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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 271 records · Page 15
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Temperature measurements in heavily-sooting ethylene/air flames using synchrotron x-ray fluorescence of krypton

High-fidelity temperature field measurements have been made for several heavily-sooting ethylene/air flames that have historically been challenging environments for conventional optical diagnostics. These challenges have largely been overcome here, in this study, by conducting x-ray fluorescence (XRF) measurements of a Kr fluorescent agent in the hard x-ray regime (15 keV). The current methodology presents a more economical diagnostic than a previously reported implementation of the Kr-XRF method, by limiting seeding of the expensive fluorescent agent to only the fuel stream flows. Detailed reacting flow simulations have been used to interpret experimental signals by tracking the mole fraction of the fluorescent agent in the flow field. Simulated Kr densities are in excellent agreement with measurements throughout the flow field. Temperature measurements of the flow field also agree well with simulations and recent literature studies. However, uncertainties in the measurements become increasingly large downstream of the burner surface as the krypton fraction drops due to mixing of the fuel and co-flow streams. Additionally, we demonstrate that soot particles in the heavily sooting flames studied do not impede the Kr-XRF measurements.

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

Machine learning and process-based modeling of spatiotemporal changes in active layer thickness across Alaska

Permafrost degradation poses a growing threat to infrastructure stability and ecosystem resilience in the rapidly warming Arctic. We investigated the spatiotemporal dynamics of active layer thickness (ALT) across Alaska by integrating field observations, environmental datasets, a physically based Stefan model, and machine learning (ML) techniques. Using weather projections from the Coupled Model Intercomparison Project Phase 6 under two Shared Socioeconomic Pathways (SSP 2-4.5 and SSP 5-8.5), we assessed ALT sensitivity to projected future weather conditions. The random forest (RF) model outperformed the Stefan approach in predicting ALT on the training dataset (R² = 0.84 vs. 0.53) but demonstrated lower generalizability on the test dataset (R² = 0.24 vs. 0.54). The root mean square error (RMSE) for the RF model for training and testing ranged from 14 to 22 cm, compared to 17 and 18 cm for the Stefan model. Variable importance analysis revealed that mean annual temperature and slope angle were the strongest predictors of ALT, accounting for 19% and 18% of the variance, respectively, followed by sediment transport index (14%) and stream power index (11%). Comparative analysis of baseline ALT predictions showed the Stefan model tended to project a thicker active layer (mean ± SD: 65 ± 16 cm), compared to the RF model (mean ± SD: 59 ± 8.8) cm). Both models indicated a latitudinal gradient in ALT, with shallower depths at higher latitudes. Projected ALT increases by 2100 were estimated at 3.3 ± 2.2 cm under SSP 2-4.5 and 5.9 ± 4.0 cm under SSP 5-8.5 for the ML model, whereas the Stefan model projected substantially larger increases of 13 ± 2.6 cm (SSP 2-4.5) and 28 ± 4.4 cm (SSP5-8.5). Spatial analysis showed the greatest ALT increases in northern Alaska, with relatively smaller changes in southern regions. These findings highlight the complex, multifactorial nature of ALT dynamics and the value of hybrid modeling approaches. As rising temperatures accelerate permafrost thaw, changes in ALT can disrupt ecosystems, damage infrastructures, and enhance the release of stored soil carbon, highlighting the urgent need for improved predictive capabilities to inform adaptation strategies in the Arctic.

Climate sciences↗
DOE OSTI2026

Catalytic resonance theory for the kinetics of photon-promoted catalysis

The illumination of catalytic surfaces with a continuous or pulsed stream of photons dynamically modulates surface chemistry for faster rates, non-equilibrium conversion, or product selectivity control. To establish fundamental principles of dynamic photon-modulated catalysis, the photocatalytic conversion of a generic surface reaction was simulated using the kinetic Monte Carlo method to understand the kinetic implications of an independent stream of photons that promotes surface product desorption. The time-averaged photocatalytic rate at differential conditions for varying photon flux and temperatures indicated three kinetic regimes described by product thermal desorption control, surface reaction control, and an intermediate kinetic regime with a zero slope Arrhenius plot, consistent with a degree of rate control dominated by the photon arrival frequency (i.e., per-site photon flux). Here, the maximum photocatalytic rate occurred orders of magnitude above the Sabatier limit at the resonance frequency, identified as the photon arrival frequency matching the surface reaction rate constant.

