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At least 1,027 records · Page 57
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Milestone 2.8: Preliminary Radiolytic Gas Generation Measurements from Helium-Backfilled Samples

The Department of Energy (DOE) is currently managing nearly 13 metric tons of aluminum-clad spent nuclear fuel (ASNF) with the intention of extended (> 50 years) dry storage in helium-backfilled canisters. Due to in-reactor and cooling pond conditions, oxyhydroxide corrosion layers have formed on the surface of the ASNF elements. These corrosion layers are susceptible to radiolysis and the formation of molecular hydrogen gas (H 2 ) due to the fuel’s inherent radiation field. Consequently, a rigorous evaluation of the effect of helium gas on radiolytic H 2 production is necessary to support the Technical Considerations and Challenges for Extended (> 50 yrs) Dry Storage of ASNF program, especially as previous Task 2 - Oxyhydroxide Layer Radiolytic Gas Generation Resolution work demonstrated a significant effect of gas composition on the radiolytic yield (G-value) of H 2 . Here we report preliminary G-values for the radiolytic formation of H 2 from the gamma irradiation of pre-corroded aluminum alloy 1100 coupons flame sealed in helium environments. Irradiations yielded G(H 2 ) values of (5.1 ± 0.5) x 10 –4 and (9.4 ± 0.9) x 10 –4 µmol J –1 for pristine coupons, and (10.1 ± 0.4) x 10 –4 and (15.1 ± 1.2) x 10 –4 µmol J –1 for pre-corroded coupons for 0% and 50% relative humidity, respectively. These helium environment G(H 2 ) values are between 28% and 58% higher than previously reported values for argon environments. This enhancement is attributed to the significant difference in first ionization energy between helium (24.59 eV) and argon (15.76) facilitating additional processes, e.g., Penning ionization. These new preliminary helium environment G(H 2 ) values will be employed by Task 3 - Sealed and Vented System Episodic Breathing and Gas Generation Prediction to model the effect of radiolytic H 2 accumulation in helium environments to evaluate the practicality of the extended storage standard canister design.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

Resolution of Tolerance Variations

The connector/adapter assembly (CAA) is one component of a higher-level assembly. A simplified representation of the CAA is illustrated in Figure 1. The location of each CAA is required to meet a specific positional requirement. Several CAAs have been measured and found to be out of tolerance. The connector and the adapter are welded to each other such that the cylindrical axes of the two components are coaxial. The positional tolerance condition requires that all points on the outer surface of the CAA must be within a defined maximum diameter, as illustrated in Figure 1. Two different methods have been developed to measure the CAA positions from coordinate measuring machine (CMM) data. One method (RevD) extrapolates the data from two circles approximately midway from the weld region to each end. The second method (RevF) measures points that are much closer to the actual ends.

42 ENGINEERING↗
DOE OSTI2024

Spatially Resolved Near Field Spectroscopy of Vibrational Polaritons at the Small N Limit

Vibrational polaritons, which have been primarily studied in Fabry–Pérot cavities with a large number of molecules (N ~ 10 6 –10 10 ) coupled to the resonator mode, exhibit various experimentally observed effects on chemical reactions. However, the exact mechanism is elusively understood from the theoretical side, as the large number of molecules involved in an experimental strong coupling condition cannot be represented completely in simulations. This discrepancy between theory and experiment arises from computational descriptions of polariton systems typically being limited to only a few molecules, thus failing to represent the experimental conditions adequately. To address this mismatch, we used surface phonon polariton (SPhP) resonators as an alternative platform for vibrational strong coupling. SPhPs exhibit strong electromagnetic confinement on the surface and thus allow for coupling to a small number of molecules. As a result, this platform can enhance nonlinearity and slow down relaxation to the dark modes. In this study, we fabricated a pillar-shaped quartz resonator and then coated it with a thin layer of cobalt phthalocyanine (CoPc). By employing scattering-type scanning near-field optical microscopy (s-SNOM), we spatially investigated the dependency of vibrational strong coupling on the spatially varying electromagnetic field strength and demonstrated strong coupling with 38,000 molecules only–reaching to the small N limit. Through s-SNOM analysis, we found that strong coupling was observed primarily on the edge of the quartz pillar and the apex of the s-SNOM tip, where the maximum field enhancement occurs. In contrast, a weak resonance signal and lack of coupling were observed closer to the center of the pillar. This work demonstrates the importance of spatially resolved polariton systems in nanophotonic platforms and lays a foundation to explore polariton chemistry and chemical dynamics at the small N limit–one step closer to reconcile with high-level quantum calculations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Functionalized Magnetic Nanoparticles for Technetium Sequestration from Groundwater

