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DOE OSTI2025

Real-time elemental analysis of liquids for process monitoring using laser-induced breakdown spectroscopy with a liquid wheel sampling approach

This article presents an engineered sampling system that used a rotating wheel to form a thin liquid layer, permitting the use of laser-induced breakdown spectroscopy (LIBS) for in situ, real-time elemental impurity quantification during liquid processing. The sampling approach was demonstrated on eight elements from across the periodic table (Na, Al, K, Ca, Ti, Sr, Mo, and Yb). Univariate and multivariate calibrations were presented for each element. The average value for percent root mean square errors of cross-validation for the multivariate models was 3.64%, highlighting the method's strong prediction accuracy. Additionally, the limits of detection for each analyte were estimated from their univariate models: Na = 0.0532, Al = 18.5, K = 0.105, Ca = 0.273, Ti = 67.7, Sr = 0.640, Mo = 22.4, and Yb = 22.9 μg mL –1 . Finally, a test in which multivariate models were used to monitor a liquid system for 80 min was performed to investigate the real-time monitoring capabilities of this liquid LIBS sampling approach. Rigorous measurements were performed to effectively predict the absence and concentrations of multiple analytes as they were spiked and diluted. This demonstration showed the feasibility of using LIBS for real-time liquid quantification models with estimated precision ≤ 8.1%. Finally, the limitations of this approach and potential future improvements are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Environmental, Health and Safety Assessment Application of a Heat Integrated, Post-combustion CO2 Capture System Using Monoethanolamine and Hitachi H3-1 Solvent at the E.W. Brown Coal-fired Power Plant

An Environmental Health and Safety (EH&S) Assessment was completed for operation of a pilot scale carbon dioxide (CO2) capture system (CCS) at the Louisville Gas & Electric (LG&E) and Kentucky Utilities (KU) Energy, LLC (LG&E-KU) E. W. Brown Generating Station in Harrodsburg, Mercer County, Kentucky. The pilot system was evaluated using two CO2 capture solvents, monoethanolamine (MEA) and Hitachi’s H3-1 solvent. The purpose of the EH&S Assessment was to determine if there were any unacceptable environmental, health or safety concerns that may prevent operation or environmental permitting of a larger scale pilot scale plant. The assessment included review of process flow diagrams, input and output flow rates for primary materials, literature describing similar processes and chemicals used or created during the process, actual air emission and wastewater test data and air emission calculations. The evaluation included identification of risks related to hazardous chemicals, air emissions, wastewater discharges, solid wastes generated and employee hazards. Most potential EH&S issues that were identified are commonly found and successfully managed at large industrial facilities. No risks were identified that could not be successfully managed or would likely prevent implementation or environmental permitting of the pilot or larger scale plant. Potential exposures and resulting health risks from exposure to low concentrations of nitrosamines generated from degradation of the Hitachi H3-1 and possibly MEA solvents may be a health concern for site workers, but additional investigation is needed to accurately assess this risk. Applying the information gained from operating the pilot plant, performing air emission testing and used solvent testing to a large-scale facility at a commercial coal-fired electric generating plant suggests additional air emission control measures may be necessary to reduce potential site worker health risks and possibly community risks. Depending upon the location and regional air quality, considerable effort may be required to obtain the necessary air permit for construction and operation of a similarly configured large-scale PCCCS facility.

gas separation↗

DOE OSTI2020

Environmental, Health and Safety Assessment Application of a Heat Integrated, Post-combustion CO 2 Capture System Using Monoethanolamine and Hitachi H3-1 Solvent at the E.W. Brown Coal-Fired Power Plant