Canavan, Jesse R. [University of Minnesota, Minnea↗
DOE OSTI2021

Winter precipitation changes in California under global warming: Contributions of CO2, uniform SST warming, and SST change patterns

Climate models project a wetting winter over California, distinct from the drying in all other Mediterranean climate regions under warming. Dynamic effect via an eastward extension of the westerly jet stream over the North Pacific is the root cause for the wetting California. Utilizing four sets of prescribed-SST (sea surface temperature) simulations, the relative effects of direct CO2 radiative forcing, uniform SST warming, and SST change pattern are investigated. The wetting winter is dominated by uniform SST warming mainly through its effect on the jet extension. As a fundamental response to the enhanced upper-tropospheric warming in the tropics, the jet extension in coupled simulations is well reproduced under uniform SST warming and robust among models. An El Niño-like SST warming pattern has a secondary contribution to the jet extension via atmospheric teleconnection, but with large inter-model spread. Relative to the SST forcing, the direct CO2 radiative effect is negligible.

Dong, Lu↗
DOE OSTI2022

Discovering hydrothermalism from Afar: In Situ methane instrumentation and change-point detection for decision-making

Seafloor hydrothermalism plays a critical role in fundamental interactions between geochemical and biological processes in the deep ocean. A significant number of hydrothermal vents are hypothesized to exist, but many of these remain undiscovered due in part to the difficulty of detecting hydrothermalism using standard sensors on rosettes towed in the water column or robotic platforms performing surveys. Here, we use in situ methane sensors to complement standard sensing technology for hydrothermalism discovery and compare sensors on a towed rosette and an autonomous underwater vehicle (AUV) during a 17 km long transect in the Northern Guaymas Basin in the Gulf of California. This transect spatially intersected with a known hydrothermally active venting site. These data show that methane signalled possible hydrothermal-activity 1.5–3 km laterally (100–150 m vertically) from a known vent. Methane as a signal for hydrothermalism performed similarly to standard turbidity sensors (plume detection 2.2–3.3 km from reference source), and more sensitively and clearly than temperature, salinity, and oxygen instruments which readily respond to physical mixing in background seawater. We additionally introduce change-point detection algorithms—streaming cross-correlation and regime identification—as a means of real-time hydrothermalism discovery and discuss related data supervision technologies that could be used in planning, executing, and monitoring explorative surveys for hydrothermalism.

58 GEOSCIENCES↗
DOE OSTI2021

Thermodynamic Analysis of Thermo-vacuum Clothes Drying Operation

Clothes drying accounts for a significant amount of energy consumed in residential and commercial sectors. A thermal vacuum clothes drying technology (TVCD) is proposed as an advanced clothes dryer which can significantly reduce the energy requirements by expediting the drying process. In the conventional convective clothes dryer, hot dry air is introduced into the drum which gets in direct contact to dry the clothes. This process is energy inefficient since the significant amount of heat and the water carried out with the exhaust stream are wasted. In contrast to the conventional convective drying technique, the drying mechanism of TVCD is through nucleate boiling at low temperature due to reduced vessel pressure. The process is not only efficient but also reduces the required time for drying. The objective of this paper is to develop a comprehensive thermodynamic model to predict the transient drying process of TVCD. The three-stage system model including the detail analysis of individual components is capable of simulating the variation of the water content in the textile under various operational conditions. The preliminary results show that the drying time of 3 lb textile from 70% to 2.5% in TVCD is approximately four times less than the time required in the conventional clothes dryer. Parametric studies are carried out to understand the effect of operation conditions and component geometry on the system performance. Energy consumption of the system is also analyzed.

