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At least 1,369 records · Page 76

All sources NASA NTRS DOE OSTI

DOE OSTI2018

Optimal design of microtube recuperators for an indirect supercritical carbon dioxide recompression closed Brayton cycle

This paper presents a baseline design and optimization approach developed in Aspen Custom Modeler (ACM) for microtube shell-and-tube exchangers (MSTEs) used for high- and low-temperature recuperation in a 10 MWe indirect supercritical carbon dioxide (sCO 2 ) recompression closed Brayton cycle (RCBC). The MSTE-type recuperators are designed using one-dimensional models with thermal-hydraulic correlations appropriate for sCO 2 and properties models that capture considerable nonlinear changes in CO 2 properties near the critical and pseudo-critical points. Using the successive quadratic programming (SQP) algorithm in ACM, optimal recuperator designs are obtained for either custom or industry-standard microtubes considering constraints based on current advanced manufacturing techniques. The three decision variables are the number of tubes, tube pitch-to-diameter ratio, and tube diameter. Five different objective functions based on different key design measures are considered: minimization of total heat transfer area, heat exchanger volume, metal weight, thermal residence time, and maximization of compactness. Sensitivities studies indicate the constraint on the maximum number of tubes per shell does affect the number of parallel heat exchanger trains but not the tube selection, total number of tubes, tube length and other key design measures in the final optimal design when considering industry-standard tubes. In this study, the optimally designed high- and low-temperature recuperators have 47,000 3/32 inch tubes and 63,000 1/16 inch tubes, respectively. In addition, sensitivities to the design temperature approach and maximum allowable pressure drop are studied, since these specifications significantly impact the optimal design of the recuperators as well as the thermal efficiency and the economic performance of the entire sCO 2 Brayton cycle.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2014

Control of waveguide properties by tuning femtosecond laser induced compositional changes

Local compositional changes induced by high repetition rate fs-laser irradiation can be used to produce high performance optical waveguides in phosphate-based glasses. The waveguide refractive index contrast is determined by the local concentration of La, which can be changed by the action of the writing laser pulses. In this work, we have investigated the degree of control that can be exerted using this waveguide writing mechanism over the cross-section of the guiding region, and the local refractive index and compositional changes induced. These variables can be smoothly controlled via processing parameters using the slit shaping technique with moderate Numerical Aperture (NA 0.68) writing optics. The combined use of X-ray microanalysis and near field refractive index profilometry evidences a neat linear correlation between local La content and refractive index increase over a broad Δn interval (>3 × 10{sup −2}). This result further confirms the feasibility of generating efficient, integrated optics elements via spatially selective modification of the glass composition.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Finite boundary effects on the spherical Rayleigh–Taylor instability between viscous fluids

For the Rayleigh–Taylor unstable arrangement of a viscous fluid sphere embedded in a finite viscous fluid spherical shell with a rigid boundary and a radially directed acceleration, a dispersion relation is developed from a linear stability analysis using the method of normal modes. [Formula: see text] is the radially directed acceleration at the interface. ρ i denotes the density, μ i is the viscosity, and R i is the radius, where i = 1 is the inner sphere and i = 2 is the outer sphere. The dispersion relation is a function of the following dimensionless variables: viscosity ratio [Formula: see text], density ratio [Formula: see text], spherical harmonic mode n, [Formula: see text], [Formula: see text], and the dimensionless growth rate [Formula: see text], where σ is the exponential growth rate. We show that the boundedness provided by the outer spherical shell has a strong influence on the instability behavior, which is reflected not only in the modulation of the growth rate but also in the selection of the most unstable modes that are physically possible. This outer boundary effect is quantified by the relative magnitude of the radius ratio H. We find that when H is close to unity, lower order harmonics are excluded from becoming the most unstable within a vast region of the parameter space. In other words, the effect of H has precedence over the other controlling parameters d, B, and a wide range of s in establishing what the lowest most unstable mode can be. When H ~ 1, low order harmonics can become the most unstable only for s >> 1. However, in the limit when s → ∞, we show that the most unstable mode is n = 1 and derive the dispersion relation in this limit. The exclusion of most unstable low order harmonics caused by a finite outer boundary is not realized when the outer boundary extends beyond a certain threshold length-scale in which case all modes are equally possible depending on the value of B.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2017

