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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 595 records · Page 33
All sourcesNASA NTRSDOE OSTI
NASA NTRS2018

A Two-Stage Biological Reactor for Treatment of Space Based Waste Waters

Previous works on Membrane Aerobic Biological Reactors (MABR) CoMANDR 1.0, CoMANDR 2.0, and R-CoMANDAR have demonstrated their ability to stabilize various space based waste streams over operating periods of ~1 year. Biological pretreatment by MABR systems can stabilize space based waste streams. Biological stabilization includes reducing the pH, conversion of organic N to NOx- and oxidation of dissolved organic matter to CO2. These processes produce a more stable waste product (brine), facilitate the distillation processes, and enable evaporative or membrane based systems. An alternative to aerobic operation would be to include anoxic operation to promote denitrification and production of N2 gas. This results in a reduced O2 demand and increases ammonia oxidation efficiency. Denitrifictaion can be accomplished in either a single reactor (Simultaneous Nitrification Denitrification) or in a two-stage system with separate aerobic and anoxic reactors. We evaluated the performance of both architectures in pilot scale systems (1-2 crew/d). Each system was continuously operated for over 2 years during which they processed a variety of habitation waste streams (ISS, Transit, and EPB) in both a continuous and on production feed mode. Here we report the results of the two stage system. Results indicate that the two stage system can successfully remove organic carbon, lower pH and convert organic N to N2 gas. Organic carbon and organic N oxidation reaction rates for the two stage system are similar to past studies for single stage aerobic systems. The two stage system is more complex and requires an additional pump. While no maintenance was required on the system during the nearly two year period of operation, the packed bed did produce N2 gas for many operational test points. The performance and comparison of operational conditions are detailed below

Water↗
DOE OSTI2024

High-Temperature Oxidation Behavior of Wrought and Additive Manufactured H282 in Direct-Fired Supercritical CO2 Power Cycle Environments

Materials selection is a key concern for corrosion resistance in high temperature and pressure direct-fired supercritical CO2 power cycles. The effect of elevated pressure on corrosion resistance can be critical, as impurities within the supercritical fluid such as H2O and O2 can result in additional corrosion behaviors. Utilizing additive manufacturing (AM) methods for construction of power cycle components requiring both compact and complex designs could be advantageous. AM H282 produced by laser powder bed fusion was exposed to direct-fired conditions (95CO2 – 4H2O – 1 O2) at 750 °C at both atmospheric pressure and supercritical conditions (20 MPa) for up to 4,000 hours. Oxidation behavior, sub-surface carbide formation, and chromia scale volatilization was dependent upon AM preparation techniques and surface modifications. These results are discussed in terms of the potential compatibility issues that may arise when using AM alloys in high temperature regions of direct-fired sCO2 power cycles, particularly for thin-walled components.

Carney, Casey↗
NASA NTRS2020

Did a Complex Carbon Cycle Operate in the Inner Solar System?

Solids in the interstellar medium consist of an intimate mixture of silicate and carbonaceous grains. Because 99% of silicates in meteorites were reprocessed at high temperatures in the inner regions of the Solar Nebula, we propose that similar levels of heating of carbonaceous materials in the oxygen-rich Solar Nebula would have converted nearly all carbon in dust and grain coatings to CO. We discuss catalytic experiments on a variety of grain surfaces that not only produce gas phase species such as CH4, C2H6, C6H6, C6H5OH, or CH3CN, but also produce carbonaceous solids and fibers that would be much more readily incorporated into growing planetesimals. CH4 and other more volatile products of these surface-mediated reactions were likely transported outwards along with chondrule fragments and small Calcium Aluminum-rich Inclusions (CAIs) to enhance the organic content in the outer regions of the nebula where comets formed. Carbonaceous fibers formed on the surfaces of refractory oxides may have significantly improved the aggregation efficiency of chondrules and CAIs. Carbonaceous fibers incorporated into chondritic parent bodies might have served as the carbon source for the generation of more complex organic species during thermal or hydrous metamorphic processes on the evolving asteroid.

