, Y. Archean cratonic mantle recycled at a mid-ocean ridge. Science Advances, 8(22), (2022): eabn6749, https://doi.org/10.1126/sciadv.abn6749.
    Description: Basalts and mantle peridotites of mid-ocean ridges are thought to sample Earth’s upper mantle. Osmium isotopes of abyssal peridotites uniquely preserve melt extraction events throughout Earth history, but existing records only indicate ages up to ~2 billion years (Ga) ago. Thus, the memory of the suspected large volumes of mantle lithosphere that existed in Archean time (〉2.5 Ga) has apparently been lost somehow. We report abyssal peridotites with melt-depletion ages up to 2.8 Ga, documented by extremely unradiogenic 187Os/188Os ratios (to as low as 0.1095) and refractory major elements that compositionally resemble the deep keels of Archean cratons. These oceanic rocks were thus derived from the once-extensive Archean continental keels that have been dislodged and recycled back into the mantle, the feasibility of which we confirm with numerical modeling. This unexpected connection between young oceanic and ancient continental lithosphere indicates an underappreciated degree of compositional recycling over time.
    Description: This study was financially supported by the National Science Fund for Distinguished Young Scholars 42025201 (to C.-Z.L.), the National Key Research and Development Project of China 2020YFA0714801 (to C.-Z.L.), the Strategic Priority Research Program of the Chinese Academy of Sciences XDA13010106 (to C.-Z.L.), the Strategic Priority Research Program of the Chinese Academy of Sciences XDB42020301 (to C.-Z.L.), and NSF grants 2114652 and 1657983 (to H.J.B.D.).
    Repository Name: Woods Hole Open Access Server
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  • 2
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    Serpentinite-derived slab fluids control the oxidation state of the subarc mantle (2022)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-05-27
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Zhang, Y., Gazel, E., Gaetani, G. A., & Klein, F. Serpentinite-derived slab fluids control the oxidation state of the subarc mantle. Science Advances, 7(48), (2021): eabj2515, https://doi.org/10.1126/sciadv.abj2515.
    Description: Recent geochemical evidence confirms the oxidized nature of arc magmas, but the underlying processes that regulate the redox state of the subarc mantle remain yet to be determined. We established a link between deep subduction-related fluids derived from dehydration of serpentinite ± altered oceanic crust (AOC) using B isotopes and B/Nb as fluid proxies, and the oxidized nature of arc magmas as indicated by Cu enrichment during magma evolution and V/Yb. Our results suggest that arc magmas derived from source regions influenced by a greater serpentinite (±AOC) fluid component record higher oxygen fugacity. The incorporation of this component into the subarc mantle is controlled by the subduction system’s thermodynamic conditions and geometry. Our results suggest that the redox state of the subarc mantle is not homogeneous globally: Primitive arc magmas associated with flat, warm subduction are less oxidized overall than those generated in steep, cold subduction zones.
    Description: Y.Z. acknowledges funding from the National Science Foundation of China (91958213), the Chinese Academy of Sciences (XDB42020402), and the Shandong Provincial Natural Science Foundation, China (ZR2020QD068). This study was supported in part by the U.S. National Science Foundation NSF EAR 1826673 to E.G. and G.A.G. and OCE 1756349 to E.G.
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  • 3
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    Rapid degradation of cellulose diacetate by marine microbes (2022)
    American Chemical Society
    Details
    Publication Date: 2022-05-27
    Description: © The Author(s), 2022. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Mazzotta, M. G., Reddy, C. M., & Ward, C. P. Rapid degradation of cellulose diacetate by marine microbes. Environmental Science & Technology Letters, 9(1), (2022): 37-41. https://doi.org/10.1021/acs.estlett.1c00843.
    Description: The persistence of cellulose diacetate (CDA), a biobased plastic used in textiles and single-use consumer products, in the ocean is currently unknown. Here, we probe the disintegration and degradation of CDA-based materials (25 μm films, 510 μm foam, and 97 g/m2 fabric) by marine microbes in a continuous flow seawater mesocosm. Photographic evidence and mass loss measurements demonstrate that CDA-based materials disintegrate in months. Disintegration is marked by the increasing esterase and cellulase activity of the biofilm community, suggesting that marine microbes degrade CDA. The natural abundance stable (13C) and radiocarbon (14C) isotopic signature of carbon dioxide respired during short-term bottle incubations confirms the rapid degradation of both acetyl and cellulosic components of CDA by seawater microbial communities. These findings challenge the paradigm set by governmental agencies and advocacy groups that CDA-based materials persist in the ocean for decades, and represent a positive step toward identifying high-utility, biobased plastics with low environmental persistence.
    Description: M.G.M., C.M.R., and C.P.W. thank Eastman Chemical Co. and Woods Hole Oceanographic Institution (WHOI) for scientific and financial support.
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  • 4
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    Environmentally friendly and efficient hornet nest envelope-based photothermal absorbers (2022)
    American Chemical Society
    Details
    Publication Date: 2022-05-27
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Xie, L., Liu, X., Caratenuto, A., Tian, Y., Chen, F., DeGiorgis, J. A., Wan, Y., & Zheng, Y. Environmentally friendly and efficient hornet nest envelope-based photothermal absorbers. Acs Omega, 6(50), (2021): 34555–34562, https://doi.org/10.1021/acsomega.1c04851.
    Description: Water shortage is a critical global issue that threatens human health, environmental sustainability, and the preservation of Earth’s climate. Desalination from seawater and sewage is a promising avenue for alleviating this stress. In this work, we use the hornet nest envelope material to fabricate a biomass-based photothermal absorber as part of a desalination isolation system. This system realizes an evaporation rate of 3.98 kg m–2 h–1 under one-sun illumination, with prolonged evaporation rates all above 4 kg m–2 h–1. This system demonstrates a strong performance of 3.86 kg m–2 h–1 in 3.5 wt % saltwater, illustrating its effectiveness in evaporation seawater. Thus, with its excellent evaporation rate, great salt rejection ability, and easy fabrication approach, the hornet nest envelope constitutes a promising natural material for solar water treatment applications.
    Description: The authors acknowledge the support from the National Science Foundation, USA, through grant number CBET-1941743 and the National Science Foundation under EPSCoR Cooperation Agreement OIA-1655221.
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  • 5
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    Sunlight-driven dissolution is a major fate of oil at sea (2022)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-06-09
    Description: © The Author(s), 2022. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Freeman, D. H., & Ward, C. P. Sunlight-driven dissolution is a major fate of oil at sea. Science Advances, 8(7), (2022): eabl7605, https://doi.org/10.1126/sciadv.abl7605.
    Description: Oxygenation reactions initiated by sunlight can transform insoluble components of crude oil at sea into water-soluble products, a process called photo-dissolution. First reported a half century ago, photo-dissolution has never been included in spill models because key parameters required for rate modeling were unknown, including the wavelength and photon dose dependence. Here, we experimentally quantified photo-dissolution as a function of wavelength and photon dose, making possible a sensitivity analysis of environmental variables in hypothetical spill scenarios and a mass balance assessment for the 2010 Deepwater Horizon (DwH) spill. The sensitivity analysis revealed that rates were most sensitive to oil slick thickness, season/latitude, and wavelength and less sensitive to photon dose. We estimate that 3 to 17% (best estimate 8%) of DwH surface oil was subject to photo-dissolution, comparable in magnitude to other widely recognized fate processes. Our findings invite a critical reevaluation of surface oil budgets for both DwH and future spills at sea.
    Description: This work was supported by the Fisheries and Oceans Canada Multi-Partner Research Initiative award to C.P.W. (project #1.06), the NSF Graduate Research Fellowship awarded to D.H.F. (award #174530), and NSF-OCE grant #1841092 to C.P.W.
