Precise Control of Cu Nanoparticle Size and Catalytic Activity through Pore Templating in Zr Metal-Organic Frameworks
Abstract not provided
Mian, Mohammad Rasel↗
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Electric currents and coronal heating in NOAA active region 6952
We examine the spatial and temporal relationship between coronal structures observed with the soft X-ray telescope (SXT) on board the Yohkoh spacecraft and the vertical electric current density derived from photospheric vector magnetograms obtained using the Stokes Polarimeter at the Mees Solar Observatory. We focus on a single active region: AR 6952 which we observed on 7 days during 1991 December. For 11 independent maps of the vertical electric current density co-aligned with non-flaring X-ray images, we search for a morphological relationship between sites of high vertical current density in the photosphere and enhanced X-ray emission in the overlying corona. We find no compelling spatial or temporal correlation between the sites of vertical current and the bright X-ray structures in this active region.
Metcalf, T. R.↗
Photochemical CO 2 Reduction Using Rhenium(I) Tricarbonyl Complexes with Bipyridyl-Type Ligands with and without Second Coordination Sphere Effects
In this study, the effect of phenyl, phenol, aniline, amino, and CF 3 substituents of the 2,2'-bipyridine ligand in fac-ReCl(L)(CO) 3 (L=2,2'-bipyridine derivative) catalysts on photochemical CO 2 reduction in dimethylacetamide is examined, in order to understand the structure-function relationships and to compare the catalytic activities with the previously published electrochemical results. All complexes including ReCl(bpy)(CO) 3 have similar excited-state lifetimes and emission spectra, but complex 1 with the Ph-NH 2 moiety exhibits a significantly larger molar absorption coefficient for its metal-to-ligand charge transfer (MLCT) band. All complexes we tested produce CO with only a negligible amount of H 2 and formate in self-sensitized systems in the presence of triethanolamine (TEOA) and in some cases, BIH (1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]-imidazole). The presence of the Ph-NH 2 moiety (complex 1) has a beneficial effect on both electrochemical and photochemical activity, allowing a turnover number (TON) of 32 and 120 for photochemical CO production (without and with BIH, respectively). In the case of the Ph-OH group in the second coordination sphere (complexes 4 and 6), these complexes are active for photochemical CO 2 reduction, despite the formation of a stable 6-coordinate Re-OPh intermediate via reductive deprotonation as previously observed under electrochemical conditions. Overall, BIH accelerates the rate of formation of the one-electron reduced species (OERS) of the Re catalysts and allows higher turnover frequency (TOF) and TON for CO formation. The X-ray structures of complexes 1 and 4 were determined to have distorted octahedral Re centres, and show π-π stacking interactions with neighboring molecules as well as intramolecular hydrogen bonds to the internal chloride ligands. The unusually high absorptivity of the MLCT absorption of complex 1 has been explained by TD-DFT calculations.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
The Estimation Surface Latent Heat Flux Over the Ocean and its Relationship to Marine Atmospheric Boundary Layer (MABL) Structure
A new technique combining active and passive remote sensing instruments for the estimation of surface latent heat flux over the ocean is presented. This synergistic method utilizes aerosol lidar backscatter data, multi-channel infrared radiometer data and microwave scatterometer data acquired onboard the NASA P-3B research aircraft during an extended field campaign over the Atlantic ocean in support of the Lidar In-space Technology Experiment (LITE) in September of 1994. The 10 meter wind speed derived from the scatterometers and the lidar-radiometer inferred near-surface moisture are used to obtain an estimate of the surface flux of moisture via bulk aerodynamic formulae. The results are compared with the Special Sensor Microwave Imager (SSM/I) daily average latent heat flux and show reasonable agreement. However, the SSM/I values are biased high by about 30 W/sq m. In addition, the MABL height, entrainment zone thickness and integrated lidar backscatter intensity are computed from the lidar data and compared with the magnitude of the surface fluxes. The results show that the surface latent heat flux is most strongly correlated with entrainment zone top, bottom and the integrated MABL lidar backscatter, with corresponding correlation coefficients of 0.62, 0.67 and 0.61, respectively.
Palm, Stephen P.↗
The Estimation of Surface Latent Heat Flux Over the Ocean and its Relationship to Marine Atmospheric Boundary Layer (MABL) Structure
A new technique combining active and passive remote sensing instruments for the estimation of surface latent heat flux over the ocean is presented. This synergistic method uses aerosol lidar backscatter data, multi-channel infrared radiometer data and microwave scatterometer data acquired onboard the NASA P-3B research aircraft during an extended field campaign over the Atlantic ocean in support of the Lidar In-space Technology Experiment (LITE) in September of 1994. The 10 meter wind speed derived from the scatterometers and the lidar-radiometer inferred near-surface moisture are used to obtain an estimate of the surface flux of moisture via bulk aerodynamic formulae. The results are compared with the Special Sensor Microwave Imager (SSM/I) daily average latent heat flux and show reasonable agreement with an rms error and bias of about 50 and 25 W per square meters, respectively. In addition, the MABL height, entrainment zone thickness and integrated lidar backscatter intensity are computed from the lidar data and compared with the magnitude of the surface fluxes. The results show that the surface latent heat flux is most strongly correlated with entrainment zone top, bottom and the integrated MABL lidar backscatter, with corresponding correlation coefficients of 0.62, 0.67 and 0.61, respectively.