Joseph A Nuth↗
DOE OSTI2025

Solvation directed morphological control in metal oxide nanostructures

The development of structural hierarchy on various length scales during the crystallization process is ubiquitous in biological systems and minerals and is common in synthetic nanomaterials. The driving forces for the formation of complex architectures range from local interfacial interactions, that modify interfacial speciation, local supersaturation, and nucleation barriers, to macroscopic interparticle forces. Although it is enticing to interpret the formation of hierarchical architectures as the assembly of independently nucleated building blocks, crystallization pathways often follow monomer-by-monomer addition with structural complexity arising from interfacial chemical coupling and strongly correlated fluctuation dynamics in the electric double layers. Here, we show that the development of structural hierarchy through heterogeneous nucleation is driven by dipolar and solvation forces. Specifically, coupled simulations and experimental studies revealed that dipole build-up along the slow growth direction can trigger twinning and the development of branched architectures. Enthalpic solvation interactions were shown to either enhance or reduce the dipole moment of the nanoparticles and, thereby, control crystal morphology and architecture. The systematic studies of chemical coupling between different solvents and undercoordinated surface atoms of the growing nanocrystals revealed the mechanism of dimensionality control and the development of structural hierarchy without ligands or structure-directing agents.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Markers of mitochondrial function and oxidative metabolism in skeletal muscle do not display intrinsic circadian regulation in female mice

Mitochondria are key regulators of metabolism and ATP supply in skeletal muscle, while circadian rhythms influence many physiological processes. However, whether mitochondrial function is intrinsically regulated in a circadian manner in mouse skeletal muscle is inadequately understood. Accordingly, we measured postabsorptive transcript abundance of markers of mitochondrial autophagy, dynamics, and metabolism [extensor digitorum longus (EDL), soleus, gastrocnemius], protein abundance of electron transport chain complexes (EDL and soleus), enzymatic activity of succinate dehydrogenase (tibialis anterior and plantaris), and maximal mitochondrial respiration (tibialis anterior) in different skeletal muscles from female C57BL/6NJ mice at four zeitgeber times: 1, 7, 13, and 19. Our findings demonstrate that markers of mitochondrial function and oxidative metabolism do not display intrinsic time-of-day regulation at the gene, protein, enzymatic, or functional level. The core-clock genes Bmal1 and Dbp exhibited intrinsic circadian rhythmicity in skeletal muscle (i.e., EDL, soleus, gastrocnemius) and circadian amplitude varied by muscle type. These findings demonstrate that female mouse skeletal muscle does not display circadian regulation of markers of mitochondrial function or oxidative metabolism over 24 h.

Circadian Biology↗
DOE OSTI2026

Plutonium(III) versus uranium(III) and samarium(III) in small molecule activation chemistry

We report the PuIII complex, [PuIII(CpMe4)3] (1-Pu), and demonstrate its differences in small molecule reactivity compared to the UIII and SmIII analogs, [UIII(CpMe4)3] (1-U) and [SmIII(CpMe4)3] (1-Sm), respectively. 1-Pu reductively cleaves the small molecule (PhS)2, affording a PuIII complex, [{PuIII(CpMe4)2}2(μ-SPh)2] (2-Pu), while retaining the PuIII center and eliminating (CpMe4)2 as a by-product, a fingerprint of a sterically induced reduction (SIR) reaction. Sm is often used as a surrogate for Pu, but the analogous [SmIII(CpMe4)3], (1-Sm), is unreactive. The (PhS)2 cleavage by 1-U proceeds solely via a metal-based oxidation (i.e., UIII → UIV), to form [UIV(CpMe4)3(SPh)] (3-U). Only 1-U reacts with (PhHN)2, affording the reductive cleavage product, [UIV(CpMe4)3(NHPh)] (4-U). The difference in reactivity of 1-Pu compared to complexes 1-Sm and 1-U was unexpected, and since SIR chemistry can enable complexes to participate in otherwise impossible reductive transformation of substrates, this reinforces the importance of studying small molecule reactivity with the transuranic elements.