Technetium 99 (Tc) is among the most common environmental contaminants at DOE sites and one of the most common risk drivers in low- and high-level waste disposal sites. The majority of Tc is generated from anthropogenic sources, such as nuclear power plants, global weapons, nuclear storage facilities and medical applications. Through these sources, Tc contamination has been unintentionally introduced in to the environment. The most common chemical form of Tc is Tc(VII)O{sub 4}{sup -}. Due to its high solubility and mobility, Tc can enter the food chain and cause adverse health effects to humans. Currently, ion exchange resins and reduction processes are the most common approaches for Tc immobilization. Although these techniques have shown to be effective, they also possess major drawbacks, such as high cost, low adsorption capacity, and complex creation and maintenance. Therefore, development of more efficient and simple technologies for the remediation of Tc-contaminated systems are needed. Functionalized magnetic nanoparticles have been used to remove organic and inorganic contaminants from water resources. These nanoparticles have attracted extensive attention as an adsorbent material due to their large surface area, high efficiency, low-cost, easy functionalization and separation with a magnet. This study seek to develop functionalized magnetic iron oxide nanoparticles for the efficient removal of Tc and other heavy metal contaminants from water resources under ambient conditions. Objectives: Synthesize magnetic iron oxide nanoparticles and functionalize their surface with Cetyltrimethylammonium Bromide (CTAB) and tetraethyl-orthosilicate (TEOS). Characterize the synthesized nanoparticles using scanning electron microscopy (SEM) coupled with energy dispersive X-ray spectroscopy (EDS), Dynamic Light Scattering (DLS) and Zeta PALS. Perform adsorption studies to evaluate their adsorption behavior and capacity for (a) Technetium using Rhenium (ReO{sub 4}{sup -}) as a surrogate and (b) heavy metals, e.g. Cu{sup 2+}. Conclusions: Magnetic iron oxide nanoparticles were successfully functionalized with CTAB and TEOS. The functionalization of the iron oxide nanoparticles affects their surface charge and their hydrodynamic diameter. The addition of CTAB or TEOS decreased the hydrodynamic diameter of the nanoparticles due to repulsive and steric forces. The SEM micrographs show spherical nanoparticles of different sizes. The EDX analysis shows the presence of iron and oxygen from the iron oxide crystalline structure, and the different constituents of the CTAB and TEOS molecules. Proof-of-concept shows the successful adsorption of rhenium (ReO{sub 4}{sup -}) and copper Cu{sup 2+}) onto CTAB-Fe{sub 2}O{sub 3} and TEOS-Fe{sub 2}O{sub 3} respectively.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Controlling Oxidation of Nb in Oxygen Abundant Environments.

Superconducting Radio Frequency (SRF) cavities, the core of modern particle accelerators, rely on high-purity niobium (Nb) to achieve high quality factors and accelerating gradients. However, native oxidation in ambient conditions introduces a complex oxide layer with increased surface defects and contamination, particularly from carbon. This research explores a controlled oxidation processes in an oxygen-abundant environment to try to control this complex oxide stack, with the goal of improving surface purity and uniformity. Using standard surface preparation techniques—including electropolishing, vacuum baking, and sonication—followed by a custom oxidation protocol, we compared structural and chemical changes through Confocal Microscopy, Scanning Electron Microscopy (SEM), and X-Ray Photoelectron Spectroscopy (XPS). Results show that iterative oxidation cycles can significantly reduce carbon-related defects, even without baking. Aditionally, baked samples with a specific oxidation technique demonstrated a measurable 25\% decrease in carbide formation.

