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Physical Sciences Vistas (Issue 2 2021) [Newsletter]

I am pleased to introduce the second 2021 issue of Physical Sciences Vistas, with a focus on “excellence in mission-focused science, technology, and engineering.” Excellence in mission-focused ST&E within the Physical Sciences Directorate (ALDPS) spans a broad spectrum of accomplishments in nuclear physics and materials science that sustains and enhances LANL’s science base.

36 MATERIALS SCIENCE↗

Uncertainty Analysis and Software Verification

Uncertainty analyses are an important part of calibrations and testing. They allow researchers insight on how to reduce and mitigate errors in testing. Each device used in testing introduces error in a system, as well as other sources such as environmental conditions, electronics, analog to digital, and random errors. Each source is carefully examined to identify how much error it introduces to a system. These sources are then combined using various methods of uncertainty calculations. To verify and validate software, a manual calculation is required to ensure the software is performing as intended. Using Excel to verify the calculations, we can identify discrepancies within the software. The root of the sum of the squares uncertainty (RSS) is used to find the combined uncertainty of a device at one and two standard deviations of the mean. Calibrations on accelerometers are performed using a vibration system along with a back-toback reference accelerometer. The vibration system takes a reference point at 100Hz frequency at 10g amplitude. The sensitivities are collected at each dialed in frequency. The sensitivity of the device represents the electrical output of the UUT (mV, pC, etc.) per unit of acceleration (g). The full history of sensitivities of selected accelerometers are used to find the averaged, standard deviation, and uncertainty of the device at each frequency tested. The uncertainty calculations from excel and the software are then compared.

97 MATHEMATICS AND COMPUTING↗

Validation of the SCEPTRE Boltzmann-CSD Solver

A new Boltzmann-CSD solver has been developed within the SCEPTRE radiation-transport code, based on the 1st-order form of the transport equation, using discontinuous finite elements in space and energy and discrete ordinates in angle. The Boltzmann-CSD solver has been validated against experimental data for electron energy deposition distributions and for electron emission spectra. Comparison of the calculated results with experimental data shows excellent agreement for many of the test configurations and reasonable agreement for other test configurations. The tests have also been modeled with the ITS Monte Carlo code, which also shows excellent to reasonable agreement with the SCEPTRE results and experimental data. The SCEPTRE Boltzmann-CSD solver relies on electron cross sections generated by the legacy CEPXS code, which currently is limited to electron-only Boltzmann-CSD cross sections. Performing full electron-photon radiation transport with the Boltzmann-CSD solver will require further development in the cross section generating code. For the energy- deposition calculations, neglecting photon transport results in at most about 5% overprediction of the energy deposition for high-energy electrons on high-Z targets, and relatively insignificant difference for the other test configurations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Physics Division Strategic Plan: Science Drivers

The Physics Division Science Drivers articulate the overarching scientific objectives that we seek to address and that form the lifeblood of our Division. While many physics subfields are represented in the Physics Division’s scientific portfolio, we strive to maintain or achieve excellence and international leadership in only a few areas. While diversity of science and engineering efforts is strongly supported and provides the fertile soil for innovation, there are dominating areas in which we must excel to accomplish our mission that is stated as: “We design, execute and analyze experiments that challenge, improve and validate our understanding of fundamental physics underpinning LANL’s national security mission.”

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Integrated TBC/EBC for SiC Fiber Reinforced SiC Matrix Composites for Next Generation Gas Turbines (Final Report)