Keener, Megan↗
DOE OSTI2026

Highly-destabilized ligand field excited states of iron carbene complexes and their relation to charge transfer state lifetimes

Lifetimes of photoexcited charge transfer (CT) states in transition metal chromophores are influenced by low-lying ligand field (LF) excited states, especially for 3d metal complexes. To manipulate interactions between LF and CT states, it is important to be able to control LF excited state energies using tunable synthetic variables. In this report, we use Fe 2p3d L 3 -edge resonant inelastic X-ray scattering (RIXS) to measure LF excited state energies of three homoleptic iron chromophores coordinated by strong-field N-heterocyclic carbenes (NHCs). We investigate the effect of oxidation state and ligand scaffold on LF energies and covalency parameters. A cyclometalated bis(NHC) ligand affords both high LF excited state energies (and thus high 10 Dq) as well as high metal–ligand covalency compared to other iron complexes with very strong-field ligands. However, for the set of complexes investigated, we do not observe meaningful correlation between the LF excited state energies and the CT excited state lifetimes. These results illustrate that targeting long-lived CT excited states necessitates control of multiple molecular excited state properties, with destabilization of the LF excited state energies proving necessary, but insufficient, to control the CT excited state lifetime in Fe carbene complexes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2012

The Multiple Use Plug Hybrid for NanoSats (MUPHyN) Miniature Thruster

The Multiple Use Plug Hybrid (for) Nanosats is a prototype thruster is being developed to fill a niche application for NanoSat-scale spacecraft propulsion. When fully developed, the MUPHyN thruster will provide an effective and low-risk propulsive capability that could enable multiple NanoSats to be independently re-positioned after deployment from a parent launch vehicle. Because the environmentally benign, chemically-stable propellants are mixed only within the combustion chamber after ignition and the flow rate of the fuel is determined by a pyrolysis mechanism that is nearly independent of pressure or fuel grain defects, the system is inherently safe and can be piggy-backed near a secondary payload with little or no overall mission risk increase to the primary payload. The MUPHyN thruster uses safe-handling and inexpensive nitrous oxide (N2O) and acrylonitrile-butadiene-styrene (ABS) as propellants. Fused Deposition Modeling (FDM), a direct digital manufacturing process, is used to fabricate short-form-factor solid fuel grains with multiple helical combustion ports from ABS thermoplastic. This manufacturing process allows for the rapid development and manufacture of complex fuel grain geometries that are not possible to extrude or cast using conventional methods. This technology enables the construction of fuel grains with length-to-diameter ratios appropriate for incorporation into CubeSats while maintaining high surface areas and regression rates that allow the system to maintain a near optimal oxidizer to fuel ratio. The MUPHyN system provides attitude control torques by using secondary-injection thrust vectoring on a truncated aerospike nozzle. This configuration allows large impulse delta V burns and small impulse attitude control firings to be performed with the same system. To ensure survivability during extend duration burns, the MUPHyN incorporates a novel regenerative cooling design where the N2O oxidizer flows through a cooling path embedded in the aerospike nozzle before being injected into the combustion chamber near the nozzle base.