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  • 6
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    Surface warming-induced global acceleration of upper ocean currents (2022)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-07-25
    Description: © The Author(s), 2022. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Peng, Q., Xie, S.-P., Wang, D., Huang, R. X., Chen, G., Shu, Y., Shi, J.-R., & Liu, W. Surface warming-induced global acceleration of upper ocean currents. Science Advances, 8(16), (2022): eabj8394, https://doi.org/10.1126/sciadv.abj8394.
    Description: How the ocean circulation changes in a warming climate is an important but poorly understood problem. Using a global ocean model, we decompose the problem into distinct responses to changes in sea surface temperature, salinity, and wind. Our results show that the surface warming effect, a robust feature of anthropogenic climate change, dominates and accelerates the upper ocean currents in 77% of the global ocean. Specifically, the increased vertical stratification intensifies the upper subtropical gyres and equatorial currents by shoaling these systems, while the differential warming between the Southern Ocean upwelling zone and the region to the north accelerates surface zonal currents in the Southern Ocean. In comparison, the wind stress and surface salinity changes affect regional current systems. Our study points a way forward for investigating ocean circulation change and evaluating the uncertainty.
    Description: Q.P. is supported by the National Natural Science Foundation of China (42005035), the Science and Technology Planning Project of Guangzhou (202102020935), and the Independent Research Project Program of State Key Laboratory of Tropical Oceanography (LTOZZ2102). D.W. is supported by the National Natural Science Foundation of China (92158204), and the Innovation Group Project of Southern Marine Science and Engineering Guangdong Laboratory (Zhuhai) (311020004). S.-P.X. is supported by the National Science Foundation (AGS-1934392). Y.S. is supported by the National Key Research and Development Program of China (2016YFC1401702). G.C. is supported by National Natural Science Foundation of China (41822602). The numerical simulation is supported by the High-Performance Computing Division and HPC managers of W. Zhou and D. Sui in the South China Sea Institute of Oceanology.
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  • 7
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    Divergent forms of pyroplastic: lessons learned from the M/V X-Press Pearl ship fire (2022)
    American Chemical Society
    Details
    Publication Date: 2022-12-07
    Description: © The Author(s), 2022. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in James, B., de Vos, A., Aluwihare, L., Youngs, S., Ward, C., Nelson, R., Michel, A., Hahn, M., & Reddy, C. Divergent forms of pyroplastic: lessons learned from the M/V X-Press Pearl ship fire. ACS Environmental Au, 2(5), (2022): 467–479, https://doi.org/10.1021/acsenvironau.2c00020.
    Description: In late May 2021, the M/V X-Press Pearl container ship caught fire while anchored 18 km off the coast of Colombo, Sri Lanka and spilled upward of 70 billion pieces of plastic or “nurdles” (∼1680 tons), littering the country’s coastline. Exposure to combustion, heat, chemicals, and petroleum products led to an apparent continuum of changes from no obvious effects to pieces consistent with previous reports of melted and burned plastic (pyroplastic) found on beaches. At the middle of this continuum, nurdles were discolored but appeared to retain their prefire morphology, resembling nurdles that had been weathered in the environment. We performed a detailed investigation of the physical and surface properties of discolored nurdles collected on a beach 5 days after the ship caught fire and within 24 h of their arrival onshore. The color was the most striking trait of the plastic: white for nurdles with minimal alteration from the accident, orange for nurdles containing antioxidant degradation products formed by exposure to heat, and gray for partially combusted nurdles. Our color analyses indicate that this fraction of the plastic released from the ship was not a continuum but instead diverged into distinct groups. Fire left the gray nurdles scorched, with entrained particles and pools of melted plastic, and covered in soot, representing partial pyroplastics, a new subtype of pyroplastic. Cross sections showed that the heat- and fire-induced changes were superficial, leaving the surfaces more hydrophilic but the interior relatively untouched. These results provide timely and actionable information to responders to reevaluate cleanup end points, monitor the recurrence of these spilled nurdles, gauge short- and long-term effects of the spilled nurdles to the local ecosystem, and manage the recovery of the spill. These findings underscore partially combusted plastic (pyroplastic) as a type of plastic pollution that has yet to be fully explored despite the frequency at which plastic is burned globally.
    Description: This work was supported by the Postdoctoral Scholar Program at the Woods Hole Oceanographic Institution (WHOI), with funding provided by the Weston Howland Jr. Postdoctoral Scholarship. Additional support was provided by the WHOI Marine Microplastics Catalyst Program, the WHOI Marine Microplastics Innovation Accelerator Program, the WHOI Investment in Science Fund, the March Marine Initiative (a program of March Limited, Bermuda), The Seaver Institute, Gerstner Philanthropies, the Wallace Research Foundation, the Richard Saltonstall Charitable Foundation, the Harrison Foundation, Hollis and Ermine Lovell Charitable Foundation, and the Richard Grand Foundation. AdV was supported by funding from the Schmidt Foundation.
    Keywords: Microplastic ; Resin pellets ; Pollution ; Additives ; Open burning ; Weathering ; Maritime accident
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  • 8
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    Microplastics in the Weddell Sea (Antarctica): A Forensic Approach for Discrimination between Environmental and Vessel-Induced Microplastics (2021)
    American Chemical Society
    In:  EPIC3Environmental Science & Technology, American Chemical Society, ISSN: 0013-936X
    Details
    Publication Date: 2022-01-07
    Description: Microplastic (MP) pollution has been found in the Southern Ocean surrounding Antarctica, but many local regions within this vast area remain uninvestigated. The remote Weddell Sea contributes to the global thermohaline circulation, and one of the two Antarctic gyres is located in that region. In the present study, we evaluate MP (〉300 μm) concentration and composition in surface (n = 34) and subsurface water samples (n = 79, ∼11.2 m depth) of the Weddell Sea. All putative MP were analyzed by attenuated total reflection Fourier transform infrared (ATR-FTIR) spectroscopy. MP was found in 65% of surface and 11.4% of subsurface samples, with mean (±standard deviation (SD)) concentrations of 0.01 (±0.01 SD) MP m–3 and 0.04 (±0.1 SD) MP m–3, respectively, being within the range of previously reported values for regions south of the Polar Front. Additionally, we aimed to determine whether identified paint fragments (n = 394) derive from the research vessel. Environmentally sampled fragments (n = 101) with similar ATR-FTIR spectra to reference paints from the research vessel and fresh paint references generated in the laboratory were further subjected to micro-X-ray fluorescence spectroscopy (μXRF) to compare their elemental composition. This revealed that 45.5% of all recovered MP derived from vessel-induced contamination. However, 11% of the measured fragments could be distinguished from the reference paints via their elemental composition. This study demonstrates that differentiation based purely on visual characteristics and FTIR spectroscopy might not be sufficient for accurately determining sample contamination sources.
    Repository Name: EPIC Alfred Wegener Institut
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  • 9
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    Plastic formulation is an emerging control of its photochemical fate in the ocean (2021)
    American Chemical Society
    Details
    Publication Date: 2022-10-26
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Walsh, A. N., Reddy, C. M., Niles, S. F., McKenna, A. M., Hansel, C. M., & Ward, C. P. Plastic formulation is an emerging control of its photochemical fate in the ocean. Environmental Science & Technology, 55(18), (2021): 12383–12392, https://doi.org/10.1021/acs.est.1c02272.