Romero, Juan [Fermilab]↗
DOE OSTI2026

Advancing Mass Timber Buildings: Novel Methods Improve Thermal Assessment and Material Use

For nearly a century, thermal demand calculations for buildings have relied on simplified models developed to match the technical constraints of their era. The first standards, introduced in Germany and Austria in 1929, established climate zones and material conductivity coefficients that, with only incremental updates, still underpin many current assessments. Yet, methods such as Hot box testing, originally designed for lightweight insulation, continue to be applied for mass timber buildings, overlooking thermodynamic characteristics confer real-world advantages. Recent research at Oak Ridge National Laboratory incorporates updated methodologies, aligned with ASHRAE Standard 55 (ASHRAE, 2023) accounting for factors such as thermal inertia, inner surface temperatures, emissivity, solar gains, and dynamic outdoor conditions. These factors better reflect observed heating and cooling loads and highlight opportunities for efficient use of materials in mass timber construction. This work provides a framework for designing comfortable, resilient, and resource-efficient buildings while aligning with performance expectations in energy codes.

Pickett, Robert [International Mass Timber Allianc↗
DOE OSTI2025

Methods to Observe Tribological Failures in Self-Mated Steel Contacts

Scuffing, a type of wear found in highly stressed or poorly lubricated contacts, is characterized by a rapid increase in friction and severe plastic deformation of the near-surface material. Scuffing has proven difficult to study because it initiates unpredictably, progresses rapidly, and typically develops within an inaccessible contact interface. Although there have been successful in-situ studies of scuffing in real-time, the transparent counter body needed for these studies changes the interactions between the surfaces and the lubricant, which affects the scuffing process in unknown ways. This paper describes the development of X-ray-compatible tribometry to study the scuffing of self-mated steels in-situ and in real-time. The method uses a crossed cylinders configuration with a thin (500 μm thick) stationary component and a small (≈200 μm) contact width to maximize X-ray interactions with atoms within the stress field generated by the contact. The resulting instrument and method are used to benchmark the scuffing response of self-mated 52,100 steel under tribologically challenging ‘oil-off’ lubrication conditions. The results demonstrate reliable scuffing in this configuration despite the relatively small contact areas and loads used. Following scuffing, gross plastic deformation was observed on both surfaces along with significant subsurface grain refinement and flow only on the stationary surface, which experienced constant contact. Interestingly, high friction initiated at specific locations of the migratory surface, which experienced intermittent contact, and then propagated across the track over time, suggesting that local conditions of the migratory surface dominated friction leading into the failure event.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Defect-Driven Redox Interplay on Anatase TiO 2 : Surface-Structure Dependent Activation for CO 2 Hydrogenation Catalysis

Titanium dioxide (TiO 2 ) is one of the most extensively studied oxides as an active catalyst or catalyst support, particularly in energy and environmental applications, but the atomistic mechanisms governing its dynamic response to reactive environments and their correlation to reactivity remain largely elusive. Using in situ environmental transmission electron microscopy (ETEM), synchrotron X-ray diffraction (XRD), ambient-pressure X-ray photoelectron spectroscopy (AP-XPS), temperature-programmed reduction (TPR), reactivity measurements, and theoretical modeling, we reveal the dynamic interplay between oxygen loss and replenishment of anatase TiO 2 under varying reactive conditions. Under H 2 exposure, anatase TiO 2 undergoes surface reduction via lattice oxygen loss, forming Ti 3 O 5 . In contrast, CO 2 exposure induces oxygen replenishment, reversing stoichiometry. In mixed H2/CO 2 environments, the reverse water–gas shift (RWGS) reaction proceeds selectively on stepped and high-indexed TiO 2 surfaces, whereas the thermodynamically stable TiO 2 (101) surface remains inactive and intact. Critically, H 2 pretreatment generates oxygen vacancies on TiO 2 (101), transforming it into an active Ti 3 O 5 or defect-rich surface that catalyzes RWGS. By correlating surface structure, defect dynamics, and gas-phase interactions, this work deciphers the competition between H 2 -driven reduction and CO 2 -driven oxidation pathways at the atomic scale. Furthermore, these insights establish defect engineering as a strategic lever to activate inert TiO 2 facets, advancing the design of adaptive catalysts for sustainable fuel synthesis technologies.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Heat Generation versus Heat Dissipation Maps for Batteries (Battery Safety Maps) [SWR-21-27]