In this ambitious project, a significant challenge preventing widespread use of ceramic matrix composites in hot section components of gas power generating turbines was addressed. Hot section components made from SiC fiber reinforced SiC matrix composites (SiC/SiC composites), have the potential to achieve a combined cycle energy efficiency of above 65%. To achieve this efficiency, the temperature of the combustion gases on the turbine component surface is expected to reach as high as ~1700ºC (3100ºF). However, SiC/SiC composites suffer from volatilization at high temperature under high velocity steam environment – typical in a turbine hot chamber. This integrated collaborative project, between two research groups at Clemson University and a team of engineers and scientists at GE Gas Power, focused on design, fabrication and evaluation of a new graded environmental barrier coating. Using the excellent compositional tailorability of polymer derived ceramics (PDCs), we developed an integrated EBC/BC that smoothly transitions from bottom SiC/SiC bond interface to hermetic sesquioxide (Y 2 O 3 ) top surface. This smooth compositional transition avoided the sharp CTE mismatch at interfaces to greatly reduce the thermal stress. The developed EBC is compatible with and bonds well with the bond coat that GE uses. The top hermetic oxide surface ensures low oxygen transportation and volatilization rates under the high velocity steam environment. The graded microstructure with increasing sesquioxide concentration also decreases the amount of Si and C elements near the top hermetic sesquioxide layer. Coatings made using a process suitable for manufacturing – atmospheric plasma spraying was demonstrated. The microstructure of coatings made using this process were fully characterized. Finally, the performance of these coatings was investigated under the most demanding conditions for this application. Specifically, high temperature, high velocity steam exposure; thermal shock test; and thermal cycling tests. The graded coatings performed exceptionally well in all these tests. Specific suggestions for future development in this area have also been identified. In addition to the excellent technical progress, this project helped initiate a robust collaboration between the research groups at Clemson and GE Gas Power. It also provided a high-quality learning and mentoring opportunity for the three post-doctoral research associates and two UG students at Clemson University who worked on this project. All proposed tasks, sub-tasks were completed, and all milestones achieved.

03 NATURAL GAS↗

LANL Regular Employee Population and Demographics, FY15-21

This document summarizes an effort to compile and analyze the LANL regular employee population’s demographic attributes and trends between FY15-FY21 using MicroStrategy, a web-based data analytics and visualization tool. LANL’s HR Division collected and prepared data for the Weapons Program’s annual reporting activities for the 2017 through 2023 NNSA Stockpile Stewardship and Management Plan (SSMP). Los Alamos workforce data represent the fiscal year-end snapshot of the permanent employee population who are categorized by the Common Occupational Classification System (COCS). This work enables further analyses, including trends for all workforce attributes presented in the SSMPs as well as a definition of a crosswalk between COCS categorization and the internal laboratory job classification hierarchy. Data for other sites and the federal workforce, as shown in the SSMPs, are included and corresponding figures can be visualized within the MicroStrategy tool. A portable, Excel-based version of the tool was developed and shared with the multi-site workforce working group. This summary highlights selected aspects of the LANL regular workforce. The data analyses and visualizations communicate insights within three major themes regarding permanent LANL employees: 1) demographic transformation, 2) attrition, and 3) skills. Regarding demographic transformation, and consistent with the general trend across the enterprise, early career regular employees are the fastest growing group, with growth ranging between 12-34% year-to-year over the seven-year period analyzed. The data also reflect effects of internal and external factors on attrition; the large spike in separations in FY18 aligns with the contract transition from LANS to Triad and the dip in attrition between FY20-FY21 is likely a result of the global pandemic. The population of regular employees in general management, engineer, and operator COCS categories have the fastest growth rates amongst all the occupational categories. The MicroStrategy and Excel tools provide additional details and trends.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Industrial Assessment Center – integration of education and practice. Final progress report

The goal of the DOE’s Industrial Assessment Center (IAC) program is twofold: first, to help US manufacturing competitiveness by providing assessments and recommendations for small and medium-sized enterprises (SMEs) on energy efficiency, productivity, sustainability and competitiveness – including measuring the impacts of these recommendations on reducing greenhouse gas emissions; and second, to address a growing shortage of engineering professionals with applied energy and manufacturing-related skills by training a diverse cross-section of engineering students through hands-on involvement in these assessments. IUPUI has an IAC, which was established in 2011, in the Department of Mechanical and Energy Engineering, Purdue School of Engineering and Technology, IUPUI. The IAC has won the awards twice. We have built the center that has the expertise and infrastructure for quality energy assessments to manufactures and commercial building owners and aligned our current research and teaching activities to the DOE’ training mission with programs to train the next generation of industrial energy efficiency experts, with theory and hands-on experience in conducting energy assessment for small and median manufacturing enterprises. We have made recommendations that have the potential to save about $20M annually. We also initiated research projects to meet DOE priorities, specifically in the areas of smart manufacturing and cybersecurity. On the energy assessment side, the Center has provided energy assessments to 144 qualified companies, primarily located in Indiana. On the training side, the center has trained students in various programs, such as the department’s Bachelor of Science (BS) programs in Mechanical Engineering (ME) and BS in Energy Engineering (EEN), both are ABET accredited engineering programs, as well as a graduate level Energy Management and Assessment certificate program. At the present, the center has trained 95 students, 43 or them received the DOE issued certificates. Research projects were developed within the center to advance energy efficiency related technologies, which provided excellent opportunities for our trainees. The center has also been building a professional network with utilities, Manufacturing Extension Partnership (MEP), government agencies, and manufacturing companies, to increase our client base and promote collaborations. The center received the 2019 Center of Excellence of the Year Award and three students received the “Outstanding Achievement in Energy Engineering by an IAC Student” awards in the past five years.