An Environmental Health and Safety (EH&S) Assessment was completed for operation of a pilot scale carbon dioxide (CO 2 ) capture system (CCS) at the Louisville Gas & Electric (LG&E) and Kentucky Utilities (KU) Energy, LLC (LG&E-KU) E. W. Brown Generating Station in Harrodsburg, Mercer County, Kentucky. The pilot system was evaluated using two CO 2 capture solvents, monoethanolamine (MEA) and Hitachi’s H3-1 solvent. The purpose of the EH&S Assessment was to determine if there were any unacceptable environmental, health or safety concerns that may prevent operation or environmental permitting of a larger scale pilot scale plant. The assessment included review of process flow diagrams, input and output flow rates for primary materials, literature describing similar processes and chemicals used or created during the process, actual air emission and wastewater test data and air emission calculations. The evaluation included identification of risks related to hazardous chemicals, air emissions, wastewater discharges, solid wastes generated and employee hazards. Most potential EH&S issues that were identified are commonly found and successfully managed at large industrial facilities. No risks were identified that could not be successfully managed or would likely prevent implementation or environmental permitting of the pilot or larger scale plant. Potential exposures and resulting health risks from exposure to low concentrations of nitrosamines generated from degradation of the Hitachi H3-1 and possibly MEA solvents may be a health concern for site workers, but additional investigation is needed to accurately assess this risk. Applying the information gained from operating the pilot plant, performing air emission testing and used solvent testing to a large-scale facility at a commercial coal-fired electric generating plant suggests additional air emission control measures may be necessary to reduce potential site worker health risks and possibly community risks. Depending upon the location and regional air quality, considerable effort may be required to obtain the necessary air permit for construction and operation of a similarly configured large-scale PCCCS facility.

gas separation↗

DOE OSTI2017

'A Good Decision Is Based On Information, Not On Numbers' - A Process For National Strategic Decision Making - 17203

Waste management decision making is the process used by waste owners to determine and justify choices in across the lifecycle of a waste (from the manner of generation or retrieval to final disposition). In the UK, waste owners in the nuclear industry are obligated, by their environmental permits and authorisations, to demonstrate the application of robust and well-underpinned decision making processes for waste management. This is captured through the requirement for waste owners to demonstrate the identification and implementation of Best Available Technique (BAT). The National Waste Programme (NWP), led by LLW Repository Ltd, is a UK wide programme which leads the implementation of the UK National Strategy for the management of solid LLW from the nuclear industry [1] and which aims to deliver a self-sustaining culture for optimised management of Low Level Waste (LLW) in the UK. Recognising the requirement on waste owners, the NWP has - in conjunction with appointed contractors - led the development and publication of national strategic optioneering studies (so-called national strategic BAT studies) to support waste owners. Recognising the benefits that this approach to optioneering and strategic decision making could have for other waste producers, this paper provides an overview of the process used for the development of the suite of national strategic BAT assessments for the NWP. It details: the main phases of the process, the key features of each process phase, the benefits of the approach and key learning from its deployment in practice. Note: The legislative regime in England and Wales requires the identification and application of BAT. There is an equivalent regime in Scotland known as Best Practicable Environmental Option (BPEO) and Best Practicable Means (BPM). The requirements are comparable across the two legislative regimes and, for the purposes of simplicity, the term BAT will be utilised in this paper. The approach and outcomes of the national strategic optioneering process described are applicable across the UK. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2019

X-rays put molecules into a spin

The past decade has witnessed the emergence of a new X-ray light source technology that has been under development for some decades: the so-called self-amplified spontaneous emission-based free-electron laser (FEL). Furthermore, such lasers provide pulses with durations from just below 1 fs (10 –15 s) to over 100 fs and with energies from a few microjoules to a few millijoules, permitting the study of, for example, nonlinear optical effects (1), ultrafast processes (2), coherent diffractive imaging of biological systems such as protein crystals (3, 4), and mimivirus (5). After the opening of the first extreme-UV to soft X-ray user facility, namely FLASH in the Deutsches Elektronen-Synchrotron at Hamburg, Germany (6), a number of other machines covering the extreme-UV (FERMI FEL-1, DALIAN), soft X-ray (FERMI FEL-2, FLASH1/FLASH2), and hard X-ray spectral ranges (LCLS, PAL-XFEL, SACLA, and XFEL) have been opened to users from a wide range of scientific and engineering disciplines.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2018

Advancing Risk‐Informed Decision Making in Managing Defense Nuclear Waste in the United States: Opportunities and Challenges for Risk Analysis

