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DOE OSTI2025

Electrochemical production of H 2 O 2 on palladium-based clusters driven by metal–support interaction

Utilizing palladium (Pd) clusters as active sites offers a promising route to minimize noble metal consumption in electrochemical hydrogen peroxide (H 2 O 2 ) production. In this work, we present a synthesis approach for anchoring Pd-based clusters onto carbon-supported CeO 2 nanosubstrates to enable efficient H 2 O 2 generation via the two-electron oxygen reduction reaction (ORR) pathway. By systematically adjusting Pd loading, we evaluated its impact on H 2 O 2 yield and production rate. The catalyst with the lowest Pd content (0.027 wt%) exhibited outstanding performance, achieving 97% H 2 O 2 selectivity, 94.2 faradaic efficiency at 0.7 V vs. RHE, and a peak production rate of 195.8 mol g Pd −1 h −1 . A formulation containing 0.35 wt% Pd delivered a peak ORR mass activity nearly three times as high as that of commercial 10 wt% Pd/C, while retaining comparable electrochemical stability. These enhancements are attributed to synergistic effects among isolated PdO clusters, CeO 2 nanocrystals, and the conductive carbon support, which together facilitate oxygen adsorption and promote the two-electron ORR pathway. Analysis after accelerated durability testing further revealed a tendency toward cluster agglomeration and mass transfer from smaller to larger nanocrystals, indicative of a coarsening mechanism. Overall, this study underscores the promise of low-Pd PdO–CeO 2 –carbon hybrid catalysts for scalable and efficient H 2 O 2 electrosynthesis, while highlighting stability as a critical area for future improvement.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Data driven investigation to understand the influence of total solids on biological biogas upgrading

In situ biogas upgrading achieves CO 2 conversion to CH 4 via hydrogenotrophic methanogenesis; however, gas-liquid mass transfer constraints limit the upgrading performance. Recognizing that optimization studies often underrepresent the effects of total solids (TS) and organic loading rate (OLR), this study undertook a holistic, statistics driven assessment of operating conditions for in situ H 2 assisted biogas upgrading, centering the analysis on TS and OLR. A dataset of 31 studies was compiled and comprised 99 observations. A rigorous analytical framework was employed, combining data standardization, fixed- and random-effects (REML) weighted regressions with cluster-robust errors, stratified analyses, and machine learning. Mixed-effects meta regression indicated that TS was the main factor explaining differences of methane fraction (CH 4 %) when considering the between studies heterogeneity. Focusing on a near-stoichiometric subset (H 2 /CO 2 ≈ 4:1), TS remained significant. Stratified results showed a stronger negative relationship between TS and CH 4 % in UASB reactors than in CSTRs, with a negative effect under mesophilic conditions and no significant effect under thermophilic conditions. A Random Forest model corroborated the statistical findings, consistently ranking H 2 /CO 2 ratio, OLR, TS, and hydrogen injection rate (HIR) as the most influential predictors. These findings delineate trends across increasing TS levels, particularly between 1% and 10%, and provide preliminary insights for TS above 15% in in situ biogas upgrading. They further provide insights for the influence of TS by reactor type and temperature, thereby advancing the evidence base for implementing biological CO 2 conversion to CH 4 in practice.