Palm, Stephen P.↗
The Estimation of Surface Latent Heat Flux over the Ocean and its Relationship to Marine Atmospheric Boundary Layer (MABL) Structure
A new technique combining active and passive remote sensing instruments for the estimation of surface latent heat flux over the ocean is presented. This synergistic method utilizes aerosol lidar backscatter data, multi-channel infrared radiometer data, and microwave scatterometer data acquired onboard the NASA P-313 research aircraft during an extended field campaign over the Atlantic ocean in support of the Lidar In-space Technology Experiment (LITE) in September of 1994. The 10 meter wind speed derived from scatterometers and lidar-radiometer inferred near-surface moisture are used to obtain an estimate of the surface flux of moisture via a bulk aerodynamic formula. The results are compared with the Special Sensor Microwave Imager (SSM/I) daily average latent heat flux and show reasonable agreement. However, the SSM/I values are biased low by about 15 W/sq m. In addition, the Marine Atmospheric Boundary Layer (MABL) height, entrainment zone thickness and integrated lidar backscatter intensity are computed from the lidar data and compared with the magnitude of the surface fluxes. The results show that the surface latent heat flux is most strongly correlated with entrainment zone depth, MABL height and the integrated MABL lidar backscatter, with corresponding correlation coefficients of 0.39, 0.43 and 0.71, respectively.
Palm, Stephen P.↗
Elucidation of the physical factors that control activated transport of penetrants in chemically complex glass-forming liquids
Understanding the activated transport of penetrant or tracer atoms and molecules in condensed phases is a challenging problem in chemistry, materials science, physics, and biophysics. Many angstrom- and nanometer-scale features enter due to the highly variable shape, size, interaction, and conformational flexibility of the penetrant and matrix species, leading to a dramatic diversity of penetrant dynamics. Based on a minimalist model of a spherical penetrant in equilibrated dense matrices of hard spheres, a recent microscopic theory that relates hopping transport to local structure has predicted a novel correlation between penetrant diffusivity and the matrix thermodynamic dimensionless compressibility, S 0 ( T ) (which also quantifies the amplitude of long wavelength density fluctuations), as a consequence of a fundamental statistical mechanical relationship between structure and thermodynamics. Moreover, the penetrant activation barrier is predicted to have a factorized/multiplicative form, scaling as the product of an inverse power law of S 0 ( T ) and a linear/logarithmic function of the penetrant-to-matrix size ratio. This implies an enormous reduction in chemical complexity that is verified based solely on experimental data for diverse classes of chemically complex penetrants dissolved in molecular and polymeric liquids over a wide range of temperatures down to the kinetic glass transition. The predicted corollary that the penetrant diffusion constant decreases exponentially with inverse temperature raised to an exponent determined solely by how S 0 ( T ) decreases with cooling is also verified experimentally. Our findings are relevant to fundamental questions in glassy dynamics, self-averaging of angstrom-scale chemical features, and applications such as membrane separations, barrier coatings, drug delivery, and self-healing.
Science & Technology - Other Topics↗
Relationship between the radioemission flux from local sources in the sun with the structure of the optically observed active regions
Solar radiation analysis using radio astronomy observations
RADIO ASTRONOMY↗
Significant Centers of Tectonic Activity as Identified by Wrinkle Ridges for the Western Hemisphere of Mars
The western hemisphere region of Mars has been the site of numerous scientific investigations regarding its tectonic evolution. For this region of Mars, the dominant tectonic region is the Tharsis province. Tharsis is characterized by an enormous system of radiating grabens and a circumferential system of wrinkle ridges. Past investigations of grabens associated with Tharsis have identified specific centers of tectonic activity. A recent structural analysis of the western hemisphere region of Mars which includes the Tharsis region, utilized 25,000 structures to determine the history of local and regional centers of tectonic activity based primarily on the spatial and temporal relationships of extensional features. This investigation revealed that Tharsis is more structurally complex (heterogeneous) than has been previously identified: it consists of numerous regional and local centers of tectonic activity (some are more dominant and/or more long lived than others). Here we use the same approach as Anderson et al. to determine whether the centers of tectonic activity that formed the extensional features also contributed to wrinkle ridge (compressional) formation.