    Description: Sunlight exposure is a control of long-term plastic fate in the environment that converts plastic into oxygenated products spanning the polymer, dissolved, and gas phases. However, our understanding of how plastic formulation influences the amount and composition of these photoproducts remains incomplete. Here, we characterized the initial formulations and resulting dissolved photoproducts of four single-use consumer polyethylene (PE) bags from major retailers and one pure PE film. Consumer PE bags contained 15–36% inorganic additives, primarily calcium carbonate (13–34%) and titanium dioxide (TiO2; 1–2%). Sunlight exposure consistently increased production of dissolved organic carbon (DOC) relative to leaching in the dark (3- to 80-fold). All consumer PE bags produced more DOC during sunlight exposure than the pure PE (1.2- to 2.0-fold). The DOC leached after sunlight exposure increasingly reflected the 13C and 14C isotopic composition of the plastic. Ultrahigh resolution Fourier transform ion cyclotron resonance mass spectrometry revealed that sunlight exposure substantially increased the number of DOC formulas detected (1.1- to 50-fold). TiO2-containing bags photochemically degraded into the most compositionally similar DOC, with 68–94% of photoproduced formulas in common with at least one other TiO2-containing bag. Conversely, only 28% of photoproduced formulas from the pure PE were detected in photoproduced DOC from the consumer PE. Overall, these findings suggest that plastic formulation, especially TiO2, plays a determining role in the amount and composition of DOC generated by sunlight. Consequently, studies on pure, unweathered polymers may not accurately represent the fates and impacts of the plastics entering the ocean.
    Description: Funding was provided by the Seaver Institute, the Gerstner Family Foundation, Woods Hole Oceanographic Institution, and the National Science Foundation Graduate Research Fellowship Program (A.N.W.). The Ion Cyclotron Resonance user facility at the National High Magnetic Field Laboratory is supported by the National Science Foundation Division of Chemistry and Division of Materials Research through DMR-1644779 and the State of Florida.
    Keywords: Plastic pollution ; Marine debris ; Additives ; Dissolved organic carbon ; Photochemical oxidation ; FT-ICR-MS ; Titanium dioxide
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  • 10
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    Multiple integrated metabolic strategies allow foraminiferan protists to thrive in anoxic marine sediments (2021)
    American Association for the Advancement of Science
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    Publication Date: 2022-05-27
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Gomaa, F., Utter, D. R., Powers, C., Beaudoin, D. J., Edgcomb, V. P., Filipsson, H. L., Hansel, C. M., Wankel, S. D., Zhang, Y., & Bernhard, J. M. Multiple integrated metabolic strategies allow foraminiferan protists to thrive in anoxic marine sediments. Science Advances, 7(22), (2021): eabf1586, https://doi.org/10.1126/sciadv.abf1586.
    Description: Oceanic deoxygenation is increasingly affecting marine ecosystems; many taxa will be severely challenged, yet certain nominally aerobic foraminifera (rhizarian protists) thrive in oxygen-depleted to anoxic, sometimes sulfidic, sediments uninhabitable to most eukaryotes. Gene expression analyses of foraminifera common to severely hypoxic or anoxic sediments identified metabolic strategies used by this abundant taxon. In field-collected and laboratory-incubated samples, foraminifera expressed denitrification genes regardless of oxygen regime with a putative nitric oxide dismutase, a characteristic enzyme of oxygenic denitrification. A pyruvate:ferredoxin oxidoreductase was highly expressed, indicating the capability for anaerobic energy generation during exposure to hypoxia and anoxia. Near-complete expression of a diatom’s plastid genome in one foraminiferal species suggests kleptoplasty or sequestration of functional plastids, conferring a metabolic advantage despite the host living far below the euphotic zone. Through a unique integration of functions largely unrecognized among “typical” eukaryotes, benthic foraminifera represent winning microeukaryotes in the face of ongoing oceanic deoxygenation.
    Description: his project was funded by the U.S. NSF IOS 1557430 and 1557566. H.L.F. acknowledges support from the Swedish Research Council VR (grant number 2017-04190).
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  • 11
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    Postmelting hydrogen enrichment in the oceanic lithosphere (2021)
    American Association for the Advancement of Science
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    Publication Date: 2022-05-27
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Le Roux, V., Urann, B. M., Brunelli, D., Bonatti, E., Cipriani, A., Demouchy, S., & Monteleone, B. D. Postmelting hydrogen enrichment in the oceanic lithosphere. Science Advances, 7(24), (2021): eabf6071, https://doi.org/10.1126/sciadv.abf6071.
    Description: The large range of H2O contents recorded in minerals from exhumed mantle rocks has been challenging to interpret, as it often records a combination of melting, metasomatism, and diffusional processes in spatially isolated samples. Here, we determine the temporal variations of H2O contents in pyroxenes from a 24-Ma time series of abyssal peridotites exposed along the Vema fracture zone (Atlantic Ocean). The H2O contents of pyroxenes correlate with both crustal ages and pyroxene chemistry and increase toward younger and more refractory peridotites. These variations are inconsistent with residual values after melting and opposite to trends often observed in mantle xenoliths. Postmelting hydrogen enrichment occurred by ionic diffusion during cryptic metasomatism of peridotite residues by low-degree, volatile-rich melts and was particularly effective in the most depleted peridotites. The presence of hydrous melts under ridges leads to widespread hydrogen incorporation in the oceanic lithosphere, likely lowering mantle viscosity compared to dry models.
    Description: Funding for this study was supported by NSF EAR-P&G 1524311 and 1839128 to V.L.R. and the Andrew W. Mellon Foundation Award for Innovative Research to V.L.R. A.C. and D.B. were funded by the Italian Programma di Rilevante Interesse Nazionale PRIN 20178LPCPW and PRIN2017KY5ZX8, respectively. Revisions were performed within the duration of a “Visiting Scholar at SCIENCE 2020” award to V.L.R. (University of Copenhagen, Denmark), with support from the Department of Geosciences and Natural Resource Management, Section for Geology.
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  • 12
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    Remote and local drivers of Pleistocene South Asian summer monsoon precipitation: a test for future predictions (2021)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-05-27
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Clemens, S. C., Yamamoto, M., Thirumalai, K., Giosan, L., Richey, J. N., Nilsson-Kerr, K., Rosenthal, Y., Anand, P., & McGrath, S. M. Remote and local drivers of Pleistocene South Asian summer monsoon precipitation: a test for future predictions. Science Advances, 7(23), (2021): eabg3848, https://doi.org/10.1126/sciadv.abg3848.
    Description: South Asian precipitation amount and extreme variability are predicted to increase due to thermodynamic effects of increased 21st-century greenhouse gases, accompanied by an increased supply of moisture from the southern hemisphere Indian Ocean. We reconstructed South Asian summer monsoon precipitation and runoff into the Bay of Bengal to assess the extent to which these factors also operated in the Pleistocene, a time of large-scale natural changes in carbon dioxide and ice volume. South Asian precipitation and runoff are strongly coherent with, and lag, atmospheric carbon dioxide changes at Earth’s orbital eccentricity, obliquity, and precession bands and are closely tied to cross-equatorial wind strength at the precession band. We find that the projected monsoon response to ongoing, rapid high-latitude ice melt and rising carbon dioxide levels is fully consistent with dynamics of the past 0.9 million years.
    Description: S.C.C. and S.M.M. were supported by U.S. NSF OCE1634774. M.Y. was funded by JSPS grants JPMXS05R2900001 and 19H05595 and JAMSTEC Exp. 353 postcruise study. K.N.-K. and P.A. were supported by UK-IODP, Open University, and NERC (NE/L002493/1), K.T. was supported by the Technology and Research Initiative Fund, Arizona Board of Regents.
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  • 13
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    Groundwater residence time estimates obscured by anthropogenic carbonate (2021)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-05-27
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Seltzer, A. M., Bekaert, D. V., Barry, P. H., Durkin, K. E., Mace, E. K., Aalseth, C. E., Zappala, J. C., Mueller, P., Jurgens, B., & Kulongoski, J. T. Groundwater residence time estimates obscured by anthropogenic carbonate. Science Advances, 7(17), (2021): eabf3503, https://doi.org/10.1126/sciadv.abf3503.