In situ biogas upgrading↗

NASA NTRS2010

Potential Lunar In-Situ Resource Utilization Experiments and Mission Scenarios

The extraction and use of resources on the Moon, known as In-Situ Resource Utilization (ISRU), can potentially reduce the cost and risk of human lunar exploration while also increasing science achieved. By not having to bring all of the shielding and mission consumables from Earth and being able to make products on the Moon, missions may require less mass to accomplish the same objectives, carry more science equipment, go to more sites of exploration, and/or provide options to recover from failures not possible with delivery of spares and consumables from Earth alone. The concept of lunar ISRU has been considered and studied for decades, and scientists and engineers were theorizing and even testing concepts for how to extract oxygen from lunar soil even before the Apollo 11 mission to the Moon. There are four main areas where ISRU can significantly impact how human missions to the Moon will be performed: mission consumable production, civil engineering and construction, energy production, storage, and transfer, and manufacturing and repair. The area that has the greatest impact on mission mass, hardware design and selection, and mission architecture is mission consumable production, in particular, the ability to make propellants, life support consumables, and fuel cell reagents. Mission consumable production allows for refueling and reuse of spacecraft, increasing power production and storage, and increased capabilities and failure tolerance for crew life support. The other three areas allow for decreased mission risk due to radiation and plume damage, alternative power systems, and failure recover capabilities while also enabling infrastructure growth over Earth delivered assets. However, while lunar ISRU has significant potential for mass, cost, and risk reduction for human lunar missions, it has never been demonstrated before in space. To demonstrate that ISRU can meet mission needs and to increase confidence in incorporating ISRU capabilities into mission architectures, terrestrial laboratory and analog field testing along with robotic precursor missions are required. A stepwise approach with international collaboration is recommended. The first step is to understand the resources available through orbital and surface exploration missions. Resources of particular interest are hydrogen, hydroxyl, water, and other polar volatile resources recently measured by Chandrayaan, Lunar Reconnaissance Orbiter (LRO), and the Lunar Crater Observation and Sensing Satellite (LCROSS). The second step is to demonstrate critical aspects of ISRU systems to prove ISRU is feasible under lunar environmental and resource conditions (ex. subscale oxygen extraction from regolith). The third step is to perform integrated missions with ISRU and other connected systems, such as power, consumable storage, surface mobility, and life support at a relevant mission scale to demonstrate ISRU capabilities as well as the critical interfaces with other exploration systems. If possible, the mission should demonstrate the use of ISRU products (ex. in a rocket engine or fuel cell). This dress rehearsal mission would be the final step before full implementation of ISRU into human missions, and may be performed during human lunar exploration activities. This stepwise approach is the most conservative approach, and may only be possible with international cooperation due to the limited number of robotic missions each nation/space agency can perform within their budget.

Sanders, Gerald B.↗

DOE OSTI2024

Effect of Anoxic Iron Corrosion on WIPP Brine Geochemistry FY23 Final Report (U)

A 280-day study was completed to evaluate the effect of zero-valent iron (Fe 0 ) on the Waste Isolation Pilot Plant (WIPP) brine geochemistry under anticipated reducing conditions. Hydrogen (H 2 ) gas is expected to be present in the repository after closure due to the anoxic corrosion of a vast quantity of iron contained in the waste forms disposed at WIPP; therefore, a background argon atmosphere containing H 2 was chosen for this study. WIPP groundwater brine pH and E h will impact the mobility and fate of plutonium within the repository. Modeling and laboratory results for Castile WIPP brine indicate that equilibrium fa values relative to the standard hydrogen electrode (SHE) are 40 mV more reducing (i.e., more negative) than those for Salado WIPP brine (-480 mV vs. -440 mV, respectively) because of the higher pH of the Castile brine (pH 9 .3 for Castile vs. pH 8.8 for Salado). The E h and pH data were corrected for the effects of high ionic strength. The experimental results for both brines are consistent with thermodynamic predictions using OLI Systems' Mixed Solvent Electrolyte chemical equilibrium model. The measured and corrected pH and E h data from this study are provided in Table ES-I and Table ES-2, respectively. The experimental study, with four test conditions in triplicate, was performed in a dual glovebox with a nominally 3 vol.% H 2 in argon atmosphere (target H 2 range: 3 ± I vol.%). Simulants containing MgO only ( experimental control) and MgO+Fe 0 (WIPP base case) were prepared for both the Salado and Castile brines. MgO was included in all simulants to account for the use of bulk magnesium oxide in the WIPP repository. Fe 0 was included in some simulants to incorporate the effects of the anoxic corrosion of iron and in-situ hydrogen generation in the study. The brine compositions were developed by Sandia National Laboratory (SNL; Xiong, 2008) and have been used in previous WIPP evaluations. The test method (agitation, etc.) is partially based on ASTM D3987-12. Twelve rounds of periodic measurements of pH and E h were performed over the course of the study. Chemical analysis results for liquids and solids (ICP-MS, ICP-ES, IC Anion, TIC, SEM-EDX) are consistent with the pH, E h , and thermodynamic modeling results. This study included the following conditions that deviate from anticipated post-closure conditions following brine intrusion, but were selected to facilitate bench-scale testing to validate modeling of pH and E h for the post-closure WIP P repository: an anoxic glove box atmosphere containing ≤ 4 vol. % H 2 vs. substantially higher H 2 gas concentrations assumed in the WIPP Performance Assessment (PA); a significantly higher liquid-to-solid test ratio compared to the much lower phase ratio anticipated in the WIP P repository; agitation of the simulant bottles to maximize mass transfer; and finally the use of Fe 0 reagents having a much greater surface area than expected in the WIP P repository. Non-representative conditions were chosen for various reasons such as: to provide bounding conservative results, to provide a margin of safety for testing, or to facilitate simulant sub-sampling and analysis. In a parallel effort, aqueous electrolyte thermodynamic models were developed for the synthetic Salado and Castile brines to inform the experimental design, facilitate laboratory data interpretation, and allow extension of evaluations beyond the parameters tested. Thermodynamic modeling simulations including the MgO and Fe 0 additives that are directly relevant to the experimental measurements (e.g., pH calibration curve, ORP corrections) are included in this report. The measured fa of the simulants was close to the OLI model predictions for both brines and was largely controlled by the background H 2 partial pressure in the vapor phase as well as H 2 generated in situ in the aqueous phase by the Fe 0 corrosion. The H 2 gas-phase concentration tested and thermodynamically evaluated was much lower than is assumed in the WIPP PA; however, H 2 (g) concentrations significantly below this level are still predicted to result in very reducing conditions. In conclusion: • The experimental results are consistent with thermodynamic model predictions for fa, pH, and the effects of high ionic strength. • Evidence to date suggests that the H2 concentration in the glovebox atmosphere ultimately determined the final E h values of the simulants and resulted in highly reducing conditions. As a result, little difference was observed between the control simulants containing only MgO and the WIPP base-case simulants that contained MgO and Fe 0 . • This test methodology is recommended for future studies evaluating WIPP repository conditions. The methodology includes: (1) background H 2 in argon with agitation ( or could alternatively include in-situ-generated H 2 in sealed bottles); (2) carefully measured and corrected ORP data ( with much effort focused on allowing the probes to fully stabilize); and (3) ionic-strength-corrected pH data. Other best practices, such as simulant sparging/handling, ORP probe replacement, etc., should also be considered. • The coupling of experimental studies and thermodynamic modeling is also highly recommended because these methods inform and direct one another leading to greater confidence in and understanding of the results.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2024