Yang, Cheng-Min↗
DOE OSTI2020

Modeling Streamflow and Sediment Transport Under Current and Future Climates at the West Valley Site - 20231

Performance Assessment models often require inputs representing specific hydrologic processes such as streamflow and sediment flux. This paper details the development of a process-level hydrologic model and its use in a Probabilistic Performance Assessment (PPA) system-level model for the West Valley Site in western New York. For this PPA model, a watershed model was developed using SWAT (Soil and Water Assessment Tool) and used to evaluate water and sediment fluxes in nearby streams draining the Site. A particular challenge of probabilistic modeling over long periods of time is scaling parameters appropriately so that outcomes are not grossly over- or underestimated. This challenge is especially important when the spatial and temporal scales of process and system level models differ. In this instance, the SWAT watershed model and GoldSim PPA model have similar spatial scales of stream reaches and sub-catchments within a single watershed (approximately hundreds to tens of thousands of square meters, but the temporal scales differ considerably. The SWAT model calculates streamflow and sediment transport rates at the daily scale, while the PPA model requires long-term average values that are applied over hundreds to thousands of year-long periods. As such, distributions of daily climatic parameters such as average precipitation rate, temperature, wind speed, and relative humidity were developed to force a transient SWAT model that captures the dynamic behavior of the watershed in response to daily changes in the weather. Output from the model, which includes stream flow (m{sup 3}/y) and sediment transport rate (Mg/y) is then averaged over a 100-year period as an approximation for the long-term average values which can be applied in GoldSim. A single SWAT model was run 5000 times with varying climatic inputs and deterministic soil, land use, and elevation data, and the range of outputs were compiled into a distribution which can be implemented stochastically into the PPA Model. Additionally, this paper includes a high-level discussion of how changes in future climate affect weather input distributions, and a summary of how those changes in weather affect the outcomes from the SWAT model and the inputs into the PPA model. In this analysis, future climate distributions were developed based on climate research documenting the expected changes to precipitation and temperature in western New York. The 5,000 SWAT simulations were then repeated with these future climate distributions, and the resulting output was implemented into the PPA Model as hydrologic conditions under a future climate. In the current version of the PPA Model, hydrologic parameters change linearly from the 'current climate' conditions to the 'future climate' conditions over a period of 100 years, after which they remain constant. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Unconventional desalination: The use of cyclone separators in HDH desalination to achieve zero liquid discharge

Research in water desalination technologies is constantly growing to meet global demands for freshwater. Though acting to meet these demands, the rapid growth and spread of desalination technologies poses environmental issues due to the increasing brine concentrates that are ultimately discharged back to nature. This article presents a cyclone separator to transform a humidification-dehumidification (HDH) cycle to a dual-product cycle to produce freshwater and solid salt crystals for highly saline streams. A desalination cycle equipped with a cyclone separator is used to treat water with 3.5%–81% salinity. The separation efficiency is well above 99% and can produce potable water from hyper saline feed in a once-through process. Further, the cyclone separator performance was tested under different conditions including humidity ratios, relative humidities, and feed stream's salinities. The cyclone separator is self-cleaning and overcomes salt scaling. This behavior is a direct function of the walls' temperature and the carrier air dew point. Self-cleaning capability allows the cyclone separator to treat feed water of extreme salinities (up to 810,000ppm) down to freshwater salinity with zero liquid discharge. The cyclone separator was utilized in a novel HDH desalination technology to treat different salinities. The product was freshwater of salinity <500ppm.

42 ENGINEERING↗
DOE OSTI2023

New constraints on warm dark matter from the Lyman- α forest power spectrum

The forest of Lyman-α absorption lines detected in the spectra of distant quasars encodes information on the nature and properties of dark matter and the thermodynamics of diffuse baryonic material. Its main observable—the 1D flux power spectrum (FPS)—should exhibit a suppression on small scales and an enhancement on large scales in warm dark matter (WDM) cosmologies compared to standard Λ⁢CDM. Here, we present an unprecedented suite of 1080 high-resolution cosmological hydrodynamical simulations run with the graphics processing unit-accelerated code cholla to study the evolution of the Lyman-α forest under a wide range of physically motivated gas thermal histories along with different free-streaming lengths of WDM thermal relics in the early Universe. A statistical comparison of synthetic data with the forest FPS measured down to the smallest velocity scales ever probed at redshifts 4.0≲z≲5.2 [E. Boera et al., Revealing reionization with the thermal history of the intergalactic medium: New constraints from the Ly⁢α flux power spectrum, Astrophys. J. 872, 101 (2019)] yields a lower-limit m WDM >3.1 keV (95% C.L.) for the WDM particle mass and constrains the amplitude and spectrum of the photoheating and photoionizing background produced by star-forming galaxies and active galactic nuclei at these redshifts. Interestingly, our Bayesian inference analysis appears to weakly favor WDM models with a peak likelihood value at the thermal relic mass of m WDM =4.5 keV. In conclusion, we find that the suppression of the FPS from free-streaming saturates at k≳0.1 s km -1 because of peculiar velocity smearing, and this saturated suppression combined with a slightly lower gas temperature provides a moderately better fit to the observed small-scale FPS for WDM cosmologies.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Technology Assessment on Low-Temperature Waste Heat Recovery in Industry