42 ENGINEERING↗

Downselection of Cladding Materials for Zirconium Hydride Moderator

This report complete Milestone M3.1.1 — “Cladding downselection: Team will report to ARPA-E on at least two down-selected cladding options—one metallic and one ceramic.” In this milestone, we systematically assess FeCrAl alloys and SiC-based cladding options for a zirconium hydride (ZrHx) moderator in terms of their neutronics, radiation stability, hydrogen permeability, chemical compatibility, and fabricability. The analysis shows that FeCrAl alloys are excellent candidate cladding materials for a ZrHx moderator given their proven radiation stability, acceptable compatibility with ZrHx, and industrially established fabricability. The relative high hydrogen permeability is manageable by introducing a thin layer of an Al 2 O 3 hydrogen permeation barrier on the external surface. The SiC-cladded ZrHx moderator is promising because of its outstanding neutronics performance, excellent radiation stability, and extremely low intrinsic hydrogen permeability. However, potential interactions of SiC and Zr and the challenge in achieving a hermetic SiC-based cladding require further investigation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Hydrogen Life-Cycle Analysis in Support of Clean Hydrogen Production

Hydrogen is a basic molecule which is commonly used in the production of chemicals or as an energy carrier or a fuel. Its zero-carbon content means that it does not produce carbon dioxide upon its use. However, depending on the energy source and technology for hydrogen production and delivery, there can be greenhouse gas (GHG) emissions associated with the hydrogen for various end use applications. To provide the largest reduction in GHG emissions, hydrogen produced from clean energy sources should be used. As concerns regarding climate change grows, there is an increasing focus on economic production of clean hydrogen to displace less climate neutral sources of hydrogen. However, there are many different methods of hydrogen production with unique processes that result in different levels of life cycle GHG emissions of hydrogen production and its end use applications. Therefore, a comprehensive life cycle accounting methodology that takes all these factors into account is required. he GREET ® (Greenhouse gases, Regulated Emissions, and Energy use in Technologies) model was first developed in 1995 by Argonne National Laboratory with the support from the various offices of the U.S. Department of Energy (DOE). GREET provides in-depth Life Cycle Analysis (LCA) simulations for a variety of products and is available as an Excel spreadsheet (GREET Excel), or as an application (GREET .Net). Both versions are available for public download at no cost. This report accompanies GREET 2022 release to describe the major updates and expansions to the hydrogen technology pathways, and to provide data sources and sample carbon intensity results for each of the pathways.

08 HYDROGEN↗

Operational Energy Life Cycle Data Development for the National Institute of Standards And Technology (NIST) Building Industry Reporting and Design for Sustainability (BIRDS) Neutral Environmental Software Tool (NEST)