Identifying a novel pathway for extracellular electron uptake in Methanosarcina barkeri using shotgun

The overarching goal of this project was to identify the genetic and/or enzymatic basis for extracellular electron uptake in Methanosarcina barkeri—an organism we previously characterized to be capable of this process using poised potential electrodes and a range of electrochemical techniques. In our first aim, we will utilized proteomic techniques that labels extracellular proteins with free amine groups with biotin and perform a selective purification of these proteins from the rest of the proteome. These were identified using mass spectrometry, providing us insight into the identity of the cell surface proteins, including redox active proteins present during extracellular electron uptake. We will also used an isobaric tagging technique (iTRAQ labeling) of proteomes from different experiment conditions to look at differential proteins expression and better understand the total pathway involved in extracellular electron uptake coupled to methanogenesis. In our final aim, we will investigated the electrochemical nature of electron uptake in co-cultures, compared to our pure culture data sets. We predict the process of electron uptake from electrodes replicates what goes on in nature when these organisms for co-cultures with electrogenic microbes such as Geobacter, and to test this hypothesis we have begun to probe co-cultures electrochemically during direct interspecies electron transfer. Our final aim took much longer than expected due to challenges replicating co-cultures between Geobacter metallireducens and Methanosarcina barkeri. We found the major problem with this work was the inability of the M. barkeri strain we used (and we tried strains from three different labs) to successfully grow on acetate in the absence of hydrogen. As such, we began to use the strain Methanosarcina acetivorans—another close relative that specializes on acetate growth. We are currently in the process of comparing electrochemical observations of this microorganism between pure and co-culture experiments.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2022

Electrocatalysis in Alkaline Media and Alkaline Membrane-Based Energy Technologies