Eilers, Shannon D.↗
DOE OSTI2025

The linker protein ApcI regulates light harvesting under red light in Synechocystis sp. PCC 6803

Phycobilisomes (PBSs) are versatile cyanobacterial antenna complexes that harvest light energy to drive photosynthesis. They can adapt to various light conditions; for example, dismantling under high light to prevent photo-oxidation and arranging in rows under low light to increase light harvesting efficiency. Light quality also influences PBS structure and function, as observed under far-red light exposure. Here, we describe a PBS linker protein, ApcI (previously hypothetical protein Sll1911), expressed specifically under red light (620 nm) or upon chemically induced reduction of the plastoquinone pool. We characterized ApcI in Synechocystis sp. PCC 6803 using mutant analyses, PBS binding experiments, and protein interaction studies. Deletion of apcI conferred high light tolerance on Synechocystis sp. PCC 6803 compared to the wild-type strain, leading to reduced energy transfer from PBSs to the photosystems under high light. Binding experiments revealed that ApcI replaces the linker protein ApcG at the membrane-facing side of the PBS core via a paralogous C-terminal motif. Additionally, the N-terminal region of ApcI interacts with photosystem II. Our findings highlight the importance of PBS remodeling for adaptation to different light conditions. The characterization of ApcI provides insight into the mechanisms by which cyanobacteria optimize light harvesting in response to varying light conditions.

Photosystem↗
NASA NTRS1999

Carboxylic and dicarboxylic acids extracted from crushed magnesium oxide single crystals

Carboxylic and dicarboxylic acids (glycolic, oxalic, malonic and succinic) have been extracted with tetrahydrofuran (THF) and H2O from large synthetic MgO crystals, crushed to a medium fine powder. The extracts were characterized by infrared spectroscopy and 1H-NMR. The THF extracts were derivatized with tert-butyldimethylsilyl (t-BDMS) for GC-MS analysis. A single crystal separated from the extract was used for an x-ray structure analysis, giving the monoclinic unit cell, space group P21/c with ao = 5.543 A, bo = 8.845 A, co = 5.086 A, and beta = 91.9 degrees, consistent with beta-succinic acid, HOOC(CH2)COOH. The amount of extracted acids is estimated to be of the order of 0.1 to 0.5 mg g-1 MgO. The MgO crystals from which these organic acids were extracted grew from the 2860 degrees C hot melt, saturated with CO/CO2 and H2O, thereby incorporating small amounts of the gaseous components to form a solid solution (ss) with MgO. Upon cooling, the ss becomes supersaturated, causing solute carbon and other solute species to segregate not only to the surface but also internally, to dislocations and subgrain boundaries. The organic acids extracted from the MgO crystals after crushing appear to derive from these segregated solutes that formed C-C, C-H and C-O bonds along dislocations and other defects in the MgO structure, leading to entities that can generically be described as (HxCyOz)n-. The processes underlying the formation of these precursors are fundamental in nature and expected to be operational in any minerals, preferentially those with dense structures, that crystallized in H2O-CO2-laden environments. This opens the possibility that common magmatic and metamorphic rocks when weathering at the surface of a tectonically active planet like Earth may be an important source of abiogenically formed complex organic compounds.

NASA Discipline Exobiology↗
NASA NTRS1992

Catalytic methods using molecular oxygen for treatment of PMMS and ECLSS waste streams, volume 2

Catalytic oxidation has proven to be an effective addition to the baseline sorption, ion exchange water reclamation technology which will be used on Space Station Freedom (SSF). Low molecular weight, polar organics such as alcohols, aldehydes, ketones, amides, and thiocarbamides which are poorly removed by the baseline multifiltration (MF) technology can be oxidized to carbon dioxide at low temperature (121 C). The catalytic oxidation process by itself can reduce the Total Organic Carbon (TOC) to below 500 ppb for solutions designed to model these waste waters. Individual challenges by selected contaminants have shown only moderate selectivity towards particular organic species. The combined technology is applicable to the more complex waste water generated in the Process Materials Management System (PMMS) and Environmental Control and Life Support System (ECLSS) aboard SSF. During the phase 3 Core Module Integrated Facility (CMIF) water recovery tests at NASA MSFC, real hygiene waste water and humidity condensate were processed to meet potable specifications by the combined technology. A kinetic study of catalytic oxidation demonstrates that the Langmuir-Hinshelwood rate equation for heterogeneous catalysts accurately represent the kinetic behavior. From this relationship, activation energy and rate constants for acetone were determined.