For this analysis, regionalized life cycle assessment (LCA) results for environmental impacts (using the Tool for Reduction and Assessment of Chemicals and Other Environmental Impacts [TRACI] 2.1) and cumulative energy demand (using the Federal Life Cycle Analysis Commons Elementary Flow List [FEDEFL] Inventory Methods v1.0.0) were evaluated for the production and utilization of electricity, natural gas, fuel oil, and propane as commodities within residential and commercial buildings. These results can used as a framework for future research into net zero, high-performance buildings, such as done here for the Building Industry Reporting and Design for Sustainability (BIRDS) database by the National Institute of Standards and Technology (NIST) Engineering Laboratory. The geographical results were assigned to each United States (U.S.) Zone Improvement Plan (ZIP) code based on the ZIP code location and corresponding Balancing Authority Area, natural gas basin, and Petroleum Administration for Defense Districts (PADDs). Additionally, previously developed models were utilized to develop future life cycle profiles. Projections were based on data available from the U.S. Energy Information Administration Annual Energy Outlook 2022 through 2050 (AEO 2022). Electricity LCA models were updated based on AEO 2022 projected annual generation mixes, while the natural gas baseline model was updated based on projected shares of natural gas types (conventional, shale, tight, and coalbed methane). Projections of crude oil production rates and export rates were applied to the petroleum baseline model in five-year increments to investigate their effects on the life cycle profile of fuel oil and propane. While only 100-year Global Warming Potential (GWP-100) with climate carbon feedback (CC-FB) and Cumulative Energy Demand are shown in Section 4: Results, the complete results, including Acidification Potential, Eutrophication Potential, Freshwater Ecotoxicity Potential, GWP-100 without inclusion of CC-FB, Human Health Impacts Potentials (Cancer, Non-Cancer), Ozone Depletion Potential, Particulate Matter Formation Potential, and Photochemical Smog Formation Potential, are tabulated for each ZIP code in the Excel worksheets that accompany this analysis. For the Excel spreadsheet tools associated with this report, please go to https://www.netl.doe.gov/energy-analysis/details?id=f8890fac-be55-44ac-aaa9-e2888bfabe93

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Neutronics Calculations for EBR-II Run 137E

Neutronics calculations were performed for EBR-II Run 137E using MC2 -3/TWODANT, DIF3D, and PERSENT codes. Parameters required for system safety analysis such as the reactivity feedback coefficients and core power distribution were evaluated. The detailed results are provided in the accompanying Excel spreadsheet Run_137E_Neutronics_Results.xls. This report describes the core model of EBR-II at the beginning of Run 137E, the computation methodology, and how to interpret the results listed in the Excel spreadsheet.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

US Department of Energy, Office of Science High Performance Computing Facility Operational Assessment 2021: Oak Ridge Leadership Computing Facility

Oak Ridge National Laboratory’s (ORNL’s) Leadership Computing Facility (OLCF) continues to surpass its operational target goals of supporting users; delivering fast, reliable computational ecosystems; creating innovative solutions for high-performance computing (HPC) needs; contributing to the community to build the next generation HPC workforce, and managing risks, safety, and security associated with operating some of the most powerful computers in the world. The results can be seen in the cutting-edge science conducted by users and the praise from the research community. Calendar year (CY) 2021 saw continued excellence in research supported by the OLCF’s leadership-class computing resources, including Summit (the nation’s most powerful supercomputer), the global scratch file system Alpine, the Scalable Protected Infrastructure (SPI), the Exploratory Visualization Environment for Research in Science and Technology (EVEREST), and the archival mass-storage resource High-Performance Storage System (HPSS). While maintaining access and exceptional user support for Summit, the OLCF continued to make progress on the installation and deployment of Frontier, which will be the nation’s first exascale system when it comes online at the start of CY 2023. Users have already begun running and optimizing scientific codes on Crusher, the OLCF test and development system equipped with Frontier’s architecture. Throughout the year, the OLCF maintained a strong culture of operational excellence, including risk management, workplace safety, and cybersecurity. The OLCF’s rigorous risk management strategy anticipated and mitigated risks, and at this time there are no high-priority operational risks. Similarly, ORNL and the OLCF were committed to operating under the US Department of Energy’s (DOE’s) safety regulations that ensure a safe workplace. Technical staff tracked and monitored existing threats and vulnerabilities within the OLCF while continually developing tools and practices to enhance operations without increasing the facility’s risk. CY 2021 was filled with outstanding results and accomplishments, including a very high rating from users on overall satisfaction for the eighth consecutive year; a tremendous number of node hours delivered to 1,671 researchers on Summit; and the successful delivery of the allocation split of roughly 60%, 20%, and 20% of core-hours offered for the Innovative and Novel Computational Impact on Theory and Experiment (INCITE), Advanced Scientific Computing Research Leadership Computing Challenge (ALCC), and Director’s Discretionary (DD) programs, respectively (Section 2). COVID-19 research remained a focus in 2021, and the ALCC and DD programs allocated over 1 million Summit hours to the COVID-19 High Performance Computing Consortium. These accomplishments, coupled with the high utilization rates (i.e., overall and capability usage), represent the fulfillment of the promise of leadership class machines: efficient facilitation of leadership-class computational applications.

