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DOE OSTI2021

Results of the CHF-SERTTA In-Pile Transient Boiling Experiments at TREAT

To advance the current understanding of heat transfer between nuclear fuel rod cladding and the surrounding coolant under transient scenarios involving critical heat flux (CHF), the CHF-Static Environment Rodlet Transient Test Apparatus (CHFSERTTA), an in-pile experiment, was developed for and irradiated in the Transient Reactor Test (TREAT) facility at Idaho National Laboratory. The CHF-SERTTA experiment consists of a hollow, borated stainless steel rod submerged in a static water pool. The rod, heated via the (n, a) reaction in boron-10, was designed for investigating in-pile transient heat transfer between the rod surface and the coolant, avoiding the complexity of including the heat transfer between the fuel, gas gap, and cladding in typical light-water reactor (LWR) fuel rods. The instrumentation package for CHF-SERTTA focused on capturing those data that best describe the heat transfer behaviour between the rod and coolant. This paper outlines the CHFSERTTA experiment design and presents the initial results of the experiment campaign.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2017

Theoretical modeling of the interaction of phenylacetylene and styrene molecules with Pd{111}

The DFT-PBE method was used to calculate the structural and energy characteristics of all possible adsorption complexes of phenylacetylene (PA) and styrene (St) molecules with the Pd{111} surface. According to the calculations, the acetylene group of the PA molecule in the energetically preferred complexes is bound to three or four Pd atoms and the plane of the phenyl ring is parallel to the Pd surface. In the case of deficiency of fcc sites, the phenyl ring of the PA molecule is displaced from the Pd{111} surface. The number of Pd atoms required for the compact adsorption of two PA molecules is the same as that for the adsorption of one St molecule.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Absolute Molecular Orientation of Isopropanol at Ceria (100) Surfaces: Insight into Catalytic Selectivity from the Interfacial Structure

The initial mechanistic steps underlying heterogeneous chemical catalysis can be described in a framework where the composition, structure, and orientation of molecules adsorbed to reactive interfaces are known. However, extracting this vital information is the limiting step in most cases due in part to challenges in probing the interfacial monolayer with enough chemical specificity to characterize the surface molecular constituents. These challenges are exacerbated at complex or spatially heterogeneous interfaces where competing processes and a distribution of local environments can uniquely drive chemistry. To address these limitations, this work presents a distinctive combination of materials synthesis, surface specific optical experiments, and theory to probe and understand molecular structure at catalytic interfaces. Specifically, isopropanol was adsorbed to surfaces of the model CeO 2 catalyst that were synthesized with only the (100) facet exposed. Vibrational sum-frequency generation was used to probe the molecular monolayer, and with the guidance of density functional theory calculations, was used to extract the structure and absolute molecular orientation of isopropanol at the CeO 2 (100) surface. Our results show that isopropanol is readily deprotonated at the surface, and through the measured absolute molecular orientation of isopropanol, we obtain new insight into the selectivity of the (100) surface to form propylene. Our findings reveal key insight into the chemical and physical phenomena taking place at pristine interfaces thereby pointing to intuitive structural arguments to describe catalytic selectivity in more complex systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2001

Odyssey Comet Nucleus Orbiter: The Next Step in Cometary Exploration

Cometary nuclei are the most primitive bodies in the solar system, containing a cosmo-chemical record of the primordial solar nebula. Flyby missions to comets, such as those that encountered Comet Halley in 1986, provide a glimpse at this record. However, to study a cometary nucleus in detail requires a rendezvous mission, i.e., a nucleus orbiter. Only an orbiter provides the ability to map the entire nucleus surface at high resolution, to study the complex chemistry in the cometary coma and its variation with time, and to determine the mass and bulk density of the nucleus, key parameters in understanding how small bodies first formed in the solar nebula. A nucleus orbiter also provides the opportunity to sense the nucleus surface in preparation for more ambitious landing and sample return missions in the future. Additional information is contained in the original extended abstract.

