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  • 1
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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
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 2
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    Soothsaying DOM: A current perspective on the future of oceanic dissolved organic carbon (2020)
    Frontiers Media
    Details
    Publication Date: 2022-10-26
    Description: © The Author(s), 2020. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Wagner, S., Schubotz, F., Kaiser, K., Hallmann, C., Waska, H., Rossel, P. E., Hansmann, R., Elvert, M., Middelburg, J. J., Engel, A., Blattmann, T. M., Catala, T. S., Lennartz, S. T., Gomez-Saez, G., V., Pantoja-Gutierrez, S., Bao, R., & Galy, V. Soothsaying DOM: A current perspective on the future of oceanic dissolved organic carbon. Frontiers in Marine Science, 7, (2020): 341, doi:10.3389/fmars.2020.00341.
    Description: The vast majority of freshly produced oceanic dissolved organic carbon (DOC) is derived from marine phytoplankton, then rapidly recycled by heterotrophic microbes. A small fraction of this DOC survives long enough to be routed to the interior ocean, which houses the largest and oldest DOC reservoir. DOC reactivity depends upon its intrinsic chemical composition and extrinsic environmental conditions. Therefore, recalcitrance is an emergent property of DOC that is analytically difficult to constrain. New isotopic techniques that track the flow of carbon through individual organic molecules show promise in unveiling specific biosynthetic or degradation pathways that control the metabolic turnover of DOC and its accumulation in the deep ocean. However, a multivariate approach is required to constrain current carbon fluxes so that we may better predict how the cycling of oceanic DOC will be altered with continued climate change. Ocean warming, acidification, and oxygen depletion may upset the balance between the primary production and heterotrophic reworking of DOC, thus modifying the amount and/or composition of recalcitrant DOC. Climate change and anthropogenic activities may enhance mobilization of terrestrial DOC and/or stimulate DOC production in coastal waters, but it is unclear how this would affect the flux of DOC to the open ocean. Here, we assess current knowledge on the oceanic DOC cycle and identify research gaps that must be addressed to successfully implement its use in global scale carbon models.
    Description: This work was funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) project number 422798570. The Hanse-Wissenschaftskolleg and the Geochemical Society provided funding for the conference. Additional support was provided by the National Science Foundation OCE #1756812 to SW. TB acknowledges funding from ETH Zürich and JAMSTEC. JM was supported by the Netherlands Earth System Science Centre. SP-G was funded by COPAS Sur-Austral (CONICYT PIA APOYO CCTE AFB170006). GG-S acknowledges funding from DFG, DI 842/6-1.
    Keywords: Dissolved organic carbon ; Global carbon cycle ; Recalcitrance ; Isotopic probing ; Climate change
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 3
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    Non-breaking wave effects on buoyant particle distributions (2020)
    Frontiers Media
    Details
    Publication Date: 2022-10-26
    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. H. Non-breaking wave effects on buoyant particle distributions. Frontiers in Marine Science, 7, (2020): 148, doi:10.3389/fmars.2020.00148.
    Description: The dispersal of buoyant particles in the ocean mixed layer is influenced by a variety of physical factors including wind, waves, and turbulence. Microplastics observations are often made at the free surface, which is strongly forced by surface gravity waves. Many studies have used numerical simulations to examine how turbulence and wave effects (e.g., breaking waves, Langmuir circulation) control buoyant particle dispersal at the ocean surface. However these simulations are not wave phase-resolving. Therefore, the effects of an unsteady free surface due to surface gravity waves remain unknown in this context. To address this, we develop an analytical model for the distribution of buoyant particles as a function of wave-phase under wind-wave conditions in deep-water. Using this analytical model and complementary numerical simulations, we quantify the effects of a nonbreaking, monochromatic, progressive wave train on the equilibrium vertical and horizontal distributions of buoyant particles. We find that waves result in non-uniform horizontal distributions of particles with more particles under the wave crests than the troughs. We also find that the waves can stretch or compress the equilibrium vertical distribution. Finally, we consider the effects of waves on the sampling of microplastics with a towed net, and we show that waves have the ability to lower the measured concentrations relative to nets sampling without the influence of waves.
    Description: This work was supported by the Postdoctoral Scholar Program at the Woods Hole Oceanographic Institution, and by the US National Science Foundation under grant no. CBET-1706586.
    Keywords: Ocean waves ; Microplastics ; Particle distributions ; Sampling error ; Particle-laden flows ; Neuston nets
    Repository Name: Woods Hole Open Access Server
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  • 4
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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
    Repository Name: Woods Hole Open Access Server
    Type: Article
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