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Glucose as a Potential Chemical Marker for Ice Nucleating Activity in Arctic Seawater and Melt Pond Samples (2019)

Zeppenfeld, Sebastian ; van Pinxteren, Manuela ; Hartmann, Markus ; [weitere]

American Chemical Society (ACS)

In: EPIC3Environmental Science and Technology, American Chemical Society (ACS), 53(15), pp. 8747-8756, ISSN: 0013-936X

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Publikationsdatum: 2024-04-12

Beschreibung: Recent studies pointed to a high ice nucleating activity (INA) in the Arctic sea surface microlayer (SML). However, related chemical information is still sparse. In the present study, INA and free glucose concentrations were quantified in Arctic SML and bulk water samples from the marginal ice zone, the ice-free ocean, melt ponds, and open waters within the ice pack. T50 (defining INA) ranged from −17.4 to −26.8 °C. Glucose concentrations varied from 0.6 to 51 μg/L with highest values in the SML from the marginal ice zone and melt ponds (median 16.3 and 13.5 μg/L) and lower values in the SML from the ice pack and the ice-free ocean (median 3.9 and 4.0 μg/L). Enrichment factors between the SML and the bulk ranged from 0.4 to 17. A positive correlation was observed between free glucose concentration and INA in Arctic water samples (T50(°C) = (−25.6 ± 0.6) + (0.15 ± 0.04)·Glucose(μg/L), RP = 0.66, n = 74). Clustering water samples based on phytoplankton pigment composition resulted in robust but different correlations within the four clusters (RP between 0.67 and 0.96), indicating a strong link to phytoplankton-related processes. Since glucose did not show significant INA itself, free glucose may serve as a potential tracer for INA in Arctic water samples.

Repository-Name: EPIC Alfred Wegener Institut

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The Molecular Fingerprint of Fluorescent Natural Organic Matter Offers Insight into Biogeochemical Sources and Diagenetic State (2018)

Wünsch, Urban J ; Acar, Evrim ; Koch, Boris P ; [weitere]

American Chemical Society (ACS)

In: EPIC3Analytical Chemistry, American Chemical Society (ACS), 90(24), pp. 14188-14197, ISSN: 0003-2700

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Publikationsdatum: 2024-04-09

Beschreibung: Investigating the biogeochemistry of dissolved organic matter (DOM) requires the synthesis of data from several complementary analytical techniques. The traditional approach to data synthesis is to search for correlations between measurements made on the same sample using different instruments. In contrast, data fusion simultaneously decomposes data from multiple instruments into the underlying shared and unshared components. Here, Advanced Coupled Matrix and Tensor Factorization (ACMTF) was used to identify the molecular fingerprint of DOM fluorescence fractions in Arctic fjords. ACMTF explained 99.84% of the variability with six fully shared components. Individual molecular formulas were linked to multiple fluorescence components and vice versa. Molecular fingerprints differed in diversity and oceanographic patterns, suggesting a link to the biogeochemical sources and diagenetic state of DOM. The fingerprints obtained through ACMTF were more specific compared to traditional correlation analysis and yielded greater compositional insight. Multivariate data fusion aligns extremely complex, heterogeneous DOM data sets and thus facilitates a more holistic understanding of DOM biogeochemistry.

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Grand Canonical Monte Carlo Simulations on Phase Equilibria of Methane, Carbon Dioxide, and Their Mixture Hydrates (2018)

Qiu, Nianxiang ; Bai, Xiaojing ; Sun, Ningru ; [weitere]

American Chemical Society (ACS)

In: The Journal of Physical Chemistry B, 122 (42). pp. 9724-9737.

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Publikationsdatum: 2021-01-08

Beschreibung: The cage occupancy plays a crucial role in the thermodynamic stability of clathrate hydrates and is an important quantity for understanding the CO2–CH4 replacement phenomenon. In this work, the occupancy isotherms of pure CH4, pure CO2, and their mixture in sI and sII hydrates are studied by GCMC + MD simulations. The adsorption of CH4 and CO2 + CH4 in the sI and sII hydrates can be categorized as the one-site Langmuir type. The calculated occupancy ratio θL/θS and the abundance ratio of CO2 to CH4 vary with the temperature and pressure, which provide the prerequisite information for the prediction of CH4 recovery yield at different conditions in the CO2–CH4 gas exchange process. The phase equilibria of clathrate hydrates of pure gases and mixtures are explored and the corresponding heat of dissociation and hydration numbers are determined. The current investigation provides new perspectives to understand the mechanism behind the gas adsorption behavior of clathrate hydrates.

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Use of Waste-Derived Biochar to Remove Copper from Aqueous Solution in a Continuous-Flow System (2017)

Aran, Diego ; Antelo, Juan ; Lodeiro, Pablo ; [weitere]

American Chemical Society (ACS)

In: Industrial & Engineering Chemistry Research, 56 (44). pp. 12755-12762.

