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DOE OSTI2024

Preparation of ultrathin sputtered gold films on palladium as efficient oxygen reduction electro-catalysts

Herein, we present the preparation of ultrathin gold (Au) films on different M (M = Pd, Pt, Rh, Ir, and Ru) electrodes (Au/M) using magnetron sputtering deposition for oxygen reduction reaction (ORR). The ORR electro-catalytic activities of prepared Au/M catalysts increase as follows: Au/Ru < Au/Ir < Au/Rh < Au/Pt < Au/Pd. Accordingly, the oxygen reduction catalytic behaviors of the Au-modified palladium (Au/Pd) thin films with various Au thicknesses (0.16, 0.24, 0.5, and 1 nm) are investigated in acidic environments. It is found that Au modifications can promote oxygen reduction performances due to the development of more catalytic active sites on the Pd catalyst through the existence of Au atoms. Noticeably, Au/Pd samples exhibit a connection in oxygen reduction ability as a function of Au thickness, with the ultrathin 0.16 nm Au/Pd being the most active ORR catalyst. Significantly, the 0.16 nm Au/Pd material demonstrates superior stability after 1000 potential cycles compared with the 0.16 nm Pt/Pd owing to the influence of Au coating and structurally stable surfaces. Therefore, surface modification with the deposition of Au films on Pd represents a favorable technique to boost both the ORR capability and stability of the electro-catalysts.

Magnetron sputtering↗

DOE OSTI2023

In-field alpha spectrometry system for uranium enrichment verification of uranium hexafluoride

A portable In-Field Alpha Spectrometry (IFAS) system was developed to support on-site uranium enrichment determination for samples taken at facilities working with gaseous UF 6 . It consists of a modified commercial alpha spectrometer, a vacuum pump, a laptop computer, and associated connectors and cables. The IFAS uses specially designed Single-Use Destructive Assay (SUDA) samplers to capture gaseous UF 6 and convert and store it as UO 2 F 2 in a thin-film zeolite. To examine the quantitative performance of the IFAS system a large number of replicate SUDA samples was acquired for natural uranium (NU, 0.72 wt%, 23 samples), low enriched uranium 1 (LEU1, 2.33 wt% 235 U, 10 samples), and low enriched uranium 2 (LEU2, 4.62 wt% 235 U, 10 samples). The standard deviation (SD) values for uranium enrichment determination with the IFAS for NU, LEU1, and LEU2, in 20-hour assays, were 0.037 wt% 235 U, 0.063 wt% 235 U, and 0.072 wt% 235 U, respectively. In addition, a separate analysis suggests that comparable SD values can be achieved in less time, approximately 8-10 hours. For context, these SD values are well below the International Atomic Energy Agency’s International Target Values for the determination of uranium enrichment in non-destructive assay measurements.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2022

Computational Aspects of Single-Molecule Kinetics for Coupled Catalytic Cycles: A Spectral Analysis

Catalysis from single active sites is analyzed using methods developed from single molecule kinetics. Using a stochastic Markov state description, the observable properties of general catalytic networks of reactions are expressed using an eigenvalue decomposition of the transition matrix for the Markov process. By the use of a sensitivity analysis, the necessary eigenvalues and eigenvectors are related to the energies of controlling barriers and wells located along the reaction routes. A generalization of the energetic span theory allows the eigenvalues to be computed from several activation energies corresponding to distinct barrier-well pairings. The formalism is demonstrated accurately for model problems for a physically realistic mechanism for an alkene hydrogenation reaction on a single atom catalyst.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Radicals as Exceptional Electron-Withdrawing Groups: Nucleophilic Aromatic Substitution of Halophenols Via Homolysis-Enabled Electronic Activation

