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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 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Selective hydrogenation via precise hydrogen bond interactions on catalytic scaffolds

Abstract The active site environment in enzymes has been known to affect catalyst performance through weak interactions with a substrate, but precise synthetic control of enzyme inspired heterogeneous catalysts remains challenging. Here, we synthesize hyper-crosslinked porous polymer (HCPs) with solely -OH or -CH 3 groups on the polymer scaffold to tune the environment of active sites. Reaction rate measurements, spectroscopic techniques, along with DFT calculations show that HCP-OH catalysts enhance the hydrogenation rate of H-acceptor substrates containing carbonyl groups whereas hydrophobic HCP- CH 3 ones promote non-H bond substrate activation. The functional groups go beyond enhancing substrate adsorption to partially activate the C = O bond and tune the catalytic sites. They also expose selectivity control in the hydrogenation of multifunctional substrates through preferential substrate functional group adsorption. The proposed synthetic strategy opens a new class of porous polymers for selective catalysis.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Understanding hydrogen electrocatalysis by probing the hydrogen-bond network of water at the electrified Pt–solution interface

Rational construction of the electrode–solution interface where electrochemical processes occur is of paramount importance in electrochemistry. Efforts to gain better control and understanding of the interface have been hindered by lack of probing methods. Here, in this study, we show that the hydrogen evolution and oxidation reactions (HER/HOR) catalysed by platinum in base can be promoted by introduction of N-methylimidazoles at the platinum–water interface. In situ spectroscopic characterization together with simulations indicate that the N-methylimidazoles facilitate diffusion of hydroxides across the interface by holding the second layer of water close to platinum surfaces, thereby promoting the HER/HOR. We thus propose that the HER/HOR kinetics of platinum in acid and base is governed by diffusion of protons and hydroxides, respectively, through the hydrogen-bond network of interfacial water by the Grotthuss mechanism. Moreover, we demonstrate a 40% performance improvement of an anion exchange membrane electrolyser by adding 1,2-dimethylimidazole into the alkali fed into its platinum cathode.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Catalytic decomposition of methane into hydrogen and high-value carbons: combined experimental and DFT computational study

Thermocatalytic decomposition (TCD) of methane can produce hydrogen and valuable nanocarbon co-products with low to near-zero CO2 emission. In this study, a series of Pd promoted Ni catalysts, prepared with various Ni/Pd ratios on a CNT support, were evaluated for methane TCD performance. Characterization and calculations using density functional theory (DFT) were carried out to elucidate the activity–structure relationship and growth mechanism of carbon nanomaterials. It was found that the methane conversion and stability of the catalysts were highly dependent on the Ni/Pd ratio and reaction temperature. DFT calculations revealed that the diffusion of carbon in the metal sublayer required for CNT growth was more favorable in the Ni–Pd alloy lattice suggesting that the buildup of carbon in the metal alloy sublayer facilitated the formation of CNTs and CNFs. A cyclic reaction–regeneration process for self-sustained TCD was experimentally demonstrated. In each cycle, a portion of the separated CNT product was used to re-synthesize the Ni–Pd/CNT catalyst for use in the next reaction cycle. After five cycles of operation, the CH4 conversion, morphology and crystallinity of the carbon product remained unchanged.

Wang, I-Wen↗
DOE OSTI2023

Low hydrogen solubility in clay interlayers limits gas loss in hydrogen geological storage

Gas intercalation into clay interlayers may result in hydrogen loss in the geological storage of hydrogen; a phenomenon that has not been fully understood and quantified. Here we use metadynamics molecular simulations to calculate the free energy landscape of H 2 intercalation into montmorillonite interlayers and the H 2 solubility in the confined water; in comparison with results obtained for CO 2 . Furthermore, the results indicate that H 2 intercalation into hydrated interlayers is thermodynamically unfavorable while CO 2 intercalation can be favorable. H 2 solubility in hydrated clay interlayers is in the same order of magnitude as that in bulk water and therefore no over-solubility effect due to nanoconfinement is observed – in striking contrast with CO 2 . These results indicate that H 2 loss and leakage through hydrated interlayers due to intercalation in a subsurface storage system, if any, is limited.