Weissman, P. R.↗

DOE OSTI2024

Hidden non-collinear spin-order induced topological surface states

Abstract Rare-earth monopnictides are a family of materials simultaneously displaying complex magnetism, strong electronic correlation, and topological band structure. The recently discovered emergent arc-like surface states in these materials have been attributed to the multi-wave-vector antiferromagnetic order, yet the direct experimental evidence has been elusive. Here we report observation of non-collinear antiferromagnetic order with multiple modulations using spin-polarized scanning tunneling microscopy. Moreover, we discover a hidden spin-rotation transition of single-to-multiple modulations 2 K below the Néel temperature. The hidden transition coincides with the onset of the surface states splitting observed by our angle-resolved photoemission spectroscopy measurements. Single modulation gives rise to a band inversion with induced topological surface states in a local momentum region while the full Brillouin zone carries trivial topological indices, and multiple modulation further splits the surface bands via non-collinear spin tilting, as revealed by our calculations. The direct evidence of the non-collinear spin order in NdSb not only clarifies the mechanism of the emergent topological surface states, but also opens up a new paradigm of control and manipulation of band topology with magnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS2011

Signatures of Chemical Evolution in Protostellar Nebulae

A decade ago observers began to take serious notice of the presence of crystalline silicate grains in the dust flowing away from some comets. While crystallinity had been seen in such objects previously, starting with the recognitions by Campins and Ryan (1990) that the 10 micron feature of Comet Halley resembled that of the mineral forsterite, most such observations were either ignored or dismissed as no path to explain such crystalline grains was available in the literature. When it was first suggested that an outward flow must be present to carry annealed silicate grains from the innermost regions of the Solar Nebula out to the regions where comets could form (Nuth, 1999; 2001) this suggestion was also dismissed because no such transport mechanism was known at the time. Since then not only have new models of nebular dynamics demonstrated the reality of long distance outward transport (Ciesla, 2007; 2008; 2009) but examination of older models (Boss, 2004) showed that such transport had been present but had gone unrecognized for many years. The most unassailable evidence for outward nebular transport came with the return of the Stardust samples from Comet Wild2, a Kuiper-belt comet that contained micron-scale grains of high temperature minerals resembling the Calcium-Aluminum Inclusions found in primitive meteorites (Zolensky et aI., 2006) that formed at T > 1400K. Now that outward transport in protostellar nebulae has been firmly established, a re-examination of its consequences for nebular gas is in order that takes into account both the factors that regulate both the outward flow as well as those that likely control the chemical composition of the gas. Laboratory studies of surface catalyzed reactions suggest that a trend toward more highly reduced carbon and nitrogen compounds in the gas phase should be correlated with a general increase in the crystallinity of the dust (Nuth et aI., 2000), but is such a trend actually observable? Unlike the Fischer-Tropsch or the Haber-Bosch reactions used in industry, the surface catalyzed reactions seen in our laboratory do not produce a simple product stream of methane or ammonia, respectively. Instead, such reactions produce a wide range of both aliphatic and aromatic hydrocarbons, as well as reduced nitrogen compounds such as ammonia, amines, amides and imides, as gas phase products together with a heavy, macromolecular, kerogen-like surface coating that remains on the grains. While CO and N2 will certainly be depleted by conversion into more complex and less volatile species via reaction on grain surfaces, it may be very difficult to monitor such changes from outside the system.

Nuth, Joseph A., III↗

DOE OSTI2020

Kinetics of low-temperature methane activation on IrO 2 (1 1 0): Role of local surface hydroxide species

The ability of the IrO 2 (1 1 0) surface to promote CH 4 activation at low temperatures (~150 K) suggests possibilities for developing IrO 2 -based catalysts to selectively convert light alkanes to high-value chemicals. In this study, we present experimental results and microkinetic simulations, based on density functional theory (DFT) calculations, of temperature programmed reaction spectra (TPRS) obtained for CH 4 σ-complexes adsorbed on IrO 2 (1 1 0), and focus on clarifying how surface OH groups modify the branching between CH 4 desorption, activation and subsequent reactions during TPRS. Our DFT results predict that surface OH groups strongly destabilize CH 4 σ-complexes on IrO 2 (1 1 0) in addition to deactivating surface O-atoms that are needed to achieve CH 4 activation at low temperature. We demonstrate that a microkinetic model that incorporates the influence of surface OH groups on the CH 4 binding and reactivity reproduces experimental TPRS results which show that adsorbed CH 4 σ-complexes preferentially dissociate at low CH 4 coverage, but that an increasing fraction of the adsorbed CH 4 desorbs at low temperature (~120 K) with increasing initial CH 4 or H coverage. The simulations reveal that low-temperature CH4 desorption during TPRS arises primarily from CH 4 σ-complexes that are kinetically-trapped between adjacent surface OH groups, and are thus destabilized and unable to access reactive O-atoms. In addition, when the effect of adjacent OH groups is incorporated we find that the PBE-D3 functional incorporating dispersion provides CH 4 binding energies that agree more closely with that obtained from the TPRS experiments. Overall, our results demonstrate that the local effect of adjacent OH groups must be incorporated into any microkinetic models to properly capture the selectivity between extensive and partial oxidation in alkane conversion on IrO 2 (1 1 0) under reaction conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Surface chemical defence of the eelgrass Zostera marina against microbial foulers

