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Pierce, Eric M.

Publications and source records attributed to Pierce, Eric M..

13 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Light-independent phytoplankton degradation and detoxification of methylmercury in water

Phytoplankton serves as a key entry point for the trophic transfer and bioaccumulation of the neurotoxin methylmercury (MeHg) in aquatic food webs. However, it is unclear whether and how phytoplankton itself may degrade and metabolize MeHg in the dark. Here, using several strains of the freshwater alga Chlorella vulgaris, the marine diatom Chaetoceros gracilis and two cyanobacteria (or blue-green algae), we report a light-independent pathway of MeHg degradation in water by phytoplankton, rather than its associated bacteria. About 36–85% of MeHg could be degraded intracellularly to inorganic Hg(II) and/or Hg(0) via dark reactions. Furthermore, endogenic reactive oxygen species, particularly singlet oxygen, were identified as the main driver of MeHg demethylation. Given the increasing incidence of algal blooms in lakes and marine systems globally, these findings underscore the potential roles of phytoplankton demethylation and detoxification of MeHg in aquatic ecosystems and call for improved modelling and assessment of MeHg bioaccumulation and environmental risks.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Adsorption and intracellular uptake of mercuric mercury and methylmercury by methanotrophs and methylating bacteria

The cell surface adsorption and intracellular uptake of mercuric mercury Hg(II) and methylmercury (MeHg) are important in determining the fate and transformation of Hg in the environment. However, current information is limited about their interactions with two important groups of microorganisms, i.e., methanotrophs and Hg(II)-methylating bacteria, in aquatic systems. This study investigated the adsorption and uptake dynamics of Hg(II) and MeHg by three strains of methanotrophs, Methylomonas sp. strain EFPC3, Methylosinus trichosporium OB3b, and Methylococcus capsulatus Bath, and two Hg(II)-methylating bacteria, Pseudodesulfovibrio mercurii ND132 and Geobacter sulfurreducens PCA. Distinctive behaviors of these microorganisms towards Hg(II) and MeHg adsorption and intracellular uptake were observed. The methanotrophs took up 55–80% of inorganic Hg(II) inside cells after 24 h incubation, lower than methylating bacteria (>90%). Approximately 80–95% of MeHg was rapidly taken up by all the tested methanotrophs within 24 h. In contrast, after the same time, G. sulfurreducens PCA adsorbed 70% but took up <20% of MeHg, while P. mercurii ND132 adsorbed <20% but took up negligible amounts of MeHg. These results suggest that microbial surface adsorption and intracellular uptake of Hg(II) and MeHg depend on the specific types of microbes and appear to be related to microbial physiology that requires further detailed investigation. Despite being incapable of methylating Hg(II), methanotrophs play important roles in immobilizing both Hg(II) and MeHg, potentially influencing their bioavailability and trophic transfer. Furthermore, methanotrophs are not only important sinks for methane but also for Hg(II) and MeHg and can influence the global cycling of C and Hg.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Uncertainty quantification of machine learning models to improve streamflow prediction under changing climate and environmental conditions

Machine learning (ML) models, and Long Short-Term Memory (LSTM) networks in particular, have demonstrated remarkable performance in streamflow prediction and are increasingly being used by the hydrological research community. However, most of these applications do not include uncertainty quantification (UQ). ML models are data driven and can suffer from large extrapolation errors when applied to changing climate/environmental conditions. UQ is required to quantify the influence of data noises on model predictions and avoid overconfident projections in extrapolation. In this work, we integrate a novel UQ method, called PI3NN, with LSTM networks for streamflow prediction. PI3NN calculates Prediction Intervals by training 3 Neural Networks. It can precisely quantify the predictive uncertainty caused by the data noise and identify out-of-distribution (OOD) data in a non-stationary condition to avoid overconfident predictions. We apply the PI3NN-LSTM method in the snow-dominant East River Watershed in the western US and in the rain-driven Walker Branch Watershed in the southeastern US. Results indicate that for the prediction data which have similar features as the training data, PI3NN precisely quantifies the predictive uncertainty with the desired confidence level; and for the OOD data where the LSTM network fails to make accurate predictions, PI3NN produces a reasonably large uncertainty indicating that the results are not trustworthy and should avoid overconfidence. PI3NN is computationally efficient, robust in performance, and generalizable to various network structures and data with no distributional assumptions. It can be broadly applied in ML-based hydrological simulations for credible prediction.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Sonochemical oxidation and stabilization of liquid elemental mercury in water and soil

