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DOE OSTI2021

Assessment of tritium effluent from Prototype Generation IV Sodium-cooled Fast Reactor

We report a tritium transport model for a pool-type sodium cooled fast reactor was developed for estimation of tritium effluents from the Prototype Generation IV Sodium-cooled Fast Reactor (PGSFR). For this purpose, the transport model developed for Experimental Breeder Reactor II and Fast Flux Test Facility was updated and validated. The tritium production rate from ternary fission and activations in PGSFR were calculated by the Argonne Reactor Computation (ARC) code suite for fast reactor analysis, and due to the potential uncertainties in source terms and variations of cold trap performance and material permeability during reactor operation, the tritium distributions and tritium effluents were estimated for several bounding cases. The upper bounding gaseous and liquid tritium release rates from PGSFR are similar to ~440.7 Ci/year and 14.7 Ci/year, respectively. The gaseous tritium effluent is about few orders of magnitude smaller than the regulatory constraint of the tritium concentration in the air. The peak tritium concentration in the steam-generator feedwater is similar to ~1.1x10 -3 mu Ci/g, which is required to be diluted prior to releasing as tritiated water. The accumulated tritium in the cold trap after five cycle operations is ~ 52,000 Ci. Because of significant conservatism in these upper bounding estimations, it is expected that the tritium effluent at the nominal case with plausible source terms would be about 2 orders of magnitude smaller than that of the upper bounding case.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2022

Design and Optimization of Structured Multi-Functional Trapping Catalysts for Conversion of Hydrocarbons and NOx from Diesel and Advanced Combustion Engines

Oxides of nitrogen in the form of nitric oxide (NO) and nitrogen dioxide (NO 2 ) commonly referred to as NOx, is one of the two chemical precursors that lead to ground-level ozone, a ubiquitous air pollutant in urban areas. A major source of NOx is generated by equipment and vehicles powered by diesel engines, which have a combustion exhaust that contains NOx in the presence of excess O 2 . Vehicular emission control catalysts are ineffective in eliminating CO, hydrocarbons, and NOx during engine cold-start when exhaust temperatures are below 200°C. The objective of the project was to develop and demonstrate a multi-functional, catalyzed trap that enables vehicles with advanced combustion strategies to meet Tier 3 emissions standards while achieving the 150 °C challenge for sustained co-oxidation of HCs and CO and ≥90% NO trapping and release during warmup. Specifically, the multi-functional Lean HC+NOx (LHCNT) was developed for application in the exhaust aftertreatment of conventional diesel engines and engines having low temperature combustion (LTC) regimes. Activities included the design and synthesis of adsorbents and catalysts, screening and evaluation. Passive NOx absorbers (PNA), hydrocarbon (HC) traps, and oxidation catalysts (OC) were evaluated for use in series or as integrated devices. Predictive tools were developed utilizing the characterization and analysis of these materials, and an emission system was designed and optimized utilizing the catalyst systems. Microkinetic models were developed for the PNA for the simple NO-only feed and complex feed containing CO, H 2 , and model hydrocarbons (ethylene and dodecane). A first-principles, mechanistic-based model of the PNA was developed which utilized molecular-scale estimates (density functional theory) of energy barriers, mechanistic-based kinetics and realistic treatments of the flow and transport processes. Two new oxidation catalysts were developed (PdCu alloy, mixed copper-ceria-cobalt oxide), both of which significantly lessened the detrimental inhibition by CO on hydrocarbon and NO oxidation. A method for lessening the detrimental impact of CO on PNA activity was developed that involves use of an oxidation catalyst upstream of the PNA. The SwRI Ectolab TM burner system was applied to evaluate the baseline PNA material and confirmed performance comparable to the benchflow PNA studies using simulated exhaust. Spatially-resolved mass spectrometry (SpaciMS) was used to measure the transient spatial profiles of reacting species spanning the length of a three-function LHCNT containing PNA, HCT, and OC. The findings from this study provide diesel vehicle and catalyst companies valuable information to develop more cost effective emission control catalysts which helps to expand the use of more fuel efficient diesel power. The fundamental modeling and experimental tools and findings from this project can be applied to catalyst technologies used in the energy and chemical industries. The project led to 14 publications in the peer-reviewed literature with 2 additional currently under review. Finally, the project also led to training of several doctoral students who were placed in research jobs in industry and academia. Specifically, Mugdha Ambast (UH) has joined Cummins, Kevin Gu (UVa) has joined GM, and Abhay Gupta (UH) is to join Caterpillar.