Attribution of the July–August 2013 heat event in Central and Eastern China to anthropogenic greenhouse gas emissions

In the midsummer of 2013, Central and Eastern China (CEC) was hit by an extraordinary heat event, with the region experiencing the warmest July-August on record. To explore how human-induced greenhouse gas emissions and natural internal variability contributed to this heat event, we compare observed July-August mean surface air temperature wit h that simulated by climate models. We find that both atmospheric natural variability and anthropogenic factors contributed to this heat event. This extreme warm midsummer was associated with a positive high-pressure anomaly that was closely related to the stochastic behavior of atmospheric circulation. Diagnosis of CMIP5 models and large ensembles of two atmospheric models indicates that human influence has substantially increased the chance of warm mid-summers such as 2013 in CEC, although the exact estimated increase depends on the selection of climate models.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Suppressing Quantum Circuit Errors Due to System Variability

We present a quantum circuit optimization technique that takes into account the variability in error rates that is inherent across present-day noisy quantum computing platforms. This method can be run after qubit routing or postcompilation and consists of computing isomorphic subgraphs to input circuits and scoring each using heuristic cost functions derived from system calibration data. Using an independent standard algorithmic test suite, we show that it is possible to recover on average nearly 40% of missing fidelity using better qubit selection via efficient to compute cost functions. We demonstrate additional performance gains by considering qubit placement over multiple quantum processors. The overhead from these tools is minimal with respect to other compilation steps, such as qubit routing, as the number of qubits increases. As such, our method can be used to find qubit mappings for problems at the scale of quantum advantage and beyond.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2014

PUEBLO OF ZIA RENEWABLE ENERGY DEVELOPMENT FEASIBILITY STUDY

The Pueblo of Zia will conduct a comprehensive feasibility study for best-use application(s) for development of renewable energy resources on its tribally held TRUST lands (i.e., Trust Lands of Zia Indian Reservation). The feasibility study is essential for determining the technical and economic viability of a future renewable project(s) on Zia tribal lands, including the potential economic and environmental benefits for the Tribe. Project Objectives: The feasibility study is essential for determining the technical and economic viability of future renewable project(s) on Zia tribal lands, including the potential economic and environmental benefits for the Tribe to: 1. Provide a balanced local renewable power supply for Zia Pueblo, its members, tribal offices, schools and buildings, and businesses on tribal lands 2. Provide a firm power supply for export and commercial market distribution 3. Provide economic development for the Tribe and its members, including job training and creation, each in accordance with the goals and objectives as conveyed by the Pueblo of Zia Tribal Council, Tribal Administration, and outlined in The Pueblo of Zia Comprehensive Plan and Pueblo of Zia — Zia Enterprise Zone Master Plan. A key goal of the study is to analyze the integrated development of solar, geothermal, and wind renewable energy resources at Zia Pueblo, with added potential to combine gas-fired generation to accomplish energy firming. Geothermal offers a base load source of energy, providing power continuously for end users. Wind and solar offer intermediate and peaking sources of energy, which can be harvested throughout the day, with periods of variable but predicable output. Variability will be managed in an integrated manner, using Zia Pueblo's combined renewable resources to generate high-quality power. Tasks are intended to collect, catalog, map, and analyze existing data on Zia Pueblo's renewable energy resource base and then match resource attributes with the most suitable renewable technologies for tribal energy consumption and needs. Also, key impacts on cultural and social values of Zia Pueblo will be addressed. Selected most favorable uses and technologies will be further investigated to determine initial feasibility and market for business development for up to six sites located on tribal land. The anticipated result will be the recommended development of sites that have sufficient background study completed to warrant a business plan, detailed engineering feasibility, and acquisition of project financing. Valuable technical and economic information will accrue from this study that may be applied to scale up or down the various power technology potential on Zia Pueblo for maximum benefit and best area(s) of application, project phasing and potential for future replicability and expansion.