Abstract An omnibus spending bill in 2014 directed the Department of Energy to analyze how effectively Department of Energy (DOE) identifies, programs, and executes its plans to address public health and safety risks that remain as part of DOE's remaining environmental cleanup liabilities. A committee identified two dozen issues and associated recommendations for the DOE, other federal agencies, and the U.S. Congress to consider, as well as other stakeholders such as states and tribal nations. In regard to risk assessment, the committee described a risk review process that uses available data, expert experience, identifies major data gaps, permits input from key stakeholders, and creates an ordered set of risks based on what is known. Probabilistic risk assessments could be a follow‐up from these risk reviews. In regard to risk management, the states, in particular, have become major drivers of how resources are driven. States use different laws, different priorities, and challenge DOE's policies in different ways. Land use decisions vary, technology choices are different, and other notable variations are apparent. The cost differences associated with these differences are marked. The net result is that resources do not necessarily go to the most prominent human health and safety risks, as seen from the national level.

Greenberg, Michael R.↗

DOE OSTI2024

Influences of the South American Low-Level Jet on the Convective Environment in Central Argentina Using a Convection-Permitting Simulation

This study documents the spatial and temporal distribution of the South American low-level jet (SALLJ) and quantifies its impact on the convective environment using a 6.5-month convection-permitting simulation during the Remote Sensing of Electrification, Lightning, And Mesoscale/Microscale Processes with Adaptive Ground Observations and Clouds, Aerosols, and Complex Terrain Interactions (RELAMPAGO-CACTI) campaigns. Overall, the simulation reproduces the observed SALLJ characteristics in central Argentina near the Sierras de Córdoba (SDC), a focal point for terrain-focused upscale growth. SALLJs most frequently occur in the summer with maxima to the northwest and east of the SDC and minima over the higher terrain. The shallower SALLJs (<1750 m) have a strong overnight skew, while the elevated jets are more equally spread throughout the day. SALLJ periods often have higher amounts of low-level moisture and instability compared to non-SALLJ periods, with these impacts increasing over time when the SALLJ is present and decreasing afterward. The SALLJ may enhance low-level wind shear magnitudes (particularly when accounting for the jet height); however, enhancement is somewhat limited due to the presence of speed shear in most situations. SALLJ periods are associated with low-level directional shear favorable for organized convection and an orientation of cloud-layer wind shear parallel to the terrain, which could favor upscale growth. A case study is shown in which the SALLJ influenced both the magnitude and direction of wind shear concurrent with convective upscale growth near the SDC. This study highlights the complex relationship between the SALLJ and its impacts during periods of widespread convection.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Shallow cumulus entrainment: observational retrieval, physical interpretation, and climate impacts (Final grant report)

This document constitutes a final technical report for DE-SC0020083, a research grant awarded by the US Department of Energy Office of Science, to Prof. Daniel Kirshbaum at McGill University. The original research proposal, entitled "Shallow cumulus entrainment: observational retrieval, physical interpretation, and climate impacts", defined four scientific objectives that synthesized ARM observations with turbulence-permitting large-eddy simulations (LES) to quantify and understand the process of cumulus entrainment, whereby a cumulus cloud ingests surrounding air through its lateral edges. These objectives included developing observational climatologies of cumulus bulk entrainment rate at two ARM observatories, physical interpretation of these findings using LES, quantification of the impacts of subcloud circulations on entrainment, and the climate impacts of flow-dependent entrainment variations. In the six years that have elapsed since the grant was awarded (three funded years and three no-cost annual extensions), all four of the objectives were successfully addressed. Four personnel were trained (one B.Sc., one M.Sc. to completion, five years of Ph.D. training, and 2.5 years of postdoctoral training), eight peer-reviewed articles were published in high-impact journals, and 20 presentations were delivered (three invited).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Cathode system for electrodeposition of metals on microspheres

The present disclosure relates to an apparatus for electroplating an element. The apparatus may comprise a cathode cage assembly. The cathode cage assembly may include a cage member and at least one electrically conductive wire extending along at least a portion of the cage member. The wire may be arranged to form at least one volume within the cage member for retaining an element within the cage member. The cage member and the wire permit a degree of movement of the element during an electroplating process while retaining the element within the volume.