Hydrogen energy-based electrochemical energy conversion technologies offer the promise of enabling a transition of the global energy landscape from fossil fuels to renewable energy. Here, we present a comprehensive review of the fundamentals of electrocatalysis in alkaline media and applications in alkaline-based energy technologies, particularly alkaline fuel cells and water electrolyzers. Anion exchange (alkaline) membrane fuel cells (AEMFCs) enable the use of nonprecious electrocatalysts for the sluggish oxygen reduction reaction (ORR), relative to proton exchange membrane fuel cells (PEMFCs), which require Pt-based electrocatalysts. However, the hydrogen oxidation reaction (HOR) kinetics is significantly slower in alkaline media than in acidic media. Understanding these phenomena requires applying theoretical and experimental methods to unravel molecular-level thermodynamics and kinetics of hydrogen and oxygen electrocatalysis and, particularly, the proton-coupled electron transfer (PCET) process that takes place in a proton-deficient alkaline media. Extensive electrochemical and spectroscopic studies, on single-crystal Pt and metal oxides, have contributed to the development of activity descriptors, as well as the identification of the nature of active sites, and the rate-determining steps of the HOR and ORR. Among these, the structure and reactivity of interfacial water serve as key potential and pH-dependent kinetic factors that are helping elucidate the origins of the HOR and ORR activity differences in acids and bases. Additionally, deliberately modulating and controlling catalyst-support interactions have provided valuable insights for enhancing catalyst accessibility and durability during operation. The design and synthesis of highly conductive and durable alkaline membranes/ionomers have enabled AEMFCs to reach initial performance metrics equal to or higher than those of PEMFCs. We emphasize the importance of using membrane electrode assemblies (MEAs) to integrate the often separately pursued/optimized electrocatalyst/support and membranes/ionomer components. Operando/in situ methods, at multiscales, and ab initio simulations provide a mechanistic understanding of electron, ion, and mass transport at catalyst/ionomer/membrane interfaces and the necessary guidance to achieve fuel cell operation in air over thousands of hours. We hope that this Review will serve as a roadmap for advancing the scientific understanding of the fundamental factors governing electrochemical energy conversion in alkaline media with the ultimate goal of achieving ultralow Pt or precious-metal-free high-performance and durable alkaline fuel cells and related technologies.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2024

Steam Condensation Scaled Experiment in the Presence of Non-condensable Gas for Reactor Containment Passive Safety Analysis

This study presents scaled experiments using steam condensation with non-condensable gas (NCG)—helium, simulating hydrogen—as these experiments are pivotal for water-cooled reactor passive containment cooling system (PCCS) design and analysis. Research into PCCSs for small modular reactors (SMRs) is especially important in light of SMR system design; however, studies in the literature reflect limitations due to test geometry and operational condition variations, without considering SMR prototypic design. To address these challenges, a scaled test facility was developed to accurately replicate SMR PCCSs. This facility includes vertical down-flow condensing test sections with 1-, 2-, and 4-in.-diameter condensing tubes, accompanied by annular water cooling. Experiments were conducted using both superheated and saturated steam, with steam mass flow rates varying from 55 to 66 kg/hr., in the presence of helium as the NCG mass flow rate ranges from 1.8 to 22 kg/hr. Test data were collected on (a) the axial temperatures of the annular cooling water; (b) the outer wall temperature of the condensers; and (c) the mass flow rate, temperature, and pressure at the test section inlets and outlets. These primary test data were used in conjunction with a standard data reduction methodology to estimate essential thermal parameters such as heat fluxes, heat transfer coefficients, and condensation rates. The effects of NCGs on steam condensation within the geometry of the scaled test sections were then presented in regard to various testing conditions.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2024

Presentation: Steam Condensation Scaled Experiment in the Presence of Non-condensable Gas for Reactor Containment Passive Safety Analysis

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2020

Experimental measurements of fuel and water crossover in an active DMFC

This work measured polarization curves as well as the high-frequency resistance of active direct methanol fuel cell (DMFC) operates at around 80 °C with active controls of temperature, methanol concentration, airflow rate, and relative humidity. The relative humidity of the air did not have noticeable impacts on the fuel cell unless the operating temperature was near the evaporation temperature of water (100 °C). The hydrophobic water management layer (WML) between the membrane electrode assembly (MEA) and cathode air channel increases the mass transfer resistance and improves the water retention in MEA. Adding a WML increased the peak power density, decreased the ohmic resistance, and improved the fuel efficiency of the fuel cell, especially when it operated near 100 °C. This study also quantitatively measured methanol and water crossover as well as the fuel efficiency at different operating currents. The fuel efficiency increased significantly with the increase of the current density. Using a hydrophobic fuel management layer (FML) between the anode fuel channel and MEA reduced the fuel and water crossover rates and increased the ohmic resistance due to the decrease of the water content of the Nafion membrane. The FML improved fuel efficiency by reducing the methanol crossover. The combination of the FML and WML enabled the steady operation of DMFC using highly concentrated methanol solutions (up to 75 wt%).