14 SOLAR ENERGY↗

DOE OSTI2024

SCALE Analyses of Scenarios in the Molten Salt Reactor Fuel Cycle

In support of the US Nuclear Regulatory Commission non-light-water reactor fuel cycle demonstration project, the capabilities of SCALE 6.3.1 for radionuclide characterization, criticality, and shielding were demonstrated through several scenarios in a molten salt reactor (MSR) nuclear fuel cycle. Three scenarios were selected for this study, with the molten salt breeder reactor (MSBR) serving as the reference design. The original thorium-based fuel salt used in MSBR was replaced with a 235 U-enriched fuel salt to better reflect anticipated future MSR concepts. The first scenario focused on the fuel salt preparation stage. Criticality analyses, using SCALE/CSAS-Shift and SCALE/SAMPLER, examined potential critical configurations in the fresh fuel salt container based on variables such as 235 U enrichment, UF 4 molar fraction, temperature, and container geometry. The second scenario explored the release of fission products during reactor operation in which the tritium buildup in the primary fuel salt was quantified through depletion calculations using SCALE/TRITON with continuous fuel makeup and fractional fission product removal. This scenario also assessed radioactivity levels in the off-gas system (OGS), quantifying radiotoxic nuclides that could be released into the environment. SCALE/SAMPLER was employed to perform uncertainty quantification to identify key operating parameters influencing the buildup of radiotoxic nuclides in the OGS. Additionally, radiation dose rates were calculated using SCALE/MAVRIC to estimate the maximum exposure levels within the reactor cell complex during operation. The final scenario evaluated the decay heat and radioactivity of the primary fuel salt collected in the drain tank, as well as the radiation dose rate outside the building from the presence of the drain tank. Overall, the application of SCALE’s various capabilities for radionuclide inventory generation, criticality analysis, and shielding in MSR fuel cycles was successfully demonstrated across these scenarios.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2025

Computational materials reliability assessment of hydrogen fueled gas turbine power generation engines

The use of blended fuel sources in land based gas turbine engines drives variations in the resulting operational profile (temperatures and pressures) which can impact engine reliability. Furthermore, variability in the manufacture of components affects the resulting microstructure which directly impacts material performance and reliability. Currently, data-driven models are typically used for maintaining and inspecting fleets of engines. Without explicitly capturing material and operational sources of variability conservatism must be used in developing component-level reliability models. Therefore, there exists an opportunity to use information from materials-scale physics models to better inform reliability modeling and reduce conservatism; the impact is more cost-efficient operation and maintenance of current and future fleets. Specifically, this work establishes a computational framework for evaluating the probabilistic high temperature creep performance of hot-section Ni-based superalloys where uncertainty comes from both microstructural and operational variability. A novel high-fidelity physics model which phenomenologically captures grain-boundary sensitive phenomena has been established. A probabilistic calibration procedure was used to calibrate the model and capture uncertainty in the parameterized model coefficients. A design of experiments methodology was established for identifying informative microstructural digital representations for suitable for forward model evaluation. Results show that training a machine-learning surrogate using this design criteria outperforms random selection of microstructural representations. Finally, two surrogate models were developed: (1) a deterministic surrogate model which predicts the local field response given microstructure, constitutive model parameters, and operating conditions (stress, temperature) and (2) a probabilistic model, where uncertainty comes from constitutive law uncertainty, built using denoising diffusion probabilistic models which samples responses given (1) microstructure and (2) operating conditions. These surrogate models enable partner Siemens Energy to rapidly perform UQ analysis specific to creep deformation across a range of microstructures and operating conditions. The impact is that these ML and physics codes can be used to establish more advanced reliability models for the inspection, servicing, and maintenance of land based gas turbine engines.

36 MATERIALS SCIENCE↗

DOE OSTI2014

First Look at Smoke Emissions from Prescribed Burns in Long-unburned Longleaf Pine Forests