    Description: Groundwater is an important source of drinking and irrigation water. Dating groundwater informs its vulnerability to contamination and aids in calibrating flow models. Here, we report measurements of multiple age tracers (14C, 3H, 39Ar, and 85Kr) and parameters relevant to dissolved inorganic carbon (DIC) from 17 wells in California’s San Joaquin Valley (SJV), an agricultural region that is heavily reliant on groundwater. We find evidence for a major mid-20th century shift in groundwater DIC input from mostly closed- to mostly open-system carbonate dissolution, which we suggest is driven by input of anthropogenic carbonate soil amendments. Crucially, enhanced open-system dissolution, in which DIC equilibrates with soil CO2, fundamentally affects the initial 14C activity of recently recharged groundwater. Conventional 14C dating of deeper SJV groundwater, assuming an open system, substantially overestimates residence time and thereby underestimates susceptibility to modern contamination. Because carbonate soil amendments are ubiquitous, other groundwater-reliant agricultural regions may be similarly affected.
    Description: his work was conducted as a part of the USGS National Water Quality Assessment Program (NAWQA) Enhanced Trends Project (https://water.usgs.gov/nawqa/studies/gwtrends/). Measurements at Argonne National Laboratory were supported by Department of Energy, Office of Science under contract DE-AC02-06CH11357. Measurements at Pacific Northwest National Laboratory were part of the Ultra-Sensitive Nuclear Measurements Initiative conducted under the Laboratory Directed Research and Development Program. PNNL is operated by Battelle for the U.S. Department of Energy under Contract DE-AC05-76RL01830. This work was also partially supported by NSF award OCE-1923915 (to A.M.S. and P.H.B. at WHOI).
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  • 14
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    Production of two highly abundant 2-methyl-branched fatty acids by blooms of the globally significant marine cyanobacteria Trichodesmium erythraeum (2021)
    American Chemical Society
    Details
    Publication Date: 2022-05-27
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Gosselin, K. M., Nelson, R. K., Spivak, A. C., Sylva, S. P., Van Mooy, B. A. S., Aeppli, C., Sharpless, C. M., O’Neil, G. W., Arrington, E. C., Reddy, C. M., & Valentine, D. L. Production of two highly abundant 2-methyl-branched fatty acids by blooms of the globally significant marine cyanobacteria Trichodesmium erythraeum. ACS Omega, 6(35), (2021): 22803–22810, https://doi.org/10.1021/acsomega.1c03196.
    Description: The bloom-forming cyanobacteria Trichodesmium contribute up to 30% to the total fixed nitrogen in the global oceans and thereby drive substantial productivity. On an expedition in the Gulf of Mexico, we observed and sampled surface slicks, some of which included dense blooms of Trichodesmium erythraeum. These bloom samples contained abundant and atypical free fatty acids, identified here as 2-methyldecanoic acid and 2-methyldodecanoic acid. The high abundance and unusual branching pattern of these compounds suggest that they may play a specific role in this globally important organism.
    Description: This work was funded with grants from the National Science Foundation grants OCE-1333148, OCE-1333162, and OCE-1756254 and the Woods Hole Oceanographic Institution (IR&D). GCxGC analysis made possible by WHOI’s Investment in Science Fund.
    Keywords: Lipids ; Alkyls ; Bacteria ; Genetics ; Chromatography
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    Multiple carbon incorporation strategies support microbial survival in cold subseafloor crustal fluids (2021)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-05-27
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Trembath-Reichert, E., Shah Walter, S. R., Ortiz, M. A. F., Carter, P. D., Girguis, P. R., & Huber, J. A. Multiple carbon incorporation strategies support microbial survival in cold subseafloor crustal fluids. Science Advances, 7(18), (2021): eabg0153, https://doi.org/10.1126/sciadv.abg0153.
    Description: Biogeochemical processes occurring in fluids that permeate oceanic crust make measurable contributions to the marine carbon cycle, but quantitative assessments of microbial impacts on this vast, subsurface carbon pool are lacking. We provide bulk and single-cell estimates of microbial biomass production from carbon and nitrogen substrates in cool, oxic basement fluids from the western flank of the Mid-Atlantic Ridge. The wide range in carbon and nitrogen incorporation rates indicates a microbial community well poised for dynamic conditions, potentially anabolizing carbon and nitrogen at rates ranging from those observed in subsurface sediments to those found in on-axis hydrothermal vent environments. Bicarbonate incorporation rates were highest where fluids are most isolated from recharging bottom seawater, suggesting that anabolism of inorganic carbon may be a potential strategy for supplementing the ancient and recalcitrant dissolved organic carbon that is prevalent in the globally distributed subseafloor crustal environment.
    Description: The Gordon and Betty Moore Foundation sponsored most of the observatory components at North Pond through grant GBMF1609. This work was supported by the National Science Foundation through grants NSF OCE-1745589, OCE-1635208, and OCE-1062006 to J.A.H. and NSF OCE-1635365 to P.R.G. and S.R.S.W.; NASA Postdoctoral Fellowship with the NASA Astrobiology Institute to E.T.-R.; L’Oréal USA For Women in Science Fellowship to E.T.-R.; and Woods Hole Partnership Education Program, sponsored by the Woods Hole Diversity Initiative to M.A.F.O. The Center for Dark Energy Biosphere Investigations (C-DEBI OCE-0939564) also supported the participation of J.A.H. and P.D.C. This is C-DEBI contribution number 564.
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    Reconciling evidence of oxidative weathering and atmospheric anoxia on Archean Earth (2021)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-05-27
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Johnson, A. C., Ostrander, C. M., Romaniello, S. J., Reinhard, C. T., Greaney, A. T., Lyons, T. W., & Anbar, A. D. Reconciling evidence of oxidative weathering and atmospheric anoxia on Archean Earth. Science Advances, 7(40), (2021): eabj0108, https://doi.org/10.1126/sciadv.abj0108.
    Description: Evidence continues to emerge for the production and low-level accumulation of molecular oxygen (O2) at Earth’s surface before the Great Oxidation Event. Quantifying this early O2 has proven difficult. Here, we use the distribution and isotopic composition of molybdenum in the ancient sedimentary record to quantify Archean Mo cycling, which allows us to calculate lower limits for atmospheric O2 partial pressures (PO2) and O2 production fluxes during the Archean. We consider two end-member scenarios. First, if O2 was evenly distributed throughout the atmosphere, then PO2 〉 10–6.9 present atmospheric level was required for large periods of time during the Archean eon. Alternatively, if O2 accumulation was instead spatially restricted (e.g., occurring only near the sites of O2 production), then O2 production fluxes 〉0.01 Tmol O2/year were required. Archean O2 levels were vanishingly low according to our calculations but substantially above those predicted for an abiotic Earth system.
    Description: We would like to thank our funding sources, including FESD “Dynamics of Earth System Oxygenation” (NSF EAR 1338810 to A.D.A.), NASA Earth and Space Science Fellowship awarded to A.C.J. (80NSSC17K0498), NSF EAR PF to A.C.J. (1952809), and WHOI Postdoctoral Fellowship to C.M.O. C.T.R. acknowledges support from the NASA Astrobiology Institute. We also acknowledge support from the Metal Utilization and Selection across Eons (MUSE) Interdisciplinary Consortium for Astrobiology Research, sponsored by the National Aeronautics and Space Administration Science Mission Directorate (19-ICAR19_2-0007).
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    Fossil records of early solar irradiation and cosmolocation of the CAI factory: a reappraisal (2021)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-05-27
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Bekaert, D. V., Auro, M., Shollenberger, Q. R., Liu, M.-C., Marschall, H., Burton, K. W., Jacobsen, B., Brennecka, G. A., McPherson, G. J., von Mutius, R., Sarafian, A., & Nielsen, S. G. Fossil records of early solar irradiation and cosmolocation of the CAI factory: a reappraisal. Science Advances, 7(40), (2021): eabg8329, https://doi.org/10.1126/sciadv.abg8329.