08 HYDROGEN↗

NASA NTRS2017

In-Space Chemical Propulsion Systems Roadmap

In-space propulsion begins where the launch vehicle upper stage leaves off, performing the functions of primary propulsion, reaction control, station keeping, precision pointing, and orbital maneuvering. The main engines used in space provide the primary propulsive force for orbit transfer, planetary trajectories and extra planetary landing and ascent. The reaction control and orbital maneuvering systems provide the propulsive force for orbit maintenance, position control, station keeping, and spacecraft attitude control. Advanced in-space propulsion technologies will enable much more effective exploration of our Solar System and will permit mission designers to plan missions to "fly anytime, anywhere, and complete a host of science objectives at the destinations" with greater reliability and safety. With wide range of possible missions and candidate propulsion technologies, the question of which technologies are "best" for future missions is a difficult one. A portfolio of propulsion technologies should be developed to provide optimum solutions for a diverse set of missions and destinations. A large fraction of the rocket engines in use today are chemical rockets; that is, they obtain the energy needed to generate thrust by chemical reactions to create a hot gas that is expanded to produce thrust. A significant limitation of chemical propulsion is that it has a relatively low specific impulse (Is, or thrust per mass flow rate of propellant). A significant improvement (>30%) in Is can be obtained by using cryogenic propellants, such as liquid oxygen and liquid hydrogen, for example. Historically, these propellants have not been applied beyond upper stages.

Oxidizers↗

NASA NTRS2024

ECI Final Report: Closing of Critical Technology Gaps for Rotating Detonation Rocket Engines

NASA has successfully fired several configurations of a dual regenerative 10K lbf class Rotating Detonation Rocket Engines using cryogenic liquid methane, liquid hydrogen, and RP-1 as fuel and liquid or gaseous oxygen as the oxidizer. In addition, 3 hot fire test phases were conducted to evaluate parametrically varying combustor geometries using a subscale 500-1K lbf class thruster RDRE. Several studies were successfully completed to evaluate the impacts of contraction ratio, annulus L’, heat transfer through calorimetry, and varying injector designs. Laser powder bed fusion GRCop-42, GRX-810, and C-103 alloys were used for the outer bodies, inner bodies, nozzles, and injector variations. The development of RDRE technology is only now possible with additive manufacturing techniques and these specialized alloys. Critical design parameters, design rules of thumb, and operability limitations have been identified. Major lessons learned in the development of critical components have also been documented. All critical technology gaps have been demonstrated at one scale or another and closed. A major finding of this work is that the combustion efficiency of the RDRE is far superior to that of the traditional liquid rocket engine requiring an order of magnitude lower chamber volume and residence time to react. Because of this, the design trade space opens up significantly. More compact chamber geometries are now possible with potential mass savings and significant length savings possible to flight geometries. In addition, the ceiling for the technology, in terms of Isp, has not yet been reached. It is likely that an additional ~10% better Isp over equivalent state-of-the-art combustion devices may be achieved over the next decade should the technology continue to be developed. This technology has been shown to be viable for near term infusion (2-5 years) into space missions and enable cost effective space access for US industry. This final report documents all major findings from this early career initiative (ECI) project and lays out what is needed post ECI.

Thomas Teasley↗

NASA NTRS2019

Two-Phase Convection Heat Transfer Correlations for Liquid Hydrogen Pipe Chilldown

Recently, heat transfer correlations based on liquid nitrogen (LN2) and liquid hydrogen (LH2) pipe quenching data were developed to improve the predictive accuracy of lumped node codes like SINDA/FLUINT and the Generalized Fluid System Simulation Program (GFSSP). After implementing these correlations into both programs, updated model runs showed strong improvement in LN2 pipe chilldown modeling but only modest improvement in LH2 modeling. Due to large differences in thermal and fluid properties between the two fluids, results indicated a need to develop a separate set of LH2-only correlations to improve the accuracy of the simulations. This paper presents a new set of two-phase convection heat transfer correlations based on LH2 pipe quenching data. A correlation to predict the bulk vapor temperature was developed after analysis showed that high amounts of thermal nonequilibrium of the liquid and vapor phases occurred during film boiling of LH2. Implemented in a numerical model, the new correlations achieve a mean absolute error of 19.5 K in the predicted wall temperature when compared to recent LH2 pipe chilldown data, an improvement of 40% over recent GFSSP predictions. This correlation set can be implemented in simulations of the transient LH2 chilldown process. Such simulations are useful for predicting the chilldown time and boil-off mass of LH2 for applications such as the transfer of LH2 from a ground storage tank to the rocket vehicle propellant tank, or through a rocket engine feedline during engine startup.

critical heat flux↗

NASA NTRS1992

Pressurized Lunar Rover (PLR)