Bunn, Thomas L.↗

DOE OSTI2023

Semiannual Categorical Process Report - January Through June 2023

The Sandia National Laboratories, in California (SNL/CA) is a research and development facility, owned by the U.S. Department of Energy’s National Nuclear Security Administration agency (DOE/NNSA). The laboratory is located in the City of Livermore (the City) and is comprised of approximately 410 acres. The SNL/CA facility is operated by National Technology and Engineering Solutions of Sandia, LLC (NTESS) under a contract with the DOE/NNSA. The DOE/ NNSA’s Sandia Field Office (SFO) oversees the operations of the site. North of the SNL/CA facility is the Lawrence Livermore National Laboratory (LLNL), in which SNL/CA’s sewer system combines with before discharging to the City’s Publicly Owned Treatment Works (POTW) for final treatment and processing. The City’s POTW authorizes the wastewater discharge from SNL/CA via the assigned Wastewater Discharge Permit #1251 (the Permit), which is issued to the DOE/NNSA’s main office for Sandia National Laboratories, located in New Mexico (SNL/NM). The Monitoring and Reporting Condition 2.B of the Permit requires compliance with the semiannual reporting requirements contained in federal categorical pretreatment standards regulations (40 CFR 403.12). These regulations set numerical limits on the concentration of pollutants allowed to discharge from certain categories of industrial processes. This report is submitted to the City to satisfy this reporting requirement.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Supersaturation Variability from Scalar Mixing: Evaluation of a New Subgrid-Scale Model Using Direct Numerical Simulations of Turbulent Rayleigh–Bénard Convection

We report that supersaturation fluctuations in the atmosphere are critical for cloud processes. A nonlinear dependence on two scalars - water vapor and temperature - leads to different behavior than single scalars in turbulent convection. For modeling such multiscalar processes at subgrid scales (SGS) in large-eddy simulations (LES) or convection-permitting models, a new SGS scheme is implemented in CM1 that solves equations for SGS water vapor and temperature fluctuations and their covariance. The SGS model is evaluated using benchmark direct-numerical simulations (DNS) of turbulent Rayleigh–Bénard convection with water vapor as in the Michigan Tech Pi Cloud Chamber. This idealized setup allows thorough evaluation of the SGS model without complications from other atmospheric processes. DNS results compare favorably with measurements from the chamber. Results from LES using the new SGS model compare well with DNS, including profiles of water vapor and temperature variances, their covariance, and supersaturation variance. SGS supersaturation fluctuations scale appropriately with changes to the LES grid spacing, with the magnitude of SGS fluctuations decreasing relative to those at the resolved scale as the grid spacing is decreased. Sensitivities of covariance and supersaturation statistics to changes in water vapor flux relative to thermal flux are also investigated by modifying the sidewall conditions. Relative changes in water vapor flux substantially decrease the covariance and increase supersaturation fluctuations even away from boundaries.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Small-Scale Engineered High Flexibility Gasifier