02 PETROLEUM↗

DOE OSTI2022

Design and Optimization of Structured Multi-Functional Trapping Catalysts for Conversion of Hydrocarbons and NOx from Diesel and Advanced Combustion Engines

Oxides of nitrogen in the form of nitric oxide (NO) and nitrogen dioxide (NO 2 ) commonly referred to as NOx, is one of the two chemical precursors that lead to ground-level ozone, a ubiquitous air pollutant in urban areas. A major source of NOx is generated by equipment and vehicles powered by diesel engines, which have a combustion exhaust that contains NOx in the presence of excess O 2 . Vehicular emission control catalysts are ineffective in eliminating CO, hydrocarbons, and NO x during engine cold-start when exhaust temperatures are below 200°C. The objective of the project was to develop and demonstrate a multi-functional, catalyzed trap that enables vehicles with advanced combustion strategies to meet Tier 3 emissions standards while achieving the 150 °C challenge for sustained co-oxidation of HCs and CO and ≥90% NO trapping and release during warmup. Specifically, the multi-functional Lean HC+NOx (LHCNT) was developed for application in the exhaust aftertreatment of conventional diesel engines and engines having low temperature combustion (LTC) regimes. Activities included the design and synthesis of adsorbents and catalysts, screening and evaluation. Passive NOx absorbers (PNA), hydrocarbon (HC) traps, and oxidation catalysts (OC) were evaluated for use in series or as integrated devices. Predictive tools were developed utilizing the characterization and analysis of these materials, and an emission system was designed and optimized utilizing the catalyst systems. Microkinetic models were developed for the PNA for the simple NO-only feed and complex feed containing CO, H 2 , and model hydrocarbons (ethylene and dodecane). A first-principles, mechanistic-based model of the PNA was developed which utilized molecular-scale estimates (density functional theory) of energy barriers, mechanistic-based kinetics and realistic treatments of the flow and transport processes. Two new oxidation catalysts were developed (PdCu alloy, mixed copper-ceria-cobalt oxide), both of which significantly lessened the detrimental inhibition by CO on hydrocarbon and NO oxidation. A method for lessening the detrimental impact of CO on PNA activity was developed that involves use of an oxidation catalyst upstream of the PNA. The SwRI Ectolab TM burner system was applied to evaluate the baseline PNA material and confirmed performance comparable to the benchflow PNA studies using simulated exhaust. Spatially-resolved mass spectrometry (SpaciMS) was used to measure the transient spatial profiles of reacting species spanning the length of a three-function LHCNT containing PNA, HCT, and OC. The findings from this study provide diesel vehicle and catalyst companies valuable information to develop more cost effective emission control catalysts which helps to expand the use of more fuel efficient diesel power. The fundamental modeling and experimental tools and findings from this project can be applied to catalyst technologies used in the energy and chemical industries. The project led to 14 publications in the peer-reviewed literature with 2 additional currently under review. Finally, the project also led to training of several doctoral students who were placed in research jobs in industry and academia. Specifically, Mugdha Ambast (UH) has joined Cummins, Kevin Gu (UVa) has joined GM, and Abhay Gupta (UH) is to join Caterpillar.

42 ENGINEERING↗

DOE OSTI2024

In situ formation of pseudohalide anions induced by humid air and light passivates formamidinium‐based halide perovskites

Abstract Metal halide perovskites based on formamidinium (FA), or FA‐rich compositions have shown great promise for high‐performance photovoltaics. A deeper understanding of the impact of ambient conditions (e.g., moisture, oxygen, and illumination) on the possible reactions of FA‐based perovskite films and their processing sensitivities has become critical for further advances toward commercialization. Herein, we investigate reactions that take place on the surface of the FA 0.7 Cs 0.3 , mixed Br/I wide bandgap perovskite thin films in the presence of humid air and ambient illumination. The treatment forms a surface layer containing O, OH, and N‐based anions. We propose the latter originates from formamidine trapped at the perovskite/oxide interface reacting further to cyanide and/or formamidinate—an understudied class of pseudohalides that bind to Pb. Optimized treatment conditions improve photoluminescence quantum yield owing to both reduced surface recombination velocity and increased bulk carrier lifetime. The corresponding perovskite solar cells also exhibit improved performance. Identifying these reactions opens possibilities for better utilizing cyanide and amidinate ligands, species that may be expected during vapor processing of FA‐based perovskites. Our work also provides new insights into the self‐healing or self‐passivating of MA‐free perovskite compositions where FA and iodide damage could be partially offset by advantageous reaction byproducts. image