While heteroatom-centered radicals are understood to be highly electrophilic, their ability to serve as transient electron-withdrawing groups and facilitate polar reactions at distal sites has not been extensively developed. Here, we report a new strategy for the electronic activation of halophenols, wherein generation of a phenoxyl radical via formal homolysis of the aryl O-H bond enables direct nucleophilic aromatic substitution of the halide with carboxylate nucleophiles under mild conditions. Pulse radiolysis and transient absorption studies reveal that the neutral oxygen radical (O • ) is indeed an extraor-dinarily strong electron-withdrawing group [σ p - (O • ) = 2.79 vs. σ p - (NO 2 ) = 1.27]. Additional mechanistic and computational studies indicate that the key phenoxyl intermediate serves as an open-shell electron-withdrawing group in these reactions, lowering the barrier for nucleophilic substitution by more than 20 kcal/mol relative to the closed-shell phenol form of the substrate. Finally, by using radicals as transient activating groups, this homolysis-enabled electronic activation strategy provides a powerful platform to expand the scope of nucleophile-electrophile couplings and enable previously challenging transformations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

In situ electrochemical scanning/transmission electron microscopy of electrode–electrolyte interfaces

Insights into the dynamics of electrochemical processes are critically needed to improve our fundamental understanding of electron, charge, and mass transfer mechanisms and reaction kinetics that influence a broad range of applications, from the functionality of electrical energy-storage and conversion devices (e.g., batteries, fuel cells, and supercapacitors), to materials degradation issues (e.g., corrosion and oxidation), and materials synthesis (e.g., electrodeposition). To unravel these processes, in situ electrochemical scanning/transmission electron microscopy (ec-S/TEM) was developed to permit detailed site-specific characterization of evolving electrochemical processes that occur at electrode–electrolyte interfaces in their native electrolyte environment, in real time and at high-spatial resolution. This approach utilizes “closed-form” microfabricated electrochemical cells that couple the capability for quantitative electrochemical measurements with high spatial and temporal resolution imaging, spectroscopy, and diffraction. Here, we review the state-of-the-art instrumentation for in situ ec-S/TEM and how this approach has resulted in new observations of electrochemical processes.

25 ENERGY STORAGE↗

DOE OSTI2021

Spent Nuclear Fuel and Reprocessing Waste Inventory

This report provides information on the inventory of spent nuclear fuel (SNF) in the United States located at Nuclear Power Reactor (NPR) and Independent Spent Fuel Storage Installation (ISFSI) sites, as well as SNF and reprocessing waste located at U.S. Department of Energy (DOE) sites and other research and development (R&D) centers. Actual or estimated quantitative values for current inventories are provided along with inventory forecasts derived from examining different future nuclear power generation scenarios. The report also includes select information on the characteristics associated with the wastes examined (e.g., type, packaging, heat generation rate, decay curves).

Peters, Shan↗

DOE OSTI2021

Spent Nuclear Fuel and Reprocessing Waste Inventory

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

SB14 Source Reduction Evaluation Review and Plan for the DOE California Sites

The Department of Energy (DOE) is the owner of multiple facilities in Northern California. The facilities include Lawrence Livermore National Laboratory (LLNL), Lawrence Berkeley National Laboratory (LBNL), Sandia National Laboratories/California (SNL/CA) and SLAC National Accelerator Laboratory (SLAC) among other sites. Through their operations, the facilities generate hazardous waste and, thereby, are subject to the requirements of Chapter 31 of the Title 22 California Code of Regulations, Waste Minimization. The Northern California sites are primarily research and development facilities in the areas relating to national security, high-energy physics, bioscience and the environment.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Assessment of Offshore Wind Leasing Areas in California [Slides]

This presentation summarizes an analysis of options for dividing Morro Bay and Humboldt Wind Energy Areas (WEAs) into offshore wind lease areas. The delineation process considered input from wind energy developers, physical characteristics of the sites, and potential effects of turbine layout and mooring technology selection on the energy generation capacity of each location. Two delineation options were assessed for the Humboldt WEA and four options for the Morro Bay WEA. The lease areas within each WEA were designed to have equal value and support approximately 1 gigawatt of generation capacity.