While fire has long played a role in the longleaf pine ecosystem, there are still some stands in the southeastern United States where fire has not been reintroduced and fuels have accumulated for 50 years or more. As part of a larger study examining fuel loading and smoke emissions on Department of Defense installations in the southeastern U.S., fuels and trace emissions were measured during three prescribed burns at Ft. Jackson Army Base near Columbia, South Carolina in November 2011. These pine-forest understory fires provided valuable emissions data for fires that burned in stands that had little or no exposure to fire for decades. Smoke emissions were measured on the ground and from an aircraft by scientists from a large team of atmospheric researchers. (Akagi et al., 2013) To characterize initial emissions in the lofted plume and in point sources of residual smoldering combustion, trace-gas species were measured using an airborne FTIR and a ground-based FTIR, respectively. Whole-air sampling canisters were also collected from both ground- and airborne-based platforms. A total of 97 trace gases were quantified in this work, largely via infrared spectroscopy. Selected emissions data were compared with similar data collected from prescribed burns sampled in coastal North Carolina in 2010 in younger fuels beds of loblolly/longleaf stands near Camp Lejeune (Burling et al., 2011). The emission factors measured in this work differ by ~13-195% to EF measured from the managed stands at Camp Lejeune for organic and N-containing species, suggesting that fire emissions in similar ecosystems can exhibit large variability. Part of the differences, however, may be ascribed to burn conditions as well since the NC burns were during the wet season whereas the SC stands were burned after an extended drought. We also report the first detailed FTIR emissions data for a suite of monoterpenes. Figure 1 displays the emission factors (g/kg fuel) for several monoterpenes and isoprene as measured by the ground-based FTIR system. Due to their unsaturated structure, terpenes are highly reactive compounds emitted from plants thought to contribute to secondary organic aerosol formation (SOA) (Saathoff et al., 2009; Hennigan et al., 2011) and the formation of small oxygenated volatile organic compounds (OVOCs) (Jacob et al., 2002) in fire plumes. The known chemistry and measured abundance of monoterpenes suggests that these species impacted secondary plume processes including ozone, OVOC, and SOA formation in sampled plumes within the first few hours after emission.

biomass burning↗

DOE OSTI2020

An Overview of Neutron Irradiated SiC Layer Behavior using Micro-and Nano-Characterization Techniques

The complexity of fission product distribution and composition within the SiC layer of tristructural isotropic (TRISO) coated particles, irradiation effects on the SiC structure as well as the variable nature of metallic fission product release, has led to the exploration of multiple micro- and nano-characterization techniques. The fine scale of the fission product precipitates necessitates unique learnings and application of electron microscopic techniques with irradiated fuel during the Advanced Gas Reactor (AGR)-1 experiment analysis. A summarized discussion on the specific advanced techniques with associated method development for TRISO coated particles is provided followed by the down selected techniques currently considered to provide the highest impact. Techniques considered are electron probe micro-analyzer (EPMA), scanning transmission electron microscopy (STEM), and Precession electron diffraction (PED). SiC grain boundary characteristics are evaluated due to the mobility of specific fission products through grain boundaries. PED was performed for understanding the role of grain boundary character on fission product transport. One set of comparative analyses between AGR-1 and AGR-2 particles leads to a finding that the AGR-1, high-Ag-retention particle, had statistically more coincidence site lattice (CSL)-related grain boundaries (but fewer low-angle grain boundaries), compared to the AGR-2 particle. This implies that CSL-related grain boundaries may have a direct influence on Ag retention. However, precipitates were found on a relatively small fraction of CSL-related grain boundaries in both particles. In another set of comparison between AGR-1 and AGR-2 particles that were subjected to safety testing, there is significant differences in average SiC grain boundary distributions, but the fission product distributions on these grain boundaries are very similar.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Micro- and Nano-techniques for the Study of Fission Product Precipitation in SiC Layer

