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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 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Synthesis and Structure–Activity Characterization of a Single-Site MoO 2 Catalytic Center Anchored on Reduced Graphene Oxide

Molecularly derived single-site heterogeneous catalysts can bridge the understanding and performance gaps between conventional homogeneous and heterogeneous catalysis, guiding the rational design of next-generation catalysts. While impressive advances have been made with well-defined oxide supports, the structural complexity of other supports and the nature of the grafted surface species present an intriguing challenge. In this study, single-site Mo(=O) 2 species grafted onto reduced graphene oxide (rGO/MoO 2 ) are characterized by XPS, DRIFTS, powder XRD, N 2 physisorption, NH 3 -TPD, aqueous contact angle, active site poisoning assay, Mo EXAFS, model compound single-crystal XRD, DFT, and catalytic performance. NH 3 -TPD reveals that the anchored MoO 2 moiety is not strongly acidic, while Mo 3d 5/2 XPS assigns the oxidation state as Mo(VI), and XRD shows little rGO periodicity change on MoO 2 grafting. Contact angle analysis shows that MoO 2 grafting consumes rGO surface polar groups, yielding a more hydrophobic surface. The rGO/MoO 2 DRIFTS assigns features at 959 and 927 cm –1 to the symmetric and antisymmetric Mo=O stretching modes, respectively, of an isolated cis-(O=Mo=O) moiety, in agreement with DFT computation. Moreover, the Mo EXAFS rGO/MoO 2 structural data are consistent with isolated (C–O) 2– Mo(=O) 2 species having two Mo=O bonds and two Mo–O bonds at distances of 1.69(3) and 1.90(3) Å, respectively. rGO/MoO 2 is also more active than the previously reported AC/MoO 2 catalyst, with reductive carbonyl coupling TOFs approaching 1.81 × 10 3 h –1 . rGO/MoO 2 is environmentally robust and multiply recyclable with 69 ± 2% of the Mo sites catalytically significant. Altogether, rGO/MoO 2 is a structurally well-defined and versatile single-site Mo(VI) dioxo heterogeneous catalytic system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Modulating the dynamics of Brønsted acid sites on PtWOx inverse catalyst

Here metal-metal oxide (M-MO) inverse catalysts are broadly applied. Brønsted acid sites on the oxide overlayers are often hypothesized to drive selective C-O bond activation. However, the Brønsted acid site nature and dynamics under working conditions remain poorly understood due to multiple materials functionalities. Here, we investigate the formation and the dynamics of Brønsted acid and redox sites on PtWO x /C under working conditions. DFT-based thermodynamic calculations and microkinetic modeling reveal a complex interplay between Brønsted acid and redox sites and potentially fast catalyst dynamics at comparable time scales to the chemistry. Combining in situ characterization and probe chemistry, we demonstrate that the density of Brønsted acid sites on the PtWO x /C inverse catalyst could be modulated by up to two orders of magnitude by altering the reaction parameters and by the chemistry itself. We elicit an order of magnitude increase in the acid-catalyzed dehydration average reaction rate by periodic hydrogen pulsing.

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

Mechanistic studies of NH 3 -assisted reduction of mononuclear Cu(ii) cation sites in Cu-CHA zeolites

Cu-Exchanged zeolites catalyze various redox reactions including the selective catalytic reduction (SCR) of NO x with NH 3 and the partial oxidation of hydrocarbons. The reduction of Cu(II) cations to Cu(I) by NH 3 alone has been observed experimentally, yet fundamental details regarding the Cu active site requirements, reaction stoichiometry, and reaction mechanism remain incompletely understood. Here, we synthesized model Cu-exchanged chabazite (Cu-CHA) zeolites with varying Cu ion densities and distributions of mononuclear Cu(II) ion site types (Cu 2+ , (CuOH) + ) and studied NH 3 -assisted Cu(II) reduction reactions using a combination of spectroscopic, titrimetric, and gas-phase product analysis methods. In situ UV-visible and X-ray absorption spectroscopies were used to monitor and quantify the transient reduction of Cu(II) to Cu(I) during exposure to NH 3 (473 K), in concert with titration methods that use NO and NH 3 co-reductants to fully reduce to the Cu(I) state any residual Cu(II) ions that remained after treatments in NH 3 alone for a given time period. The techniques provide quantitative evidence that both mononuclear Cu(II) site types are able to reduce in NH 3 alone, and do so to similar extents as a function of time. NH 3 temperature programmed reduction (TPR) revealed that the reaction stoichiometry of NH 3 -assisted reduction forms approximately one equivalent of N 2 per 6 Cu sites, regardless of Cu speciation or density, consistent with a six-electron reduction process whereby two NH 3 molecules react with six Cu(II) species to produce one N 2 molecule and six Cu(I) species. Furthermore, these findings provide new insights into the reaction pathways and mechanisms by which NH 3 alone reduces mononuclear Cu(II) sites in zeolites, which are undesired side-reactions that occur during steady-state NO x SCR and can unintentionally influence SCR-relevant spectroscopic or titrimetric characterization experiments.

