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When a pinch is problematic: Detecting pertechnetate in groundwater

pertechnetate

A PNNL researcher holds a redox sensor in the project’s lab in the Radiochemical Processing Laboratory.  Andrea Starr | PNNL

PNNL develops an effective tool for measuring a tricky contaminant

March 30, 2020
March 30, 2020
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Imagine trying to detect and measure a pinch of salt in an Olympic-size swimming pool. Now pretend the tools you are using don’t work well. Some can detect the salt but can’t tell you how much is in there, and others confuse salt with chlorine.

Now swap the swimming pool for a source of groundwater and the salt for a radioactive contaminant called pertechnetate.

ACS Journal Pertechnetate
The future of groundwater contamination measurement? The large thiol claws of PNNL’s subsurface probe with custom gold tips detect and measure pertechnetate in aqueous environments. Cover illustration by Rose Perry, PNNL

Pertechnetate is a byproduct of nuclear waste. If it ends up where it is not supposed to be—like, in groundwater—it could impact human health, which is why researchers and regulators keep a close lookout for it. The environmental safety limits for pertechnetate are roughly equivalent to a pinch of salt in an Olympic pool. And there are only a few technologies to measure it, each with limitations.

PNNL research tackles this challenge with new technology to detect and accurately measure pertechnetate at super low levels in groundwater. This research, “Redox-Based Electrochemical Affinity Sensor for Detection of Aqueous Pertechnetate Anion,” was the cover article for the March 2020 edition of ACS Sensors (DOI: 10.1021/acssensors.9b01531). 

Why it matters: The Environmental Protection Agency drinking water standard for pertechnetate is 0.000000052 grams per liter (that’s roughly 1/6000th the weight of a single poppy seed). While techniques exist for detection of pertechnetate in the environment, many have their drawbacks. PNNL’s technology can accurately measure low levels of pertechnetate in groundwater. Additionally, this proof of concept has the potential to be applied to other target contaminants simultaneously, increasing efficiency for environmental sensing.

Summary: The new technology acts like a coin counter, but at a microscopic level. It sorts one type of chemical from another, providing the total amount of a target chemical at the end. The tool uses custom probes with a gold electrode that only allows the target groundwater contaminants to stick while the other chemicals bounce off.

Sulfur likes to bind to gold and it also tends to react with pertechnetate, making sulfur-containing compounds an ideal intermediate in tool development. The sulfur sticks to the gold probe, then reacts with the pertechnetate, which forms a precipitate. The precipitate inhibits an electric current pulsing through the probe, providing an inverse measurement of pertechnetate concentration.

What’s Next: While this work was specifically focused on pertechnetate, there is potential to expand the technology to simultaneous multiple targets with the goal of increasing the efficiency of environmental measurements.

Sponsors: This research was funded by the Laboratory Directed Research and Development program at PNNL and by the Deep Vadose Zone program under the U.S. Department of Energy’s (DOE’s) Office of Environmental Management. Part of this research was performed at the Environmental Molecular Sciences Laboratory, a national user facility at PNNL managed by the DOE Office of Biological and Environmental Research.

PNNL Research Team: Sayandev Chatterjee, Meghan S. Fujimoto, Yingge Du, Gabriel B. Hall, Nabajit Lahiri, Eric D. Walter, Libor Kovarik. ACS Sensors cover illustration by Rose Perry, PNNL.

 

March 27, 2020
MARCH 12, 2020
Web Feature

Tracking Toxics in the Salish Sea

With the help of a diagnostic tool called the Salish Sea Model, researchers found that toxic contaminant hotspots in the Puget Sound are tied to localized lack of water circulation and cumulative effects from multiple sources.

Creating better models to predict subsurface water flow and transport

river soil

New framework improves the predictions of subsurface sediment permeability

February 19, 2020
February 17, 2020
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The Science
Co-authors of a paper in Water Resources Research led by PNNL researchers developed a new iterative data assimilation framework to more accurately describe the permeability of subsurface sediments in numerical models when using facies, a system that classifies dissimilar sediments into distinct geological units that share important features of interest to modelers. The iterative framework applies data from field observations and experiments to inform the delineation of facies at the start of each model run. Further refinements are achieved at each iteration through the application of statistical constraints that maintain geologic continuity among adjacent locations.

Distribution of Facies
Spatial distribution of three facies (red, yellow and blue colors) in a 2D vertical cross section of a 3D case. Figures show the new method provides a more accurate and continuous estimation of facies distribution compared to the conventional method. White colors in the figures are bore samples and black dots are the conditioning points selected by the new method.

The Impact
Spatial distribution of three facies (red, yellow and blue colors) in a 2D vertical cross section of a 3D case. Figures show the new method provides a more accurate and continuous estimation of facies distribution compared to the conventional method. White colors in the figures are bore samples and black dots are the conditioning points selected by the new method.