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2019

Simulation of Spent Nuclear Fuel loading into a Final Waste Repository

Previous work towards studying repository loading have used: - spent nuclear fuel (SNF) with an average burnup composition; - a lumped capacitance thermal model for calculating temperature in a Cyclus repository model. The goal of this work is to improve on the repository models and use U.S. historical SNF inventory data in simulations to more accurately study the loading of a waste repository. These goals will be achieved by: - using UNF-ST-and-DARDS Unified Database (UDB) that has historic assembly-specific data (e.g, isotopic composition, heat) in Cyclus simulations; - implementing a more accurate thermal model within a Cyclus repository model. Objectives: - Create a Cyclus spent fuel conditioning model that packages spent fuel bundles into packages which have user-defined properties. - Create a Cyclus medium-fidelity repository model that gives accurate time and spatial dependent temperature values and loads the repository based on a user-selected loading strategy. Cyclus is an agent-based extensible framework for modeling flow of material through user-defined nuclear fuel cycles. In Cyclus, each facility in the fuel cycle is modeled individually and the facilities interact with one another as independent agents. The spent fuel conditioning model accepts spent fuel bundles and puts them into a cylindrical waste package. In the spent fuel conditioning model, the user can define variables: For each layer, radius, thermal conductivity, thermal diffusivity; For each package, Number of spent fuel bundles, Radius and height. The waste repository model accepts waste packages and emplaces them into available positions within the waste repository based on a thermal criteria. The thermal criteria is a temperature limit at the interface between the waste package surface and the host geology, that is set based on the repository's host geology. In the waste repository model, the user can define the variables: Capacity, Distance between waste packages, Distance between drifts, Repository host geology, Loading Strategy. After the addition of new waste packages at each time step, the waste repository model recalculates the temperature at each location in the repository. If the addition of this new package causes its temperature to exceed the thermal limit, it will be placed back into the buffer. A thermal model that relies on a transient 'outside' model and quasi-steady-state 'inside' model is used to accurately determine the temperature in the repository. The 'outside' model assumes a homogenous medium with the Engineered Barrier System (EBS) replaced by the geologic medium. Temperature solutions for the central waste package, adjacent point and line sources are superimposed to calculate the temperature at specific points in the repository. The central drift consists of one finite line source which represents the central waste package. The central drift also consists of point sources that represent neighboring waste packages in the central drift. The neighboring drifts are represented by infinite line sources. The 'inside' model is considered to be at a quasi-steady-state condition because EBS has a relatively low thermal mass compared to the infinite geologic medium. The steady state calculation is performed at each time step with the heat source and interface temperature as boundary conditions. Future Work: Run Cyclus simulations with U.S. historical SNF inventory data, the spent fuel conditioning and repository models to study how waste package acceptance strategies impact repository loading.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

Weatherization Assistant NEAT/MHEA

The software provides a measure selection technique indicating cost effective retrofit activities that can be applied to a home using a standard Savings to Investment Ratio (SIR). Users must provide an input file describing the characteristics of the home to be evaluated. The software takes the input data provided and calculates energy savings and cost savings predicted for a standard set of measures given the input parameters. The Weatherization Assistant computes estimates of pre-retrofit whole building space heating and cooling energy consumptions based on the house description data supplied by the user. The consumptions are computed using a monthly heating and cooling variable base degree-day method by algorithms similar to those developed for the CIRA program [LBL, 1982]. The building consumptions are needed in computing the energy savings from measures affecting the efficiencies of the heating and cooling equipment. Weatherization Assistant then computes the energy savings and costs for each individual measure applicable to the building described as if it were the only measure installed in the house. From these energy savings, a discounted dollar savings over the life of each measure is computed. The ratio of this dollar savings to the cost of installing the measure, the "savings-to-investment ratio" (SIR), is used in an initial ranking of the measures' effectiveness. The "interacted" savings and SIR of measures are then determined assuming the measures are added to the house collectively, in order of their ranking, e.g., the second ranked measure is installed in the house initially described by the user after having been modified by the first ranked measure. If this second-ranked measure's updated SIR is greater than a user-defined limit, the measure is left implemented, else it is removed so that the next measure's effectiveness is not dependent on it. The choice between two mutually exclusive measures (such as different levels of insulation) is made on the basis of their "net present value" (NPV), the difference of life-time savings and installation cost, rather than their SIR. This has been shown to be the more correct criterion on which to base the selection between two measures, both of which cannot be installed. The audit computes and reports to the user the energy savings, discounted dollar savings, installation cost, and SIR for each measure considered cost-effective. For those with SIR greater than the user-designated cutoff, a materials list gives the material name, type, and quantity required for installation of the measure. Weatherization Assistant permits entry of pre-retrofit billing data for gas or electrically heated homes or homes with electric air-conditioning. The user may then make the decision to have the savings of the measures adjusted to reflect the difference in billed consumption and that predicted by the program.