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

Appropriateness and Readiness of Cold Crucible Vitrification of Calcine Solids at the Idaho Site and H-Canyon Effluent at the Savannah River Site

This report summarizes the results from an assessment of the technology readiness and deployment of cold crucible induction melter (CCIM) technology to vitrify high level waste (HLW) calcine solids at the Idaho Site and H-Canyon liquid effluent at the Savannah River Site (SRS). The assessment was requested by the Department of Energy’s Office of Environmental Management (DOE-EM), but is not a DOE 413-3-4a assessment for technology deployment. A joint Savannah River National Laboratory (SRNL) and Fluor Idaho Cleanup Project (ICP) team with subject matter experts evaluated the existent literature and experience both within the DOE as well as relevant external experience. The technology assessment focused on the site-specific technology readiness and appropriateness based on a number of system factors including feasibility and appropriateness of the technology for the specific site application, the potential extent of the regulatory and design challenges, and evaluation of the ability to deploy within the treatment needs of each site. This initial assessment provides information to support DOE-EM in making a go/no-go decision to carry out additional work on the technology maturation for critical decisions and planning.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Hanford Site Composite Analysis: Comparison of One- and Three-Dimensional Simulation of Vadose Zone Transport and Transfer to Groundwater for Selected Waste Sites

The purpose of this document is to compare 1D and 3D technetium-99 (Tc-99) VZ transport and transfer rates to groundwater for five selected waste sites (two tanks, two cribs, and one trench) to demonstrate the need to consider 3D flow and transport mechanisms and commingling of contaminant plumes originating from adjacent waste sites. The waste sites selected for the comparison evaluation are the 241-A-105 Tank in the A Farms Area model, the 216-B-18 Crib and the 216-B-25 Trench in the BC Cribs and Trenches model, the 216-B-49 Crib in the B Complex model, and the 241-SX-115 Tank in the S Farms Area model. The selected waste sites all represent different disposal or leak conditions, with and without potential impacts due to release-fluid commingling, occurring at the Hanford Site Central Plateau.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

Streamlined Approach for Environmental Restoration (SAFER) Plan for Corrective Action Unit 578: Miscellaneous Inactive Sites Nevada National Security Site, Nevada, (Rev. 0)

This Streamlined Approach for Environmental Restoration (SAFER) Plan addresses the actions needed to achieve closure for Corrective Action Unit (CAU) 578, Miscellaneous Inactive Sites, identified in the Federal Facility Agreement and Consent Order (FFACO). CAU 578 comprises the following 11 corrective action sites (CASs) located in Areas 2, 3, 4, 6, 7, 12, and 23 of the Nevada National Security Site: • 02-26-01, Lead (Concrete Box w/Lining) • 02-26-07, Gun Turret w/Lead in Barrel • 03-16-01, U-3auS Disposal Site • 04-26-02, Lead on Instrument Bunker • 06-99-07, Sump • 07-99-01, Miscellaneous Debris • 12-02-11, UST-P-2 • 12-06-01, Muckpile • 12-06-04, Muckpile • 23-12-01, Boiler (2) • 23-99-04, Salvage Yard This plan provides the methodology for field activities needed to gather the necessary information for closing each CAS. There is sufficient information and process knowledge from historical documentation and investigations of similar sites regarding the expected nature and extent of potential contaminants to recommend closure of CAU 578 using the SAFER process. Additional information will be obtained by conducting a field investigation before selecting the appropriate corrective action for each CAS. The results of the field investigation will support a defensible recommendation that no further corrective action is necessary. This will be presented in a closure report that will be prepared and submitted to the Nevada Division of Environmental Protection (NDEP) for review and approval.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Tropopause Characteristics Based on Long-Term ARM Radiosonde Data: A Fine-Scale Comparison at the Extratropical SGP Site and Arctic NSA Site