Anderson, R.C.↗
Metal oxide-promoted calcium cuprate catalysts for diol oxidative dehydrocyclization to lactones
Here, this work investigates structure-function relationships in electronically tunable, redox-active, basic Cu-Ca mixed metal oxide catalysts for oxidative dehydrocyclization of liquid diols to lactones. Compositional screening identified Ni 2+ and Zn 2+ as effective promoters that increase the surface Cu 2+ population by ∼1.7× and Cu-normalized activity for liquid 1,4-butanediol conversion to γ-butyrolactone by ∼3–4×. In situ Raman spectroscopy, in situ X-ray absorption spectroscopy (XAS), in situ diffuse-reflectance Fourier transform infrared spectroscopy (DRIFTS), ex situ X-ray diffraction (XRD), and H 2 -temperature-programmed reduction (H 2 -TPR) show that Ni 2+ or Zn 2+ incorporation promotes the formation of Ca 0.82 Cu 1.00 O 2 nanoparticles under mild calcination conditions. This cuprate phase features stronger and shorter Cu–O bonds (1.90 Å) than inactive bulk CuO (1.95 Å) and square-planar Cu 2+ O 4 sites with enhanced d z2 electrophilicity, strengthening alkoxy adsorption. Pyridine-DRIFTS confirms the purely basic nature of the catalyst surface, while methanol-DRIFTS indicates Cu 2+ surface enrichment with Ni or Zn promotion, where Cu–O(Ca)–Cu sites can exist as amorphous domains or a truncation layer on crystalline nanoparticles.
09 BIOMASS FUELS↗
Operando methods: A new era of electrochemistry
One of the grand challenges facing electrochemistry is to directly resolve the complex nature of (electro)catalyst active sites and capture real-time “movies” of reaction dynamics, i.e. “watching chemistry in action”. The need for such fundamental understanding has stimulated the development of operando/in situ methods, which have greatly enhanced our ability to identify activity descriptors of electrocatalysts and establish structure–property relationships of energy materials. Here, this review summarizes the frontiers of operando electrochemical liquid-cell scanning transmission electron microscopy and correlative synchrotron X-ray methods, which are complementary tools to comprehensively investigate reaction dynamics across multiple spatiotemporal scales. In an effort to encourage greater adoption of advanced operando methods by the general electrochemistry community, this review points out the need to benchmark electrochemistry in confined and heterogenous liquid environment with minimal beam-induced damage. We anticipate that multimodal operando methods will become indispensable for understanding interfacial reaction mechanisms for the broad chemistry and energy materials communities.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Catalytic oxidative coupling of arenes and alkanes: applications for efficient chemical synthesis and for hydrocarbon oligomerization. Progress Report 2016-7. Final report
This is the final report for DE-FG02-08ER15997 with a grant period of 8/15/2008-8/14/2018 (plus 1 year NCE); Program: Basic Energy Sciences; PI: Melanie S. Sanford; co-PI: Adam J. Matzger. The project resulted in 20 publications, 12 supported entirely by this grant and 8 supported substantially by this grant. The overall goals of this project were design catalysts (both homogeneous catalysts and MOF-supported catalysts) to control reactivity and selectivity in energy relevant C–H bond functionalization reactions. The proposed research led to a variety of new catalysts and catalytic processes which are currently finding application in organic synthesis. These efforts were well aligned with the goals of the DOE BES Catalysis Science Program. C–H functionalization reactions have extensive applications in energy-related industries, including petroleum and biofuels processing. The research activities also matched many of the priority areas identified by the Catalysis Science Program, including: investigating problems at the interface of heterogeneous and homogeneous catalysis as a means to derive new catalysts; incorporating 2° interactions to modulate catalyst stability, reactivity, and selectivity; using these new catalysts to tune molecular-level catalytic activity and selectivity; and studying structure-reactivity relationships of inorganic, organic, or hybrid catalytic materials in solution.
02 PETROLEUM↗
Development of Hybrid Product Breakdown Structure for NASA Ground Systems
The Product Breakdown Structure is traditionally a method of identification of the products of a project in a tree structure. It is a tool used to assess, plan, document, and display the equipment requirements for a project. It is part of a product based planning technique, and attempts to break down all components of a project in as much detail as possible, so that nothing is overlooked. The PBS for ground systems at the Kennedy Space Center is being developed to encompass the traditional requirements including the alignment of facility, systems, and components to the organizational hierarchy. The Ground Operations Product Breakdown Structure is a hybrid in nature in that some aspects of a work breakdown structure will be incorporated and merged with the Architecture Concept of Operations, Master Subsystem List, customer interface, and assigned management responsibility. The Ground Operations Product Breakdown Structure needs to be able to identify the flexibility of support differing customers (internal and external) usage of ground support equipment within the Kennedy Space Center launch and processing complex. The development of the Product Breakdown Structure is an iterative activity Initially documenting the organization hierarchy structure and relationships. The Product Breakdown Structure identifies the linkage between the customer program requirements, allocation of system resources, development of design goals, and identification logistics products. As the Product Breakdown Structure progresses the incorporation of the results of requirement planning for the customer occurs identifying facility needs and systems. The mature Product Breakdown Structure is baselined with a hierarchical drawing, the Product Breakdown Structure database, and an associated document identifying the verification of the data through the life cycle of the program/product line. This paper will document, demonstrate, and identify key aspects of the life cycle of a Hybrid Product Breakdown Structure. The purpose is to show how a project management and system engineering approach can be utilized for providing flexible customer service in an evolving manned space flight launch processing environment.
