Publications

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Publications in peer reviewed journals

8 Publications found
  • Acesulfame allows the tracing of multiple sources of wastewater and riverbank filtration

    Miguel Angel Marazuela, Giovanni Formentin, Klaus Erlmeier, Thilo Hofmann
    2023 - Environmental Pollution, in press

    Abstract: 

    Aquifers providing drinking water are increasingly threatened by emerging contaminants due to wastewater inputs from multiple sources. These inputs have to be identified, differentiated, and characterized to allow an accurate risk assessment and thus ensure the safety of drinking water through appropriate management. We hypothesize, that in climates with seasonal temperature variations, the sweetener acesulfame potassium (ACE) provides new pathways to study wastewater inputs to aquifers. Specifically, this study investigates the temperature-driven seasonal oscillation of ACE to assess multiple sources of wastewater inputs at a riverbank filtration site. ACE concentrations in the river water varied from 0.2 to 1 μg L−1 in the cold season (T < 10 °C) to 0–0.1 μg L−1 in the warm season (T > 10 °C), due to temperature-dependent biodegradation during wastewater treatment. This oscillating signal could be traced throughout the aquifer over distances up to 3250 m from two different infiltration sources. A transient numerical model of groundwater flow and ACE transport was calibrated over hydraulic heads and ACE concentrations, allowing the accurate calculation of mixing ratios, travel times, and flow-path directions for each of the two infiltration sources. The calculated travel time from the distant infiltration source was of 67 days, while that from the near source was of 20 days. The difference in travel times leads to different potential degradation of contaminants flowing into the aquifer from the river, thus demonstrating the importance of individually assessing the locations of riverbank infiltration. The calibrated ACE transport model allowed calculating transient mixing ratios, which confirmed the impact of river stage and groundwater levels on the mixing ratio of the original groundwater and the bank filtrate. Therefore, continuous monitoring of ACE concentrations can help to optimize the management of the water works with the aim to avoid collection of water with very short travel times, which has important regulative aspects. Our findings demonstrate the suitability of ACE as a transient tracer for identifying multiple sources of wastewater, including riverbank filtration sites affected by wastewater treatment plant effluents. ACE seasonal oscillation tracking thus provides a new tool to be used in climates with pronounced seasonal temperature variations to assess the origins of contamination in aquifers, with time and cost advantages over multi-tracer approaches.

  • Analytical strategies to measure gadolinium as a wastewater marker in surface and groundwater systems

    Miguel Angel Marazuela, Martin Stockhausen, Thilo Hofmann
    2023 - MethodsX, 10: in press

    Abstract: 

    The increasing use of gadolinium (Gd)-based contrast agents in magnetic resonance imaging and the recalcitrant behavior of Gd during municipal wastewater treatment have led to increased concentrations of the tracer in aquatic environments. These anthropogenic Gd emissions to wastewater and, subsequently, to surface and groundwater systems can be exploited to calculate groundwater travel times and mixing ratios, identify wastewater inputs, and calibrate groundwater models. However, analytical complexity, costs, and the time needed to directly measure anthropogenic inputs hinder the practical use of Gd. While direct measurements with inductively coupled plasma-mass spectrometry (ICP-MS) are highly efficient and feasible, only total Gd can be detected with this approach. In unknown hydrogeological systems, the differentiation between total, anthropogenic, and geogenic Gd by interpolating rare earth element patterns requires complex sample pre-treatment and pre-concentration. Direct measurements of Gd can be obtained using anion-exchange chromatography coupled to ICP-MS but the limit of quantification will be higher. Here we provide guidelines for selecting the optimal method for the analysis of Gd as a wastewater tracer in surface-groundwater systems.

