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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 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Final Technical Report: In-Silico Heterogeneous Catalyst Design for GHG Reduction via Bulk Chemicals

This project has advanced the understanding of ammonia synthesis by developing novel thermochemical catalysts, setting a new benchmark for energy and carbon efficiency in large-scale bulk chemicals production. This research leverages a proprietary computational discovery platform and high-throughput experimental validation, significantly accelerating catalyst optimization and enabling ammonia synthesis at lower temperature and pressure conditions than conventional processes. As a result, green ammonia can be produced at a cost that meets or exceeds established targets, supporting a viable pathway toward decarbonized ammonia for fuel, fertilizers, and hydrogen supply applications.

Grose, Jacob E [Copernic Catalysts, Inc.]↗
DOE OSTI2022

Plasmon mediated deposition of Ni on titanium nitride nanoparticles: Applications in enhanced photoreduction of bicarbonate

A suitably designed plasmonic catalyst can provide versatile and energy-efficient strategies to utilize visible light to drive different catalytic reactions. Here we have successfully developed composite plasmonic catalysts by visible-light-induced deposition of popular transition metal nanocatalysts such as Ni and Pt on refractory plasmonic titanium nitride (TiN) nanoparticles. Here, the catalytic properties of the TiN composite nanoparticles were evaluated using the visible light-mediated bicarbonate to formate reduction reaction in the presence of glycerol as the hole-scavenger. Deposition of Ni and Pt nanocatalysts on TiN significantly improves its catalytic efficiency towards the reaction. However, Ni deposited on TiN nanoparticles exhibited better catalytic properties in comparison to that of TiN_Pt composites. The findings of this study can be used to develop stable and efficient visible light-responsive plasmonic composite catalysts which can accelerate different energy extensive reactions.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Catalyst design for small molecule activation of energy consequence

This project targets the conversion of ubiquitous small molecules (e.g. NO, CO, H 2 O) into viable precursors to synthetic fuels. Current state of the art catalyst design has not directly targeted transition metal complexes capable of mediating the multi-electron redox processes necessary to reduce the overpotential (energy loss) required achieve efficient activation of small molecule substrates. In this vein, a new strategy has been developed for the assembly of polynuclear architectures; allowing for the construction of tunable polymetallic centers that assemble easily within a pre-organized template (conferring stability, selectivity and tunability) that can effect multi-electron redox processes for reactions. Catalyst development has commenced with the following target design elements: (1) catalysts featuring multiple transition metal ions in the same reaction space to greatly expand accessible molecular redox capabilities; (2) catalysts are assembled in a polynucleating ligand framework that permits control over the cluster morphology as well as the local steric and electronic environment of the transition metal ions within the cluster. The high-tunability of the catalyst composition (metal content) and geometric flexibility has permitted a rigorous assessment of electronic-structure-to-function relationship to be developed, further guiding synthetic efforts to realize more potent catalysts. The numerous permutations possible showcase the high degree of generality to this approach with many synthetic handles to tune redox and reaction chemistry. Trinuclear complexes have been synthesized featuring homo- and hetero-trinuclear cores featuring a variety of first row transition metal ions (Cr→Ni). The molecular clusters have been shown to successfully mediate multi-electron redox processes in a cooperative fashion without requiring strong chemical reductants or oxidants. The reactive molecular complexes are being utilized to activate and breakdown the robust bonds within typical waste stream small molecules (e.g., greenhouse gases) and convert them into value-added commodity chemicals. Ultimately, the catalysts developed by this approach will be required to convert energy acquired via renewable resources (e.g., solar or wind) into synthetic fuels as an energy storage mechanism.

