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  • 1
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    Nitrogen cycling in sediments on the NW African margin inferred from N and O isotopes in benthic chambers (2022)
    Frontiers
    Details
    Publication Date: 2024-02-07
    Description: Benthic nitrogen cycling in the Mauritanian upwelling region (NW Africa) was studied in June 2014 from the shelf to the upper slope where minimum bottom water O 2 concentrations of 25 µM were recorded. Benthic incubation chambers were deployed at 9 stations to measure fluxes of O 2 , dissolved inorganic carbon (DIC) and nutrients (NO 3 - , NO 2 - , NH 4 + , PO 4 3- , H 4 SiO 4 ) along with the N and O isotopic composition of nitrate (δ 15 N-NO 3 - and δ 18 O-NO 3 - ) and ammonium (δ 15 N-NH 4 + ). O 2 and DIC fluxes were similar to those measured during a previous campaign in 2011 whereas NH 4 + and PO 4 3- fluxes on the shelf were 2 – 3 times higher and possibly linked to a long-term decline in bottom water O 2 concentrations. The mean isotopic fractionation of NO 3 - uptake on the margin, inferred from the loss of NO 3 - inside the chambers, was 1.5 ± 0.4 ‰ for 15/14 N ( 15 ϵ app ) and 2.0 ± 0.5 ‰ for 18/16 O ( 18 ϵ app ). The mean 18 ϵ app : 15 ϵ app ratio on the shelf (〈 100 m) was 2.1 ± 0.3, and higher than the value of 1 expected for microbial NO 3 - reduction. The 15 ϵ app are similar to previously reported isotope effects for NO 3 - respiration in marine sediments but lower than determined in 2011 at a same site on the shelf. The sediments were also a source of 15 N-enriched NH 4 + (9.0 ± 0.7 ‰). A numerical model tuned to the benthic flux data and that specifically accounts for the efflux of 15 N-enriched NH 4 + from the seafloor, predicted a net benthic isotope effect of N loss ( 15 ϵ sed ) of 3.6 ‰; far above the more widely considered value of ~0‰. This result is further evidence that the assumption of a universally low or negligible benthic N isotope effect is not applicable to oxygen-deficient settings. The model further suggests that 18 ϵ app : 15 ϵ app trajectories > 1 in the benthic chambers are most likely due to aerobic ammonium oxidation and nitrite oxidation in surface sediments rather than anammox, in agreement with published observations in the water column of oxygen deficient regions.
    Type: Article , PeerReviewed
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    OceanRep: Article in a Scientific Journal - peer-reviewed
  • 2
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    Design optimization of a submersible chemiluminescent sensor (DISCO) for improved quantification of reactive oxygen species (ROS) in surface waters (2023)
    MDPI
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    Publication Date: 2023-03-08
    Description: © The Author(s), 2022. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Grabb, K., Pardis, W., Kapit, J., Wankel, S., Hayden, E., & Hansel, C. Design optimization of a submersible chemiluminescent sensor (DISCO) for improved quantification of reactive oxygen species (ROS) in surface waters. Sensors, 22(17), (2022): 6683, https://doi.org/10.3390/s22176683.
    Description: Reactive oxygen species (ROS) are key drivers of biogeochemical cycling while also exhibiting both positive and negative effects on marine ecosystem health. However, quantification of the ROS superoxide (O2−) within environmental systems is hindered by its short half-life. Recently, the development of the diver-operated submersible chemiluminescent sensor (DISCO), a submersible, handheld instrument, enabled in situ superoxide measurements in real time within shallow coral reef ecosystems. Here, we present a redesigned and improved instrument, DISCO II. Similar to the previous DISCO, DISCO II is a self-contained, submersible sensor, deployable to 30 m depth and capable of measuring reactive intermediate species in real time. DISCO II is smaller, lighter, lower cost, and more robust than its predecessor. Laboratory validation of DISCO II demonstrated an average limit of detection in natural seawater of 133.1 pM and a percent variance of 0.7%, with stable photo multiplier tube (PMT) counts, internal temperature, and flow rates. DISCO II can also be optimized for diverse environmental conditions by adjustment of the PMT supply voltage and integration time. Field tests showed no drift in the data with a percent variance of 3.0%. Wand tip adaptations allow for in situ calibrations and decay rates of superoxide using a chemical source of superoxide (SOTS-1). Overall, DISCO II is a versatile, user-friendly sensor that enables measurements in diverse environments, thereby improving our understanding of the cycling of reactive intermediates, such as ROS, across various marine ecosystems.
    Description: The development and verification of DISCO was funded by Schmidt Marine Technology Partners (G-2010-59878 to C.M.H., S.D.W. and J.K.). This research was further supported, in part, by grants from NSF GRFP (2016230168 to K.C.G.), WHOI Ocean Ventures Fund (2020 and 2021 to K.C.G.), and the MIT Wellington and Irene Loh Fund Fellowship (4000111995 to K.C.G.).