NREL's Battery Safety Map (Heat Generation versus Heat Dissipation Maps for Batteries) generates a response surface that is grouped into regions where the battery is deemed safe from the propagation of thermal runaway, those where an engineering solution would render the battery safe, and finally instances where thermal runaway is inevitable. The demarcation for the different regions is provided by specifications or constraints imposed by the end user. NREL's Battery Safety Map is a user-defined subroutine that sweeps through a set of parameters describing the operating conditions and short-circuit scenarios for battery safety simulations. For each run, the electrochemical-thermal model implementing reaction kinetics and gas generation are run to evaluate the amount of heat generated. A thermal model then captures the amount of heat dissipation based on boundary conditions defined (e.g., forced convection, constant temperature at the surface, etc.). Based on the rate of heat transfer and the amount of heat generated, each run is classified into "safe," "mitigation possible," or "unsafe" zones. These categories are defined based on constraints or tolerance specifications provided by the end user.

Santhanagopalan, Shriram↗
DOE OSTI2021

Effects of water on the kinetics of acetone hydrogenation over Pt and Ru catalysts

We employed an approach combining reaction kinetics measurements at steady state conditions, electronic structure calculations employing density functional theory, and microkinetic modeling for acetone hydrogenation to provide insights into the effects of water on metal catalyst surfaces for the hydrogenation of oxygenates over a wide range of reaction conditions. Elucidation of the repulsive interactions due to adsorbed water molecules at various reaction conditions provides a basis to formulate rate expressions for heterogeneous catalytic processes of biomass oxygenates. Reaction kinetics experiments were carried out at partial pressures of H 2 , acetone, water and helium in the range of 0.51-0.79, 0.02-0.13, 0.08-0.23, 0-0.28 atm, respectively. We show that the addition of water enhances the hydrogenation rate at 353 K and 1 atm on oxophilic metal catalysts such as Ru/C, whereas the same promotional effect of water is not observed for Pt-based catalysts. Microkinetic model predictions for the hydrogenation of acetone on Ru in the absence and presence of water, using enthalpies and entropies obtained from DFT calculations, were in agreement with the experimentally observed reaction orders and activation barriers. The model shows that a water-assisted hydroxypropyl path is expected to be the favored path on Ru with a rate-determining step of H-OH-mediated hydrogenation of C 3 H 6 OH (i.e., the hydroxypropyl intermediate formed by H 2 O-mediated initial hydrogenation of acetone) to produce isopropyl alcohol (IPA). Furthermore, hydrogen, acetone, hydroxypropyl intermediate and hydroxyl species were predicted to be abundant on the Ru surface with a high coverage of nearly 85%. Lastly, the combined studies of computational and experimental catalysis on hydrogenation reactions help to elucidate the mechanistic role of water on metal catalyzed reactions for producing chemical building blocks from biomass-derived oxygenates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Methane emission hotspots in a boreal forest-fen mosaic potentially linked to deep taliks