Plants rely on both mechanical and chemical defence mechanisms to protect their surfaces against microorganisms. The recently completed genome of the eelgrass Zostera marina , a marine angiosperm with fundamental importance for coastal ecosystems, showed that its re-adaptation from land to the sea has led to the loss of essential genes (for chemical communication and defence) and structural features (stomata and thick cuticle) that are typical of terrestrial plants. This study was designed to understand the molecular nature of surface protection and fouling-control strategy of eelgrass against marine epiphytic yeasts. Different surface extraction methods and comparative metabolomics by tandem mass spectrometry (LC-MS/MS) were used for targeted and untargeted identification of the metabolite profiles of the leaf surface and the whole tissue extracts. Desorption electrospray ionization-imaging mass spectrometry (DESI-IMS) coupled with traditional bioassays revealed, for the first time, the unique spatial distribution of the eelgrass surface-associated phenolics and fatty acids, as well as their differential bioactivity against the growth and settlement of epiphytic yeasts. This study provides insights into the complex chemical defence system of the eelgrass leaf surface. It suggests that surface-associated metabolites modulate biotic interactions and provide chemical defence and structural protection to eelgrass in its marine environment.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2017

Effect of reducible oxide–metal cluster charge transfer on the structure and reactivity of adsorbed Au and Pt atoms and clusters on anatase TiO 2

We carried out density functional theory calculations to study the influence of oxide–metal charge transfers on the structure, energetics, and reactivity of Au and Pt atoms, dimers, and trimers adsorbed on the (101) surface of reduced anatase TiO 2 . Pt clusters interact much more strongly with the TiO 2 support than Au clusters, and, with the exception of single Pt adatoms, generally behave as electron acceptors on reduced TiO 2 , whereas Au clusters can both accept and donate charge on the reduced surface. The reactivity of the supported clusters was probed by considering their interaction with CO and co-adsorbed O 2 . The effect of surface reduction on the interaction with CO is particularly significant when the CO adsorption site is an interfacial metal atom directly in contact with the TiO 2 surface and/or in the presence of co-adsorbed O 2 . Pt clusters interact strongly with co-adsorbed O 2 and form Pt–O 2 complexes that can easily accept electrons from reduced surfaces. In contrast, Au clusters donate charge to co-adsorbed O 2 even in the presence of excess electrons from a reduced support. In conclusion, the computed differences in the properties of the supported Pt and Au clusters are consistent with several experimental observations and highlight the important role of excess surface electrons in the behavior of supported metal catalysts on reducible oxides

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRSDate not supplied

Surface Systems and Interface Standardization

Space exploration on planetary surfaces will require the use of various surface systems which will likely need to interface with one another. These systems must communicate and share data, as well as distribute power and transfer fluids for sustainable surface operations. Such systems can range from landers, surface habitats, mobility systems, cargo, and In-Situ Resource Utilizations (ISRUs). Previous and current programs have developed space interoperability standards that help aid in reducing potential risks of interface integration. One example of this is the International Deep Space Interoperability Standards (IDSIS) which focuses on deep space exploration. A goal of the Artemis program is to develop a sustained human presence on the lunar surface that would be a training ground for future Mars exploration. Therefore, it will be beneficial to identify interface standards between the surface assets which will help mitigate risk and reduce complexity in the harsh environments of space exploration. A key contribution to sustainability is commonality between hardware and software interfaces. Generic interfaces for data, power, and fluids will reduce risk, promote interoperability, and define standard interfaces across surface exploration projects and programs. Standardized interfaces would be advantageous for improving efficiency and reducing overall complexity, which are critical considerations for future space exploration. Furthermore, it will provide cost reductions to the Artemis programs over their life cycle (in Operations & Maintenance (O&M) and Logistics). Unique proprietary interfaces if considered or allowed would not only increase complexity but also add cost to the programs. Of course, understanding what will work and not work effectively in these unique environments such as the lunar surface is important. These unique environments require much needed intelligent design, prototyping, comprehensive testing, and field experience, utilizing consensus on common interface solutions.