14 SOLAR ENERGY↗

DOE OSTI2022

Probing electronic dead layers in homoepitaxial n-SrTiO 3 (001) films

We combine state-of-the-art oxide epitaxial growth by hybrid molecular beam epitaxy with transport, x-ray photoemission, and surface diffraction, along with classical and first-principles quantum mechanical modeling to investigate the nuances of insulating layer formation in otherwise high-mobility homoepitaxial n-SrTiO 3 (001) films. Our analysis points to charge immobilization at the buried n-SrTiO 3 /undoped SrTiO 3 (001) interface as well as within the surface contamination layer resulting from air exposure as the drivers of electronic dead-layer formation. As Fermi level equilibration occurs at the surface and the buried interface, charge trapping reduces the sheet carrier density (n 2D ) and renders the n-STO film insulating if n 2D falls below the critical value for the metal-to-insulator transition.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Molecular Additive Engineering for Process-Humidity Robustness and Reproducible Fabrication of Perovskite Solar Cells and Modules

The commercialization of perovskite solar cells (PSCs) faces significant challenges due to their sensitivity to environmental humidity, which compromises film crystallization and device stability. Here, we introduce diphenylvinylphosphine (DPVP) as a Lewis base additive that enhances the performance and reproducibility of PSCs fabricated under ambient-air conditions. DPVP suppresses moisture-induced defect formation and stabilizes crystallization within realistic process-humidity ranges (20–40% relative humidity) commonly encountered in laboratory and pilot-scale manufacturing environments. It improves film uniformity, reduces trap densities, and yields highly reproducible device performance, enabling champion PCEs of 24.2% in small-area devices and 20.5% in blade-coated 12 cm 2 mini-modules. Furthermore, DPVP-assisted modules exhibit enhanced stability, retaining over 85% of their initial efficiency after 900 h of maximum power point tracking (MPPT) at 65 °C. This study demonstrates a humidity-resilient and scalable additive strategy for ambient-air perovskite photovoltaic manufacturing.

defect passivation↗

DOE OSTI2025

Evidence for I 2 loss from the perovskite–gas interface upon light-induced halide segregation

Sunlight-induced halide segregation in (CH 3 NH 3 )Pb(Br x I 1−x ) 3 (1 > x > 0.2), which limits obtainable voltages from solar cells with these perovskite absorbers, reverses upon resting in the dark. However, sustained illumination at ca. 1 sun opens a new decomposition pathway, leading to irreversible I 2 loss in an open system. We conclusively show I 2 off-gassing from halide-segregated (CH 3 NH 3 )Pb(Br 0.75 I 0.25 ) 3 by trapping gaseous I 2 and tracking the electronic conductivity of the perovskite, which increases from electron-doping as iodides are oxidized to iodine. Importantly, we show that this reaction occurs across the perovskite-air solid–gas interface, without confounding effects from solvent or reactive solid interfaces. This characterization was conducted under a nitrogen atmosphere, avoiding vacuum- and oxygen-driven I 2 loss pathways. Consistent observations of I 2 loss upon light-soaking CsPb(Br 0.75 I 0.25 ) 3 films show that this reaction is intrinsic to the inorganic framework. We propose that the disruption of iodide-rich domains in the halide-segregated films through I 2 loss can masquerade as a light-induced healing or apparent remixing of the segregated film, when in fact it leads to irreversible decomposition. Although I 2 off-gassing is less likely in bromide-rich solid solutions, light-induced halide segregation brings the iodides into proximity and forms electronic states that are energetically poised to trap and accumulate holes, providing a driving force for I 2 loss. Thus, even bromide-rich mixed-halide perovskite absorbers will benefit from I 2 -impermeable encapsulation for long-term stability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Experimental Rexolite Outgassing Measurements for Particle Accelerator Technology Development [Slides]