    • The cost-effectiveness of existing analytical strategies to measure Gd when used as a wastewater tracer in surface-groundwater systems is addressed
    • A novel analytical strategy for direct determination of total Gd is presented

     

  • Benchmarking biochar with activated carbon for immobilizing leachable PAH and heterocyclic PAH in contaminated soils

    Carlotta Carlini, Sampriti Chaudhuri, Oliver Mann, Daniel Tomsik, Thorsten Hüffer, Nicolas Greggio, Diego Marazza, Thilo Hofmann, Gabriel Sigmund
    2023 - Environmental Pollution, in press

    Abstract: 

    Remediation of residually contaminated soils remains a widespread problem. Biochar can immobilize polycyclic aromatic hydrocarbons (PAH). However, studies on its ability to immobilize PAH and N, S, and O substituted PAH (hetero-PAH) in real soils, and benchmarking with commercial activated carbon are missing. Here, we compared the ability of pristine biochar (BC), steam-activated biochar (SABC), and commercial activated carbon (AC) to immobilize PAH and hetero-PAH. The three carbons were tested on soils from four different contaminated sites in Austria. Different amendment rates (w/w) of the carbons were investigated (BC: 1.0, 2.5, and 5%; SABC: 0.5, 1.0, and 2.0%; AC: 1%) in batch experiments to cover meaningful ranges in relation to their performance. SABC performed better than AC, removing at least 80% PAH with the lowest application rate of 0.5%, and achieving a complete removal at an application rate of 1.0%. BC performed slightly worse but still acceptable in residually contaminated soils (40 and 100% removal at 1 and 5% amendment, respectively). The ability of BC and SABC to immobilize PAH decreased as the PAH-molar volume increased. PAH with three or more rings were preferentially removed by AC compared to SABC or BC. This can be explained by the difference in pore size distribution of the carbons which could limit the accessibility of PAH and hetero-PAH to reach sorption sites for π- π electron donor-acceptor interactions, which drive PAH and hetero-PAH sorption to carbons. Column percolation tests confirmed the results obtained in batch tests, indicating, that decisions for soil remediation can be derived from simpler batch experiments. In soil samples with 1% BC, a reduction of over 90% in the total concentration of PAH in the leached water was observed. Overall, BC and SABC were demonstrated to be valid substitutes for AC for stabilizing residually contaminated soils.

  • Key Principles for the Intergovernmental Science–Policy Panel on Chemicals and Waste

    Marlene Ågerstrand, Kenneth Arinaitwe, Thomas Backhaus, Ricardo O. Barra, Miriam L. Diamond, Joan O. Grimalt, Ksenia Groh, Faith Kandie, Perihan Binnur Kurt-Karakus, Robert J. Letcher, Rainer Lohmann, Rodrigo O. Meire, Temilola Oluseyi, Andreas Schäffer, Mochamad Septiono, Gabriel Sigmund, Anna Soehl, Temitope O. Sogbanmu, Noriyuki Suzuki, Marta Venier, Penny Vlahos, Martin Scheringer
    2023 - Environ. Sci. Technol., 57: in press

    Abstract: 

    In 2021, the United Nations Environment Programme (UNEP) recognized chemical pollution as a planetary crisis tantamount to climate change and biodiversity decline. In an important next step, the international community agreed in March 2022 on establishing an independent, intergovernmental science–policy panel on chemicals, waste, and pollution prevention (hereafter termed “the Panel”). This Panel will take its place among two other intergovernmental bodies, the Intergovernmental Panel on Climate Change (IPCC) and the Intergovernmental Science-Policy Platform on Biodiversity and Ecosystem Services (IPBES). Now is a crucial time for establishing the Panel, following a process facilitated by UNEP to negotiate the Panel’s scope, functions, and institutional design, with the ambition to formally establish the Panel in 2024.
    As a group of international scientists working on chemical pollution, we applaud this milestone of progress to initiate the establishment of a panel for chemicals, waste, and pollution prevention. At the beginning of the negotiating process, we would like to highlight the following 10 critical aspects for consideration in determining the settings of the Panel.