58 GEOSCIENCES↗
DOE OSTI2026

Data for Photoenzymatic Stereoablative Enantioconvergence of γ-chiral Oximes via Hydrogen Atom Transfer

Producing enantioenriched molecules from racemic mixtures is essential for manufacturing. Traditional methods such as resolution, deracemization and enantioconvergent catalysis primarily involve separating or converting enantiomers without altering their structures, or functionalization of stereocentres at or proximal to functional groups. However, there are challenges in enantioselectively forging C–H bonds that are remote from functional groups via hydrogen atom transfer (HAT) with these methods. Here we introduce a strategy for the photoenzymatic stereoablative enantioconvergence of γ-chiral oximes using repurposed flavin-dependent ene-reductases. A photoinduced single-electron reduction of the γ-chiral oxime by an ene-reductase generates an iminyl radical, which then undergoes stereoablative 1,5-HAT at the γ-stereocentre. Subsequent chiral reconstruction through enzymatic HAT and spontaneous imine hydrolysis yields the γ-chiral ketone with high enantioselectivity. This work provides a robust method for remote stereoablative enantioconvergent HAT and broadens the synthetic utility of photobiocatalysis.

Bioproducts↗
DOE OSTI2024

Prospects of hydrogen cogeneration and carbon dioxide utilization in electrochemical refineries for ethylene production via oxidative coupling of methane: A techno-economic assessment

Ethylene is recognized as one of the most significant chemicals globally. The projected ethylene production for 2023 stands at 227.6 million tonnes, with expectations of continued demand growth. The primary use of ethylene, accounting for over 76%, lies in the production of plastics such as polyethylene, polyvinyl chloride, and polystyrene. Despite the enduring carbon retention potential of plastics themselves, traditional ethylene feedstock production from fossil resources contributes substantially to greenhouse gas emissions, ranging from 0.29 to 2.29 kg CO2 /kg Ethylene depending on various factors like feedstock and process design. Various decarbonization strategies, including the utilization of hydrogen as a primary heat source, have been proposed to reduce the carbon footprint of ethylene production, but their efficacy remains limited, offering at best a 0–30% reduction in on-site CO 2 emissions.

09 BIOMASS FUELS↗
DOE OSTI2024

A Photochemical Phosphorus-Hydrogen-Oxygen Network for Hydrogen-dominated Exoplanet Atmospheres

Due to the detection of phosphine (PH 3 ) in the solar system gas giants Jupiter and Saturn, PH 3 has long been suggested to be detectable in exosolar substellar atmospheres too. However, to date, direct detection of phosphine has proven to be elusive in exoplanet atmosphere surveys. We construct an updated phosphorus-hydrogen-oxygen (PHO) photochemical network suitable for the simulation of gas giant hydrogen-dominated atmospheres. Using this network, we examine PHO photochemistry in hot Jupiter and warm Neptune exoplanet atmospheres at solar and enriched metallicities. Our results show for HD 189733b-like hot Jupiters that HOPO, PO, and P 2 are typically the dominant P carriers at pressures important for transit and emission spectra, rather than PH 3 . For GJ1214b-like warm Neptune atmospheres our results suggest that at solar metallicity PH 3 is dominant in the absence of photochemistry, but is generally not in high abundance for all other chemical environments. At 10 and 100 times solar, small oxygenated phosphorus molecules such as HOPO and PO dominate for both thermochemical and photochemical simulations. The network is able to reproduce well the observed PH 3 abundances on Jupiter and Saturn. Despite progress in improving the accuracy of the PHO network, large portions of the reaction rate data remain with approximate, uncertain, or missing values, which could change the conclusions of the current study significantly. Improving understanding of the kinetics of phosphorus-bearing chemical reactions will be a key undertaking for astronomers aiming to detect phosphine and other phosphorus species in both rocky and gaseous exoplanetary atmospheres in the near future.

atmospheric composition↗
DOE OSTI2026

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

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

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