Baking Rexolite removes gases trapped on the surface and in the bulk material, reduces outgassing, and reduces gas load inside the vacuum system. Outgassing performance degrades over time for samples exposed to ambient air and dry nitrogen. Longer vacuum storage leads to lower outgassing rates in the observed time frame.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Investigation of Flux Spreading in a Light-Trapping, Planar-Cavity Receiver for Enclosed Solar Particle Heating

Concentrating solar thermal power (CSP) technology development has recently focused on increasing the operating temperatures to accommodate high efficiency power cycles and thermochemical processes. Inert solid particles as heat transfer media enable solar receivers to operate above 700 degrees Celsius resulting in increased system thermal efficiency compared to the conventional molten salt based CSP system. An open-cavity falling-particle solar receiver that can efficiently heat particles by direct heating from concentrated solar radiation faces challenges with large particle losses from wind and unable to support thermochemical reactions. A light-trapping, planar cavity reiver (LTPCR) where particles are indirectly heated can significantly minimize the particle losses during the operation, support thermochemical reactions, and offer scalability potential. The LTPCR features an array of vertical planar receiver/absorber panels arranged within a cavity configuration. Concentrated solar radiation from heliostats is focused onto the receiver walls, where heat is indirectly transferred to solid particles flowing inside the receiver channels. Heat transfer occurs through direct contact between the receiver panel walls and particles, and can be enhanced by fluidizing particles with air. This fluidization increases particle-wall contact and extends particle residence time, maximizing heat transfer efficiency. The unique vertical planar receiver structure originated from a near-blackbody tubular light absorber, effectively distributing the incoming solar beam spread across the panel walls and trapping light. This flux spreading effect, driven by cosine projection, converts high incident solar flux into a lower, more uniform heat flux on the panel walls. This redistribution enhances heat transfer efficiency between particle-wall or reaction gases-wall, while preventing localized overheating of the receiver panel. Indirect planar cavity solar receivers completely separate solid particles from the ambient environment that can greatly reduce the thermal losses in heated particles resulting in high efficiency at high temperatures above 700 degrees Celsius. This design ensures no particle losses to the environment during the operation while open-cavity designs can experience significant particle losses from wind. An experimental investigation was conducted to observe flux spreading on the receiver panel wall. A lab-scale prototype planar receiver, fabricated using Haynes 230 alloy, was tested under direct concentrated solar radiation using the high-flux solar furnace (HFSF) facility at NREL. The experiment was performed under normal peak radiative heat fluxes ranging from 800 to 1900 kW/m2. A temperature distribution on the panel wall was measured using a thermal imaging camera (FLIR A 6600). To prevent overheating at the receiver front tip, prism-shaped heat shields (Zircar UNIFROM C1) were placed in front of the receiver, and their influence on flux spreading was also studied. Absorbed flux distribution on the panel wall was modeled using SolTrace. The total solar power and flux distributions delivered from HFSF were determined based on the heliostat mirror optical properties, direct normal irradiance (DNI) on the on-sun testing days, peak flux measurement during the on-sun testing, and shutter/attenuator settings Due to the large incident angles of the solar beam on the panel wall, the angular optical properties of Haynes 230 alloy and Zircar heat shields were incorporated into the model. This flux distribution model was then integrated into a computational fluid dynamics (CFD) simulation to predict the receiver panel wall temperature, which was compared with the experimental measurements. Both prediction and measurements identified a temperature hotspot at the backside of the panel, indicating that the incident solar beam can fully reach to the rear of the receiver. The heat shields positioned at the front of the receiver effectively reduced the excessive temperature rise at the receiver front tip. Overall, the temperature was well distributed over the panel wall, with a minor hotspot at the back of the receiver. The model slightly overpredicted the temperature, possibly due to discrepancies in optical properties of the panel and an underprediction of thermal loss in the receiver. The advancement of the particle LTPCR offers a viable alternative to open-cavity receivers by addressing particle loss issues. Additionally, it presents a pathway for enabling solar thermochemical processes, extending CSP technology beyond power generation to fuel and chemical production.

