Publications

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Publications in peer reviewed journals

5 Publications found
  • Demystifying mercury geochemistry in contaminated soil–groundwater systems with complementary mercury stable isotope, concentration, and speciation analyses

    David S. McLagan, Lorenz Schwab, Jan G. Wiederhold, Lu Chen, Jan Pietrucha, Stephan M. Kraemer, Harald Biester
    2022 - Environmental Science: Processes & Impacts, Advance Article

    Abstract: 

    Interpretation of mercury (Hg) geochemistry in environmental systems remains a challenge. This is largely associated with the inability to identify specific Hg transformation processes and species using established analytical methods in Hg geochemistry (total Hg and Hg speciation). In this study, we demonstrate the improved Hg geochemical interpretation, particularly related to process tracing, that can be achieved when Hg stable isotope analyses are complemented by a suite of more established methods and applied to both solid- (soil) and liquid-phases (groundwater) across two Hg2+-chloride (HgCl2) contaminated sites with distinct geological and physicochemical properties. This novel approach allowed us to identify processes such as Hg2+ (i.e., HgCl2) sorption to the solid-phase, Hg2+ speciation changes associated with changes in groundwater level and redox conditions (particularly in the upper aquifer and capillary fringe), Hg2+ reduction to Hg0, and dark abiotic redox equilibration between Hg0 and Hg(II). Hg stable isotope analyses play a critical role in our ability to distinguish, or trace, these in situ processes. While we caution against the non-critical use of Hg isotope data for source tracing in environmental systems, due to potentially variable source signatures and overprinting by transformation processes, our study demonstrates the benefits of combining multiple analytical approaches, including Hg isotope ratios as a process tracer, to obtain an improved picture of the enigmatic geochemical behavior and fate of Hg at contaminated legacy sites.

  • Identifying Functional Groups that Determine Rates of Micropollutant Biotransformations Performed by Wastewater Microbial Communities

    Stephanie L. Rich, Michael Zumstein, Damian E. Helbling
    2022 - Environmental Science & Technology, 56: 984–994

    Abstract: 

    The goal of this research was to identify functional groups that determine rates of micropollutant (MP) biotransformations performed by wastewater microbial communities. To meet this goal, we performed a series of incubation experiments seeded with four independent wastewater microbial communities and spiked them with a mixture of 40 structurally diverse MPs. We collected samples over time and used high-resolution mass spectrometry to estimate biotransformation rate constants for each MP in each experiment and to propose structures of 46 biotransformation products. We then developed random forest models to classify the biotransformation rate constants based on the presence of specific functional groups or observed biotransformations. We extracted classification importance metrics from each random forest model and compared them across wastewater microbial communities. Our analysis revealed 30 functional groups that we define as either biotransformation promoters, biotransformation inhibitors, structural features that can be biotransformed based on uncharacterized features of the wastewater microbial community, or structural features that are not rate-determining. Our experimental data and analysis provide novel insights into MP biotransformations that can be used to more accurately predict MP biotransformations or to inform the design of new chemical products that may be more readily biodegradable during wastewater treatment.

  • Pharmaceutical pollution of the world’s rivers

    John L. Wilkinson, Alistair B. A. Boxall, Dana W. Kolpin, Kenneth M. Y. Leung, Racliffe W. S. Lai, Cristobal Galban-Malagon, Aiko D. Adell, Julie Mondon, Marc Metian, Robert A. Marchant, Alejandra Bouzas-Monroy, Aida Cuni-Sanchez, Anja Coors, Pedro Carriquiriborde, Macarena Rojo, Chris Gordon, Magdalena Cara, Monique Moermond, Thais Luarte, Vahagn Petrosyan, Yekaterina Perikhanyan, Clare S. Mahon, Christopher J. McGurk, Thilo Hofmann, Tapos Kormoker, Volga Iniguez, Jessica Guzman-Otazo, Jean L. Tavares, Francisco Gildasio De Figueiredo, Maria T. P. Razzolini, Victorien Dougnon, Gildas Gbaguidi, Oumar Traore, Jules M. Blais, Linda E. Kimpe, Michelle Wong, Donald Wong, Romaric Ntchantcho, Jaime Pizarro, Guang-Guo Ying, Chang-Er Chen, Martha Paez, Jina Martinez-Lara, Jean-Paul Otamonga, John Pote, Suspense A. Ifo, Penelope Wilson, Silvia Echeverria-Saenz, Nikolina Udikovic-Kolic, Milena Milakovic, Despo Fatta-Kassinos, Lida Ioannou-Ttofa, Vladimira Belusova, Jan Vymazal, Maria Cardenas-Bustamante, Bayable A. Kas
    2022 - PNAS, 119: e2113947119

    Abstract: 