The purpose of this report is to discuss the magnitude of low-temperature waste heat available in the US manufacturing sector and to identify current and emerging low-temperature heat recovery technologies and equipment. The primary focus of the study is on the industries that produce the lowest-temperature waste heat: the chemical, primary metal, petroleum, nonmetallic mineral, fabricated metal, food, paper, and wood industries. In addition to identifying the waste streams, their characteristics, and currently available heat recovery technologies, the study also explored future research opportunities and economic barriers for recovery technology implementation. Special attention was given to applicable heat to power conversion technologies such as the organic Rankine cycle, thermoelectric conversion, and the supercritical CO 2 cycle. The study included investigations in research and new developments, including turbine and heat exchanger cost for waste heat to power systems, size, efficiency, and intermittency of waste heat streams.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2022

Tunable Oxygen Reduction Electrocatalysis by Phenazine-Modified Carbons (Final Report)

This project aims to systematically investigate the fundamental interfacial chemistry that underlies the four-electron, four-proton oxygen reduction reaction (ORR) mediated by heteroatom-doped graphitic carbon electrodes. Heteroatom-doped (Fe, N, etc.) graphitic carbons have emerged as a rich class of materials that are promising ORR catalysts in low temperature fuel cells because of their earth-abundant elements, extremely low cost, environmental harmlessness, and high tolerance to impurities in the fuel stream. However, despite decades of research, systematic efforts to improve the activity, selectivity, and durability of these catalysts has been hampered both by a complex heterogeneous distribution of potential N- and Fe-dopant active sites and by the inability to tune the local electronic structure and environment of the active site with molecular precision. Understanding the fundamental chemistry that influences the turnover-limiting and selectivity determining steps for ORR and other multielectron/multiproton electrocatalytic transformations requires new and innovative methods to prepare heteroatom active sites with molecular precision on carbon surfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Comparison of basin-scale in situ and meteoric 10 Be erosion and denudation rates in felsic lithologies across an elevation gradient at the George River, northeast Tasmania, Australia

Long-term erosion rates in Tasmania, at the south ern end of Australia’s Great Dividing Range, are poorly known; yet, this knowledge is critical for making informed land-use decisions and improving the ecological health of coastal ecosystems. Here, we present quantitative, geologically relevant estimates of erosion rates for the George River basin, in northeast Tasmania, based on in situ-produced 10 Be ( 10 Be i ) measured from stream sand at two trunk channel sites and seven tributaries (mean: 24.1 ± 1.4 Mg km -2 yr -1 ; 1σ). These new 10 Bei-based erosion rates are strongly related to elevation, which appears to control mean annual precipitation and temperature, suggesting that elevation-dependent surface processes influence rates of erosion in northeast Tas mania. Erosion rates are not correlated with slope in contrast to erosion rates along the mainland portions of Australia’s Great Dividing Range. We also extracted and measured meteoric 10 Be ( 10 Be m ) from grain coatings of sand-sized stream sediment at each site, which we normalize to measured concentrations of reactive 9 Be and use to estimate 10 Be m -based denudation rates for the George River. 10 Bem/ 9 Be reac denudation rates replicate 10 Be i erosion rates within a factor of 3 but are highly sensitive to the value of 9 Be that is found in bedrock ( 9 Be parent ), which was unmeasured in this study. 10 Bem/ 9 Be reac denudation rates seem sensitive to recent mining, forestry, and agricultural land use, all of which resulted in widespread topsoil disturbance. Our findings suggest that 10 Bem/ 9 Be reac denudation metrics will be most useful in drainage basins that are geologically homogeneous, where recent disturbances to topsoil profiles are minimal, and where 9 Be parent is well constrained.