Akse, James R.↗
DOE OSTI2024

Theoretical analysis of the OH-initiated atmospheric oxidation reactions of imidazole

Imidazoles are present in Earth's atmosphere in both the gas-phase and in aerosol particles, and have been implicated in the formation of brown carbon aerosols. The gas-phase oxidation of imidazole (C 3 N 2 H 4 ) by hydroxyl radicals has been shown to be preferentially initiated via OH-addition to position C5, producing the 5-hydroxyimidazolyl radical adduct. However, the fate of this adduct upon reaction with O 2 in the atmospheric gas-phase is currently unknown. We employed an automated approach to investigate the reaction mechanism and kinetics of imidazole's OH-initiated gas-phase oxidation, in the presence of O 2 and NO x . The explored mechanism included reactions available to first-generation RO 2 radicals, as well as alkoxyl radicals produced from RO 2 + NO reactions. Product distributions were obtained by assembling and solving a master equation, under conditions relevant to the Earth's atmosphere. Our calculations show a complex, branched reaction mechanism, which nevertheless converges to yield two major closed-shell products: 4H-imidazol-4-ol (4H-4ol) and N,N′-diformylformamidine (FMF). At 298 K and 1 atm, we estimate the yields of 4H-4ol and FMF from imidazole oxidation initiated via OH-addition to position C5 to be 34 : 66, 12 : 85 and 2 : 95 under 10 ppt, 100 ppt and 1 ppb of NO respectively. This work also revealed O 2 -migration pathways between the α-N-imino peroxyl radical isomers. This reaction channel is fast for the first-generation RO 2 radicals, and may be important during the atmospheric oxidation of other unsaturated organic nitrogen compounds as well.

Almeida, Thomas Golin↗
NASA NTRS1996

Turbulent flame propagation in partially premixed flames

Turbulent premixed flame propagation is essential in many practical devices. In the past, fundamental and modeling studies of propagating flames have generally focused on turbulent flame propagation in mixtures of homogeneous composition, i.e. a mixture where the fuel-oxidizer mass ratio, or equivalence ratio, is uniform. This situation corresponds to the ideal case of perfect premixing between fuel and oxidizer. In practical situations, however, deviations from this ideal case occur frequently. In stratified reciprocating engines, fuel injection and large-scale flow motions are fine-tuned to create a mean gradient of equivalence ratio in the combustion chamber which provides additional control on combustion performance. In aircraft engines, combustion occurs with fuel and secondary air injected at various locations resulting in a nonuniform equivalence ratio. In both examples, mean values of the equivalence ratio can exhibit strong spatial and temporal variations. These variations in mixture composition are particularly significant in engines that use direct fuel injection into the combustion chamber. In this case, the liquid fuel does not always completely vaporize and mix before combustion occurs, resulting in persistent rich and lean pockets into which the turbulent flame propagates. From a practical point of view, there are several basic and important issues regarding partially premixed combustion that need to be resolved. Two such issues are how reactant composition inhomogeneities affect the laminar and turbulent flame speeds, and how the burnt gas temperature varies as a function of these inhomogeneities. Knowledge of the flame speed is critical in optimizing combustion performance, and the minimization of pollutant emissions relies heavily on the temperature in the burnt gases. Another application of partially premixed combustion is found in the field of active control of turbulent combustion. One possible technique of active control consists of pulsating the fuel flow rate and thereby modulating the equivalence ratio (Bloxsidge et al. 1987). Models of partially premixed combustion would be extremely useful in addressing all these questions related to practical systems. Unfortunately, the lack of a fundamental understanding regarding partially premixed combustion has resulted in an absence of models which accurately capture the complex nature of these flames. Previous work on partially premixed combustion has focused primarily on laminar triple flames. Triple flames correspond to an extreme case where fuel and oxidizer are initially totally separated (Veynante et al. 1994 and Ruetsch et al. 1995). These flames have a nontrivial propagation speed and are believed to be a key element in the stabilization process of jet diffusion flames. Different theories have also been proposed in the literature to describe a turbulent flame propagating in a mixture with variable equivalence ratio (Muller et al. 1994), but few validations are available. The objective of the present study is to provide basic information on the effects of partial premixing in turbulent combustion. In the following, we use direct numerical simulations to study laminar and turbulent flame propagation with variable equivalence ratio.