97 MATHEMATICS AND COMPUTING↗

Development of Corrosion Resistant Coatings for Structural Materials for Liquid Fueled Molten Salts Reactors Applications (Final Report)

Current structural alloys, code certified for the MSRs temperature ranges, contain high levels of chromium, making them highly susceptible to molten halide salt corrosion. One potential solution to circumvent the need for code certification of novel alloys, which is expensive and time consuming, is to design claddings that will protect the underlying code certified materials from corrosion damage during operation. In this work, we examined the corrosion of Ni and Cu electroplated, Ni and CuNi weld overlay, Mo-laser clad, and carburized claddings on SS316H for use in molten salt reactor environments. After characterization of the cladded materials (Task 1), static corrosion tests were used to assess corrosion resistance of the claddings in typical molten fluoride salts (Task 2). The corrosion tests were performed in molten FLiNaK at 700°C up to 1000 hours. Pre- and post-corrosion Scanning Electron Microscopy (SEM), energy-dispersive-spectroscopy (EDS), Transmission Electron Microscopy (TEM), X-ray Diffraction (XRD) and glow-discharge-optical-emission-spectroscopy (GDOES) were performed on cladding cross-sections and surfaces to evaluate degradation. The Cu and Ni electroplated samples, as well as the carburized samples, showed excellent corrosion resistance relative to the bare SS316H. To assess high temperature cladding stability, ageing experiments were performed at temperatures up to 900 C in inert atmosphere for the electroplated and carburized samples and a diffusion model was developed to predict long term cladding behavior (Task 3). It was found that the Cu cladding was basically insensitive to the high temperature ageing, except for small secondary phases forming at the interface. On the other hand, the Ni electroplated cladding experienced significant interdiffusion. Nevertheless, the gain in corrosion resistance for a 100μm Ni electroplated cladding is phenomenal, with more than 50% reduction in chromium dissolution from the substrate material for the first 15 years of salt exposure at 700°C. To assess radiation resistance and phase stability, high-temperature 4MeV Ni heavy ion irradiation was performed across the cladding/substrate interface up to 50 displacement-per-atom (DPA) at 500°C and 700°C to assess the phase stability and irradiation behaviors of the electroplated systems (Task 4). The Ni and Cu electroplated systems did not experience void swelling at the contrary to the SS316H substrate due to their nanocrystalline nature. Some level of recrystallization was observed in the cladding, as well as radiation induced segregation and enhanced diffusion. The interface acted as a potent sink for point defects with the presence of a void denuded zone. The mechanical properties of the claddings were assessed using thermal shock, micro-indentation, nano-indentation, and four-point bend testing experiments (Task 5). These experiments were performed on the claddings in as-received, corroded, irradiated, and thermally aged states to determine the effects of typical molten salt reactor environments on cladding integrity. No significant mass loss was observed after repeated thermal shocks. While the electroplated samples softened after high-temperature ageing, irradiation hardening compensate this effect, such that there is little different with the as-received materials. The results of these experiments suggest that the electroplated (copper/nickel) show the greatest promise for application in molten salt reactor development. These claddings prevented any chromium dissolution from occurring during the static corrosion experiments. Additionally, they demonstrated favorable properties for high temperature diffusion, phase stability, interfacial mechanical properties, and irradiation resistance. Weld-overlay cladding are also of great interest and could reach properties similar to the electroplated samples upon optimization (especially with multiple weld passes). The carburized SS316H showed excellent behavior as well, but more work needs to be done to assess their long-term stability. Finally, the Mo-laser clad system was not pursued further due to the manufacturing challenges. It is also worth noting that the Ni cladding systems should behave relatively well in terms of weldability since the Ni-weld overlay microstructure and associated corrosion rate are sound. While the NiCu weld-overlay has even lower corrosion rates than the Ni-weld overlay, more studies on welding of Cu-electroplated systems are necessary since Cu clusters are known to embrittle steels.