    Description: Calcium-aluminum–rich inclusions (CAIs) in meteorites carry crucial information about the environmental conditions of the nascent Solar System prior to planet formation. Based on models of 50V–10Be co-production by in-situ irradiation, CAIs are considered to have formed within ~0.1 AU from the proto-Sun. Here, we present vanadium (V) and strontium (Sr) isotopic co-variations in fine- and coarse-grained CAIs and demonstrate that kinetic isotope effects during partial condensation and evaporation best explain V isotope anomalies previously attributed to solar particle irradiation. We also report initial excesses of 10Be and argue that CV CAIs possess essentially a homogeneous level of 10Be, inherited during their formation. Based on numerical modeling of 50V–10Be co-production by irradiation, we show that CAI formation during protoplanetary disk build-up likely occurred at greater heliocentric distances than previously considered, up to planet-forming regions (~1AU), where solar particle fluxes were sufficiently low to avoid substantial in-situ irradiation of CAIs.
    Description: This study was funded by NASA Emerging Worlds grant NNX16AD36G to S.G.N. and prepared by LLNL under contract DE-AC52-07NA27344 with release number LLNL-JRNL-819045. M.C.L acknowledges the support by the NASA grant 80NSSC20K0759. The UCLA ion microprobe facility is partially supported by a grant from the NSF Instrumentation and Facilities program.
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    A global environmental crisis 42,000 years ago (2021)
    American Association for the Advancement of Science
    In:  EPIC3Science, American Association for the Advancement of Science, 371(6531), pp. 811-818
    Details
    Publication Date: 2022-10-01
    Description: Geological archives record multiple reversals of Earth's magnetic poles, but the global impacts of these events, if any, remain unclear. Uncertain radiocarbon calibration has limited investigation of the potential effects of the last major magnetic inversion, known as the Laschamps Excursion 41 to 42 thousand years ago (ka). We use ancient New Zealand kauri trees (Agathis australis) to develop a detailed record of atmospheric radiocarbon levels across the Laschamps Excursion. We precisely characterize the geomagnetic reversal and perform global chemistry-climate modeling and detailed radiocarbon dating of paleoenvironmental records to investigate impacts. We find that geomagnetic field minima ~42 ka, in combination with Grand Solar Minima, caused substantial changes in atmospheric ozone concentration and circulation, driving synchronous global climate shifts that caused major environmental changes, extinction events, and transformations in the archaeological record.
    Repository Name: EPIC Alfred Wegener Institut
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    Crystal aggregates record the pre-eruptive flow field in the volcanic conduit at Kilauea, Hawaii (2021)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-05-26
    Description: © The Author(s), 2020. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in DiBenedetto, M., Qin, Z., & Suckale, J. Crystal aggregates record the pre-eruptive flow field in the volcanic conduit at Kilauea, Hawaii. Science Advances, 6(49), (2020): eabd4850, doi:10.1126/sciadv.abd4850.
    Description: Developing reliable, quantitative conduit models that capture the physical processes governing eruptions is hindered by our inability to observe conduit flow directly. The closest we get to direct evidence is testimony imprinted on individual crystals or bubbles in the conduit and preserved by quenching during the eruption. For example, small crystal aggregates in products of the 1959 eruption of Kīlauea Iki, Hawaii contain overgrown olivines separated by large, hydrodynamically unfavorable angles. The common occurrence of these aggregates calls for a flow mechanism that creates this crystal misorientation. Here, we show that the observed aggregates are the result of exposure to a steady wave field in the conduit through a customized, process-based model at the scale of individual crystals. We use this model to infer quantitative attributes of the flow at the time of aggregate formation; notably, the formation of misoriented aggregates is only reproduced in bidirectional, not unidirectional, conduit flow.
    Description: M.D. acknowledges support the Stanford Gerald J. Lieberman Fellowship and the Postdoctoral Scholarship from Woods Hole Oceanographic Institution.
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    Small-molecule mimicry hunting strategy in the imperial cone snail, Conus imperialis (2021)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-05-26
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Torres, J. P., Lin, Z., Watkins, M., Salcedo, P. F., Baskin, R. P., Elhabian, S., Safavi-Hemami, H., Taylor, D., Tun, J., Concepcion, G. P., Saguil, N., Yanagihara, A. A., Fang, Y., McArthur, J. R., Tae, H. S., Finol-Urdaneta, R. K., Özpolat, B. D., Olivera, B. M., & Schmidt, E. W. Small-molecule mimicry hunting strategy in the imperial cone snail, Conus imperialis. Science Advances, 7(11), (2021): eabf2704, https://doi.org/10.1126/sciadv.abf2704.
    Description: Venomous animals hunt using bioactive peptides, but relatively little is known about venom small molecules and the resulting complex hunting behaviors. Here, we explored the specialized metabolites from the venom of the worm-hunting cone snail, Conus imperialis. Using the model polychaete worm Platynereis dumerilii, we demonstrate that C. imperialis venom contains small molecules that mimic natural polychaete mating pheromones, evoking the mating phenotype in worms. The specialized metabolites from different cone snails are species-specific and structurally diverse, suggesting that the cones may adopt many different prey-hunting strategies enabled by small molecules. Predators sometimes attract prey using the prey’s own pheromones, in a strategy known as aggressive mimicry. Instead, C. imperialis uses metabolically stable mimics of those pheromones, indicating that, in biological mimicry, even the molecules themselves may be disguised, providing a twist on fake news in chemical ecology.
    Description: Research reported in this publication was supported by NIH R35GM12252, with contributions to biological work from NIH Fogarty International Center U19TW008163, NIH P01GM48677, and DOD CDMRP W81XWH-17-1-0413. The content is solely the responsibility of the authors and does not necessarily represent the official views of the NIH.
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    Thermal stress reduces pocilloporid coral resilience to ocean acidification by impairing control over calcifying fluid chemistry (2021)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-05-26
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Guillermic, M., Cameron, L. P., De Corte, I., Misra, S., Bijma, J., de Beer, D., Reymond, C. E., Westphal, H., Ries, J. B., & Eagle, R. A. Thermal stress reduces pocilloporid coral resilience to ocean acidification by impairing control over calcifying fluid chemistry. Science Advances, 7(2), (2021): eaba9958, https://doi.org/10.1126/sciadv.aba9958.
    Description: The combination of thermal stress and ocean acidification (OA) can more negatively affect coral calcification than an individual stressors, but the mechanism behind this interaction is unknown. We used two independent methods (microelectrode and boron geochemistry) to measure calcifying fluid pH (pHcf) and carbonate chemistry of the corals Pocillopora damicornis and Stylophora pistillata grown under various temperature and pCO2 conditions. Although these approaches demonstrate that they record pHcf over different time scales, they reveal that both species can cope with OA under optimal temperatures (28°C) by elevating pHcf and aragonite saturation state (Ωcf) in support of calcification. At 31°C, neither species elevated these parameters as they did at 28°C and, likewise, could not maintain substantially positive calcification rates under any pH treatment. These results reveal a previously uncharacterized influence of temperature on coral pHcf regulation—the apparent mechanism behind the negative interaction between thermal stress and OA on coral calcification.
    Description: R.A.E. and J.B.R. acknowledge support from National Science Foundation grants OCE-1437166 and OCE-1437371. The work was also supported by the “Laboratoire d’Excellence” LabexMER (ANR-10-LABX-19), cofunded by a grant from the French government under the program “Investissements d’Avenir,” and an IAGC student grant 2017. R.A.E. acknowledges financial and logistical support from the Pritzker Endowment to UCLA IoES, and J.B.R. acknowledges support from the ZMT and the Hanse-Wissenschaftskolleg Fellowship Program and the NSF OCE award #1437371.
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    Offshore pelagic subsidies dominate carbon inputs to coral reef predators (2021)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-05-26
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Skinner, C., Mill, A. C., Fox, M. D., Newman, S. P., Zhu, Y., Kuhl, A., & Polunin, N. V. C. Offshore pelagic subsidies dominate carbon inputs to coral reef predators. Science Advances, 7(8), (2021): eabf3792, https://doi.org/10.1126/sciadv.abf3792.