Poinsot, T.↗
DOE OSTI2026

Unveiling Swift Heavy Ion Track Morphology in Sr-Based High-Entropy Perovskites

The incorporation of multiple cations on a single lattice site in the high-entropy oxides is considered the key driving factor for modifying the known atomic-level response to energetic ion irradiation due to the presence of structural disorder; however, these effects are not well-understood yet. In this work, we present atomic-level insight into irradiation-induced nanoscale phase transformations in a perovskite-structured high-entropy oxide, Sr(Zr 0.2 Sn 0.2 Ti 0.2 Hf 0.2 Nb 0.2 )O 3 (Sr(HE)O 3 ), subjected to 774 MeV swift Xe heavy ions, where damage is dominated by inelastic ion−lattice interactions. While these ions generally are known to create nanoscale disordered channels, “ion tracks”, along the penetration direction in the material, this study shows the formation of discontinuous and partially recrystallized ion tracks in Sr(HE)O 3 . Compared to SrTiO 3 irradiated under identical energy loss conditions, the ion tracks in Sr(HE)O 3 exhibit significantly reduced diameters and a markedly different interfacial structure. Notably, the crystalline−amorphous interface in Sr(HE)O 3 shows minimal lattice distortion, confined to approximately 2−3 monolayers, in contrast to the extended disordered shell commonly observed in SrTiO 3 . Using in situ atomic-resolution electron microscopy, we further demonstrate that the amorphous/disordered regions within Sr(HE)O 3 ion tracks remain highly stable under electron irradiation, whereas tracks in SrTiO 3 readily recrystallize. This enhanced stability is attributed to the dominance of structural and chemical complexity arising from multiple B-site cations, which suppress defect migration and templated recrystallization driven by electronic excitations and local heating. Overall, this study highlights how high-entropy oxide chemistry fundamentally reshapes irradiation damage evolution, offering insights into defect formation and phase stability under extreme conditions.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Exploring Anomalous Photoelectron Angular Distributions in the Photoelectron Spectra of Gd 3 O 3 – : Study of Gd 3 O 2 – and Gd 3 O 3 – Using Photoelectron Spectroscopy and Density Functional Theory Calculations

Anion photoelectron (PE) spectra of lanthanide oxide clusters obtained previously have exhibited anomalous photoelectron angular distributions which were attributed to strong PE–valence electron (PEVE) interactions. Here, to further explore this effect, we have obtained the PE spectra of Gd 3 O 2 – and Gd 3 O 3 – , two clusters that have similarly complex electronic structures but contrasting symmetries. The spectra exhibit manifolds of detachment transitions at similar binding energies in a 0.5 eV window of energy. The electron affinity of Gd 3 O 2 is measured to be 1.29 ± 0.05 eV, and that of Gd 3 O 3 is 1.31 ± 0.05 eV. As seen in previous studies on lanthanide oxide cluster anions in lower than conventional oxidation states, transitions in spectra obtained lower photon energies are more congested than those obtained with higher photon energy, a signature of strong PEVE interactions. While the detachment transitions have predominantly parallel photoelectron angular distributions (PAD), the PAD varies across the manifold of transitions in the PE spectrum of Gd 3 O 3 – in a way that suggests four different subgroups of transitions. Results of calculations on Gd 3 O 2 – suggest kite or V-shape structures with antiferromagnetic coupling between one of the 4f 7 subshells with the two others. Calculations on Gd 3 O 3 – more definitively point to ring structures with a nearly isoenergetic ferromagnetically coupled high spin (24-tet) state and a dectet state in which one of the 4f 7 subshells is antiferromagnetically coupled with the other two. Taking these results as qualitative, we propose that strong mixing between the unperturbed states predicted computationally leads to overlapping transitions with different PADs.