The objective of this project was to design a manned pressurized lunar rover (PLR) for long-range transportation and for exploration of the lunar surface. The vehicle must be capable of operating on a 14-day mission, traveling within a radius of 500 km during a lunar day or within a 50-km radius during a lunar night. The vehicle must accommodate a nominal crew of four, support two 28-hour EVA's, and in case of emergency, support a crew of six when near the lunar base. A nominal speed of ten km/hr and capability of towing a trailer with a mass of two mt are required. Two preliminary designs have been developed by two independent student teams. The PLR 1 design proposes a seven meter long cylindrical main vehicle and a trailer which houses the power and heat rejection systems. The main vehicle carries the astronauts, life support systems, navigation and communication systems, lighting, robotic arms, tools, and equipment for exploratory experiments. The rover uses a simple mobility system with six wheels on the main vehicle and two on the trailer. The nonpressurized trailer contains a modular radioisotope thermoelectric generator (RTG) supplying 6.5 kW continuous power. A secondary energy storage for short-term peak power needs is provided by a bank of lithium-sulfur dioxide batteries. The life support system is partly a regenerative system with air and hygiene water being recycled. A layer of water inside the composite shell surrounds the command center allowing the center to be used as a safe haven during solar flares. The PLR 1 has a total mass of 6197 kg. It has a top speed of 18 km/hr and is capable of towing three metric tons, in addition to the RTG trailer. The PLR 2 configuration consists of two four-meter diameter, cylindrical hulls which are passively connected by a flexible passageway, resulting in the overall vehicle length of 11 m. The vehicle is driven by eight independently suspended wheels. The dual-cylinder concept allows articulated as well as double Ackermann steering. The primary power of 8 kW is supplied by a dynamic isotope system using a closed Brayton cycle with a xenon-hydrogen mixture as the working fluid. A sodium-sulfur battery serves as the secondary power source. Excess heat produced by the primary power system and other rover systems is rejected by radiators located on the top of the rear cylinder. The total mass of the PLR 2 is 7015 kg. Simplicity and low total weight have been the driving principles behind the design of PLR 1. The overall configuration consists of a 7-m-long, 3-m-diameter cylindrical main vehicle and a two-wheeled trailer. The cylinder of the main body is capped by eight-section, faceted, semi-hemispherical ends. The trailer contains the RTG power source and is not pressurized. The shell of the main body is constructed of a layered carbon fiber/foam/Kevlar sandwich structure. Included in the shell is a layer of water for radiation protection. The layer of water extends from the front of the rover over the crew compartment and creates a safe haven for the crew during a solar flare-up. The carbon fiber provides the majority of the strength and stiffness and the Kevlar provides protection from micrometeoroids. The Kevlar is covered with a gold foil and multi-layer insulation (MLI) to reduce radiation degradation and heat transfer through the wall. A thin thermoplastic layer seals the fiber and provides additional strength.

Creel, Kenneth↗

DOE OSTI2025

Decoupling electrode kinetics to elucidate reaction mechanisms in alkaline water electrolysis

Alkaline water electrolysis (AWE) presents key advantages, including reduced material costs, enhanced operational stability, and compatibility with non-precious metal catalysts, positioning it as a scalable route for hydrogen production. In this study, we introduce a minimally invasive single-cell configuration incorporating a reference electrode via diaphragm extension to form an internal ion channel. This setup, combined with an interfaced potentiostat and auxiliary electrometer, enables real-time, independent monitoring of anode and cathode behavior, offering high-resolution electrochemical diagnostics. While it is well established that the hydrogen evolution reaction (HER) exhibits sluggish kinetics in alkaline media, our study reveals that this limitation persists even in practical AWE systems where nickel-based substrates are used as electrodes. This observation is supported by both experimental data and voltage breakdown modeling. Arrhenius-type analysis reveals that localized electric fields induced by catalysts shift the reaction kinetics from classical Butler–Volmer behavior toward a Marcus-like regime, where interfacial molecular dynamics and bimolecular charge transfer dominate. We propose a semi-empirical model and a surficial reaction mechanism to describe these dynamics. This work underscores the critical need for cathode innovation and provides a rational framework for designing advanced catalysts and electrode architectures to optimize AWE performance.