10 SYNTHETIC FUELS↗
DOE OSTI2020

Discovery of single-atom alloy catalysts for CO 2 -to-methanol reaction by density functional theory calculations

The transformations of CO 2 molecules into valuable products are of increasing interest due to the negative impact of anthropogenic CO 2 emissions on global warming. The CO 2 -to-methanol hydrogenation is an economically profitable reaction of carbon fixation, but it still steps away from widespread industrialization because of the lack of efficient and selective catalysts. Recently, single-atom alloy (SAA) catalysts have been developed to work remarkably in CO 2 hydrogenation reactions. Doping isolated single atoms into metallic catalyst can dramatically alter the catalytic performance of the host. Here, we have performed a screening discovery on Ru and 6 RuX (X = Fe, Co, Ni, Cu, Ir and Pt) SAAs using density functional theory (DFT) computations. We considered 13 possible elementary reactions in 4 possible reaction pathways on Ru and all RuX surfaces. In the computed mechanisms, we found that the formation of *H 2 COOH and *HCOO intermediates plays a critical role in determining catalysts’ activities. Doping Co and Pt isolated single atoms into Ru surface can thermodynamically and kinetically facilitate these intermediates formation processes, eventually promoting the production of methanol. The combination of weak binding and enhanced charge redistribution on RuCo and RuPt surfaces give them improved catalytic activities over pure Ru. This work will ultimately facilitate the discovery and development of SAAs for CO 2 to methanol, serving as guidance to experiments and theoreticians alike.

25 ENERGY STORAGE↗
DOE OSTI2023

Outstanding Platinum Group Metal-free Bifunctional Catalysts for Rechargeable Zinc-Air Batteries

Developing highly active and durable catalysts for zinc-air batteries (ZAB) is critical for energy conversion and storage. Herein, we prepared Fe-N-C catalysts at a kilogram scale by the commercial VariPore™ method and the effect of synthesis conditions on the catalyst performance at ZAB air electrode was investigated. The results show the PA-450-HT exhibits excellent electrocatalytic activity toward oxygen reduction reaction (ORR) and it is the most suitable catalyst for primary ZAB with the galvanostatic polarization discharge peak power density of 149 mW cm -2 , outperforming commercial Pt-Ru/C catalysts. Additionally, the NCB-600-HT catalyst displays the half-wave potential of 0.87 V vs. RHE for ORR and ΔE value of 0.81 V (indicating outstanding ORR and OER reversibility) and exhibits excellent charge-discharge cycling durability similar to NCB-550-LT around 160 h for the secondary ZAB. This work reports outstanding bifunctional Fe-N-C catalysts for rechargeable ZAB at mass production for the first time.

25 ENERGY STORAGE↗
DOE OSTI2023

Oxidative Grafting for Catalyst Synthesis in Surface Organometallic Chemistry

The development of new methods of catalyst synthesis with the potential to generate active site structures orthogonal to those accessible by traditional protocols is of great importance for discovering new materials for addressing challenges in the evolving energy and chemical economy. Here, in this work, the generality of oxidative grafting of organometallic and well-defined molecular metal precursors onto redox-active surfaces such as manganese dioxide (MnO 2 ) and lithium manganese oxide (LiMn 2 O 4 ) is investigated. Nine molecular metal precursors are explored, spanning groups 4–11 and each of the three periods of the transition metal series. The byproducts of the oxidative grafting reaction, a mixture of protodemetalation and ligand homocoupling for several organometallic precursors, was found to provide insights into the mechanism of the grafting reaction, suggesting oxidation of both the metal d-orbitals, as well as the metal–carbon σ-bonds, resulting in ejection of the ligand radical fragment. Analysis of the supported structures and oxidation state by X-ray absorption spectroscopy (XAS) and X-ray photoelectron spectroscopy (XPS) suggests that several of the chemisorbed metal ions are intercalated into interstitial vacancies of the surface structure while other complexes form intact molecular fragments on the surface. Proof of concept for the use of this metalation protocol to generate diverse, metal-dependent catalytic performance is demonstrated by the application of these materials in the conversion of cyclohexane to K/A oil (cyclohexanol and cyclohexanone) with tert-butyl hydroperoxide, as well as in the low-temperature (T ≤ 50 °C) oxidation of carbon monoxide to carbon dioxide.