Over 3000 mercury (Hg)-contaminated sites worldwide contain liquid metallic Hg [Hg(0) 1 ] representing a continuous source of elemental Hg(0) in the environment through volatilization and solubilization in water. Currently, there are few effective treatment technologies available to remove or sequester Hg(0) 1 in situ. We investigated sonochemical treatments coupled with complexing agents, polysulfide and sulfide, in oxidizing Hg(0) 1 and stabilizing Hg in water, soil and quartz sand. Results indicate that sonication is highly effective in breaking up and oxidizing liquid Hg(0) 1 beads via acoustic cavitation, particularly in the presence of polysulfide. Without complexing agents, sonication caused only minor oxidation of Hg(0) 1 but increased headspace gaseous Hg(0) g and dissolved Hg(0) aq in water. However, the presence of polysulfide essentially stopped Hg(0) volatilization and solubilization. As a charged polymer, polysulfide was more effective than sulfide in oxidizing Hg(0) 1 and subsequently stabilizing the precipitated metacinnabar (β-HgS) nanocrystals. Sonochemical treatments with sulfide yielded incomplete oxidation of Hg(0) 1 , likely resulting from the formation of HgS coatings on the dispersed µm-size Hg(0) 1 bead surfaces. Sonication with polysulfide also resulted in rapid oxidation of Hg(0) 1 and precipitation of HgS in quartz sand and in the Hg(0) 1 -contaminated soil. This research indicates that sonochemical treatment with polysulfide could be an effective means in rapidly converting Hg(0) 1 to insoluble HgS precipitates in water and sediments, thereby preventing its further emission and release to the environment. We suggest that future studies are performed to confirm its technical feasibility and treatment efficacy for remediation applications.

36 MATERIALS SCIENCE↗
DOE OSTI2022

High methylation potential of mercury complexed with mixed thiolate ligands by Geobacter sulfurreducens PCA

We report some thiols, such as cysteine (CYS) at moderate concentrations (10–500 µM), can enhance methylmercury (MeHg) formation by Geobacter sulfurreducens PCA, whereas others such as dithiol 2,3-dimercaptopropanesulfonate (DMPS) and 2,3-dimercaptosuccinic acid (DMSA) abolish mercury [Hg(II)] methylation. Little is known, however, about whether Hg(II) methylation could be enhanced or inhibited by the presence of mixed thiol ligands at low concentrations observed in the environment. Surprisingly we found that mixing CYS (1 µM) with DMPS (0.025–0.5 µM) or DMSA (0.025–1 µM) substantially increased MeHg production by 1.5–3.5-fold, compared to the no-thiol control, whereas complexation with a single DMPS, or DMSA, or CYS (1 µM) strongly inhibited Hg(II) methylation. Pre-equilibration between Hg(II) and thiols before the addition of cells was necessary to observe enhanced methylation. Spectroscopic analyses indicated the formation of mixed or heteroleptic coordinated Hg(II)-S 3 /S 4 complexes, which likely facilitated exchange of Hg(II) with cells and its uptake and internal transfer to the HgcAB proteins required for methylation. These results suggest that the effects of thiols on Hg(II) methylation were more complex than previously thought (using a single thiol) and thus underscore the importance of understanding how mixed thiols and their interactions with Hg(II) may ultimately influence MeHg production in the natural environment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Integrated Disposal Facility FY2011 Glass Testing Summary Report [Erratum]