17 WIND ENERGY↗

DOE OSTI2023

Cultural Resource Management Plan for Brookhaven National Laboratory

The Cultural Resource Management Plan (CRMP) for Brookhaven National Laboratory (BNL) provides an organized guide that describes or references the facets and interrelationships of cultural resources at BNL. Management strategies included within this CRMP are designed to adequately identify the cultural resources that BNL and DOE consider significant and to acknowledge associated management actions. A principal objective of the CRMP is to reduce the need for additional regulatory documents and to serve as the basis for a formal agreement between the DOE and the New York State Historic Preservation Officer (NYSHPO). The BNL CRMP is designed to be a “living document.” Each section includes identified gaps in the management plan, with proposed goals and actions for addressing each gap. The plan will be periodically revised to incorporate new documentation. The current (2023) update incorporates new findings and/or updated text based on completed or ongoing projects related to cultural resources at BNL since inception of the last updated CRMP in 2013. Historically, Brookhaven National Laboratory had little need for cultural resource management because many of its buildings were less than 50 years old. Most of the features that are potentially eligible for inclusion in the National Register of Historic Places were protected simply by avoiding the features. Compliance with cultural resource laws and regulations has included archeological surveys, such as those associated with the 1977 Final Environmental Impact Statement for Brookhaven National Laboratory and the 1978 Final Environmental Impact Statement for the Proton-Proton Storage Accelerator Facility (ISABELLE). In 1979, World War I trenches associated with the former Camp Upton and located near ISABELLE were determined to be eligible for inclusion in the National Register of Historic Places; however, many of these trenches had been destroyed by construction work. In 1991, the NYSHPO provided BNL with a letter indicating that only three structures and features were likely to be eligible for inclusion in the National Register of Historic Places. Between 1991 and 1999, little work associated with cultural resource management was accomplished. Beginning in 1999, awareness for the need of a program to manage cultural resources grew out of the realization that over half of the buildings at BNL were either 50 years old or were reaching that age and were, therefore, subject to the requirements in Section 106 of the National Historic Preservation Act. This fact, concomitant with the decontamination and decommissioning of the Brookhaven Graphite Research Reactor (BGRR) and the subsequent determination of BGRR’s eligibility for listing as an historical site, fueled the need for developing and implementing a more structured program for managing cultural resources at BNL.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Spent Nuclear Fuel and Reprocessing Waste Inventory: Spent Fuel and Waste Disposition

This report provides information on the inventory of spent nuclear fuel (SNF) in the United States located at Nuclear Power Reactor (NPR) and Independent Spent Fuel Storage Installation (ISFSI) sites, as well as SNF and reprocessing waste located at U.S. Department of Energy (DOE) sites and other research and development (R&D) centers as of the end of calendar year 2021. Actual or estimated quantitative values for current inventories are provided along with inventory forecasts derived from examining different future nuclear power generation scenarios, based on information available and assumptions made at the time the scenarios were developed in the spring of 2022. The report also includes select information on the characteristics associated with the wastes examined (e.g., type, packaging, heat generation rate, decay curves).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Front End Engineering Design Study on Gasification of Coal and Biomass to Generate Carbon- Free Electric Power and Hydrogen

A 2nd Phase Front End Engineering Design study of a gasification plant concept to co-produce electric power and hydrogen with net-negative CO2 emissions is being completed under the U.S. Department of Energy’s (DOE’s) 21st Century Power Plants initiative, whose goal is to advance innovative power plant concepts that are capable of flexible, net-zero carbon emission operations while producing cost-effective hydrogen to support economy-wide decarbonization goals. The proposed standalone plant would be constructed in Nebraska, USA. The specified design feedstock is a hybrid blend of Powder River Basin (PRB) subbituminous coal from Wyoming and local Nebraska biomass (corn stover), 50% each by weight (dry basis). Other potential feedstocks, including woody biomass (eastern red cedar) and waste plastic (auto shredder residue) were evaluated as alternates. The process block comprises a high-pressure, oxygen-blown fluidized bed gasifier coupled with water-gas shift, Selexol process for acid gas (H2S and CO2) removal, and pressure-swing adsorption (PSA) to yield 8,500 kg/h of high-purity hydrogen. Off-gas from the PSA unit is used in a gas turbine combined cycle plant (the power block) to supply 50 MWe net electric power to the grid. Overall thermal efficiency of the plant is 50% (HHV) with net atmospheric CO2 removal at a rate of 32 t/h. Design activities necessary to provide input to the current front-end engineering design (FEED) study, including, site selection, gasifier technology selection, investment case preparation, and the development of the Environmental Information Volume (EIV) for the host site, have been completed. These, as well as the current FEED activities, are described in this presentation.