     

  • Policy options to account for multiple chemical pollutants threatening biodiversity

    Leonie Katharina Mueller, Marlene Ågerstrand, Thomas Backhaus, Miriam Diamond, Walter Erdelen, David Evers, Ksenia Groh, Martin Scheringer, Gabriel Sigmund, Zhanyun Wang, Andreas Schäffer
    2023 - Environmental Science: Advances, in press

    Abstract: 

    Chemical pollution poses a threat to biodiversity on a global scale. This has been acknowledged in the Post-2020 Biological Diversity Framework which proposes to regulate the release of chemicals to the environment and names specific indicators focusing on pesticides, nutrients and plastic waste. We fully endorse the inclusion of these substances but argue that in order to protect biodiversity from hazardous chemicals, the scope of Target 7 should feature other groups of pollutants with potential to contribute to biodiversity loss. We propose the inclusion of non-agricultural biocides, per- and polyfluoroalkyl substances (PFASs), toxic metal(loid)s, and endocrine disrupting chemcials (EDCs). Furthermore, data on emerging pollutants (e.g., rare earth elements, industrial chemicals, liquid crystal monomers, pharmaceuticals, personal care products) need to be regularly scanned and these pollutants added to Target 7 in case of biodiversity risk. We suggest to amend Target 7 to postulate the aim for the overall reduction of chemical production and emissions, as well as the addition of the described substance groups of high concern to biodiversity for discussion and implementation in the Post-2020 Biodiversity Framework. We further elaborate on different strategies for the reduction of emissions of hazardous chemicals through chemical simplification and grouping, reduction of chemicals with non-essential use, and innovative synthesis strategies (“benign by design”). In this context the full life cycle of chemicals, i.e., production, use, end of life needs to be considered. Lastly, we propose to set up data inventories that transparently inform about production, transport and emissions of chemicals in cooperation with industry, that can serve as basis for indicators related to monitoring the effectiveness of the goals set under Target 7.

  • Seasonal biodegradation of the artificial sweetener acesulfame enhances its use as a transient wastewater tracer

    Miguel Angel Marazuela, Giovanni Formentin, Klaus Erlmeier, Thilo Hofmann
    2023 - Water Research, 232: in press

    Abstract: 

    The persistence of the artificial sweetener acesulfame potassium (ACE) during wastewater treatment and subsequently in the aquatic environment has made it a widely used tracer of wastewater inputs to both surface water and groundwater. However, the recently observed biodegradation of ACE during wastewater treatment has questioned the validity of this application. In this study, we assessed the use of ACE not only as a marker of wastewater, but also as a transient wastewater tracer that allows both the calculation of mixing ratios and travel times through the aquifer as well as the calibration of transient groundwater flow and mass transport models. Our analysis was based on data obtained in a nearly 8-year river water and groundwater sampling campaign along a confirmed wastewater-receiving riverbank filtration site located close to a drinking water supply system. We provide evidence that temperature controls ACE concentration and thus its seasonal oscillation. River water data showed that ACE loads decreased from 1.5–4 mg·s−1 in the cold season (December to June; T<10 °C) to 0–0.5 mg·s−1 in the warm season (July to November; T>10 °C). This seasonal variability of >600% was detectable in the aquifer and preserved >3 km, with ACE concentrations oscillating between <LOQ in the warm season up to 1 μg·L−1 in the cold season. The large seasonal variation in ACE concentrations during wastewater treatment, compared to the other sweeteners (sucralose, cyclamate, and saccharin) and chloride enables its use as a transient tracer of wastewater inflows and riverbank filtration. In addition, the arrival time of the ACE concentration peak can be used to estimate groundwater flow velocity and mixing ratios, thereby demonstrating its potential in the calibration of groundwater numerical models.