Pacific Northwest National Laboratory was contracted by Washington River Protection Solutions, LLC to provide the technical basis for estimating radionuclide release from the engineered portion of the disposal facility (e.g., source term). Vitrifying the low-activity waste at Hanford is expected to generate over 1.6 x 10 5 m 3 of glass (Certa and Wells 2010). The volume of immobilized low-activity waste (ILAW) at Hanford is the largest in the DOE complex and is one of the largest inventories (approximately 8.9 x 10 14 Bq total activity) of long-lived radionuclides, principally 99 Tc (t 1/2 = 2.1 x 10 5 ), planned for disposal in a low-level waste (LLW) facility. Before the ILAW can be disposed, DOE must conduct a performance assessment (PA) for the Integrated Disposal Facility (IDF) that describes the long-term impacts of the disposal facility on public health and environmental resources. As part of the ILAW glass testing program PNNL is implementing a strategy, consisting of experimentation and modeling, in order to provide the technical basis for estimating radionuclide release from the glass waste form in support of future IDF PAs. The purpose of this report is to summarize the progress made in fiscal year (FY) 2011 toward implementing the strategy with the goal of developing an understanding of the long-term corrosion behavior of low-activity waste glasses.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

ORNL Second Target Station Project: Biological & Environmental Science Workshop

Recent advances in neutron sources and instrumentation have opened up many new opportunities for the application of neutron scattering techniques in the biological and environmental sciences. Neutrons enable studies of the structure and dynamics of biological and environmental samples with a particular sensitivity to light elements, such as hydrogen, which is a key component of biological and environmental samples. Studies using neutrons are complementary to X-rays and have the unique advantage of being non-destructive and highly-penetrating. Oak Ridge National Laboratory’s upcoming Spallation Neutron Source (SNS) Second Target Station (STS) will provide high brightness cold neutron sources that significantly advance the scientific capabilities of neutron scattering instruments. The STS will advance our understanding of biological and environmental processes across spatial and temporal scales. The capabilities will enhance our ability to discover, design, and develop new materials essential for advanced sustainable technologies to address society’s most pressing needs. This report summarizes the discussions and recommendations from a joint workshop held by the STS Project and the Biological and Environmental Systems Science Directorate (BESSD) in June 2022. The purpose of the workshop was to explore science opportunities and capabilities related to biological and environmental systems that could be incorporated into both current and future STS instrument designs, as well as additional instruments at the SNS First Target Station (FTS) and High Flux Isotope Reactor (HFIR). With six breakout sessions, each with two invited plenary speakers from other institutions, the participants discussed a wide range of topics relevant to biological and environmental research. Based on the input from participants, a number of recommendations on instrumentation, sample environments, complementary multi-modal methods, data processing and analysis and sample deuteration are provided in the report. The participants also identified science opportunities that are emerging from the planned instrument capabilities at STS. Selected recommendations and science opportunities are listed in the Executive Summary.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Unravelling biogeochemical drivers of methylmercury production in an Arctic fen soil and a bog soil

Arctic tundra soils store a globally significant amount of mercury (Hg), which could be transformed to the neurotoxic methylmercury (MeHg) upon warming and thus poses serious threats to the Arctic ecosystem. However, our knowledge of the biogeochemical drivers of MeHg production is limited in these soils. Using substrate addition (acetate and sulfate) and selective microbial inhibition approaches, we investigated the geochemical drivers and dominant microbial methylators in 60-day microcosm incubations with two tundra soils: a circumneutral fen soil and an acidic bog soil, collected near Nome, Alaska, United States. Results showed that increasing acetate concentration had negligible influences on MeHg production in both soils. However, inhibition of sulfate-reducing bacteria (SRB) completely stalled MeHg production in the fen soil in the first 15 days, whereas addition of sulfate in the low-sulfate bog soil increased MeHg production by 5-fold, suggesting prominent roles of SRB in Hg(II) methylation. Without the addition of sulfate in the bog soil or when sulfate was depleted in the fen soil (after 15 days), both SRB and methanogens contributed to MeHg production. Analysis of microbial community composition confirmed the presence of several phyla known to harbor microorganisms associated with Hg(II) methylation in the soils. Lastly, the observations suggest that SRB and methanogens were mainly responsible for Hg(II) methylation in these tundra soils, although their relative contributions depended on the availability of sulfate and possibly syntrophic metabolisms between SRB and methanogens.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Competitive exchange between divalent metal ions [Cu(II), Zn(II), Ca(II)] and Hg(II) bound to thiols and natural organic matter