gasification, biomass, coal, hydrogen, power gener↗

DOE OSTI2024

Characterize and control the multi-range structure of solution-phase systems with resonant x-ray scattering

This work aims at demonstrating the feasibility and impact of Anomalous X-ray Scattering (AXS) in characterizing the multi-range structures of solution-state systems. We will show preliminary investigation of long-range correlations in concentrated aqueous electrolytes with a combination of AXS and molecular dynamics (MD) simulations. We will also start exploring the capability of AXS to capture intra- and inter-molecular structure of dilute molecular systems, and specifically its sensitivity to the chemical environment surrounding active metal sites. We anticipate that the development of this method will help us to understand ion solvation and transport, which affect the performances of, for instance, electrocatalytic cells, as well as to identify/control the intrinsic structural factors that lead to selectivity, efficiency, and stability control during catalysis.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Long-Term Evaluation of Remedial Technology Performance in the Laboratory: Multi-year Experimental Test Plan

An understanding of the long-term effectiveness of remediation technologies is central to sustainable environmental cleanup. Long-term experiments are valuable for reducing uncertainty and predicting remediation outcomes at scales required for regulatory compliance. However, these types of tests can be costly and challenging to interpret. Therefore, contaminated sites often rely on short-term laboratory experiments that may not account for the potentially significant effects of gradual, time- dependent processes governing contaminant retention, release, and species transformation. For example, short-term lab experiments (from months to a year) conducted with sediments from the unsaturated and saturated zones at the Hanford Site play an important role in initial evaluations of remediation technologies but cannot capture the full extent of time-dependent reactions, leaving uncertainties in field-scale deployment. Here, long-term testing will be conducted on select technologies based on their performance in short-term testing. The overall objective is to directly address the challenges described above by generating and analyzing data on long-term (2–10 years) efficacy of selected remediation technologies, integrating this understanding into models, and providing critical input for remediation planning, monitoring, and 5-year review cycles for field-implemented remedies. Specific objectives include: 1. Evaluating long-term efficiency of promising remedies under site-specific conditions. 2. Generating robust parameters for modeling, reducing uncertainty in predictive simulations. 3. Advancing integrated monitoring by combining geochemical and geophysical observations. 4. Informing field-scale implementation by incrementally advancing technologies, identifying failure mechanisms early, and prioritizing robust, cost-effective remedies. Through systematic evaluation of technologies in laboratory-scale column experiments, integrated monitoring, and modeling support, this project is designed to bolster confidence in the long-term robustness of selected technologies. The ultimate outcome is the identification and deployment of more reliable, cost-effective remedies that safeguard human health and the environment while reducing the uncertainties that have historically hindered cleanup progress at Hanford Site. An experimental approach was developed and initiated for long-term testing potentially up to 10 years. The table below summarizes the experimental approach developed for testing select technologies and presented in this multi-year experimental test plan.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Spent Nuclear Fuel and Reprocessing Waste Inventory

This report provides information on the inventory of spent nuclear fuel (SNF) in the United States located at Nuclear Power Reactor (NPR) and Independent Spent Fuel Storage Installation (ISFSI) sites, as well as SNF and reprocessing waste located at U.S. Department of Energy (DOE) sites and other research and development (R&D) centers as of the end of calendar year 2024. Actual quantitative values for current inventories are provided along with inventory forecasts derived from examining different future nuclear power generation scenarios, based on information available and assumptions made at the time the scenarios were developed. The report also includes select information on the characteristics associated with the wastes examined (e.g., type, packaging, heat generation rate, decay curves).