08 HYDROGEN↗

DOE OSTI2026

Background-Oriented Schlieren Velocimetry of Helium Coolant Flow in Additively Manufactured Channels

High-pressure helium gas cooling is an attractive solution for thermal management of the fusion blanket first wall, as this coolant is chemically and neutronically inert and separable from hydrogenic species. However, due to the low thermal mass of helium, geometric optimization of these channels is required to provide sufficient cooling at manageable flow rates and pumping burdens. Increasingly, analysis and optimization of these coolant channels rely on computational fluid dynamics (CFD) simulations, and these require relevant experimental data for turbulence model validation. Toward this end, a high-pressure helium gas flow visualization system has been employed to image the flow of helium in flow channels with one-sided heating, mimicking the blanket first wall environment. Flow of helium at 4 MPa pressure and flow rates up to 68 g/s (Reynolds number 57 000) is supplied to rectangular channel test sections, with uniform heating applied to the bottom wall of the channel at heat fluxes varied between roughly 50 and 130 kW/m2. A high-speed camera is used to image index of refraction (IOR) gradients in the fluid via background-oriented schlieren (BOS), and temperature and pressure instrumentation are used to characterize thermal-hydraulic performance of each channel. Cross correlation of time-resolved BOS images is then used to calculate time-averaged 2-D helium velocity fields. Flow in additively manufactured (AM) channels is examined in this manner, including both featureless channels and those containing baffling as a heat transfer enhancement. The flow distribution seen in the featureless case differs significantly from that seen in prior simulations, whereas the flow in the baffled case shows the predicted behavior of flow forced along the heated wall. This augmented flow distribution is seen to increase the heat transfer coefficient in the baffled test section. Here, strategies are discussed for ongoing and future validation of these simulations, with the aim of model deployment for blanket cooling design and optimization.

Additive manufacturing↗

DOE OSTI2024

Corrosion-Resistant Non-Carbon Electrocatalyst Supports for PEFCS

Insufficient durability of commercial catalysts is a persistent issue for PEFC applications.1 Herein, Pt on Nb-doped-TiO 2 is reported as a highly durable electrocatalyst on which the direct 4-electron reduction of oxygen to water is more facile compared to Pt/C. All performance metrics are reported comparing Pt/Nb-TiO2 with a 15% Pt loading, against a commercial Pt/C catalyst (46.5% Pt loading, Tanaka, K. K.). Nb-doped-TiO 2 with high surface area and high electronic conductivity was synthesized using the supercritical fluid method. Initially, the durability of the catalyst was characterized using accelerated stability tests (ASTs) involving 10,000 high potential cycles (DOE/FCCJ protocol) and the Pt/Nb-TiO 2 was found to retain 78% of its initial electrochemically active surface area (ECSA) compared to the 57.6 % retained by Pt/C. These observations were in excellent agreement with previous reports that the Pt particle size of Pt/C grew from 2nm to 8nm during the AST protocol along with severe corrosion and amorphization of the carbon surface.2, 3 TEM and XPS studies of the Pt-Nb-doped-TiO 2 catalyst showed that the Pt particle size grew from 3nm to 6nm and the Nb(IV) and Ti(III) in the support were oxidized to Nb(V) and Ti(IV) after the durability test. Thus, the improvement in Pt/Nb-TiO 2 ECSA retention was attributed to the lower extent of particle growth and lack of oxidative support loss upon oxidation as compared to Pt/C. The oxygen reduction reaction (ORR) performance was characterized by linear polarization using a rotating disk electrode (RDE). The electrochemical surface areas of Pt/Nb-TiO 2 and Pt/C were found to be 48m2·g -1 and 83m2·g -1 respectively, and the mass activity for the ORR at 0.9V vs. RHE were found to be 150 mA·mg-1Pt and 124 mA·mg-1Pt respectively. The improved mass activity on Pt/Nb-TiO 2 was attributed to strong metal support interaction (SMSI) between the Nb-TiO 2 support and the Pt catalyst based on the 625 meV decrease in the binding energy of the Pt4f x-ray photo-electron spectroscopy (XPS) peaks of Pt/Nb-TiO 2 compared to Pt/C. To quantify the impact of the SMSI, a kinetic model was applied to calculate the elementary reaction rate constants for the various steps of the ORR on both catalysts. The reaction rate constant (k1) for the direct 4-electron transfer pathway to produce H 2 O was significantly larger in Pt/Nb-TiO 2 as compared to Pt/C. Thus, the reduction in the electron binding energy as observed in the XPS was found to aid the facile filling of the higher energy 2p orbitals of O 2 thereby leading to improved 4-electron transfer kinetics and improved overall activity.

