Machine Learning Prediction of Nitric Acid Extraction Behavior in PUREX Process.

Plutonium uranium reduction extraction (PUREX) is a liquid-liquid extraction process used to recover plutonium (Pu) and uranium (U) from irradiated uranium fuel for various nuclear-related applications. Despite extensive efforts, quantitative prediction of liquid-liquid extraction parameters, i.e.

Review of iodine behavior from nuclear fuel dissolution to environmental release.

During nuclear fuel reprocessing, radioiodine, can be released. The speciation of iodine drives its volatility, and partitioning processes are highly variable because they depend on facility operating conditions. Starting from iodine behavior in the fuel and progressing to its behavior in the environment, this review article describes the current understanding of iodine partitioning during aqueous fuel reprocessing.

Ruthenium speciation and distribution in the environment: A review.

The review focuses on speciation and migration of anthropogenic ruthenium (Ru) originated from nuclear industry releases and presents updated information regarding Ru in the environment. It provides analysis of the main pathways of Ru species distribution in the aqueous and terrestrial environment, starting from its natural occurrence, generation and release from anthropogenic sources, predominant speciation, and ending with bioaccumulation, which can be directly or indirectly related to human health. Literature sources belonging to the post-Chernobyl time frame were preferentially considered, in which Ru-103 and Ru-106 are the major fission isotopes studied due to their traceability in the environment and their relatively long half-lives.

Long-term, sustainable solutions to radioactive waste management.

Nuclear power plays a pivotal role in ensuring a scalable, affordable, and reliable low-carbon electricity supply. Along with other low-carbon energy technologies, nuclear energy is essential for reducing our reliance on fossil fuels, addressing climate change and air pollution, and achieving a sustainable economy. Whilst significant progress has been made in reducing the volume of final radioactive waste, its management remains one of the most important challenges when considering the continued use and expansion of nuclear energy.

Accumulation mechanisms for contaminants on weak-base hybrid ion exchange resins.

Mechanism of hexavalent chromium removal (Cr(VI) as CrO) by the weak-base ion exchange (IX) resin ResinTech® SIR-700-HP (SIR-700) from simulated groundwater is assessed in the presence of radioactive contaminants iodine-129 (as IO), uranium (U as uranyl UO), and technetium-99 (as TcO), and common environmental anions sulfate (SO) and chloride (Cl). Batch tests using the acid sulfate form of SIR-700 demonstrated Cr(VI) and U(VI) removal exceeded 97%, except in the presence of high SO concentrations (536 mg/L) where Cr(VI) and U(VI) removal decreased to ≥ 80%. However, Cr(VI) removal notably improved with co-mingled U(VI) that complexes with SO at the protonated amine sites.

Reductive removal of pertechnetate and chromate by zero valent iron under variable ionic strength conditions.

Radioactive technetium-99 (Tc) present in waste streams and subsurface plumes at legacy nuclear reprocessing sites worldwide poses potential risks to human health and environment. This research comparatively evaluated efficiency of zero-valent iron (ZVI) toward reductive removal of Tc(VII) in presence of Cr(VI) from NaCl and NaSO electrolyte solutions under ambient atmospheric conditions. In both electrolytes, anticorrosive Cr(VI) suppressed oxidation of ZVI at elevated concentrations resulting in the delay of initiation of Tc(VII) reduction to Tc(IV).

Water Defect Stabilizes the Bi Lone-Pair Electronic State Leading to an Unusual Aqueous Hydration Structure.

The aqueous hydration structure of the Bi ion is probed using a combination of extended X-ray absorption fine structure (EXAFS) spectroscopy and density functional theory (DFT) simulations of ion-water clusters and condensed-phase solutions. Anomalous features in the EXAFS spectra are found to be associated with a highly asymmetric first-solvent water shell. The aqueous chemistry and structure of the Bi ion are dramatically controlled by the water stabilization of a lone-pair electronic state involving the mixed 6s and 6p orbitals.

Removable coatings: Thermal stability and decontamination of steel surfaces from Am.

This study presents a comparative analysis of several commercial removable materials for radioactive decontamination of steel surfaces using Am as representative radionuclide. The selection criteria of removable coatings for this study included a history of application, commercial availability, easy handling conditions and different composition and formulation. Carbon steel and stainless steel coupons were utilized as common industrial materials, and the experimental series were expanded to include the rusting treatment of these surfaces as it is common for decommissioned nuclear facilities.