Jaime Gomez↗

NASA NTRS1992

Volatile processes in Triton's atmosphere and surface

A basic model for latitudinal transport of nitrogen is reviewed focusing on its limitations and some complications associated with surface and atmospheric physics. Data obtained by 1989 Voyager encounter with the Neptune system revealed the complexity in the pure nitrogen transport which is caused by the nonuniform albedo of the frosts. It is concluded that Triton is similar to Mars in terms of the complexity of volatile transport and to understand Triton's surface-atmosphere system, Mars may be a very good analog.

Lunine, J. I.↗

NASA NTRS1994

Recalibration of the Viyager PRA antenna for polarization sense measurement

The Voyager Planetary Radio Astronomy (PRA) antenna and receiver system provides an indication of the sense of elliptical or circular polarization of radiation that is not correct for all directions of incidence. The true sense could be determined for all directions if accurate calibration data were available. It was not feasible to make the calibration before the Voyagers were launched. Lecacheux & Ortega-Molina (1987), however, were able to derive such calibration data from planetary radio observations made in flight. They expressed their results in terms of the tilt of a plane (the E-plane) that divides the incident ray directions for which the indicated polarization sense is correct from those directions for which the indicated sense is reversed. We demonstrate that there are certain directions for which this calibration is itself in error, and that the surface dividing the two sets of incident rays is more complex than a tilted plane. We are able to make a crude approximation to the true surface from the limited data available.

Wang, L.↗

DOE OSTI2021

Unraveling the Formation Mechanism of a Hybrid Zr-Based Chemical Conversion Coating with Organic and Copper Compounds for Corrosion Inhibition

Environmental-friendly chromate-free, zirconium (Zr)-based conversion coating is a promising green technology for corrosion protection. Additives in the surface treatment provides critical functionalities and performance improvements; however, mechanistic understanding as of how the additives influence the coatings remains unclear. In this study, a new organic-inorganic hybrid Zrbased conversion coating which combines copper (Cu) compounds and polyamidoamine (PAMAM), taking advantages of a complementary nature of organic and inorganic additives. Here, a multimodal approach combining electron and X-ray characterization is applied to study the interaction of Cu 2+ and PAMAM and the resulting impacts on the coating formation. Adding PAMAM changed the surface morphology, thickness, distribution of Cu in the cluster and void formation of the coatings. High PAMAM (100-200 pm) leads to little conversion coating formation, and low PAMAM (0-25 ppm) shows voids formation under the coatings. Moreover, PAMAM incorporates in the coating in a form of PAMAM-Cu complex with a higher concentration towards the surface, provides an organic layer at the surface of the coating. X-ray absorption near-edge structure (XANES) spectroscopy shows a difference between the conventional and hybrid coating treatments in an alkaline solution to simulate the E-coat process, suggesting the contribution of PAMAM in the enhanced chemical stability in an alkaline environment. Therefore, an intermediate range of addition of PAMAM (50 ppm) is optimal to 1) avoid excessive voids formation, 2) promote some Cu cluster formation and thus enhancing the Zr-based coating formation and 3) incorporate organic components into the coating to improve the adhesion of the subsequent coatings. Overall, this work furthers our knowledge on the formation mechanism of an effective and environmentally friendly hybrid conversion coating for corrosion inhibition, demonstrating a critical processing-structureproperty relationship. This study will benefit future development of green and effective surface treatment technology.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

NASA NTRS1988

Growth and characterization of large YBa2Cu3O(7-x) single crystals

Centimeter-sized crystal plates of YBa2Cu3O(7-x) have been obtained using a bulk composition and method described by Schneemeyer at al. (1987) modified for growth in a pure oxygen atmosphere. A porous MgO crucible and long soak time promote large crystals. Mg was not detectable in the crystals. Electron microbeam analysis using a 60 A monochromator crystal for the oxygen determination gave the composition Y(1.05)Ba(2.02)Cu(2.94)O(6.52 + or - 0.06). As-grown crystals from the melt surface exhibit a fairly sharp Tc with zero resistance at 80 K, and show complex twinning and crack patterns. Optical micrographs of a lightly polished surface normal to the c-axis of a 3-mm crystal delineate twinning and fine scale microcracking; this crystal surface now has a zero resistance at 68 K. Microhardness measurements and microfracture observations indicate intrinsic properties that may inhibit or impede large scale manufacture of electronic ceramics.