    Description: Coral reefs were traditionally perceived as productive hot spots in oligotrophic waters. While modern evidence indicates that many coral reef food webs are heavily subsidized by planktonic production, the pathways through which this occurs remain unresolved. We used the analytical power of carbon isotope analysis of essential amino acids to distinguish between alternative carbon pathways supporting four key reef predators across an oceanic atoll. This technique separates benthic versus planktonic inputs, further identifying two distinct planktonic pathways (nearshore reef-associated plankton and offshore pelagic plankton), and revealing that these reef predators are overwhelmingly sustained by offshore pelagic sources rather than by reef sources (including reef-associated plankton). Notably, pelagic reliance did not vary between species or reef habitats, emphasizing that allochthonous energetic subsidies may have system-wide importance. These results help explain how coral reefs maintain exceptional productivity in apparently nutrient-poor tropical settings, but also emphasize their susceptibility to future ocean productivity fluctuations.
    Description: Sample analysis funding was provided by NERC LSMSF grant BRIS/102/0717 and BRIS/125/1418. C.S. was supported by a Newcastle University SAgE DTA studentship and a cooperative agreement with Banyan Tree.
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    Quantification of amine- and alcohol-containing metabolites in saline samples using pre-extraction benzoyl chloride derivatization and ultrahigh performance liquid chromatography tandem mass spectrometry (UHPLC MS/MS) (2021)
    American Chemical Society
    Details
    Publication Date: 2022-05-26
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Widner, B., Kido Soule, M. C., Ferrer-González, F. X., Moran, M. A., & Kujawinski, E. B. Quantification of amine- and alcohol-containing metabolites in saline samples using pre-extraction benzoyl chloride derivatization and ultrahigh performance liquid chromatography tandem mass spectrometry (UHPLC MS/MS). Analytical Chemistry, 93(11), (2021): 4809-4817, https://doi.org/10.1021/acs.analchem.0c03769.
    Description: Dissolved metabolites serve as nutrition, energy, and chemical signals for microbial systems. However, the full scope and magnitude of these processes in marine systems are unknown, largely due to insufficient methods, including poor extraction of small, polar compounds using common solid-phase extraction resins. Here, we utilized pre-extraction derivatization and ultrahigh performance liquid chromatography electrospray ionization tandem mass spectrometry (UHPLC-ESI-MS/MS) to detect and quantify targeted dissolved metabolites in seawater and saline culture media. Metabolites were derivatized with benzoyl chloride by their primary and secondary amine and alcohol functionalities and quantified using stable isotope-labeled internal standards (SIL-ISs) produced from 13C6-labeled benzoyl chloride. We optimized derivatization, extraction, and sample preparation for field and culture samples and evaluated matrix-derived biases. We have optimized this quantitative method for 73 common metabolites, of which 50 cannot be quantified without derivatization due to low extraction efficiencies. Of the 73 metabolites, 66 were identified in either culture media or seawater and 45 of those were quantified. This derivatization method is sensitive (detection limits = pM to nM), rapid (∼5 min per sample), and high throughput.
    Description: Funding included the Gordon and Betty Moore Foundation (Award GBMF5503 to M.A.M. and E.B.K.), Simons Foundation International (Award 409923 to E.B.K.), and the National Science Foundation (Award 1656311 to M.A.M.).
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    Flow-through quantification of microplastics using impedance spectroscopy (2021)
    American Chemical Society
    Details
    Publication Date: 2022-10-21
    Description: © The Author(s), 2021. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Colson, B. C., & Michel, A. P. M. Flow-through quantification of microplastics using impedance spectroscopy. ACS Sensors, 6(1), (2021): 238–244, doi:10.1021/acssensors.0c02223.
    Description: Understanding the sources, impacts, and fate of microplastics in the environment is critical for assessing the potential risks of these anthropogenic particles. However, our ability to quantify and identify microplastics in aquatic ecosystems is limited by the lack of rapid techniques that do not require visual sorting or preprocessing. Here, we demonstrate the use of impedance spectroscopy for high-throughput flow-through microplastic quantification, with the goal of rapid measurement of microplastic concentration and size. Impedance spectroscopy characterizes the electrical properties of individual particles directly in the flow of water, allowing for simultaneous sizing and material identification. To demonstrate the technique, spike and recovery experiments were conducted in tap water with 212–1000 μm polyethylene beads in six size ranges and a variety of similarly sized biological materials. Microplastics were reliably detected, sized, and differentiated from biological materials via their electrical properties at an average flow rate of 103 ± 8 mL/min. The recovery rate was ≥90% for microplastics in the 300–1000 μm size range, and the false positive rate for the misidentification of the biological material as plastic was 1%. Impedance spectroscopy allowed for the identification of microplastics directly in water without visual sorting or filtration, demonstrating its use for flow-through sensing.
    Description: The authors thank the Richard Saltonstall Charitable Foundation and the National Academies Keck Futures Initiative (NAKFI DBS13) for their funding support.
    Keywords: Microplastics ; Plastics ; Impedance spectroscopy ; Dielectric properties ; Instrumentation ; Particle detection ; Flow-through ; Environmental sensing
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  • 25
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    Differences in Leaf Chemistry and Glandular Trichome Density between Wild Southwestern American Hop ( Humulus neomexicanus ) and Commercial Hop Cultivars (2021)
    American Chemical Society
    In:  Journal of Agricultural and Food Chemistry, 69 (27). pp. 7798-7814.
    Details
    Publication Date: 2022-01-07
    Description: The female flowers (“cones”) of the hop plant (Humulus L.) produce compounds that contribute to the flavor and other properties of beer. Hop leaves and cones produce many of the same compounds, which also confer agronomic traits such as insect and disease resistance. Targeted and untargeted ultraperformance liquid chromatography-quadrupole time-of-flight–mass spectrometry with Waters MSE technology (UPLC-QTof-MSE) metabolomics were used to compare leaf phytochemical compositions of greenhouse-grown southwestern American wild Humulus neomexicanus (A. Nelson and Cockerell) Rydb. against a group of commercial hop cultivars consisting of both pure European Humulus lupulus L. and European–North American hybrids. Principal component analysis showed a clear distinction in chemical profiles between the two groups. H. neomexicanus leaves had a significantly higher content of total α acids (p = 4.4 × 10–9), total bitter acids (p = 2.6 × 10–6), cohumulone (p = 1.0 × 10–13), humulone + adhumulone (p = 9.1 × 10–4), and the prenylflavonoids xanthohumol (p = 0.013) and desmethylxanthohumol (p = 0.029) as well as significantly higher densities of glandular trichomes (p = 1.3 × 10–6), the biosynthetic site of those compounds. Most flavonol glycosides measured were also significantly more abundant in H. neomexicanus (p = 1.5 × 10–22 to 0.0027), whereas phenolic acids were consistently, but generally nonsignificantly (p 〉 0.05), more abundant in the cultivars. The higher bitter acid, prenylflavonoid, and flavonol glycoside content of H. neomexicanus leaves may help to confer more favorable insect and disease-resistance properties.
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    Iron Acquisition Systems of Gram-negative Bacterial Pathogens Define TonB-Dependent Pathways to Novel Antibiotics (2021)
    American Chemical Society
    In:  Chemical Reviews, 121 (9). pp. 5193-5239.