14 SOLAR ENERGY↗

DOE OSTI2022

Short communication: Mechanism and prevention of irreversible trapping of atmospheric He during mineral crushing

A pervasive challenge in noble gas geochemistry is to ensure that analytical techniques do not modify the composition of the noble gases in the samples. Noble gases are present in the atmosphere and are used in a number of manufacturing procedures and by laboratory equipment. Of particular concern is the introduction of atmospheric or laboratory noble gases to samples during preparation before samples are placed in a vacuum chamber for analysis. Recent work has shown the potential for contamination of crushed samples with air-derived He that is not released by placing the samples under vacuum at room temperature. Using pure He gas as a tracer, we show that the act of crushing samples to a fine powder itself can introduce He contamination but that this is easily avoided by crushing under liquid or in an inert atmosphere. Because the He is trapped during crushing, the same concern does not extend to samples that are naturally fine-grained when collected. We also show model results that demonstrate when this effect might significantly impact samples for (U–Th) / He geochronology or 3 He cosmogenic nuclide dating. The degree of He contamination from crushing samples to sizes smaller than the > 63 µm range typically used for geochronology is insignificant for samples with a date of at least 1 Ma and 1 ppm U, and the degree of He contamination from crushing samples to sizes smaller than the 100–500 µm range typically used for cosmogenic nuclide dating is also insignificant for samples with a date of at least 10 ka with typical 3 He production rates.

58 GEOSCIENCES↗

DOE OSTI2025

Enhanced reactivity at the oil–water interface accelerates the synthesis of zymonic acid in microemulsions

Chemical reactions in microscale compartments, such as aerosols and emulsions, can exhibit significantly faster reaction rates relative to macroscale containers. This enhancement in chemistry is often due to the elevated importance of surfaces as reaction vessels are reduced to picoliter volumes. While most studies have focused on the air-water interface of droplets, there are comparably fewer studies of reactions in micron-scale aqueous solutions encapsulated by oil. Here we investigate the condensation reaction of pyruvic acid (PA) to form zymonic acid (ZA) and water. Using microfluidics and optical trapping, chemical kinetics are measured in monodisperse micron-sized emulsion droplets in situ via Raman spectroscopy. Relative to a macroscopic bulk solution, which exhibits little to no reaction over many days, we find efficient production of ZA over the same time period. A kinetic model is developed to elucidate the role of the interface in accelerating the microdroplet reaction kinetics. After quantifying the surface partitioning of PA from interfacial tension measurements, the rate coefficient for the condensation reaction at the oil-water interface is determined to be 1.8 × 10-2 M-1 s-1. This rate coefficient is estimated to be 105 larger than the reaction rate in bulk aqueous solutions. Compared to previous studies of accelerated ZA formation at the air-water interface on nanodroplets, we find that the reaction at the oil-water interface is 20 times more efficient. Despite this difference, the overall ZA formation rate in emulsions is significantly slower than in the same-sized aerosols, which arises from the weaker partitioning of PA to the oil-aqueous relative to air-water interface. These results highlight the interplay between interfacial partitioning and reactivity in accelerating chemistry in microcompartments and provides new insights into how interfacial composition influences condensation reactions.

Wallace, Brandon J↗

DOE OSTI2024

Dynamic Copper Site Redispersion through Atom Trapping in Zeolite Defects

Single-site copper-based catalysts have shown remarkable activity and selectivity for a variety of reactions. However, deactivation by sintering in high-temperature reducing environments remains a challenge and often limits their use due to irreversible structural changes to the catalyst. Here, we report zeolite-based copper catalysts in which copper oxide agglomerates formed after reaction can be repeatedly redispersed back to single sites using an oxidative treatment in air at 550 °C. Under different environments, single-site copper in Cu–Zn–Y/deAlBeta undergoes dynamic changes in structure and oxidation state that can be tuned to promote the formation of key active sites while minimizing deactivation through Cu sintering. For example, single-site Cu 2+ reduces to Cu 1+ after catalyst pretreatment (270 °C, 101 kPa H 2 ) and further to Cu0 nanoparticles under reaction conditions (270–350 °C, 7 kPa EtOH, 94 kPa H 2 ) or accelerated aging (400–450 °C, 101 kPa H 2 ). After regeneration at 550 °C in air, agglomerated CuO was dispersed back to single sites in the presence and absence of Zn and Y, which was verified by imaging, in situ spectroscopy, and catalytic rate measurements. Ab initio molecular dynamics simulations show that solvation of CuO monomers by water facilitates their transport through the zeolite pore, and condensation of the CuO monomer with a fully protonated silanol nest entraps copper and reforms the single-site structure. Importantly, the capability of silanol nests to trap and stabilize copper single sites under oxidizing conditions could extend the use of single-site copper catalysts to a wider variety of reactions and allows for a simple regeneration strategy for copper single-site catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Perovskite Solar Cells with Enhanced Fill Factors Using Polymer-Capped Solvent Annealing