Time dependent zero valent iron oxidation and the reductive removal of pertechnetate at variable pH.

Elemental iron Fe is a promising reductant for removal of radioactive technetium-99 (Tc) from complex aqueous waste streams that contain sulfate, halides, and other inorganic anions generated during processing of legacy radioactive waste. The impact of sulfate on the kinetics of oxidation and reduction capacity of Fe in the presence of Tc has not been examined. We investigated the oxidative transformation of Fe and reductive removal of TcO in 0.

Simultaneous immobilization of aqueous co-contaminants using a bismuth layered material.

The remediation of co-located contaminants in the vadose zone can be challenging due to accessibility and responses of different contaminants to remedial actions. At the Hanford Site (WA, USA), multiple radionuclides and other hazardous contaminants are present in the vadose zone and groundwater, including iodine-129 (I), technetium-99 (Tc), uranium-238 (U), chromium (Cr), and nitrate (NO). We evaluated a layered Bi oxyhydroxide material for its potential to remove individual and co-located contaminants with a series of batch experiments that investigated a range of plume conditions, followed by solid phase characterization of the reacted bismuth material.

Identification and Quantification of Technetium Species in Hanford Waste Tank AN-102.

Technetium-99 (Tc), a high yield fission product generated in nuclear reactors, is one of the most difficult contaminants to address at the U.S. Department of Energy Hanford, Savannah River, and other sites.

Spontaneous redox continuum reveals sequestered technetium clusters and retarded mineral transformation of iron.

The sequestration of metal ions into the crystal structure of minerals is common in nature. To date, the incorporation of technetium(IV) into iron minerals has been studied predominantly for systems under carefully controlled anaerobic conditions. Mechanisms of the transformation of iron phases leading to incorporation of technetium(IV) under aerobic conditions remain poorly understood.

Hybrid Sorbents for I Capture from Contaminated Groundwater.

Radioiodine (I) poses a risk to the environment due to its long half-life, toxicity, and mobility. It is found at the U.S.

Mechanisms of Plutonium Redox Reactions in Nitric Acid Solutions.

Plutonium (Pu) exhibits a complex redox behavior in aqueous solutions. This is due to the ability of the element to adapt a wide range of oxidation states typically from +3 to +6 and the tendency for dynamic interconversion between the oxidation states that primarily depend upon acid concentration and presence of coordinating ligands. This work interrogates the Pu redox behavior in aqueous nitric acid via a combination of voltammetry and in situ vis-NIR spectroelectrochemistry under controlled potentials to map the interconversion between the various Pu oxidation states.

Evolution of Acid-Dependent Am and Eu Organic Coordination Environment: Effects on the Extraction Efficiency.

Coordination of trivalent lanthanide and actinide metal ions by lipophilic diglycolamides and phosphonic acids has been proposed for their separation through extraction from aqueous nitric acid solutions. However, the nature of M coordination complexes in these combined solvent systems is not well understood, resulting in low predictability of their behavior. This work demonstrates that a combination of ,,','-tetrakis(2-ethylhexyl)diglycolamide (T2EHDGA) and weakly acidic 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) in -dodecane exhibits a complicated extraction mechanism for Eu and Am, which continuously evolves as a function of the aqueous phase acidity.

Technetium immobilization by materials through sorption and redox-driven processes: A literature review.

The objective of this review is to evaluate materials for use as a barrier or other deployed technology to treat technetium-99 (Tc) in the subsurface. To achieve this, Tc interactions with different materials are considered within the context of remediation strategies. Several naturally occurring materials are considered for Tc immobilization, including iron oxides and low solubility sulfide phases.

Iodine immobilization by materials through sorption and redox-driven processes: A literature review.

Radioiodine-129 (I) in the subsurface is mobile and limited information is available on treatment technologies. Scientific literature was reviewed to compile information on materials that could potentially be used to immobilize I through sorption and redox-driven processes, with an emphasis on ex-situ processes. Candidate materials to immobilize I include iron minerals, sulfur-based materials, silver-based materials, bismuth-based materials, ion exchange resins, activated carbon, modified clays, and tailored materials (metal organic frameworks (MOFS), layered double hydroxides (LDHs) and aerogels).