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2026

Defining Infrastructure Feasibility for Hub-Scale Offshore Atlantic Carbon Storage in the Northeastern United States

In the Northeast U.S., deep rock formations along the Atlantic outer continental shelf may have the potential to sequester 150–1136 million metric tons of CO2. However, the design and infrastructure necessary to develop offshore carbon storage in this region is not well defined because there has been little oil and gas exploration and no commercial production. Consequently, an infrastructure feasibility design was completed for a hub-scale offshore CO2 storage system along the Northeast U.S. Atlantic. The design included development of a detailed, site-specific geological model for a location near the Great Stone Dome geological structure in the Baltimore Canyon Trough off the coast of Delaware, Maryland, and New Jersey. A field injection system topology design was completed to portray a design with eight wells in two clusters connected by central manifolds. Reservoir simulations were completed for the injection system that showed the hub may be able to inject 17 million metric tons (MMT) of CO2 per year for thirty years, but injection rates varied substantially across the eight wells. A CO2 pipeline design determined feasible routes from the east coast shoreline to the injection field. Finally, the CO2 injection system design included subsea injection trees, manifolds, and power umbilicals. This is the first study to define large-scale carbon storage design and infrastructure options for the offshore Atlantic, which can help to progress this region towards field characterization and early-mover deployment for future decarbonization in the region.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2024

Locating Equitable Solar Opportunities by Census Tract: A Guide to the Screening Tool for Equitable Adoption and Deployment of Solar (STEADy Solar)

The Screening Tool for Equitable Adoption and DeploYment of Solar (STEADy Solar) is a database and mapping tool that indicates locations that may be eligible for the Investment Tax Credit bonus adders defined in the 2022 Inflation Reduction Act (IRA). The tool combines publicly available information on demographics, solar technical potential, solar economics (modeled net present value), building counts by use-type, and eligibility for tax credit adders. It can be used by states, municipalities, community-based organizations, developers, and researchers to identify sites where solar projects may be economical and where federal incentives may be available to support equitable adoption of solar. This report describes the STEADy dataset and presents high level insights from the data.

census tract↗

DOE OSTI2024

Field Study of 120-volt Heat Pump Water Heaters in the Big Easy

To meet long-term goals for reducing carbon emissions and lessen the impacts of climate change, the U.S. plans to decarbonize its building stock, which includes the replacement of fossil fuel-burning end uses with energy efficient electric alternatives. As part of this strategy, the replacement of fossil fuel water heaters with heat pump water heaters (HPWH) has the potential to avoid substantial carbon emissions. An estimated 10-15 million single-family homes with fossil fuel water heaters do not have the electrical panel capacity to install a 240-volt, 30-amp HPWH. For these homes, a technology recently introduced to the market, the 120-volt plug-in HPWH, can provide energy efficient electrification of water heating without an expensive panel and wiring retrofit. This paper presents the results of an ongoing 120-volt HPWH field study conducted in 17 homes in New Orleans, LA. Key installation scenarios are profiled for retrofitting from gas-fired water heaters to 120-volt HPWHs, accounting for space, air volume, air temperature, condensate drainage, and electrical. Each HPWH had its surrounding air temperature, relative humidity, inlet and outlet water temperature, flow, and energy consumption monitored. Using these data, hot water delivery and energy efficiency performance were analyzed based on home characteristics. Hot water run outs were investigated to understand how hot water usage, inlet water temperature, and surrounding air temperature impact the HPWH’s ability to meet load. From these results, best practices for 120-volt HPWH siting, sizing, and installation were developed. In addition, results are explored further to add insight for electrification policies and product development.

heat pump water heater, 120-volt, Residential buil↗