anions↗
DOE OSTI2025

Continuous Encodable Reshaping of Gold Nanocrystals through Facet Modulation

Shape control of nanocrystals (NCs) is crucial for tuning their assembly behavior and functional properties, yet the precise manipulation of facet composition remains challenging. Here, we present a nanocrystal reshaping strategy to control and modulate the facets of gold (Au) NCs. Our one-pot approach, conducted at room temperature, requires only initial Au NCs, Au 3+ ions, and surfactants, distinguishing it from conventional reduction-mediated “etching-and-regrowth” methods. Detailed structural studies using electron microscopy, small-angle X-ray scattering (SAXS), and UV−vis spectroscopy reveal the surfactant-encoded pathway for NC transformation from shaped particles to spheres and then into various polyhedral shapes while preserving the individual particles' volume. The proposed reshaping mechanism involves the dissolution of surface Au atoms into Au + complexes in the presence of Au 3+ and surfactant, followed by surfactant-guided redeposition and formation of facets with different atomic planes. Using the ethanol oxidation reaction (EOR) as a probe, we observe a quasi-linear decrease in onset potential and an increase in activity with increasing {100} facet exposure. This work broadens synthetic strategies by offering precise NC reshaping and facet control.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Active learning path-dependent properties using a cloud-based materials acceleration platform

Solid state materials are central to many modern technologies in which a given material may be exposed to a variety of environments. The material properties often vary with the sequence of environments in an irreversible manner, resulting in a quintessential path-dependency in experimental observables. While sequential learning techniques have been effectively deployed for accelerating learning of state properties of materials, they often use a consistent environment path in all experiments. To elevate such techniques for making optimal decisions in experimental investigations of path-dependent properties, we introduce an iterated expected information gain acquisition function that optimizes over entire experimental trajectories. This approach is implemented within a cloud-based Materials Acceleration Platform architecture utilizing an event-driven stateful broker coupled with remote HELAO (Hierarchical Experimental Laboratory Automation and Orchestration) instances and an AI science manager. The platform's efficacy was demonstrated through a case study optimizing multi-step spectro-electrochemical experiments to identify optically stable potential windows in (Co–Ni–Sb)O z metal oxides. The system successfully integrated AI-driven experiment design, remote laboratory automation, and cloud-based data infrastructure, validating the platform's capability for managing complex, adaptive, path-dependent workflows in materials discovery.

Guevarra, Dan [California Institute of Technology ↗
DOE OSTI2025

Nickel promotes selective ethylene epoxidation on silver

Over the last 80 years, chlorine (Cl) has been the primary promoter of the ethylene epoxidation reaction valued at ~40 billion USD per year, providing a ~25% selectivity increase over unpromoted silver (Ag) (~55%). Promoters such as cesium, rhenium, and molybdenum each add a few percent of selectivity enhancements to achieve 90% overall, but their codependence on Cl makes optimizing and understanding their function complex. Here, we took a theory-guided, single-atom alloy approach to identify nickel (Ni) as a dopant in Ag that can facilitate selective oxidation by activating molecular oxygen (O 2 ) without binding oxygen (O) too strongly. Surface science experiments confirmed the facile adsorption/desorption of O 2 on NiAg, as well as demonstrating that Ni serves to stabilize unselective nucleophilic oxygen. Supported Ag catalyst studies revealed that the addition of Ni in a 1:200 Ni to Ag atomic ratio provides a ~25% selectivity increase without the need for Cl co-flow and acts cooperatively with Cl, resulting in a further 10% initial increase in selectivity.

36 MATERIALS SCIENCE↗