Gettings, Michael↗

DOE OSTI2019

Hybrid Inverse Parameter Identification of Fully Coupled Ductile Damage Model for Steel Sheet DP600 with Two Different Algorithms: Trust Region and Genetic Algorithms

Ductile damage model has been widely regarded as a valuable method to predict the failure of sheet metal. Based on the thermodynamic theory and continuum damage mechanics, the fully coupled ductile damage model can be developed, which also can better predict the initiation and growth of the fracture. But the identifications of model parameters with theoretical methodology are difficult due to the complex coupling relationships existing among all state variables. The inverse methodology is regarded as a good method to resolve the problem. In this paper, the recently proposed fully coupled ductile damage model is chosen to investigate the deformation behavior of DP600 steel, in which the mixed saturation isotropic and kinematic hardenings are taken into account and fully coupled with the ductile damage. During the identification process, the least square formula of the error between experimental and numerical results is selected as the target function. The trust region algorithm and genetic algorithm are used with the help of MATLAB for the identification of three damage parameters. Finally, by comparing the experimental and numerical results, the validations of two algorithms are proved. The efficiency of the optimization process with trust region algorithm is higher, but with lower accuracy. Meanwhile, the optimization process is greatly affected by the chosen initial values of the ductile damage parameters.

36 MATERIALS SCIENCE↗

DOE OSTI2023

The value of fusion energy to a decarbonized United States electric grid

Fusion could be a part of future decarbonized electricity systems, but it will need to compete with other technologies. In particular, pulsed tokamak plants have a unique operational mode, and evaluating which characteristics make them economically competitive can help select between design pathways. Using a capacity expansion and operations model, here we determined cost thresholds for pulsed tokamaks to reach a range of penetration levels in a future decarbonized US Eastern Interconnection. The required capital cost to reach a fusion capacity of 100 GW varied from $2,700 to $7,500 kW -1 , and the equilibrium penetration increases rapidly with decreasing cost. The value per unit power capacity depends on the variable operational cost and on the cost of its competition, particularly fission, much more than on the pulse cycle parameters. These findings can therefore provide initial cost targets for fusion more generally in the United States.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2024

Environmental stress mediates groundwater microbial community assembly

Community assembly describes how different ecological processes shape microbial community composition and structure. How environmental factors impact community assembly remains elusive. Here we sampled microbial communities and >200 biogeochemical variables in groundwater at the Oak Ridge Field Research Center, a former nuclear waste disposal site, and developed a theoretical framework to conceptualize the relationships between community assembly processes and environmental stresses. We found that stochastic assembly processes were critical (>60% on average) in shaping community structure, but their relative importance decreased as stress increased. Dispersal limitation and ‘drift’ related to random birth and death had negative correlations with stresses, whereas the selection processes leading to dissimilar communities increased with stresses, primarily related to pH, cobalt and molybdenum. Assembly mechanisms also varied greatly among different phylogenetic groups. As a result, our findings highlight the importance of microbial dispersal limitation and environmental heterogeneity in ecosystem restoration and management.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2014

X-ray source considerations in operation of digital detector arrays

Digital Detector Arrays (DDA) are increasingly replacing film in radiography applications. Standards exist for characterizing the performance of these detectors, and for using them in specific inspections. We have observed that the selection of the x-ray source to use with these detectors can also have a significant influence on the performance. We look at differences between standard, and micro-focus x-ray tubes, and end-window vs. side-window micro-focus tubes. We find that for best results, one must calibrate the DDA for the source settings used during an inspection. This is particularly true for variable-focus sources.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Rational Selection of Transition-Metal Oxide Electrocatalysts from Structure Electronic Structure-Activity Relations: The Role of Defects, Strain, and Sub-Surface Layering

This BES research investigates the physicochemical properties of metal oxides and how they affect electrocatalytic functionalities. The goal is to develop a predictive framework for realizing top-performing electrocatalytic materials for energy-critical reactions. The hypothesis is that well-defined thin films allow detailed mapping of structural-activity relationships because flat surfaces are more straightforward to characterize. Furthermore, the well-defined nature of thin-film metal oxides allows precise tuning of structural and chemical variables for structure-activity-relationship mapping. The proposed research has two technical objectives. The first is to experimentally assess whether the binding energies of surface oxygen can serve as an activity descriptor for oxygen electrocatalysis on metal oxides and then how to control them by tuning the structure and chemical variables. The second is to find the rate-limiting process in oxygen electrocatalysis and other small-molecule reactions. Similar mechanistic insights have been developed on well-defined platinum surfaces but not yet on oxides. This research addresses this gap and uses electrochemistry and X-ray photoemission spectroscopy to study oxide surface chemistry. The obtained insights are collectively analyzed to reveal how the oxides’ structural and chemical variables affect kinetics and can be used to design more active electrocatalysts for energy-critical reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