The variations in the characteristics of the tropopause are sensitive indicators for the climate system and climate change. By using Atmospheric Radiation Measurement (ARM) radiosonde data that were recorded at the extratropical Southern Great Plains (SGP) and Arctic North Slope of Alaska (NSA) sites over an 18-year period (January 2003 to December 2020), this study performs a fine-scale comparison of the climatological tropopause features between these two sites that are characterized by different climates. The static stability increases rapidly above the tropopause at both sites, indicating the widespread existence of a tropopause inversion layer. The structures of both the tropopause inversion layer and the stability transition layer are more obvious at NSA than at SGP, and the seasonal variation trends of the tropopause inversion layer and stability transition layer are distinctly different between the two sites. A fitting method was used to derive the fitted tropopause height and tropopause sharpness (λ). Although this fitting method may determine a secondary tropopause rather than the primary tropopause when multiple tropopause heights are identified on one radiosonde profile, the fitted tropopause heights generally agree well with the observed tropopause heights. Broad tropopause sharpness values (λ > 2 km) occur more frequently at SGP than at NSA, resulting in a greater average tropopause sharpness at SGP (1.0 km) than at NSA (0.6 km). Significant positive trends are exhibited by the tropopause heights over the two sites, with rates of increase of 23.7 ± 6.5 m yr ⁻1 at SGP and 28.0 ± 4.0 m yr ⁻1 at NSA during the study period.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Session 077 - Panel: Wednesday US DOE Featured Site: Lexington, KY Office (Portsmouth and Paducah Sites) (R1.14)

This panel featured the DoE's Portsmouth Paducah Project Office (PPPO), which is responsible for the management and cleanup of at the Portsmouth, Ohio and Paducah, Kentucky former Gaseous Diffusion Plant sites. Portsmouth is primed for the first major skyline change at the site the upcoming demolition of the X-326 process building and initial operations of the Onsite Waste Disposal Facility. The Paducah site is working on the C-400 city block initiative allowing DOE to tackle the main source of groundwater contamination at the site, in conjunction with deactivation and demolition of the C-400 Cleaning Building. PPPO's DUF6 conversion plants have 7 lines in continuous operation at both sites providing the opportunity to ramp up cylinder processing. Panelists with presentations: DOE PPO Update (Robert Edwards, Joel Bradburne); Portsmouth/Paducah Project Office (PPPO) (Joel Bradburne, Robert Edwards); PADUCAH (Jennifer Woodard, Myrna Espinosa Redfield); Depleted Uranium Hexafluoride Conversion Project (Reinhard Knerr, Zack Smith); Paducah Deactivation and Remediation Project (Myrna Espinosa Redfield); Mid-America Conversion Services - Seven Lines One Project (Zack Smith)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Effects of penta‐coordinated Al 3+ sites and Ni defective sites on Ni/ Al 2 O 3 for CO methanation

Abstract Engineering sophisticated structure of Al 2 O 3 and controlling the structure of counterpart metal active sites remain challenges to achieve a high catalytic‐performance in heterogeneous catalysis. Herein, we present a confinement strategy to stabilize homogeneous Ni by penta‐coordinated Al 3+ anchoring sites in Al 2 O 3 . This approach is involved in using a metal–organic framework as host to load Ni 2+ ions, by the aim of producing a confined Ni/Al 2 O 3 catalyst after a standard calcination. Metal–support interaction between Ni and Al 2 O 3 was tailored to be medium to avoid the formation of inactive NiAl 2 O 4 , which favors the generation of more available Ni active sites accessible to the reactants. The resultant Ni/Al 2 O 3 exhibited superior catalytic performance in comparison with the control Ni/Al 2 O 3 in CO methanation owing to the presence of defective sites on sufficient Ni 0 surface. Furthermore, the presence of oxygen vacancies on Al 2 O 3 and hydrogen spillover contributed toward excellent coke resistance properties in the reaction.

Engineering↗
DOE OSTI2023

Tuning Active Site Flexibility by Defect Engineering of Graphene Ribbon Edge‐hosted Fe−N 3 Sites

Abstract Nitrogen‐doped, carbon‐supported transition metal catalysts are excellent for several reactions. Structural engineering of M−N x sites to boost catalytic activity is rarely studied. Here, we demonstrate that the structural flexibility of Fe−N 3 site is vital for tuning the electronic structure of Fe atoms and regulating the catalytic transfer hydrogenation (CTH) activity. By introducing carbon defects, we construct Fe−N 3 sites with varying Fe−N bond lengths distinguishable by X‐ray absorption spectroscopy. We investigate the CTH activity by density‐functional theory and microkinetic calculations and reveal that the vertical displacement of the Fe atom out of the plane of the support, induced by the Fe−N 3 distortion, raises the Fe orbital and strengthens binding. We propose that the activity is controlled by the relaxation of the reconstructed site, which is further affected by Fe−N bond length, an excellent activity descriptor. We elucidate the origin of the CTH activity and principles for high‐performing Fe−N−C catalysts by defect engineering.

Yang, Piaoping↗