Permafrost thaw is transforming boreal forests into mosaics of wetlands and drier uplands. Topographic controls on hydrological and ecological conditions impact methane (CH 4 ) fluxes, contributing to uncertainty in local and regional CH 4 budgets and underlying drivers. The objective of this study was to explore CH 4 fluxes and their drivers in a transitioning boreal forest-fen ecosystem (Goldstream Valley, Alaska, USA). This landscape is characterized by thawing discontinuous permafrost and heterogeneous mosaics of fens, collapse-scar channels, and small mounds of permafrost soils. From a survey in July 2021, observed chamber CH4 fluxes included fen areas with intermediate to very high emissions (29.8–635.3 mg CH 4 m −2 d −1 ), clustered locations with CH 4 uptake (−2.11 to −0.7 mg CH 4 m −2 d −1 ), and three anomalous emission hotspots (342.4–772.4 mg CH 4 m −2 d −1 ) that were located near samples with lower emissions. Some surface and near-surface variables partially explained the spatial variation in CH 4 flux. Log-transformed CH 4 flux had a positive linear relationship with soil moisture at 20 cm depth ( R 2 = 0.31, p -value < 1e-5) and negative linear relationships with microtopography ( R 2 = 0.13, p -value < 0.006) and slope ( R 2 = 0.28, p -value < 2e-5). Methane emissions generally occurred in flat, wet, graminoid-dominated fens, whereas CH 4 uptake occurred on permafrost mounds dominated by feather mosses and woody vegetation. However, the CH 4 hotspots occurred on drier, slightly sloped locations with low or undetectable near-surface methanogen abundance, suggesting that CH 4 was produced in deeper soils. When the hotspot samples were omitted, log-transformed CH 4 flux had a positive linear relationship with near-surface methanogen abundance ( R 2 = 0.29, p -value = 0.0023), and stronger linear relationships with soil moisture, slope, and soil macronutrient concentrations. Our findings suggest that some CH 4 emission hotspots could arise from CH 4 in deep taliks. The inference that methanogenesis occurs in deep taliks was strengthened by the identification of intrapermafrost taliks across the study area using low-frequency geophysical induction. This study assesses surface spatial heterogeneity in the context of subsurface permafrost conditions and highlights the complexity of CH 4 flux patterns in transitioning forest-wetland ecosystems. To better inform regional CH 4 budgets, further research is needed to understand the spatial distribution of terrestrial CH 4 hotspots and to resolve their surface, near-surface, and subsurface drivers.

boreal↗
DOE OSTI2021

Processes contributing to cloud dissipation and formation events on the North Slope of Alaska

Abstract. Clear-sky periods across the high latitudes have profound impacts on the surface energy budget and lower atmospheric stratification; however an understanding of the atmospheric processes leading to low-level cloud dissipation and formation events is limited. A method to identify clear periods at Utqiaġvik (formerly Barrow), Alaska, during a 5-year period (2014–2018) is developed. A suite of remote sensing and in situ measurements from the high-latitude observatory are analyzed; we focus on comparing and contrasting atmospheric properties during low-level (below 2 km) cloud dissipation and formation events to understand the processes controlling clear-sky periods. Vertical profiles of lidar backscatter suggest that aerosol presence across the lower atmosphere is relatively invariant during the periods bookending clear conditions, which suggests that a sparsity of aerosol is not frequently a cause for cloud dissipation on the North Slope of Alaska. Further, meteorological analysis indicates two active processes ongoing that appear to support the formation of low clouds after a clear-sky period: namely, horizontal advection, which was dominant in winter and early spring, and quiescent air mass modification, which was dominant in the summer. During summer, the dominant mode of cloud formation is a low cloud or fog layer developing near the surface. This low cloud formation is driven largely by air mass modification under relatively quiescent synoptic conditions. Near-surface aerosol particles concentrations changed by a factor of 2 around summer formation events. Thermodynamic adjustment and increased aerosol presence under quiescent atmospheric conditions are hypothesized as important mechanisms for fog formation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Capillary-driven Condensation for Heat Transfer Enhancement in Steam Power Plants