Despite huge improvements in power conversion efficiencies of perovskite solar cells, the technology is still limited by fill factors at around 80%. In this work, we report perovskite solar cells having exceptionally high fill factors of 85% and enhanced open-circuit voltage without sacrificing short-circuit current through a polymer-capped solvent-annealing process assisted by a hot air blower. Additionally, during the solvent-annealing, the perovskite surface flattens and the perovskite grains agglomerate into micrometer-sized clusters having enlarged α-phase crystallites, while the δ-phase simultaneously disappears. The optimized structure reduces energetic disorder and trap-assisted recombination in the perovskite layer, resulting in an enhanced efficiency from 18.2% to 19.8% and improved device lifetime. Our results provide a pathway to increase the device efficiency and stability of perovskite solar cells, and have the potential to stimulate research on scalable poly-crystal perovskite layer fabrication in optoelectronic devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2021

Ultra-clean condensing gas furnace enabled with acidic gas reduction

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Transformation of CeO 2 Nanoparticles into Atomically Dispersed Ce Cations Leads to Enhanced Reactivity for Automotive Emissions Control

Nanosized cerium oxide (CeO 2 ) has been extensively used as the oxygen storage component in automotive emission control systems. However, the possible influence of atomically dispersed Ce in these catalysts has not been recognized. Here, in this study, we demonstrate the controllable transformation of ceria nanoparticles into isolated cerium cations on γ-Al 2 O 3 via reductive atom trapping in 10% H 2 at 800 °C, achieving over half-monolayer coverage. Dispersed Ce 1 ions anchored by surface penta- and octa-coordinated Al sites exhibit outstanding thermal stability in air up to 500 °C, enabling further loading of active metals with well-defined catalyst structures. With this strategy, supported single-atom Rh 1 surrounded by dispersed Ce 1 is confirmed to exhibit much superior performance to Rh 1 on bare Al 2 O 3 or nanocrystalline CeO 2 in catalyzing NO reduction by CO, exhibiting a striking one-order-of-magnitude increase in activity. Dispersed Ce 1 exhibits greatly enhanced oxygen transfer capability compared to ceria nanoparticles and introduces a modified reaction mechanism that involves an adjacent Rh 1 –Ce 1 motif, resulting in a greatly decreased activation barrier (from 192 to 96 kJ/mol). The reactivity enhancements are also seen with Ce 1 -promoted Pt nanoparticles for oxidation of CO and hydrocarbons.

Jiang, Dong [Washington State Univ., Pullman, WA (↗

DOE OSTI2024

Bridging gaps in permafrost-shrub understanding

Permafrost, permanently frozen ground which underlies much of the Arctic and sub-Arctic, is influenced by deciduous shrubs, yet our understanding of permafrost-shrub interactions is limited. This is largely due to a lack of widespread, long-term, high-quality observations across Arctic and sub-Arctic systems, which are difficult to study due to their remote locations. Shrubs are rapidly expanding in many areas of Arctic tundra and can either amplify or inhibit permafrost thaw, making it crucial that we can understand and predict permafrost-shrub interactions. As we have limited time and resources to make observations, we must design our field campaigns to be as impactful as possible. Below we outline the current state of knowledge and give suggestions about how we can maximize our fieldwork’s impact. From field studies conducted around the Arctic, we know that shrubs generally have a cooling effect on permafrost in the summer, largely caused by the shrub canopy shading the soil. However, summertime cooling can be counteracted by a warming effect in winter, caused by the trapping of blowing snow by shrubs, which leads to increased snow depths. In addition to these commonly observed effects, both observations and models show that other local factors such as climate, soil, snow, and disturbances can interact to cause contrasting dominant effects on permafrost temperatures. For example, shrubs that protrude through the snowpack have been observed to cool permafrost in winter via thermal bridging between the air above the snow and the soil below. However, at other research sites, protruding shrubs lower the surface albedo and cause earlier snowmelt in spring, amplifying permafrost thaw by exposing the soil to thawing earlier. Protruding shrubs have also been observed to induce snow melt in autumn, creating ice layers at the snow surface that prevent further snow accumulation and eliminate the ability of shrubs to trap blowing snow, thereby reducing the winter warming effect. While we understand the physical processes that lead to these effects, we cannot explain why we observe different effects between sites.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Revealing the Formation of the <20 MeV Inner Proton Radiation Belt at L ∼ 2 During the 10–11 May 2024 Superstorm