This project advances a small-scale gasification unit as the first step in syngas-based hydrogen, chemicals, and synthetic fuels production. This unit is associated with an enhanced flexibility to different carbonaceous feedstocks including different types of coals, biomass, and plastics. The purpose of the project was to demonstrate feasibility and efficiency of coal pyrolysis in an auger reactor (pyrolyzer); supplemental methane and pyrolysis gas conversion into syngas in a proprietary non-catalytic converter; combined performance of pyrolyzer and non-catalytic converter to convert coal into syngas The proposed technology is based on an application of an intermediate speed pyrolysis at the temperature range 400-600°C as the first stage of biomass processing. At an industrial scale, an incorporation of coal pyrolysis into a feeding machine – auger-reactor allows to decrease its capital cost. At a pilot scale, it permits to employ electricity to build a compact device for testing of downstream equipment. The auger-reactor (pyrolyzer) generates pyrolysis gas and char practically from any carbonaceous feedstocks but their compositions and quantities are determined by their types. Pyrolysis gas is converted into syngas (mix of H 2 and CO) in a novel, proprietary hydrogen flame assisted non-catalytic converter which employs O 2 instead of air as an oxidizer. This reactor (converter) allows an easy adjustment to different pyrolysis gas compositions and tolerates a presence of sulfur and nitrogen contaminants. Our technology assumes carbonaceous feedstocks gasification with oxygen to allow the products H 2 , CO or CO 2 to be not diluted in N 2 and ready for the following synthesis of chemicals and fuels. Due to the same reason, it permits a more efficient CO 2 capture for its transport and storage. An implementation of our small-scale gasification process may overcome economic constrains by a flexible acceptance of coal, biomass, and plastics as well as their unsorted mixtures to make syngas for the following production of pure hydrogen, chemical and/or synthetic fuels.

42 ENGINEERING↗

DOE OSTI2023

Direct Imaging of Antiferromagnet-Ferromagnet Phase Transition in van der Waals Antiferromagnet CrSBr

The advent of van der Waals (vdW) ferromagnetic (FM) and antiferromagnetic (AFM) materials offers unprecedented opportunities for spintronics and magneto-optic devices. Combining magnetic Kerr microscopy and density functional theory calculations, the AFM-FM transition is investigated and a surprising abnormal magneto-optic anisotropy in vdW CrSBr associated with different magnetic phases (FM, AFM, or paramagnetic state) is discovered. This unique magneto-optic property leads to different anisotropic optical reflectivity from different magnetic states, permitting direct imaging of the AFM Néel vector orientation and the dynamic process of the AFM-FM transition within a magnetic field. Using Kerr microscopy, not only the domain nucleation and propagation process is imaged but also the intermediate spin-flop state in the AFM-FM transition is identified. In conclusion, the unique magneto-optic property and clear identification of the dynamics process of the AFM-FM phase transition in CrSBr demonstrate the promise of vdW magnetic materials for future spintronic technology.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Sputter-deposited CdMgTe for rear contact to CdSeTe/CdTe solar cells

CdTe-based photovoltaic device performance improvement is predominantly limited by open-circuit voltage. This work approaches the voltage deficit challenge through the incorporation of a cadmium magnesium telluride (CdMgTe) electron reflector layer at the back of 1.5- μm CdSeTe/CdTe absorbers to reduce back-surface recombination through a conduction band offset. A sputtered CdMgTe electron reflector layer permitted low fabrication temperatures and circumvented the intolerance of CdMgTe to thermal processing present in traditional close-space sublimation (CSS)-deposited CdMgTe devices. Here, we demonstrate that sputtered CdMgTe simultaneously promotes the retention of chlorine passivation and magnesium which is not feasible with CSS fabrication. We also show the importance of the Cu and Te back contact order in CdMgTe devices. Through the optimization of the sputtered CdMgTe substrate temperature, doping, and back structure configuration, 1.5 μm CdSeTe/CdTe devices with a sputtered CdMgTe layer achieved an efficiency of 16.0%, significantly higher than with CSS CdMgTe, and demonstrated partial enactment of electron-reflector behavior.

14 SOLAR ENERGY↗

DOE OSTI2017

Phase-Transfer Ligand Exchange of Lead Chalcogenide Quantum Dots for Direct Deposition of Thick, Highly Conductive Films