Monaghan, Mark W.↗
Development of Hybrid Product Breakdown Structure for NASA Ground Systems
The Product Breakdown Structure is traditionally a method of identification of the products of a project in a tree structure. It is a tool used to assess, plan, document, and display the equipment requirements for a project. It is part of a product based planning technique, and attempts to break down all components of a project in as much detail as possible, so that nothing is overlooked. The PBS for ground systems at the Kennedy Space Center is being developed to encompass the traditional requirements including the alignment of facility, systems, and components to the organizational hierarchy. The Ground Operations Product Breakdown Structure is a hybrid in nature in that some aspects of a work breakdown structure will be incorporated and merged with the Architecture Concept of Operations, Master Subsystem List, customer interface, and assigned management responsibility. The Ground Operations Product Breakdown Structure needs to be able to identify the flexibility of support differing customers (internal and external) usage of ground support equipment within the Kennedy Space Center launch and processing complex. The development of the Product Breakdown Structure is an iterative activity Initially documenting the organization hierarchy structure and relationships. The Product Breakdown Structure identifies the linkage between the customer program requirements, allocation of system resources, development of design goals, and identification logistics products. As the Product Breakdown Structure progresses the incorporation of the results of requirement planning for the customer occurs identifying facility needs and systems. The mature Product Breakdown Structure is baselined with a hierarchical drawing, the Product Breakdown Structure database, and an associated document identifying the verification of the data through the life cycle of the program/product line. This paper will document, demonstrate, and identify key aspects of the life cycle of a Hybrid Product Breakdown Structure. The purpose is to show how a project management and system engineering approach can be utilized for providing flexible customer service in an evolving manned space flight launch processing environment.
Monaghan, Mark W.↗
Simulation of an array-based neural net model
Research in cognitive science suggests that much of cognition involves the rapid manipulation of complex data structures. However, it is very unclear how this could be realized in neural networks or connectionist systems. A core question is: how could the interconnectivity of items in an abstract-level data structure be neurally encoded? The answer appeals mainly to positional relationships between activity patterns within neural arrays, rather than directly to neural connections in the traditional way. The new method was initially devised to account for abstract symbolic data structures, but it also supports cognitively useful spatial analogue, image-like representations. As the neural model is based on massive, uniform, parallel computations over 2D arrays, the massively parallel processor is a convenient tool for simulation work, although there are complications in using the machine to the fullest advantage. An MPP Pascal simulation program for a small pilot version of the model is running.
Barnden, John A.↗
A morphological study of waves in the thermosphere using DE-2 observations
Theoretical model and data analysis of DE-2 observations for determining the correlation between the neutral wave activity and plasma irregularities have been presented. The relationships between the observed structure of the sources, precipitation and joule heating, and the fluctuations in neutral and plasma parameters are obtained by analyzing two measurements of neutral atmospheric wave activity and plasma irregularities by DE-2 during perigee passes at an altitude on the order of 300 to 350 km over the polar cap. A theoretical model based on thermal nonlinearity (joule heating) to give mode-mode coupling is developed to explore the role of neutral disturbance (winds and gravity waves) on the generation of plasma irregularities.
Gross, S. H.↗
Machine-Learned Structure-Property Relationship in Metallic Glasses (Final Report)
The goal of the proposed work was to gain the ability to predict properties from the known coordinates (relative positions) of atoms in a metallic glass, presuming that information about which regions of the glass are fertile for rearrangment (defects) are encoded in this structural information. This goal is important to the science of metallic glasses. This research of applied machine learning methods to automate the development of a relationship between structural measures and thermally and stress-activated events in the metallic glass. In this way, the work aimed to building a bridge between structure and properties for this class of materials. The work is expected to have timely impact on guiding the tuning of internal structures of metallic glasses for desired properties. It also represents an advance in applying machine learning techniques to discerning the properties of materials.
36 MATERIALS SCIENCE↗
Active regions and the interplanetary magnetic field.
Solar active region relationship to large scale sector interplanetary field structure
Ness, N. F.↗