A new proton radiation belt was identified during the geomagnetic superstorm of 10–11 May 2024. To investigate its origin, we use an MHD-test particle simulation to model solar energetic proton (SEP) trapping and the evolution of the initial trapped proton population during the storm. The simulation weights the injected SEP population with interplanetary proton measurements and the initial trapped proton radial profile with energy-resolved Weather System Follow-on-Microwave (WSF-M) proton data, enabling quantitative comparison with observations. Results show that SEP contributions are minimal; the new ∼2–18 MeV belt at L ∼ 2 forms mainly through redistribution and energization of the initial trapped population within hours of the CME shock, driven by subsequent electric field impulses, rather than the initial shock alone. These results provide quantitative evidence based on realistic, plasma-dependent field dynamics and significantly advance understanding of inner radiation belt formation.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Clean Condensing Gas Furnace

Natural gas furnaces are the most common space heating equipment in the U.S. residential and commercial building markets. However, current residential natural gas condensing furnaces generate substantial acidic condensate as well as significant emissions of sulfur oxides (SOx), nitrogen oxides (NOx), carbon monoxide (CO), hydrocarbons (HC), and methane (CH 4 ) contributing to environmental degradation of air, water, and soil. This report describes a novel solution to reduce the environmental impact of natural gas condensing furnaces based on the technology of a monolithic acidic gas reduction (AGR) catalyst for SOx trapping, NOx redox to nitrogen, and oxidation of formic acid, CO, HC, and CH 4 . The AGR technology offers the following benefits: (1) a neutral furnace condensate with a pH of ~7, allowing its safe release into the sewer system thus eliminating a second drainage system; (2) trapping and removing nearly all SOx emissions; (3) NOx emissions nearly at nearly 1-2 ng/J, more than 95% lower than new emissions standards in California; (4) the use of a low-cost heat exchanger as a condensing heat exchanger (HX) since the condensate is not acidic, avoiding the need for expensive stainless steel alloys; and (5) unburnt fuel energy recovery to boost efficiency.The AGR component and AGR-enabled furnace performance were broadly tested to determine their effects on long-term reliability and durability, as well as SOx storage and regeneration activity. The AGR regeneration does not impair the performance in achieving neutral condensate and ultra-low NOx emissions, and the AGR catalyst subjected to regeneration activities continued to function well and achieved slightly better annual fuel utilization efficiency (AFUE). The 400-hour reliability and durability test of the retrofitted condensing furnace with the AGR component shows that the furnace unit still achieves a neutral furnace condensate with a pH of ~7 and enables 0~3 ng/J of NOx emissions. However, the 400-hour operation slightly degraded the AFUE because of soot particle accumulation caused by frequent incomplete combustion owing to inappropriate condensate drainage during testing. Thus, proper condensate drainage is critical for AGR-enabled furnaces. Furthermore, neutron computed tomography was employed to survey the aged AGR component and demonstrate high-resolution 2D and 3D representations for the nondestructive diagnosis of the AGR component. The tomography showed that the AGR component did not deform or suffer broken AGR channels. A new AGR catalyst with low precious metal loading was preliminarily explored to identify a pathway of optimizing AGR material loading and maximizing acidic gas reduction at low cost. The new AGR component can reduce precious metal loading by 38% and still achieve neutral condensate and ultralow NOx emissions. The furnace with the AGR component of low Pt/Rh loading enables a maximum AFUE of 97%, which is meaningfully higher than the original furnace. Long-duration testing for the furnace enabled with the low precious metal loading AGR component will be vital in future research. Although the current work demonstrates a proof of concept for the AGR-enabled furnace, the AGR assembly needs to be optimized and integrated into the design of new OEM furnace products. Furthermore, the AGR technology can be applied not only for residential gas furnaces, but also for commercial rooftop units, gas heat pumps, gas-fired water heaters, combustion boilers, and other systems.

03 NATURAL GAS↗