Mercuric Hg(II) ion forms exceptionally strong complexes with various organic ligands, particularly thiols and dissolved organic matter (DOM) in natural water. Few studies, however, have experimentally determined whether or not the presence of base cations and transition metal ions, such as Ca(II), Cu(II), and Zn(II), would compete with Hg(II) bound to these ligands, as concentrations of these metal ions are usually orders of magnitude higher than Hg(II) in aquatic systems. Different from previous model predictions, a significant fraction of Hg(II) bound to cysteine (CYS), glutathione (GSH), or DOM was found to be competitively exchanged by Cu(II), but not by Zn(II) or Ca(II). About 20–75% of CYS-bound-Hg(II) [at 2:1 CYS:Hg(II)] and 14–40% of GSH-bound-Hg(II) [at 1:1 GSH:Hg(II)] were exchanged by Cu(II) at concentrations 1–3 orders of magnitude greater than Hg(II). Competitive exchange was also observed between Cu(II) and Hg(II) bound to DOM, albeit to a lower extent, depending on relative abundances of thiol and carboxylate functional groups on DOM and their equilibrium time with Hg(II). When complexed with ethylenediaminetetraacetate (EDTA), most Hg(II) could be exchanged by Cu(II) and Zn(II), as well as Ca(II) at increasing concentrations. Furthermore, these results shed additional light on competitive exchange reactions between Hg(II) and coexisting metal ions and have important implications in Hg(II) chemical speciation and biogeochemical transformation, particularly in contaminated environments containing relatively high concentrations of Hg(II) and metal ions.

36 MATERIALS SCIENCE↗
DOE OSTI2021

The future low-temperature geochemical data-scape as envisioned by the U.S. geochemical community

Data sharing benefits the researcher, the scientific community, and the public by allowing the impact of data to be generalized beyond one project and by making science more transparent. However, many scientific communities have not developed protocols or standards for publishing, citing, and versioning datasets. One community that lags in data management is that of low-temperature geochemistry (LTG). This paper resulted from an initiative from 2018 through 2020 to convene LTG and data scientists in the U.S. to strategize future management of LTG data. Through webinars, a workshop, a preprint, a townhall, and a community survey, the group of U.S. scientists discussed the landscape of data management for LTG – the data-scape. Currently this data-scape includes a “street bazaar” of data repositories. This was deemed appropriate in the same way that LTG scientists publish articles in many journals. The variety of data repositories and journals reflect that LTG scientists target many different scientific questions, produce data with extremely different structures and volumes, and utilize copious and complex metadata. Nonetheless, the group agreed that publication of LTG science must be accompanied by sharing of data in publicly accessible repositories, and, for sample-based data, registration of samples with globally unique persistent identifiers. LTG scientists should use certified data repositories that are either highly structured databases designed for specialized types of data, or unstructured generalized data systems. Recognizing the need for tools to enable search and cross-referencing across the proliferating data repositories, the group proposed that the overall data informatics paradigm in LTG should shift from “build data repository, data will come” to “publish data online, cybertools will find”. Funding agencies could also provide portals for LTG scientists to register funded projects and datasets, and forge approaches that cross national boundaries. Finally, the needed transformation of the LTG data culture requires emphasis in student education on science and management of data.

58 GEOSCIENCES↗