36 MATERIALS SCIENCE↗

Exploring New Diamond Surfaces with Precision Chemistry and Quantum Spectroscopy

Point defects in diamond known as color centers are a promising platform for quantum sensing. As atom-like systems, they can exhibit excellent spin coherence and can be manipulated with light. As solid-state defects, they can be produced at high densities and be incorporated into scalable devices. Diamond is a uniquely excellent host; it has a large band gap, can be synthesized with sub-ppb impurity concentrations, and can be isotopically purified to eliminate magnetic noise from nuclear spins. Specifically, the nitrogen vacancy (NV) center has been demonstrated to be a highly sensitive, non-invasive magnetic probe capable of resolving the magnetic field of a single electron spin with nanometer spatial resolution. However, the development of NV centers and other color centers in diamond as a quantum platform crucially relies on developing methods to functionalize and process diamond surfaces. Diamond is the hardest material, making polishing and processing challenging, and diamond surfaces are inert and sterically hindered, making them notoriously difficult to chemically terminate and functionalize. Our approach is to discover new surface chemistries for diamond by combining multimodal surface spectroscopy with NV-based quantum spectroscopy to carefully characterize the diamond surface. We have developed a suite of techniques for characterizing the diamond surface using rapid tools for reaction screening and detailed surface spectroscopy tools for definitive identification of the surface bonding.

36 MATERIALS SCIENCE↗

Catalyst Layer Design, Manufacturing and In-line Quality Control

In this project we successfully demonstrated the capabilities of the Reactive Spray Deposition Technology (RSDT) to fabricate large-scale CCMs for advanced PEMWEs that have one-order of magnitude lower PGM loading in their catalyst layers, and performance comparable with the commercial state-of-the-art CCMs. The RSDT is a unique methodology that combines the catalyst synthesis and CCM fabrication in one step and reduces dramatically the time for CCM manufacturing. As fabricated large-scale CCMs with geometric area of 680 cm2 demonstrated excellent activity and durability performance, and the novel duo-recombination layer design paves the way for solving the safety concerns related to PEMWEs. In addition, excellent activity and durability performance has been demonstrated with RSDT fabricated CCMs with thinner membranes and duo RL design. This is a novel approach for further performance improvement of the MEAs for PEMWEs that has been successfully demonstrated for the first time in this project. The integration of the in-situ laser diagnostics system along with the in-line optical quality control system within the RSDT that has been achieved and demonstrated in this project, is an example for possibility of designing and building advanced manufacturing technologies that can meet the requirements of the future manufacturing. Therefore, the RSDT offers a precise real-time monitoring and control of the particles size, composition, loading, porosity, thickness, and defects in the catalysts’ layers, which render this technology as the best candidate for manufacturing of cost effective CCMs for PEMWEs. By using RSDT we successfully met all project’s milestones, Go/No-Go decision, objectives, goals, and deliverables.

08 HYDROGEN↗

RESIN: Responsible Innovation for Highly Recyclable Plastics - TASK 4: Risk Assessment Framework

This report covers the entirety of Task 4, but its main purpose is to deliver milestones ML4.4 and ML4.5, the last two SOPO milestones under Task 4. ML4.4 reports on the compatibility of polymer properties that affect both environmental performance and functional performance and the tradeoffs involved in turning these properties to the benefit of each. ML4.5 presents a complete set of information on the critical properties of benign target products, where benign products are defined as those with the shortest environmental lifetime which meet performance requirements. To support and provide context to the discussions of ML4.4 and ML4.5 and to provide a complete picture of Task 4, milestones 4.1-4.3 are briefly summarized at the beginning of the report. The discussion of ML4.4 introduces the notion of polymer persistence as a proxy for environmental risk. It then discusses the development and comparison of two machine leaning models explored for estimating polymer degradation rates, a random forest (RF) classifier and an RF regressor. Given the advantage of continuous outputs rather than simple classes, the RF regressor was incorporated in the Excel risk calculator, which to this point could implement the objectives of subtasks 4.1-4.3, estimating polymer release and redistribution. The ML4.4 discussion then addresses the effect of each of the three polymer features used by the RF regressor on polymer functional performance. These features are number molecular weight (Mn), glass transition temperature (T g ) and heat of fusion (H fus ). The discussion of ML4.5 reviews the conceptual framework of the risk model, which served as the foundation for developing the Excel risk calculator and describes the use of, and assumptions within, the calculator. Appendix A is further provided as a user’s guide for the calculator. To demonstrate how the calculator is intended to be used by developers in the design of low-risk polymers, an analysis of 27 hypothetical polymers defined by varying values for the three polymer features used by the RF regressor is presented. The range of parameter values selected produces estimates of polymer degradation rates and lifetimes that may be typical of various consumer products made from polyurethane polymers and shows how changes in polymer features affect lifetimes. The demonstration also predicts the final distribution of released polymer materials in environmental compartments as a function of consumer product mix and assumed leakage rates of end-of-life processes. Lastly, this report summarizes the achievement of Task 4 goals from original conception to final delivery and discusses how and to what degree to which each subtask goal was achieved.