A novel condensation method was developed to enhance the efficiency of steam power plants. The method consists of a hierarchical structure on the surface of condenser tubes consisting of a wicking structure overlaid with a porous hydrophobic membrane. The project is divided into two main efforts. First, a structure with highly defined geometry was made utilizing microfabrication on silicon. This structure helped us elucidate the physics of steam condensation at the surface, more easily model the heat transfer coefficient, and demonstrate the first proof-of-concept for our proposed condensation approach. The structures on silicon achieved a heat transfer coefficient ~ 240% higher than the theoretical filmwise value at the same operating condition. Second, the method is explored for scalability by fabricating surfaces with industrial class materials followed by heat transfer measurements on flat surfaces. An HTC enhancement of 50% over the experimental filmwise value was achieved on hierarchical copper surfaces made of commercially available copper foams and meshes, showing the potential of achieving heat transfer enhancement using low cost and scalable materials. Scalable fabrication of the hydrophobic membrane and the porous copper wick were also investigated. Our heat and mass transfer model predicts a > 5x heat transfer enhancement on a scalable version of capillary driven condenser made of membrane covered porous copper. The results demonstrate the promise of capillary-driven condensation surfaces for heat transfer applications.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2021

Solution Chemistry to Control Boron-Containing Monolayers on Silicon: Reactions of Boric Acid and 4-Fluorophenylboronic Acid with H- and Cl-terminated Si(100)

In this work, the reactions of boric acid and 4-fluorophenylboronic acid with H- and Cl-terminated Si(100) surfaces in solution were investigated. X-ray photoelectron spectroscopy (XPS) studies reveal that both molecules react preferentially with Cl–Si(100) and not with H–Si(100) at identical conditions. On Cl–Si(100), the reactions introduce boron onto the surface, forming a Si–O–B structure. The quantification of boron surface coverage demonstrates that the 4-fluorophenylboronic acid leads to ~2.8 times higher boron coverage compared to that of boric acid on Cl–Si(100). Consistent with these observations, density functional theory studies show that the reaction of boric acid and 4-fluorophenylboronic acid is more favorable with the Cl- versus H-terminated surface and that on Cl–Si(100) the reaction with 4-fluorophenylboronic acid is ~55.3 kJ/mol more thermodynamically favorable than the reaction with boric acid. The computational studies were also used to demonstrate the propensity of the overall approach to form high-coverage monolayers on these surfaces, with implications for selective-area boron-based monolayer doping.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Impact of vegetation physiology and phenology on watershed hydrology in a semiarid watershed in the Pacific Northwest in a changing climate

Concurrent with changes in climate conditions, increases in atmospheric composition and transport can affect land surface processes by regulating physiological and phenological responses of plants, and consequently perturb water, carbon, and nitrogen (N) dynamics at multiple scales. Howerver, the relationships bwtween plants physiological and phenological and land surface processes in a changing climate are less well known due to the limitation of representing palnts properties in traditional hydrological models. In this study, we use the Community Land Model version 5 (CLM5) to investigate how projected changes in large scale atmospheric conditions can affect hydrologic and biogeochemical dynamics in the Upper Columbia-Priest Rapids (UCPR) watershed, a typical semi-arid watershed located in the north-western United States dominated by croplands. Six numerical experiments considering climate change, CO2 concentration, and N deposition consistent with the Representative Concentration Pathways (RCPs) 4.5 and 8.5 are performed at 1-km resolution over the period of 2015-2099. Our results show that, compared with historical results (1985-2014), the elevated CO2 directly increases plants N uptake rates that provide additional leaf N to enhance photosynthesis by the end of 21st century (2070-2099). The higher GPP leads to changes in stomatal resistance and increased leaf area index (LAI) that affect evaporatranspiration (ET) and its components. As a result of stomatal responses to a higher CO2 concentration, ET over corn fields declines by 24.6 mm yr-1 under RCP4.5, and by 64.0 mm yr-1 under RCP8.5, respectively by the end of the century from its historical mean of 428 mm yr-1. Meanwhile, ET over soybean fields increases by 27.7 mm yr-1 under RCP4.5 and 9.98 mm yr-1 under RCP8.5 from its historical mean of 507 mm yr-1 as a result of CO2 fertilization as soybeans are able to uptake more N to increase LAI significantly. Furtherfore, the changes in physiological and phenological in corn and soybean can strongly modulate water budget terms over the watershed in response to expected changes in greenhouse gas concentrations and atmospheric composition. Additionally, increases in CO2 concentration and N deposition are beneficial for improving water use efficiency of corn and soybean, therefore lead to less water consumption per unit gram of carbon produced from these crops. Our study elucidates the need to jointly consider effects of surface climate and atmospheric composition and transport in understanding and predicting watershed hydrologic and biogeochemical responses, especially for an agricultural watershed.