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Publikationsdatum: 2020-02-06

Beschreibung: The discharges from industrial processes constitute the main source of copper contamination in aqueous ecosystems. In this study we investigated the capacity of different types of biochar (derived from chicken manure, eucalyptus, corncob, olive mill and pine sawdust) to remove copper from aqueous solution in a continuous-flow system. The flow rate of the system strongly influenced the amount of copper retained. The adsorption to the corncob biochar varied from 5.51 to 3.48 mg Cu g-1 as the flux decreased from 13 to 2.5 mL min-1. The physicochemical characteristics of biochar determine the copper retention capacity and the underlying immobilization mechanisms. Biochars with high inorganic contents retain the largest amounts of copper and may be suitable for using in water treatment systems to remove heavy metals. The copper retention capacity of the biochars ranged between ~1.3 and 26 mg g-1 and varied in the following order: chicken manure 〉 olive mill 〉〉 corncob 〉 eucalyptus 〉 sawdust pine.

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Methane Bubble Size Distributions, Flux, and Dissolution in a Freshwater Lake (2017)

Delwiche, Kyle B. ; Hemond, Harold F.

American Chemical Society (ACS)

In: Environmental Science & Technolog, 51 (23). pp. 13733-13739.

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Publikationsdatum: 2020-02-06

Beschreibung: The majority of methane produced in many anoxic sediments is released via ebullition. These bubbles are subject to dissolution as they rise, and dissolution rates are strongly influenced by bubble size. Current understanding of natural methane bubble size distributions is limited by the difficulty in measuring bubble sizes over wide spatial or temporal scales. Our custom optical bubble size sensors recorded bubble sizes and release timing at 8 locations in Upper Mystic Lake, MA continuously for 3 months. Bubble size distributions were spatially heterogeneous even over relatively small areas experiencing similar flux, suggesting that localized sediment conditions are important to controlling bubble size. There was no change in bubble size distributions over the 3 month sampling period, but mean bubble size was positively correlated with daily ebullition flux. Bubble data was used to verify the performance of a widely used bubble dissolution model, and the model was then used to estimate that bubble dissolution accounts for approximately 10% of methane accumulated in the hypolimnion during summer stratification, and at most 15% of the diffusive air–water–methane flux from the epilimnion.

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Comparison of Raman and Fourier Transform Infrared Spectroscopy for the Quantification of Microplastics in the Aquatic Environment (2018)

Cabernard, Livia ; Roscher, Lisa ; Lorenz, Claudia ; [weitere]

American Chemical Society (ACS)

In: Environmental Science & Technology, 52 (22). pp. 13279-13288.

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Publikationsdatum: 2020-01-02

Beschreibung: Microplastics (MPs, 〈5 mm) have been reported as emerging environmental contaminants, but reliable data are still lacking. We compared the two most promising techniques for MP analysis, namely, Raman and Fourier transform infrared (FTIR) spectroscopy, by analyzing MPs extracted from North Sea surface waters. Microplastics 〉500 μm were visually sorted and manually analyzed by μ-Raman and attenuated total reflection (ATR)-FTIR spectroscopy. Microplastics ≤500 μm were concentrated on gold-coated filters and analyzed by automated single-particle exploration coupled to μ-Raman (ASPEx-μ-Raman) and FTIR imaging (reflection mode). The number of identified MPs 〉500 μm was slightly higher for μ-Raman (+23%) than ATR-FTIR analysis. Concerning MPs ≤500 μm, ASPEx-μ-Raman quantified two-times higher MP numbers but required a four-times higher analysis time compared to FTIR imaging. Because ASPEx-μ-Raman revealed far higher MP concentrations (38–2621 particles m–3) compared to the results of previous water studies (0–559 particles m–3), the environmental concentration of MPs ≤500 μm may have been underestimated until now. This may be attributed to the exceptional increase in concentration with decreasing MP size found in this work. Our results demonstrate the need for further research to enable time-efficient routine application of ASPEx-μ-Raman for reliable MP counting down to 1 μm.

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Continuous Seasonal River Ebullition Measurements Linked to Sediment Methane Formation (2015)

Wilkinson, Jeremy ; Maeck, Andreas ; Alshboul, Zeyad ; [weitere]

American Chemical Society (ACS)

In: Environmental Science & Technology, 49 (22). pp. 13121-13129.

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Publikationsdatum: 2019-10-24

Beschreibung: Laboratory sediment incubations and continuous ebullition monitoring over an annual cycle in the temperate Saar River, Germany confirm that impounded river zones can produce and emit methane at high rates (7 to 30 (g CH4 m–3 d–1) at 25 °C and 270 to 700 (g CH4 m–2 yr–1), respectively). Summer methane ebullition (ME) peaks were a factor of 4 to 10 times the winter minima, and sediment methane formation was dominated by the upper sediment (depths of 0.14 to 0.2 m). The key driver of the seasonal ME dynamics was temperature. An empirical model relating methane formation to temperature and sediment depth, derived from the laboratory incubations, reproduced the measured daily ebullition from winter to midsummer, although late summer and autumn simulated ME exceeded the observed ME. A possible explanation for this was substrate limitation. We recommend measurements of methanogenically available carbon sources to identify substrate limitation and help characterize variation in methane formation with depth and from site to site.

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