36 MATERIALS SCIENCE↗

Durable and High-Performance SOECs Based on Proton Conductors for Hydrogen Production

Proton-conducting solid oxide electrolysis cells (P-SOECs) are a promising technology for cost-effective and efficient production of green hydrogen. Breakthroughs in materials development, optimization of cell structure, and achievement of high performance and durability are essential to significantly increase the commercial competitiveness of these technologies. The main objective of this project is to gain scientific knowledge for the rational design, fabrication, and demonstration of a robust, highly efficient, and low-cost SOEC technology based on a proton-conducting electrolyte membrane for hydrogen production. We focused on better understanding the degradation mechanisms of proton-conducting electrolytes, air electrodes, and catalyst materials under electrolysis mode to develop an effective strategy for rationalizing new materials that are vital for enhancing cell performance and durability. The scope includes enhancing the performance and durability of the electrolyte and electrode materials under realistic operating conditions, developing highly active and robust catalysts to minimize electrode losses while improving tolerance to contaminant poisoning, revealing the mechanism of enhanced activity and stability of the catalyst, and understanding the underlying degradation mechanisms. In addition, various characterization techniques were employed to gain a fundamental understanding of the materials’ behavior and their impact on cell performance, providing vital information to guide materials discovery and cell design. After defect chemistry engineering, the optimized donor and acceptor co-doped electrolytes BaMo/W 0.03 Ce 0.71 Yb 0.26 O 3-δ (BM/W03) showed substantially improved chemical stability against high concentrations of CO 2 and H 2 O compared to the state-of-the-art electrolyte (BaZr 0.1 Ce 0.7 Y 0.1 Yb 0.1 O 3-δ , BZCYYb1711) while maintaining comparable ionic conductivity and ionic transference number. To bypass the inherent trade-off between conductivity and chemical stability, we fabricated a bi-layer electrolyte composed of BZCYYb1711 coated with a highly-stable thin layer of BaHf 0.83 Yb 0.17 O 3-δ (BHYb). This bi-layer electrolyte displayed excellent chemical stability against high concentration CO 2 ; there was no detectable formation of BaCO 3 after exposure to 97% CO 2 (with 3% H 2 O) at 500 °C for 1000 hours and the rate of degradation in resistance was about 0.4% per 1,000 hours (kh). In contrast, the same BZCYYb1711 electrolyte without a BHYb coating degraded significantly under the same testing conditions; the degradation rate was increased to 5.1%/kh. In addition, a triple conducting air electrode Ba 0.9 Pr 0.1 Hf 0.1 Y0.1Co 0.8 O 3-δ (BPHYC) was developed by heavily doping transition metal ions into a proton-conducting material. This air electrode material, composed of 3 distinct phases, exhibits superior electrocatalytic activity due to the synergistic effect from the three component phases. Moreover, an active and durable catalyst, La 2 Ni 0.5 Fe 0.5 O 4+δ (LNF), was developed, showing excellent catalytic activity and contaminant tolerance, with a degradation rate of only 0.49%/kh when exposed to high concentrations of steam and Cr. Finally, single cells were constructed from the best electrolytes, electrodes, and catalyst coatings developed in this project. These cells demonstrated superior high current density at a given cell voltage, high roundtrip efficiency, and remarkable durability (up to 1000 hours of operation).

08 HYDROGEN↗