Zhu, Bowen↗
DOE OSTI2020

Visualization of R410A Flow Boiling Inside Horizontal Smooth Tubes under Diabatic Conditions

This article presents a novel approach to visualize the flow boiling in round tubes under “diabatic conditions”. In the visualization test section, a 3D printed round tube is placed inside a glass tube with secondary fluid at a higher temperature flowing in the annulus between the two tubes thus providing diabatic conditions. Experimental work was conducted for evaporating R410A flow in a horizontal smooth round tube with the inner diameter of 6.3 mm. Compared to the traditional adiabatic visualization technique, the more realistic evaporative condition is simulated and the developing evaporation process is captured. New insights for the flow behavior at low vapor quality are brought by this diabatic method. The vapor plug occurs at very low vapor quality, and this is attributed to the coalescence of bubbles generated on the heated tube wall. For the intermittent flow, liquid slug triggered by Kelvin–Helmholtz instability affects the nucleation on the tube wall. It brings the fresh liquid to rewet the dry surface and activate the nucleation sites. Finally, heat flux condition affects the heat transfer mechanisms during the flow boiling, and the heat transfer through the nucleate boiling mechanism increases as the heat flux increases.

3D printed↗
DOE OSTI2022

Bridge Sites of Au Surfaces Are Active for Electrocatalytic CO 2 Reduction

Prior in-situ attenuated total reflectance Fourier transform infrared (ATR-FTIR) studies of electrochemical CO 2 reduction catalyzed by Au, one of the most selective and active electrocatalysts to produce CO from CO 2 , suggest that the reaction proceeds solely on the top sites of the Au surface. This finding is worth updating with an improved spectroelectrochemical system where in-situ IR measurements can be performed under real reaction conditions that yield high CO selectivity. Herein, we report the preparation of a Au-coated Si ATR crystal electrode with both high catalytic activity for CO 2 reduction and strong surface enhancement of IR signals validated in the same spectroelectrochemical cell, which allows us to probe the adsorption and desorption behavior of bridge-bonded *CO species (*CO B ). In this study we find that the Au surface restructures irreversibly to give an increased number of bridge sites for CO adsorption within the initial tens of seconds of CO 2 reduction. By studying the potential-dependent desorption kinetics of *CO B and quantifying the steady-state surface concentration of *CO B under reaction conditions, we further show that *CO B are active reaction intermediates for CO 2 reduction to CO on the Au surface. At medium overpotential, as high as 38% of the reaction occurs on the bridge sites.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Theoretical Investigation of the Adsorbate and Potential–Induced Stability of Cu Facets During Electrochemical CO 2 and CO Reduction

The activity and product selectivity of electrocatalysts for reactions like the carbon dioxide reduction reaction (CO 2 RR) are intimately dependent on the catalyst's structure and composition. While engineering catalytic surfaces can improve performance, discovering the key sets of rational design principles remains challenging due to limitations in modeling catalyst stability under operating conditions. Herein, we perform first-principles density functional calculations adopting implicit solvation methods with potential control to study the influence of adsorbates and applied potential on the stability of different facets of model Cu electrocatalysts. Using coverage dependencies extracted from microkinetic models, we describe an approach for calculating potential and adsorbate-dependent contributions to surface energies under reaction conditions, where Wulff constructions are used to understand the morphological evolution of Cu electrocatalysts under CO 2 RR conditions. Here we identify that CO*, a key reaction intermediate, exhibits higher kinetically and thermodynamically accessible coverages on (100) relative to (111) facets, which can translate into an increased relative stabilization of the (100) facet during CO 2 RR. Our results support the known tendency for increased (111) faceting of Cu nanoparticles under more reducing conditions and that the relative increase in (100) faceting observed under CO 2 RR conditions is likely attributed to differences in CO* coverage between these facets.

30 DIRECT ENERGY CONVERSION↗