    Details
    Publication Date: 2022-01-07
    Description: Iron is an indispensable metabolic cofactor in both pro- and eukaryotes, which engenders a natural competition for the metal between bacterial pathogens and their human or animal hosts. Bacteria secrete siderophores that extract Fe3+ from tissues, fluids, cells, and proteins; the ligand gated porins of the Gram-negative bacterial outer membrane actively acquire the resulting ferric siderophores, as well as other iron-containing molecules like heme. Conversely, eukaryotic hosts combat bacterial iron scavenging by sequestering Fe3+ in binding proteins and ferritin. The variety of iron uptake systems in Gram-negative bacterial pathogens illustrates a range of chemical and biochemical mechanisms that facilitate microbial pathogenesis. This document attempts to summarize and understand these processes, to guide discovery of immunological or chemical interventions that may thwart infectious disease.
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    Synthase-Selective Exploration of a Tunicate Microbiome by Activity-Guided Single-Cell Genomics (2021)
    American Chemical Society
    In:  ACS Chemical Biology .
    Details
    Publication Date: 2022-01-07
    Description: While thousands of environmental metagenomes have been mined for the presence of novel biosynthetic gene clusters, such computational predictions do not provide evidence of their in vivo biosynthetic functionality. Using fluorescent in situ enzyme assay targeting carrier proteins common to polyketide (PKS) and nonribosomal peptide synthetases (NRPS), we applied fluorescence-activated cell sorting to tunicate microbiome to enrich for microbes with active secondary metabolic capabilities. Single-cell genomics uncovered the genetic basis for a wide biosynthetic diversity in the enzyme-active cells and revealed a member of marine Oceanospirillales harboring a novel NRPS gene cluster with high similarity to phylogenetically distant marine and terrestrial bacteria. Interestingly, this synthase belongs to a larger class of siderophore biosynthetic gene clusters commonly associated with pestilence and disease. This demonstrates activity-guided single-cell genomics as a tool to guide novel biosynthetic discovery.
    Type: Article , PeerReviewed
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    Future climate response to Antarctic Ice Sheet melt caused by anthropogenic warming (2020)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-05-25
    Description: © The Author(s), 2020. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Sadai, S., Condron, A., DeConto, R., & Pollard, D. Future climate response to Antarctic Ice Sheet melt caused by anthropogenic warming. Science Advances, 6(39), (2020): eaaz1169, doi:10.1126/sciadv.aaz1169.
    Description: Meltwater and ice discharge from a retreating Antarctic Ice Sheet could have important impacts on future global climate. Here, we report on multi-century (present–2250) climate simulations performed using a coupled numerical model integrated under future greenhouse-gas emission scenarios IPCC RCP4.5 and RCP8.5, with meltwater and ice discharge provided by a dynamic-thermodynamic ice sheet model. Accounting for Antarctic discharge raises subsurface ocean temperatures by 〉1°C at the ice margin relative to simulations ignoring discharge. In contrast, expanded sea ice and 2° to 10°C cooler surface air and surface ocean temperatures in the Southern Ocean delay the increase of projected global mean anthropogenic warming through 2250. In addition, the projected loss of Arctic winter sea ice and weakening of the Atlantic Meridional Overturning Circulation are delayed by several decades. Our results demonstrate a need to accurately account for meltwater input from ice sheets in order to make confident climate predictions.
    Description: This research was supported by the NSF Office of Polar Programs through NSF grant 1443347, the Biological and Environmental Research (BER) division of the U.S. Department of Energy through grant DE-SC0019263, the NSF through ICER 1664013, and by a grant to the NASA Sea Level Science Team 80NSSC17K0698.
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    A continuous pathway for fresh water along the East Greenland shelf (2020)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-05-25
    Description: © The Author(s), 2020. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Foukal, N. P., Gelderloos, R., & Pickart, R. S. A continuous pathway for fresh water along the East Greenland shelf. Science Advances, 6(43), (2020): eabc4254, doi:10.1126/sciadv.abc4254.
    Description: Export from the Arctic and meltwater from the Greenland Ice Sheet together form a southward-flowing coastal current along the East Greenland shelf. This current transports enough fresh water to substantially alter the large-scale circulation of the North Atlantic, yet the coastal current’s origin and fate are poorly known due to our lack of knowledge concerning its north-south connectivity. Here, we demonstrate how the current negotiates the complex topography of Denmark Strait using in situ data and output from an ocean circulation model. We determine that the coastal current north of the strait supplies half of the transport to the coastal current south of the strait, while the other half is sourced from offshore via the shelfbreak jet, with little input from the Greenland Ice Sheet. These results indicate that there is a continuous pathway for Arctic-sourced fresh water along the entire East Greenland shelf from Fram Strait to Cape Farewell.
    Description: Funding for this work comes from the NSF under grant numbers OCE-1756361 and OCE-1558742 (N.P.F. and R.S.P.) and grant numbers OCE-1756863 and OAC-1835640 (R.G.).
    Repository Name: Woods Hole Open Access Server
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    AutoTuner: high fidelity and robust parameter selection for metabolomics data processing (2020)
    American Chemical Society
    Details
    Publication Date: 2022-05-26
    Description: © The Author(s), 2020. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in McLean, C., & Kujawinski, E. B. AutoTuner: high fidelity and robust parameter selection for metabolomics data processing. Analytical Chemistry, 92(8), (2020): 5724-5732, doi:10.1021/acs.analchem.9b04804.
    Description: Untargeted metabolomics experiments provide a snapshot of cellular metabolism but remain challenging to interpret due to the computational complexity involved in data processing and analysis. Prior to any interpretation, raw data must be processed to remove noise and to align mass-spectral peaks across samples. This step requires selection of dataset-specific parameters, as erroneous parameters can result in noise inflation. While several algorithms exist to automate parameter selection, each depends on gradient descent optimization functions. In contrast, our new parameter optimization algorithm, AutoTuner, obtains parameter estimates from raw data in a single step as opposed to many iterations. Here, we tested the accuracy and the run-time of AutoTuner in comparison to isotopologue parameter optimization (IPO), the most commonly used parameter selection tool, and compared the resulting parameters’ influence on the properties of feature tables after processing. We performed a Monte Carlo experiment to test the robustness of AutoTuner parameter selection and found that AutoTuner generated similar parameter estimates from random subsets of samples. We conclude that AutoTuner is a desirable alternative to existing tools, because it is scalable, highly robust, and very fast (∼100–1000× speed improvement from other algorithms going from days to minutes). AutoTuner is freely available as an R package through BioConductor.
    Description: We thank Titus Brown and Ben Temperton for advice on the algorithm validation, Arthur Eschenlauer for constructive feedback on the software design, Krista Longnecker for continuous support and discussions, Gabriel Leventhal for mathematics advice, the users of AutoTuner for debugging help through Github, and David Angeles-Albores and two anonymous reviewers for critical feedback on the manuscript. Funding support included the National GEM Consortium and NSF graduate research program fellowships (C.M.) and grants from the MIT Microbiome Center (Award 6936800, E.B.K.) and the Simons Foundation (Award ID #509034, E.B.K.).
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    The Ah receptor: adaptive metabolism, ligand diversity, and the xenokine model (2020)
    American Chemical Society
    Details
    Publication Date: 2022-05-26
    Description: Author Posting. © American Chemical Society, 2020. This is an open access article published under an ACS AuthorChoice License. The definitive version was published in Chemical Research in Toxicology, 33(4), (2020): 860-879, doi:10.1021/acs.chemrestox.9b00476.
    Description: The Ah receptor (AHR) has been studied for almost five decades. Yet, we still have many important questions about its role in normal physiology and development. Moreover, we still do not fully understand how this protein mediates the adverse effects of a variety of environmental pollutants, such as the polycyclic aromatic hydrocarbons (PAHs), the chlorinated dibenzo-p-dioxins (“dioxins”), and many polyhalogenated biphenyls. To provide a platform for future research, we provide the historical underpinnings of our current state of knowledge about AHR signal transduction, identify a few areas of needed research, and then develop concepts such as adaptive metabolism, ligand structural diversity, and the importance of proligands in receptor activation. We finish with a discussion of the cognate physiological role of the AHR, our perspective on why this receptor is so highly conserved, and how we might think about its cognate ligands in the future.