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

Unveiling Highly Sensitive Active Site in Atomically Dispersed Gold Catalysts for Enhanced Ethanol Dehydrogenation

Developing a desirable ethanol dehydrogenation process necessitates a highly efficient and selective catalyst with low cost. Herein, we show that the “complex active site” consisting of atomically dispersed Au atoms with the neighboring oxygen vacancies (Vo) and undercoordinated cation on oxide supports can be prepared and display unique catalytic properties for ethanol dehydrogenation. The “complex active site” Au-Vo-Zr 3+ on Au 1 /ZrO 2 exhibits the highest H 2 production rate, with above 37,964 mol H 2 per mol Au per hour (385 g H 2 $g^{-1}_{Au}$ h -1 ) at 350 °C, which is 3.32, 2.94 and 15.0 times higher than Au 1 /CeO 2 , Au 1 /TiO 2 , and Au 1 /Al 2 O 3 , respectively. Combining experimental and theoretical studies, we demonstrate the structural sensitivity of these complex sites by assessing their selectivity and activity in ethanol dehydrogenation. Our study sheds new light on the design and development of cost-effective and highly efficient catalysts for ethanol dehydrogenation. Fundamentally, atomic-level catalyst design by colocalizing catalytically active metal atoms forming a structure-sensitive “complex site”, is a crucial way to advance from heterogeneous catalysis to molecular catalysis. In conclusion, our study advanced the understanding of the structure sensitivity of the active site in atomically dispersed catalysts.

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

Unveiling Highly Sensitive Active Site in Atomically Dispersed Gold Catalysts for Enhanced Ethanol Dehydrogenation

Developing a desirable ethanol dehydrogenation process necessitates a highly efficient and selective catalyst with low cost. Herein, we show that the “complex active site” consisting of atomically dispersed Au atoms with the neighboring oxygen vacancies (Vo) and undercoordinated cation on oxide supports can be prepared and display unique catalytic properties for ethanol dehydrogenation. The “complex active site” Au–Vo–Zr 3+ on Au 1 /ZrO 2 exhibits the highest H 2 production rate, with above 37,964 mol H 2 per mol Au per hour (385 g H 2 $\text{g}^{-1}_{\text{Au}} \text{h}^{–1}$) at 350 °C, which is 3.32, 2.94 and 15.0 times higher than Au 1 /CeO 2 , Au 1 /TiO 2 , and Au 1 /Al 2 O 3 , respectively. Combining experimental and theoretical studies, we demonstrate the structural sensitivity of these complex sites by assessing their selectivity and activity in ethanol dehydrogenation. Our study sheds new light on the design and development of cost-effective and highly efficient catalysts for ethanol dehydrogenation. Fundamentally, atomic-level catalyst design by colocalizing catalytically active metal atoms forming a structure-sensitive “complex site”, is a crucial way to advance from heterogeneous catalysis to molecular catalysis. Finally, our study advanced the understanding of the structure sensitivity of the active site in atomically dispersed catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Intrinsic kinetics of water-inhibited ultra-lean methane oxidation over PtPd-Mg/ θ -Al 2 O 3 catalyst

Here, this study develops intrinsic methane oxidation kinetics for ultra-lean methane conditions in the presence of water over a highly active and stable PtPd–Mg/θ-Al 2 O 3 catalyst. Comprehensive laboratory experiments were conducted over a wide range of methane concentrations (150–1200 ppm CH 4 ), water contents (1–5% H 2 O), and industrially relevant space velocities (80,000 ≤ GHSV ≤ 160,000 h -1 ). These systematic experiments informed a two-dimensional, axisymmetric, multiscale reactor model that was used to develop and validate methane oxidation kinetics under practically relevant conditions, including non-isothermal operation and high conversion regimes. Combined experimental and modeling results revealed significant intraparticle diffusion resistance and transport-induced reaction exotherm at elevated temperatures, which limited catalyst utilization despite high intrinsic activity. These transport effects were explicitly incorporated into the reactor model, enabling accurate estimation of intrinsic kinetic parameters without reliance on conventional effectiveness-factor corrections. The resulting kinetic model successfully captured both kinetically controlled and mass-transfer-limited regimes and reliably predicted CH 4 conversion across broad ranges of temperature, methane concentration, and water content