08 HYDROGEN↗

NASA NTRS2011

Lightweight Magnetic Cooler With a Reversible Circulator

A design of a highly efficient and lightweight space magnetic cooler has been developed that can continuously provide remote/distributed cooling at temperatures in the range of 2 K with a heat sink at about 15 K. The innovative design uses a cryogenic circulator that enables the cooler to operate at a high cycle frequency to achieve a large cooling capacity. The ability to provide remote/distributed cooling not only allows flexible integration with a payload and spacecraft, but also reduces the mass of the magnetic shields needed. The active magnetic regenerative refrigerator (AMRR) system is shown in the figure. This design mainly consists of two identical magnetic regenerators surrounded by their superconducting magnets and a reversible circulator. Each regenerator also has a heat exchanger at its warm end to reject the magnetization heat to the heat sink, and the two regenerators share a cold-end heat exchanger to absorb heat from a cooling target. The circulator controls the flow direction, which cycles in concert with the magnetic fields, to facilitate heat transfer. Helium enters the hot end of the demagnetized column, is cooled by the refrigerant, and passes into the cold-end heat exchanger to absorb heat. The helium then enters the cold end of the magnetized column, absorbing heat from the refrigerant, and enters the hot-end heat exchanger to reject the magnetization heat. The efficient heat transfer in the AMRR allows the system to operate at a relatively short cycle period to achieve a large cooling power. The key mechanical components in the magnetic cooler are the reversible circulator and the magnetic regenerators. The circulator uses non-contacting, self-acting gas bearings and clearance seals to achieve long life and vibration- free operation. There are no valves or mechanical wear in this circulator, so the reliability is predicted to be very high. The magnetic regenerator employs a structured bed configuration. The core consists of a stack of thin GGG disks alternating with thin polymer insulating films. The structured bed reduces flow resistance in the regenerator and therefore the pumping work by the cryogenic circulator. This magnetic cooler will enable cryogenic detectors for sensing infrared, x-ray, gamma-ray, and submillimeter radiation in future science satellites, as well as the detector systems in the Constellation-X (Con-X) and the Single Aperture Far-Infrared observatory (SAFIR). Scientific ap p - lica tions for this innovation include cooling for x-ray micro calorimeter spectrometers used for microanalysis, cryogenic particle detectors, and superconducting tunnel junction de tectors for biomolecule mass spectrometry. The cooler can be scaled to provide very large cooling capacities at very low temperatures, ideal for liquid helium and liquid hydrogen productions.

Chen, Weibo↗

NASA NTRSDate not supplied

Nodal Modeling of Tank Pressurization and Draining using a Multi-Node-Ullage Approach

The purpose of the pressurization system in liquid rocket propulsion is to control the pressure in the gas space of the propellant tank (known as the ullage space) and the propellant mass flowrate to the engine. A mathematical model is required to predict the amount of pressurant necessary to ensure that pressure and temperature levels inside the tank remain within acceptable limits and that the propellant pressure leaving the tank satisfies the net positive suction pressure (NPSP) requirement of the pump feeding the engine. Nodal codes typically model tank pressurization and draining using a single node to represent the ullage and a single node to represent the propellant. As the tank drains, the ullage node grows and the propellant node shrinks. The heat transfer between ullage to wall and ullage to propellant is governed by natural convection. Designers of liquid propulsion systems often use empirical correlations to estimate the “Collapse Factor” which represents the ratio of pressurant required with heat transfer and the amount of pressurant required without heat transfer. A single node ullage model of tank pressurization was developed using GFSSP to compute the collapse factor reasonably well and later was used to model tank pressurization during test firing of the FASTRAC rocket engine. The predicted tank pressure compared well with the test data. In the early 1970’s, pressurization and drain tests with liquid methane were performed at NASA Lewis Research Center in a vacuum chamber. A 5 ft diameter spherical aluminum tank was tested to drain from 95% to 5% full using gaseous helium, hydrogen, nitrogen and methane as pressurant. Tests were conducted with different pressurant inlet temperatures and drain times. Measured data include pressurant requirement, amount of pressurant condensed, and ullage and wall temperatures at various heights in the ullage space at the end of draining. A single node GFSSP model was developed to simulate helium pressurization of the methane tank. Predicted helium consumption was 8-23% less than measured. The average error of the six test cases was 16%. A single ullage node with multiple solid node model was developed using Thermal Desktop. Predicted helium consumption compares with the test data within 2%. This paper describes the development of a GFSSP multi-node ullage model of the test configuration and compares the predicted pressurant consumption for both helium and autogenous pressurization using gaseous methane with experimental as well as TD predictions.

Nodal Model↗