    Description: This review is dedicated in memory of the career of Alan Poland, one of the truly great minds in pharmacology and toxicology. This work was supported by the National Institutes of Health Grants R35-ES028377, T32-ES007015, P30-CA014520, P42-ES007381, and U01-ES1026127, The UW SciMed GRS Program, and The Morgridge Foundation. The authors would like to thank Catherine Stanley of UW Media Solutions for her artwork.
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    The role of northeast pacific meltwater events in deglacial climate change (2020)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-05-26
    Description: © The Author(s), 2020. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Praetorius, S. K., Condron, A., Mix, A. C., Walczak, M. H., McKay, J. L., & Du, J. The role of northeast pacific meltwater events in deglacial climate change. Science Advances, 6(9), (2020): eaay2915, doi:10.1126/sciadv.aay2915.
    Description: Columbia River megafloods occurred repeatedly during the last deglaciation, but the impacts of this fresh water on Pacific hydrography are largely unknown. To reconstruct changes in ocean circulation during this period, we used a numerical model to simulate the flow trajectory of Columbia River megafloods and compiled records of sea surface temperature, paleo-salinity, and deep-water radiocarbon from marine sediment cores in the Northeast Pacific. The North Pacific sea surface cooled and freshened during the early deglacial (19.0-16.5 ka) and Younger Dryas (12.9-11.7 ka) intervals, coincident with the appearance of subsurface water masses depleted in radiocarbon relative to the sea surface. We infer that Pacific meltwater fluxes contributed to net Northern Hemisphere cooling prior to North Atlantic Heinrich Events, and again during the Younger Dryas stadial. Abrupt warming in the Northeast Pacific similarly contributed to hemispheric warming during the Bølling and Holocene transitions. These findings underscore the importance of changes in North Pacific freshwater fluxes and circulation in deglacial climate events.
    Description: The research was partly supported by the NSF through grants ARC-257 1204045 and PLR-1417667. The numerical model simulations used resources from the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility operated under contract no. DE-AC02-05CH11231.
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    The United States' contribution of plastic waste to land and ocean (2020)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-05-26
    Description: © The Author(s), 2020. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Law, K. L., Starr, N., Siegler, T. R., Jambeck, J. R., Mallos, N. J., & Leonard, G. H. The United States' contribution of plastic waste to land and ocean. Science Advances, 6(44), (2020): eabd0288, doi:10.1126/sciadv.abd0288.
    Description: Plastic waste affects environmental quality and ecosystem health. In 2010, an estimated 5 to 13 million metric tons (Mt) of plastic waste entered the ocean from both developing countries with insufficient solid waste infrastructure and high-income countries with very high waste generation. We demonstrate that, in 2016, the United States generated the largest amount of plastic waste of any country in the world (42.0 Mt). Between 0.14 and 0.41 Mt of this waste was illegally dumped in the United States, and 0.15 to 0.99 Mt was inadequately managed in countries that imported materials collected in the United States for recycling. Accounting for these contributions, the amount of plastic waste generated in the United States estimated to enter the coastal environment in 2016 was up to five times larger than that estimated for 2010, rendering the United States’ contribution among the highest in the world.
    Description: This work was funded by Ocean Conservancy through support from the Arthur Vining Davis Foundations.
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    An early cretaceous subduction-modified mantle underneath the ultraslow spreading Gakkel Ridge, Arctic Ocean (2020)
    American Association for the Advancement of Science
    Details
    Publication Date: 2022-05-26
    Description: © The Author(s), 2020. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Richter, M., Nebel, O., Maas, R., Mather, B., Nebel-Jacobsen, Y., Capitanio, F. A., Dick, H. J. B., & Cawood, P. A. An early cretaceous subduction-modified mantle underneath the ultraslow spreading Gakkel Ridge, Arctic Ocean. Science Advances, 6(44), (2020): eabb4340, doi:10.1126/sciadv.abb4340.
    Description: Earth’s upper mantle, as sampled by mid-ocean ridge basalts (MORBs) at oceanic spreading centers, has developed chemical and isotopic heterogeneity over billions of years through focused melt extraction and re-enrichment by recycled crustal components. Chemical and isotopic heterogeneity of MORB is dwarfed by the large compositional spectrum of lavas at convergent margins, identifying subduction zones as the major site for crustal recycling into and modification of the mantle. The fate of subduction-modified mantle and if this heterogeneity transmits into MORB chemistry remains elusive. Here, we investigate the origin of upper mantle chemical heterogeneity underneath the Western Gakkel Ridge region in the Arctic Ocean through MORB geochemistry and tectonic plate reconstruction. We find that seafloor lavas from the Western Gakkel Ridge region mirror geochemical signatures of an Early Cretaceous, paleo-subduction zone, and conclude that the upper mantle can preserve a long-lived, stationary geochemical memory of past geodynamic processes.
    Description: O.N. was supported by the Australian Research Council (grant FT140101062). P.A.C. was supported by the Australian Research Council (grant FL160100168). H.J.B.D. was supported by the NSF (grants PLR 9912162, PLR 0327591, OCE 0930487, and OCE 1434452). M.R. was supported by a graduate scholarship of Monash University and the SEAE.
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    Genetic and Biochemical Reconstitution of Bromoform Biosynthesis in Asparagopsis Lends Insights into Seaweed Reactive Oxygen Species Enzymology (2020)
    American Chemical Society
    In:  ACS Chemical Biology, 15 (6). pp. 1662-1670.
    Details
    Publication Date: 2022-01-07
    Description: Marine macroalgae, seaweeds, are exceptionally prolific producers of halogenated natural products. Biosynthesis of halogenated molecules in seaweeds is inextricably linked to reactive oxygen species (ROS) signaling as hydrogen peroxide serves as a substrate for haloperoxidase enzymes that participate in the construction these halogenated molecules. Here, using red macroalga Asparagopsis taxiformis, a prolific producer of the ozone depleting molecule bromoform, we provide the discovery and biochemical characterization of a ROS-producing NAD(P)H oxidase from seaweeds. This discovery was enabled by our sequencing of Asparagopsis genomes, in which we find the gene encoding the ROS-producing enzyme to be clustered with genes encoding bromoform-producing haloperoxidases. Biochemical reconstitution of haloperoxidase activities establishes that fatty acid biosynthesis can provide viable hydrocarbon substrates for bromoform production. The ROS production haloperoxidase enzymology that we describe here advances seaweed biology and biochemistry by providing the molecular basis for decades worth of physiological observations in ROS and halogenated natural product biosyntheses.
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    Mass Spectrometry-Based Metabolomics Reveals a Concurrent Action of Several Chemical Mechanisms in Arabidopsis-Fusarium oxysporum Compatible and Incompatible Interactions (2020)
    American Chemical Society
    In:  Journal of Agricultural and Food Chemistry, 68 (51). pp. 15335-15344.
    Details
    Publication Date: 2022-01-07
    Description: Fusarium oxysporum is a destructive root-infecting plant pathogen that causes significant yield losses in many economically important crop species. Hence, a deeper understanding of pathogen infection strategies is needed. With liquid chromatography-tandem mass spectrometry and gas chromatography-time of flight mass spectrometry platforms, we analyzed the metabolic changes in a time-course experiment with Arabidopsis accessions either resistant (Col-0) or susceptible (Ler-0) to isolates of Fusarium oxysporum forma specialis matthioli infection. We showed a concurrent effect of Fusarium-derived polyols and the mycotoxin beauvericin in the suppression of the immune response of susceptible hosts. A significant increase in oxidized glutathione in the resistant host was probably associated with effective reactive oxygen species-mediated resistance responses. Through a combination of targeted and untargeted metabolomics, we demonstrated the concurrent action of several Arabidopsis defense systems as well as the concurrent action of several virulence systems in the fungal attack of susceptible Arabidopsis.
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