Heat and mass transfer limitations↗
DOE OSTI2019

Atomic-Scale Insights into Surface Lattice Oxygen Activation at the Spinel/Perovskite interface of Co 3 O 4 /La 0.3 Sr 0.7 CoO 3

Surface lattice oxygen in transition-metal oxides plays a vital role in catalytic processes. Mastering activation of surface lattice oxygen and identifying the activation mechanism are crucial for the development and design of advanced catalysts. A strategy is now developed to create a spinel Co 3 O 4 /perovskite La 0.3 Sr 0.7 CoO 3 interface by in situ reconstruction of the surface Sr enrichment region in perovskite LSC to activate surface lattice oxygen. XAS and XPS confirm that the regulated chemical interface optimizes the hybridized orbital between Co 3d and O 2p and triggers more electrons in oxygen site of LSC transferred into lattice of Co 3 O 4 , leading to more inactive O 2- transformed into active O 2-x . Furthermore, the activated Co 3 O 4 /LSC exhibits the best catalytic activities for CO oxidation, oxygen evolution, and oxygen reduction. This work would provide a fundamental understanding to explain the activation mechanism of surface oxygen sites.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Dehydrogenation of Propane and n -Butane Catalyzed by Isolated PtZn 4 Sites Supported on Self-Pillared Zeolite Pentasil Nanosheets

Propene and 1,3-butadiene are important building-block chemicals that can be produced by dehydrogenation of propane and butane over Pt catalysts. The challenge is to develop highly active and selective catalysts that are resistant to deactivation by Pt sintering and coke formation. We have recently shown that these objectives can be met for propane dehydrogenation using atomically dispersed Pt atoms anchored to neighboring ≡SiOZn-OH groups bonded to the framework dealuminated zeolite BEA. In the present study, we demonstrate that significantly superior performance can be achieved by using self-pillared pentasil (SPP) zeolite nanosheets. Following catalyst reduction in H 2 , atomic-resolution, scanning transmission electron microscopy (STEM) and X-ray absorption spectroscopy (XAS) indicate that Pt is stabilized in structures well approximated as (≡Si-O-Zn) 4-5 Pt. These species are highly active, selective, and stable for propane dehydrogenation (PDH) to give propene and for n-butane dehydrogenation (BDH) to give 1,3-butadiene. No catalyst deactivation was observed after 12 days of time on stream, and the selectivity remained at nearly 100% for PDH conducted at 823 K and a weight hourly space velocity (WHSV) of 1,350 h -1 . The apparent rate coefficient for PDH over this catalyst is significantly higher than that reported previously for Pt-containing catalysts. For BDH at 823 K and a WHSV of 3560 h -1 , the selectivity to butene isomers and 1,3-butadiene is 98.9%, and the selectivity to 1,3-butadiene is 45%. Here, we propose that the high catalyst stability observed during PDH and BDH is a consequence of a large fraction of the Pt-containing centers being located on the external surface of the zeolite nanosheets, where nascent coke precursors can desorb before condensing to form coke.