Evaluation of materials for iodine and technetium immobilization through sorption and redox-driven processes.

Radioactive iodine-129 (I) and technetium-99 (Tc) pose a risk to groundwater due to their long half-lives, toxicity, and high environmental mobility. Based on literature reviewed in Moore et al. (2019) and Pearce et al.

Author Correction: Closing the Nuclear Fuel Cycle with a Simplified Minor Actinide Lanthanide Separation Process (ALSEP) and Additive Manufacturing.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Closing the Nuclear Fuel Cycle with a Simplified Minor Actinide Lanthanide Separation Process (ALSEP) and Additive Manufacturing.

Expanded low-carbon baseload power production through the use of nuclear fission can be enabled by recycling long-lived actinide isotopes within the nuclear fuel cycle. This approach provides the benefits of (a) more completely utilizing the energy potential of mined uranium, (b) reducing the footprint of nuclear geological repositories, and (c) reducing the time required for the radiotoxicity of the disposed waste to decrease to the level of uranium ore from one hundred thousand years to a few hundred years. A key step in achieving this goal is the separation of long-lived isotopes of americium (Am) and curium (Cm) for recycle into fast reactors.

Comparative analysis of ZVI materials for reductive separation of Tc(VII) from aqueous waste streams.

Technetium-99 (Tc) is a long-lived radioactive contaminant present in legacy nuclear waste streams and contaminated plumes of the nuclear waste storage sites worldwide that poses risks for human health and the environment. Pertechnetate (TcO), the most common chemical form of Tc under oxidative conditions, is of particular concern due to its high aqueous solubility and mobility in the subsurface. One approach to treatment and remediation of TcO is reduction of Tc to less soluble and mobile Tc and its removal from the contaminated streams such as liquid secondary waste generated during vitrification of the Hanford low activity tank waste.

Combinations of NIR, Raman spectroscopy and physicochemical measurements for improved monitoring of solvent extraction processes using hierarchical multivariate analysis models.

The reliability of chemical processes can be greatly improved by implementing inline monitoring systems. Combining multivariate analysis with non-destructive sensors can enhance the process without interfering with the operation. We present here hierarchical models using both principal component analysis and partial least square analysis developed for different chemical components representative of solvent extraction process streams.

Spectroscopic Characterization of Aqua [ fac-Tc(CO)] Complexes at High Ionic Strength.

Understanding fundamental Tc chemistry is important to both the remediation of nuclear waste and the reprocessing of nuclear fuel; however, current knowledge of the electronic structure and spectral signatures of low-valent Tc compounds significantly lags behind the remainder of the d-block elements. In particular, identification and treatment of Tc speciation in legacy nuclear waste is challenging due to the lack of reference data especially for Tc compounds in the less common oxidation states (I-VI). In an effort to establish a spectroscopic library corresponding to the relevant conditions of extremely high ionic strength typical for the legacy nuclear waste, compounds with the general formula of [ fac-Tc(CO)(OH)(OH) ] (where n = 0-3) were examined by a range of spectroscopic techniques including Tc/C NMR, IR, XPS, and XAS.

Theoretical Modeling of (99)Tc NMR Chemical Shifts.

Technetium-99 (Tc) displays a rich chemistry due to its wide range of accessible oxidation states (from -I to +VII) and ability to form coordination compounds. Determination of Tc speciation in complex mixtures is a major challenge, and (99)Tc nuclear magnetic resonance (NMR) spectroscopy is widely used to probe chemical environments of Tc in odd oxidation states. However, interpretation of (99)Tc NMR data is hindered by the lack of reference compounds.

Highly Selective Colorimetric and Luminescence Response of a Square-Planar Platinum(II) Terpyridyl Complex to Aqueous TcO4(-).

Molecular recognition of an aqueous pertechnetate (TcO4(-)) anion is fundamentally challenging partly due to the charge-diffuse nature of this anion, which hampers design of new technologies for its separation and detection. To address this gap, simple salts of transition metal complexes that undergo a distinct spectroscopic change upon exposure to aqueous anions were explored. The Pt(II) complex [Pt(tpy)Br]SbF6 (tpy = 2,2';6',2″-terpyridine) undergoes a dramatic color change and intense luminescence response upon TcO4(-) uptake due to concomitant enhancement of Pt···Pt interactions.