More realistic numerical representations of the permeability of subsurface sediments lead to improved predictions of groundwater flow and the concentration of constituents that are transported with the flow. The data assimilation framework can also be applied to estimate other subsurface properties from field measurements, or from data from other systems such as watersheds, as long as they can be categorized into a few discrete representative units.

Summary
Observational data on subsurface permeability is limited for most watersheds because of the impracticality of digging enough boreholes or wells to capture the heterogeneous nature of the subsurface environment. To solve for this limitation, researchers have widely adopted approaches that estimate permeability from field experiments such as a) measuring how water levels at a cluster of wells change when water is pumped at a nearby well, or b) monitoring how quickly a tracer released at one well reaches other wells in the aquifer. The U.S. Department of Energy’s Hanford 300 Area Integrated Field Research Challenge site, for example, is well characterized from data assimilation methods that were used to understand the long-term persistence of nuclear fuel fabrication wastes disposal from 1943 to 1975.

The use of a facies approach to segment the subsurface reduces complexity in numerical models by grouping heterogeneous sediments into distinct homogenous units defined by hydraulic, physical and or chemical properties. A major difficulty with existing facies-based approaches in numerical models is that each facies is treated as its own, independent unit. Therefore, these models fail to capture the spatial continuity of subsurface sediments. The authors of this paper developed a framework that maintains continuity between neighboring facies in numerical models and thus better reflects true subsurface geology, and thereby groundwater movement. The improvements come from an iterative data assimilation approach that incorporates direct and indirect data about subsurface permeability gathered from field observations and experiments at the start of each model run as well as the application of statistical constraints about subsurface geology. The data assimilation and statistical constraint steps are re-imposed for each iteration, leading to refined facies delineation. This framework reduces uncertainty about the spatial distribution of sediment types in the subsurface, which results in more accurate predictions of groundwater flow and constituent transport.

The authors evaluated the performance of the new framework on a two-dimensional, two-facies model and a three-dimensional, three-facies model of DOE’s well-characterized Hanford 300 Area that were conceptualized from borehole and field tracer experiments. The results of the research shows that the framework can identify facies spatial patterns and reproduce tracer breakthrough curves with much improved accuracy over facies-based approaches that lack spatial continuity constraints. With additional data, the authors say that the framework can also be used to categorize biogeochemical reactive units in an aquifer.

Contact
Xingyuan Chen, Earth Scientist, Xingyuan.Chen@pnnl.gov

Funding
Funding for this research came from DOE Office of Science BER, PNNL Subsurface Biogeochemical Research SFA.

Song, X., Chen, X., Ye, M., Dai, Z., Hammond, G., And Zachara, J.M. (2019). Delineating facies spatial distribution by integrating ensemble data assimilation and Indicator Geostatistics with level-set transformation. Water Resources Research, 55. https://doi.org/10.1029/2018WR023262

March 9, 2019
JANUARY 21, 2020
Web Feature

Forensic Proteomics: Beyond DNA Profiling

A new book by PNNL biochemist Erick Merkley details forensic proteomics, a technique that directly analyzes proteins in unknown samples, in pursuit of making proteomics a widespread forensic method when DNA is missing or ambiguous.
JANUARY 10, 2020
Web Feature

Clark Recognized for Nuclear Chemistry Research

The world’s largest scientific society honored Sue B. Clark, a PNNL and WSU chemist, for contributions toward resolving our legacy of radioactive waste, advancing nuclear safeguards, and developing landmark nuclear research capabilities.
DECEMBER 6, 2019
Web Feature

Converging on Coastal Science

Advancing a more collective understanding of coastal systems dynamics and evolution is a formidable scientific challenge. PNNL is meeting the challenge head on to inform decisions for the future.

PNNL Launches Marine Renewable Energy Database

Logo of Tethys Engineering

PNNL created an online database to share information related to the marine renewable energy industry.

Tethys Engineering addresses industry’s technical and engineering challenges

November 18, 2019
November 18, 2019
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Marine renewable energy (MRE) has the potential to provide 90 gigawatts of power in the United States through waves and tidal and ocean currents.

To harness the ocean’s energy, the MRE industry needs to understand how to address technical and engineering challenges such as efficient power takeoff, device survivability, and grid integration.

PNNL developed Tethys Engineering in September 2019 to allow sharing resources around the deployment of devices in corrosive, high-energy marine environments. The recently launched Tethys Engineering online database includes collected and curated documents surrounding the technical and engineering development of MRE devices. Users can search and filter results to intuitively identify information relevant to developers, researchers, and regulators.

Tethys Engineering includes more than 3,000 journal articles, conference papers, reports, and presentations related to wave, current, salinity gradient, and ocean thermal energy conversion technologies. The database contains information from around the world.

The Tethys Engineering database was created as a companion to the already established Tethys website, which focuses on the environmental effects of the MRE industry.

November 18, 2019