58 GEOSCIENCES↗
DOE OSTI2024

Griffin: A MOOSE-based reactor physics application for multiphysics simulation of advanced nuclear reactors

Griffin is a Multiphysics Object-Oriented Simulation Environment (MOOSE) based reactor physics application for multiphysics simulations of advanced reactor designs jointly developed by Idaho National Laboratory and Argonne National Laboratory. This paper summarizes the motivation, significance, architecture, design, and features of Griffin. Griffin offers flexible and extensible features to address the challenges associated with advanced reactor designs. These features range from fundamental particle transport to specific reactor physics tasks. The features cover a wide range including on-the-fly and traditional two-step cross-section generation methods, steady-state and transient transport solvers suitable for both heterogeneous and homogeneous models, high-fidelity depletion where thousands of isotopes can be tracked and low-fidelity depletion characterized by burnup, etc. The most fundamental aspect that sets Griffin apart from other reactor analysis codes is that it is developed based on the MOOSE framework. A modular development approach is strongly enforced, with multiphysics being an essential element considered since the beginning of Griffin’s development. Griffin links various MOOSE physics modules and couples to other MOOSE-based applications and non-MOOSE-based applications for multiphyiscs simulations. Griffin includes three modules: ISOXML for preparing and managing multigroup cross sections, radiation transport for solving the neutron transport equation, and reactor analysis for user-oriented reactor physics analysis functionalities. Griffin uses various finite element methods for spatial discretization, multigroup approximation for energy discretization and discrete ordinates method, spherical harmonics expansion method, and diffusion approximation for streaming direction discretization to solve the neutron transport equation. Griffin’s flexibility is evidenced through Griffin’s various applications to fast reactor, high-temperature reactor, pebble bed reactor, molten salt reactor, and microreactor designs. Griffin development follows the software quality assurance procedure for MOOSE-based applications and with software requirements consistent with the ASME NQA-1 standard. Griffin has been adopted into the reactor analysis system for the U.S. NRC and is in use at U.S. companies, universities and national laboratories.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

The influence of natural variability on extreme monsoons in Pakistan

The monsoons in Pakistan have been exceptionally harsh in recent decades, resulting in extraordinary drought conditions and record flooding events. The changing characteristics of extreme events are widely attributed to climate change. However, given this region’s long history of floods and droughts, the role of natural climate variability cannot be rejected without a careful diagnosis. Here, we examine how oceanic and atmospheric variability has contributed to unusual precipitation distributions in West South Asia. Variations in sea surface temperatures in the tropical Pacific and northern Arabian Sea, and internal atmospheric variability related to the circumglobal teleconnection pattern and the subtropical westerly jet stream, explain more than 70% of monthly summer precipitation variability in the 21st century. Several of these forcings have co-occurred with record strength during episodes of extreme monsoons, which have exacerbated the overall effect. Climate change may have contributed to increased variability and the in-phase co-occurrences of the identified mechanisms, but further research is required to confirm any such connection.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Radiative transfer in stars by feebly interacting bosons

Starting from first principles, we study radiative transfer by new feebly-interacting bosons (FIBs) such as axions, axion-like particles (ALPs), dark photons, and others. Our key simplification is to include only boson emission or absorption (including decay), but not scattering between different modes of the radiation field. Based on a given distribution of temperature and FIB absorption rate in a star, we derive explicit volume-integral expressions for the boson luminosity, reaching from the free-streaming to the strong-trapping limit. The latter is seen explicitly to correspond to quasi-thermal emission from a “FIB sphere” according to the Stefan-Boltzmann law. Our results supersede expressions and approximations found in the recent literature on FIB emission from a supernova core and, for radiatively unstable FIBs, provide explicit expressions for the nonlocal (“ballistic”) transfer of energy recently discussed in horizontal-branch stars.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