    Keywords: Reactive oxygen species ; Superoxide ; Chemiluminescent ; In situ analysis ; Ocean sensor ; Corals
    Repository Name: Woods Hole Open Access Server
    Type: Article
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  • 3
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    Dark biological superoxide production as a significant flux and sink of marine dissolved oxygen (2020)
    National Academy of Sciences
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    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 Sutherland, K. M., Wankel, S. D., & Hansel, C. M. Dark biological superoxide production as a significant flux and sink of marine dissolved oxygen. Proceedings of the National Academy of Sciences of the United States of America, 117(7), (2020): 3433-3439, doi:10.1073/pnas.1912313117.
    Description: The balance between sources and sinks of molecular oxygen in the oceans has greatly impacted the composition of Earth’s atmosphere since the evolution of oxygenic photosynthesis, thereby exerting key influence on Earth’s climate and the redox state of (sub)surface Earth. The canonical source and sink terms of the marine oxygen budget include photosynthesis, respiration, photorespiration, the Mehler reaction, and other smaller terms. However, recent advances in understanding cryptic oxygen cycling, namely the ubiquitous one-electron reduction of O2 to superoxide by microorganisms outside the cell, remains unexplored as a potential player in global oxygen dynamics. Here we show that dark extracellular superoxide production by marine microbes represents a previously unconsidered global oxygen flux and sink comparable in magnitude to other key terms. We estimate that extracellular superoxide production represents a gross oxygen sink comprising about a third of marine gross oxygen production, and a net oxygen sink amounting to 15 to 50% of that. We further demonstrate that this total marine dark extracellular superoxide flux is consistent with concentrations of superoxide in marine environments. These findings underscore prolific marine sources of reactive oxygen species and a complex and dynamic oxygen cycle in which oxygen consumption and corresponding carbon oxidation are not necessarily confined to cell membranes or exclusively related to respiration. This revised model of the marine oxygen cycle will ultimately allow for greater reconciliation among estimates of primary production and respiration and a greater mechanistic understanding of redox cycling in the ocean.
    Description: This work was supported by NASA Earth and Space Science Fellowship NNX15AR62H to K.M.S., NASA Exobiology grant NNX15AM04G to S.D.W. and C.M.H., and NSF Division of Ocean Sciences grant 1355720 to C.M.H. This research was further supported in part by Hanse-Wissenschaftskolleg Institute of Advanced Study fellowships to C.M.H. and S.D.W. We thank Danielle Hicks for assistance with figures and Community Earth Systems Model (CESM) Large Ensemble Project for the availability and use of its data product. The CESM project is primarily supported by the NSF.
    Keywords: Microbial superoxide ; Reactive oxygen species ; Marine dissolved oxygen
    Repository Name: Woods Hole Open Access Server
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  • 4
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    Development of a deep-sea submersible chemiluminescent analyzer for sensing short-lived reactive chemicals (2022)
    MDPI
    Details
    Publication Date: 2022-10-20
    Description: © The Author(s), 2022. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Taenzer, L., Grabb, K., Kapit, J., Pardis, W., Wankel, S. D., & Hansel, C. M. Development of a deep-sea submersible chemiluminescent analyzer for sensing short-lived reactive chemicals. Sensors, 22(5), (2022): 1709, https://doi.org/10.3390/s22051709.
    Description: Based on knowledge of their production pathways, and limited discrete observations, a variety of short-lived chemical species are inferred to play active roles in chemical cycling in the sea. In some cases, these species may exert a disproportionate impact on marine biogeochemical cycles, affecting the redox state of metal and carbon, and influencing the interaction between organisms and their environment. One such short-lived chemical is superoxide, a reactive oxygen species (ROS), which undergoes a wide range of environmentally important reactions. Yet, due to its fleeting existence which precludes traditional shipboard analyses, superoxide concentrations have never been characterized in the deep sea. To this end, we have developed a submersible oceanic chemiluminescent analyzer of reactive intermediate species (SOLARIS) to enable continuous measurements of superoxide at depth. Fluidic pumps on SOLARIS combine seawater for analysis with reagents in a spiral mixing cell, initiating a chemiluminescent reaction that is monitored by a photomultiplier tube. The superoxide in seawater is then related to the quantity of light produced. Initial field deployments of SOLARIS have revealed high-resolution trends in superoxide throughout the water column. SOLARIS presents the opportunity to constrain the distributions of superoxide, and any number of chemiluminescent species in previously unexplored environments.
    Description: This research was funded by the NSF Oceanographic Technology and Interdisciplinary Coordination (OTIC) program grant number 1736332 and NSF Chemical Oceanography program grant number 1924236. Partial support was provided by the Link Foundation Ocean Engineering and Instrumentation Fellowship (L.T.).
    Keywords: Superoxide ; Chemiluminescence ; Deep-sea
    Repository Name: Woods Hole Open Access Server
    Type: Article
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