  • Small biochar particles hardly disintegrate under cryo-stress

    Gabriel Sigmund, Andrea Schmid, Hans-Peter Schmidt, Nikolas Hagemann, Thomas D. Bucheli, Thilo Hofmann
    2023 - Geoderma, 430: in press

    Abstract: 

    Physical disintegration of biochar has been postulated to determine the persistence and mobility in soil of this recalcitrant carbon pool. Therein, freeze–thaw cycling can induce substantial physical stress to biochars. We here investigated the physical disintegration and subsequent mobilisation of five different biochars under “realistic worst-case scenarios” in a laboratory soil column setup as well as in shaking and sonication batch experiments. The mobilization of carbon from biochar particles (0.25–1 mm) was investigated in the absence of clay at a pH of 6.3 with and without 80 freeze–thaw cycles. The small biochar particles used in this study did not strongly disintegrate after freeze–thaw cycling, possibly because of freezing point depression in biochar micropores. Our results in comparison with findings in literature suggest that freeze–thaw-induced physical disintegration of biochar is a process more pronounced for large biochar particles containing substantial meso- and macropores. Biochars with larger ash fractions disintegrated more, presumably because of the ash-associated formation of unstable cavities within the biochar. Physical stability of biochars produced from the same feedstock at different pyrolysis temperatures decreased with increasing aromaticity, which may be linked to a higher rigidity of more aromatic structures. Moisture content in the soil increased carbon mobilization from biochar more than physical stress such as freeze–thaw cycling. The physical disintegration of biochar and subsequent mobilization of micro-and nanosized carbon should thus be considered of minor relevance and is often not a driving factor for biochar stability in soil.

  • Stromatolitic carbonates from the Middle Miocene of the western Pannonian Basin reflect trace metal availability in microbial habitats during the Badenian Salinity Crisis

    Sebastian Viehmann, Robert Kujawa, Simon V. Hohl, Nathalie Tepe, Alexandra S. Rodler, Thilo Hofmann, Erich Draganits
    2023 - Chemical Geology, 618: in press

    Abstract: 

    Stromatolitic carbonates of the Middle Miocene Oberpullendorf Basin (Austria) provide a great opportunity to study the evolution of microbial habitats under extreme environmental changes during the Badenian (Langhian and early Serravallian) Salinity Crisis. We here present the first geochemical data for Badenian stromatolites and show in a combined approach using major, trace element, and C – O isotope compositions obtained in individual stromatolitic carbonate laminae that short-term variations of palaeo-environmental conditions within the Oberpullendorf Basin coincide with individual microbialite morphologies.

    The studied carbonates were affected by both detrital contamination and post-depositional alteration processes to different degrees. While fluid-mobile elements show clear evidence for post-depositional alteration processes, the rare earth element and yttrium (REY) as well as bio-essential element (Fe, Mn, Co, Zn, Mo, W) compositions of the carbonates remained unaffected. Stromatolitic carbonates that are devoid of detrital contamination (< 300 ppm Al) show typical shale-normalized seawater-like rare earth element and yttrium (REYSN) patterns with positive LaSN, GdSN anomalies, super-chondritic Y/Ho ratios, and heavy over light REYSN enrichments in the lower stromatolite units. These features suggest an open ocean seawater influenced depositional setting at the north-western margin of the Paratethys Sea. Stratigraphically upwards, pure stromatolitic carbonates show suppressed seawater-like REYSN signatures that argue for the development of a (semi)closed lagoon with restricted access to the open sea. Seawater-like REYSN patterns in the uppermost part resemble a reappearance of open marine environmental conditions. Interestingly, geochemical data of the upper part of the section contradict the ambient fossil record, showing the urge for future interdisciplinary approaches targeting the understanding and interplay of geochemistry, palaeontology, and geomicrobiology in modern and ancient microbial habitats. Enrichment factors of bio-essential trace elements that are either used as co-factors in metalloenzymes or metal-activated enzymes in biochemical reactions can be directly linked to the reconstructed environmental conditions: Sufficient element availability is ensured during marine conditions in the lower and uppermost stratigraphic sections; in contrast, continuous decreasing element availability of these elements is directly related to the temporary development of a (semi)closed lagoon.

Book chapters and other publications

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