Polar Bear™ – Innovative Capture of Storage Tank Vapors

Polar Bear™ is a patented technology developed by the Energy & Environmental Research Center (EERC) to capture storage tank vapors and eliminate methane emissions from upstream oil- and gas-producing facilities. Sparked by early commercial investment, the EERC licensed the technology and extended the intellectual property to storage tanks. Polar Bear™ is uniquely engineered and adapted to individual lower-producing facilities where there is otherwise no economic alternative for capturing tank vapors. A high number of small producing oil and gas wells are distributed across the country. The aggregate contributes to a significant volume of emissions. Because of the lack of economy of scale, gas volumes from these facilities are typically not recovered and contribute to methane emissions. Polar Bear™ provides a fit-for-purpose compression solution that addresses cost by reducing complexity with respect to conventional vapor recovery units and eliminating oil changes. Unique to Polar Bear™ is the capability to separate oxygenated gas from storage tank vapors. Storage tanks are designed to “breathe,” allowing gas to enter and escape during internal level and temperature changes. This infiltration of air into the tank headspace imparts undesirable oxygen content with respect to pipeline gathering. Polar Bear™ separates the vapor stream, allowing oxygen-rich gas to be used as fuel on-site while recovering the liquids-rich portion of the gas where oxygen content is minimized. A prototype system was tested to verify process models, evaluate operational performance, and advance the technology readiness level from 5 to 6. Results provide a good match between experimental measurements and process models, indicating the models are useful for future scale-up and field design. Various mixtures of nitrogen and liquefied petroleum gas were tested to understand the mass balance of nitrogen and how it relates to the potential control of oxygen content. Findings indicate that less than 2000 ppm of oxygen is likely to remain in the liquid portion of the gas in field applications. The research and development prepare the technology for field implementation to eliminate routine and fugitive methane emissions from storage tanks.

02 PETROLEUM↗
DOE OSTI2026

Impact of Hydrogen on Methane and Pollutant Emissions over Three-Way Catalysts with Natural Gas–Hydrogen Blends

Blending natural gas (NG) with hydrogen (H₂) can improve combustion and engine performance while potentially facilitating the catalytic conversion of methane and other pollutants, resulting in cleaner tailpipe emissions. This study evaluates the impact of H2 on the conversion of methane, CO, and NOx emissions on a commercial three-way catalyst (TWC) in a flow reactor using synthetic gas mixtures that simulate stoichiometric engine exhausts with NG or NG+H₂ combustion. The work examines whether, and how, the additional amount of H₂ in the exhaust stream affects the conversion efficiency of methane and other pollutants. Experiments were conducted with both degreened and aged catalysts under controlled conditions, systematically varying temperature, the air-to-fuel equivalence ratio (λ), and λ modulation. Test conditions covered λ values from 0.996 to 1.000 to represent nominally stoichiometric engine operation with different λ modulation amplitudes, as well as a range of temperatures to inform control strategies for effective CH₄, CO, and NOₓ reduction. Overall, the results show that hydrogen addition significantly improves the conversion efficiency of CH₄ and NOₓ, particularly at temperatures below 500 °C. More significantly, this study highlights that exhaust gas composition, operating temperature, λ management, and the oxygen storage capacity of the TWC all play major roles in affecting the tailpipe emissions from NG and NG+H₂ combustion.

Prikhodko, Vitaly [ORNL] (ORCID:0000000244685836)↗
DOE OSTI2026

The ever-evolving active site: transformation of single atoms to extended structures during the Rh-catalyzed reverse water–gas shift reaction

At low temperatures (< 400°C), single atoms of Rh supported on rutile TiO 2 (rTiO 2 ) are responsible for the formation of CO during the reverse water gas shift (RWGS), while methane production is associated with the Rh-TiO 2 interface due to the correlation between methane formation rates and the volume-averaged Rh nanoparticle diameter. As the temperature is increased to >540°C, there is a notable increase in CO selectivity and methane production rates tend towards zero. The time to reach zero depends on the temperature but independent of the initial Rh structure (single atoms and/or nanoparticles), which is controlled by the catalyst preparation method (wetness impregnation versus colloidal nanoparticles). At 600°C and > 4 h time on stream, the catalytic behaviour becomes completely agnostic to the initial Rh structure as well as weight loading, and the catalysts are highly selective for the reverse water gas-shift reaction. Post-reaction HR-TEM image analysis confirms Rh nanoparticles crystallize/order during the reaction; at 400°C, most of the Rh particles are disordered, while at 600°C, they are more ordered (i.e., development of defined faceting). Infrared spectroscopy of CO adsorption on Rh nanoparticles confirms the appearance of defined facets after annealing in nitrogen at high temperatures. Annealing the Rh/rTiO 2 catalysts prior to the RWGS reaction demonstrates the structural transformation of Rh depends only on time and temperature and not on reactant or product fugacity. Sites responsible for stabilizing Rh single atoms are no longer competent at higher temperatures, enabling their integration into existent nanoparticles. As the reaction temperature is increased to temperatures >540°C, the dominant active site for CO production evolves from single atoms to extended Rh structures.

36 MATERIALS SCIENCE↗