    Environmental exposure to active pharmaceutical ingredients (APIs) can have negative effects on the health of ecosystems and humans. While numerous studies have monitored APIs in rivers, these employ different analytial methods, measure different APIs, and have ignored many of the countries of the world. This makes it difficult to quantify the scale of the problem from a global perspective. Furthermore, comparison of the existing data, generated for different studies/regions/continents, is challenging due to the vast differences between the analytical methodologies employed. Here, we present a global-scale study of API pollution in 258 of the world’s rivers, representing the environmental influence of 471.4 million people across 137 geographic regions. Samples were obtained from 1,052 locations in 104 countries (representing all continents and 36 countries not previously studied for API contamination) and analyzed for 61 APIs. Highest cumulative API concentrations were observed in sub-Saharan Africa, south Asia, and South America. The most contaminated sites were in low- to middle-income countries and were associated with areas with poor wastewater and waste management infrastructure and pharmaceutical manufacturing. The most frequently detected APIs were carbamazepine, metformin, and caffeine (a compound also arising from lifestyle use), which were detected at over half of the sites monitored. Concentrations of at least one API at 25.7% of the sampling sites were greater than concentrations considered safe for aquatic organisms, or which are of concern in terms of selection for antimicrobial resistance. Therefore, pharmaceutical pollution poses a global threat to environmental and human health, as well as to delivery of the United Nations Sustainable Development Goals.

  • Towards Standardization for Determining Dissolution Kinetics of Nanomaterials in Natural Aquatic Environments: Continuous Flow Dissolution of Ag Nanoparticles

    Lucie Stetten, Aiga Mackevica, Nathalie Tepe, Thilo Hofmann, Frank von der Kammer
    2022 - Nanomaterials, 12: 519

    Abstract: 

    The dissolution of metal-based engineered nanomaterials (ENMs) in aquatic environments is an important mechanism governing the release of toxic dissolved metals. For the registration of ENMs at regulatory bodies such as REACH, their dissolution behavior must therefore be assessed using standardized experimental approaches. To date, there are no standardized procedures for dissolution testing of ENMs in environmentally relevant aquatic media, and the Organisation for Economic Co-operation and Development (OECD) strongly encourages their development into test guidelines. According to a survey of surface water hydrochemistry, we propose to use media with low concentrations of Ca2+ and Mg2+ for a better simulation of the ionic background of surface waters, at pH values representing acidic (5 < pH < 6) and near-neutral/alkaline (7 < pH < 8) waters. We evaluated a continuous flow setup adapted to expose small amounts of ENMs to aqueous media, to mimic ENMs in surface waters. For this purpose, silver nanoparticles (Ag NPs) were used as model for soluble metal-bearing ENMs. Ag NPs were deposited onto a 10 kg.mol−1 membrane through the injection of 500 µL of a 5 mg.L−1 or 20 mg.L−1 Ag NP dispersion, in order to expose only a few micrograms of Ag NPs to the aqueous media. The dissolution rate of Ag NPs in 10 mM NaNO3 was more than two times higher for ~2 µg compared with ~8 µg of Ag NPs deposited onto the membrane, emphasizing the importance of evaluating the dissolution of ENMs at low concentrations in order to keep a realistic scenario. Dissolution rates of Ag NPs in artificial waters (2 mM Ca(NO3)2, 0.5 mM MgSO4, 0–5 mM NaHCO3) were also determined, proving the feasibility of the test using environmentally relevant media. In view of the current lack of harmonized methods, this work encourages the standardization of continuous flow dissolution methods toward OECD guidelines focused on natural aquatic environments, for systematic comparisons of nanomaterials and adapted risk assessments.

  • Tracking the legacy of early industrial activity in sediments of Lake Zurich, Switzerland: using a novel multi-proxy approach to find the source of extensive metal contamination

    Remo Luis Roethlin, Adrian Gilli, Bernhard Wehrli, Robin Sue Gilli, Jan Georg Wiederhold, Nathalie Dubois
    2022 - Environmental Science and Pollution Research, in press

    Abstract: 

    Historical industrial activities at the Horn Richterwil, on the shore of Lake Zurich (Switzerland), caused widespread metal contamination on land and in the adjacent lake sediments. This study provides an estimation of the age and source of the contamination by using XRF core scanning, ICP-OES, and Hg-AFS for quantitative measurements of trace metals and MC-ICP-MS for the stable isotope analysis of mercury. Radiometric dating ( 137Cs, 210Pb, and Pu dating) of two proximal cores and varve chronology in a distal core suggest two different contaminations, one stemming from around 1960 (Zn, Cd) and an earlier one from 1880 (Cr, Cu, Hg, Pb, Sn). The XRF data suggest two different contamination pathways: one by landfill of contaminated soil and another one by industrial wastewater effluents. Maximum concentrations found within all samples are in the range of per mil (dry weight) for Cr, Cu, Hg, Pb, Sn, and Zn and lie within the top 10 cm of the sediment cores. The analysis of the mercury isotopic composition ( 𝛿202 Hg and Δ199Hg) shows a significantly different signature for one of the cores, indicating a second mercury source. We could not identify the exact source or process leading to the isotopic fractionation of mercury, but the isotopic data confirm two different sources.

Book chapters and other publications

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