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

Chemical and Biological Catalysis for Plastics Recycling and Upcycling

Plastics pollution is causing an environmental crisis, prompting the development of new approaches for recycling, and upcycling. Here, we review challenges and opportunities in chemical and biological catalysis for plastics deconstruction, recycling, and upcycling. We stress the need for rigorous characterization and use of widely available substrates, such that catalyst performance can be compared across studies. Where appropriate, we draw parallels between catalysis on biomass and plastics, as both substrates are low-value, solid, recalcitrant polymers. Innovations in catalyst design and reaction engineering are needed to overcome kinetic and thermodynamic limitations of plastics deconstruction. Either chemical and biological catalysts will need to act interfacially, where catalysts function at a solid surface, or polymers will need to be solubilized or processed to smaller intermediates to facilitate improved catalyst–substrate interaction. Overall, developing catalyst-driven technologies for plastics deconstruction and upcycling is critical to incentivize improved plastics reclamation and reduce the severe global burden of plastic waste.

28 EE - Advanced Manufacturing Office (EE-5A)↗
NASA NTRS1975

Development of advanced fuel cell system, phase 3

A multiple task research and development program was performed to improve the weight, life, and performance characteristics of hydrogen-oxygen alkaline fuel cells for advanced power systems. Gradual wetting of the anode structure and subsequent long-term performance loss was determined to be caused by deposition of a silicon-containing material on the anode. This deposit was attributed to degradation of the asbestos matrix, and attention was therefore placed on development of a substitute matrix of potassium titanate. An 80 percent gold 20 percent platinum catalyst cathode was developed which has the same performance and stability as the standard 90 percent gold - 10 percent platinum cathode but at half the loading. A hybrid polysulfone/epoxy-glass fiber frame was developed which combines the resistance to the cell environment of pure polysulfone with the fabricating ease of epoxy-glass fiber laminate. These cell components were evaluated in various configurations of full-size cells. The ways in which the baseline engineering model system would be modified to accommodate the requirements of the space tug application are identified.

Handley, L. M.↗
DOE OSTI2024

Production of 1,3-Butadiene from Renewable Feedstocks Ethanol and 1,3-Butanediol - CRADA 560 (Final Report)

1,3-butadiene is a commodity chemical currently produced from petroleum sources. Producing 1,3-butadiene from renewable resources will contribute to decarbonization, provide new green jobs, and reduce our dependance on oil. Development of multifunctional catalysts that are active, selective, and stable for this reaction has been an area of research and development. This effort reported here builds on our prior work for the 1-step conversion of ethanol to butadiene. The goal of the additional scope performed here was to accelerate the commercial deployment of sustainable butadiene production. We demonstrated that the PNNL Ag-based catalyst is significantly more active than the WWII-era catalyst when operated under the same conditions. A butadiene selectivity of 68% was obtained at 64% conversion for the production of butadiene from ethanol. It was found that ethanol feedstock is preferred over 1,3-butanediol feedstock to produce butadiene due to higher yield resulting in lower butadiene selling price (i.e., $\$$0.4-1.7/ lb). Production of 3.0 Liter of butadiene solution in hexane containing 100 grams of butadiene was achieved and delivered to Bridgestone for producing a butadiene-derived test piece.

09 BIOMASS FUELS↗
DOE OSTI2024

Thoughts on the past, present and future of UHV surface chemistry and the birth of Single-Atom Alloys

Throughout its relatively short lifetime, ultra-high vacuum (UHV) surface chemistry has progressed quickly. In the 1960's, pioneers like Ertl and Somorjai started the field using single crystals and gained significant insight into catalytic processes by relating surface structure to reactivity. The more recent proliferation of scanning probes has significantly increased the power of the single crystal approach by enabling the atomic-scale structure of active sites to be correlated with their reactivity. In this perspective we briefly discuss how the field developed, identify some challenges, and highlight Single-Atom Alloys (SAAs), a new class of heterogeneous catalyst that was developed from a fundamental surface science approach. However, despite recent successes, funding for fundamental surface science has declined. Academic hires in the discipline are also declining in part due to the start-up costs. We make the case that fundamental UHV surface chemistry is still too young a field to be in recession.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