Here, the use of semiconductor nanocrystal quantum dots (QDs) in optoelectronic devices typically requires postsynthetic chemical surface treatments to enhance electronic coupling between QDs and allow for efficient charge transport in QD films. Despite their importance in solar cells and infrared (IR) light-emitting diodes and photodetectors, advances in these chemical treatments for lead chalcogenide (PbE; E = S, Se, Te) QDs have lagged behind those of, for instance, II–VI semiconductor QDs. Here, we introduce a method for fast and effective ligand exchange for PbE QDs in solution, resulting in QDs completely passivated by a wide range of small anionic ligands. Due to electrostatic stabilization, these QDs are readily dispersible in polar solvents, in which they form highly concentrated solutions that remain stable for months. QDs of all three Pb chalcogenides retain their photoluminescence, allowing for a detailed study of the effect of the surface ionic double layer on electronic passivation of QD surfaces, which we find can be explained using the hard/soft acid–base theory. Importantly, we prepare highly conductive films of PbS, PbSe, and PbTe QDs by directly casting from solution without further chemical treatment, as determined by field-effect transistor measurements. This method allows for precise control over the surface chemistry, and therefore the transport properties of deposited films. It also permits single-step deposition of films of unprecedented thickness via continuous processing techniques, as we demonstrate by preparing a dense, smooth, 5.3-μm-thick PbSe QD film via doctor-blading. As such, it offers important advantages over laborious layer-by-layer methods for solar cells and photodetectors, while opening the door to new possibilities in ionizing-radiation detectors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

TRACER-BC2-SP2 Field Campaign Report

The focus of this project was to assess black carbon and brown carbon aerosol in Houston, Texas during the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) user facility Tracking Aerosol Convection Interactions Experiment (TRACER) through the co-located deployment of a single-particle soot photometer (SP2) with the University of Houston/Baylor aerosol optical instrumentation in the Texas (BC)2 network in and around Houston. The deployment of the SP2 enables us to expand the spatial assessment of black carbon (BC) in Houston during TRACER by permitting a more thorough characterization of BC, including sources, transport, and potential processing. BC is well known to undergo physical and chemical changes during local and long-range transport that will impact its optical properties. By deploying multiple SP2s in the Houston area, the impacts of local and long-range transport can be assessed. The TRACER-BC2-SP2 campaign will expand spatial and temporal characterization of BC in the Houston area during TRACER and link the TRACER-carbon analysis to ongoing black and brown carbon monitoring (Texas [BC]2 network) in Houston.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Electrochemistry-induced deposition for controlled formation of metal–organic framework films on insulator and conductor substrates

A number of technological applications of metal–organic frameworks (MOFs) require the formation of their thin films on insulator and/or conductor substrates at selected areas with desired thicknesses. However, fabrication of such MOF films often requires multi-step processes and/or sophisticated instruments. Herein, we discuss electrochemistry-induced MOF deposition, which permits the direct formation of a thin MOF film with controlled thickness at a desired area on various substrates. So far, we have reported the applicability of this deposition method for the formation of zeolitic imidazolate framework-8 (ZIF-8) films. In this method, a ZIF-8 film is formed on an insulator or a conductor substrate upon applying a cathodic potential to a working electrode that is placed above the substrate. Importantly, the film is formed just below the cathodic working electrode, indicating that the position and lateral dimensions (on the mm- to μm-scale) of the film can be controlled by those of the working electrode. In addition, film thickness is controllable in the range of tens to hundreds of nanometers by adjusting potential application conditions at the cathodic working electrode. These results show that the electrochemistry-induced deposition method will provide a simple means for the fabrication of a patterned MOF film on various substrates without additional lithographic processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Battery Energy Storage System (BESS) Licensing and Permitting [Slides]

This presentation provides an overview of the licensing, permitting, and regulatory frameworks governing Battery Energy Storage Systems (BESS) across multiple international contexts. It outlines foundational permitting considerations - including safety standards, siting requirements, regulatory and environmental obligations, and interconnection processes - alongside typical pathways for installation, approval, and inspection. The presentation summarizes key technical standards such as NFPA 855 and IEEE guidelines, and emphasizes best practices for safe and effective deployment. A series of detailed case studies from South Africa, Chile, Mexico, Brazil, Costa Rica, Honduras, and the Dominican Republic illustrates how different countries structure approval authority, evaluate environmental impacts, and integrate BESS into national grid systems. The deck concludes with insights on emerging challenges, including evolving regulatory frameworks, financial viability, and the need for pricing mechanisms that accurately value storage services.

24 POWER TRANSMISSION AND DISTRIBUTION↗