Keester, Kenneth L.↗

NASA NTRS2005

Mars Orbiter Sample Return Power Design

Mars has greatly intrigued scientists and the general public for many years because, of all the planets, its environment is most like Earth's. Many scientists believe that Mars once had running water, although surface water is gone today. The planet is very cold with a very thin atmosphere consisting mainly of CO2. Mariner 4, 6, and 7 explored the planet in flybys in the 1960s and by the orbiting Mariner 9 in 1971. NASA then mounted the ambitious Viking mission, which launched two orbiters and two landers to the planet in 1975. The landers found ambiguous evidence of life. Mars Pathfinder landed on the planet on July 4, 1997, delivering a mobile robot rover that demonstrated exploration of the local surface environment. Mars Global Surveyor is creating a highest-resolution map of the planet's surface. These prior and current missions to Mars have paved the way for a complex Mars Sample Return mission planned for 2003 and 2005. Returning surface samples from Mars will necessitate retrieval of material from Mars orbit. Sample mass and orbit are restricted to the launch capability of the Mars Ascent Vehicle. A small sample canister having a mass less than 4 kg and diameter of less than 16 cm will spend from three to seven years in a 600 km orbit waiting for retrieval by a second spacecraft consisting of an orbiter equipped with a sample canister retrieval system, and a Earth Entry Vehicle. To allow rapid detection of the on-orbit canister, rendezvous, and collection of the samples, the canister will have a tracking beacon powered by a surface mounted solar array. The canister must communicate using RF transmission with the recovery vehicle that will be coming in 2006 or 2009 to retrieve the canister. This paper considers the aspect and conclusion that went into the design of the power system that achieves the maximum power with the minimum risk. The power output for the spherical orbiting canister was modeled and plotted in various views of the orbit by the Satellite Orbit Analysis Program (SOAP).

Mardesich, N.↗

DOE OSTI2018

Excimer Emission of Acridine Orange Adsorbed on Gadolinium-Yttrium Orthovanadate Nanoparticles

Studying the complexes of inorganic nanoparticles – organic dye molecules is of great importance for their theranostics application. In this paper, we report gadolinium-yttrium orthovanadate nanoparticles (VNPs) – Acridine Orange (AO) complex formation in water solutions. To study the interactions between VNPs and AO, the methods of steady-state and time-resolved spectroscopy were used. It was shown that in aqueous solutions containing VNPs, AO aggregation takes place with a sandwich-like stacking of AO molecules in the near-surface layer of VNPs. The VNPs–AO complex formation causes significant changes in the AO fluorescence spectrum, namely, the appearance of a new broad, structureless band in the long-wavelength spectral edge, which was not observed in AO spectrum in a pure water solution. By analyzing of the absorption, fluorescence excitation spectra and fluorescence decay, the static excimer origin of the long-wavelength fluorescence band has been established.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2024

Flashback characterization of additively manufactured swirl-stabilized fuel injector with varying surface roughness

This work investigates the effects of as-built surface roughness on the flashback propensity in additively manufactured (AM) swirl-stabilized lean premixed (LPM) fuel injectors. Adoption of AM for rapid prototyping and fabrication of complex fuel-flexible injector designs requires investigating surface roughness effects on the flow and flame stability characteristics of the combustor. Wall roughness increases the near-wall shear, which could alter the boundary layer structure and change the propensity for flame flashback. Accounting for the realistic as-built surface roughness is crucial in carrying out computational modeling and experimental analysis to establish a feedback loop for the precision designing of fuel-flexible injectors. The presented numerical analysis of as-built AM injector is an essential consideration to optimize injector design for aerodynamics and additive manufacturability.

Mohanty, Pratikshya↗

DOE OSTI2022

Use of diffusive gradients in thin films (DGT) to measure potentially bioavailable metals in southeastern USA blackwater streams

Here, we used diffusive gradients in thin films (DGT) to measure potentially bioavailable metals in coastal plain streams in the southeastern USA that exhibited strong to moderate blackwater characteristics. Metals were partitioned into particulate metals, DGT-inert metals (i.e., colloidal and refractory organic complexes not accumulated by DGT), and DGT-labile metals (i.e., free metal ions, small inorganic complexes, and labile organic complexes). We also examined the influence of different DGT deployment times using data collected from the field and a follow-up laboratory study. The DGT-measured fraction of dissolved metals in the streams was 15% for Cd, 21% for Zn, 33% for Cu, 37% for Pb, and 98% for Mn. Metals bound to particulates predominated only for Pb. Most of the Cd, Pb, Zn, and Cu were associated with colloids, refractory organic complexes, or particles. Relatively small amounts were in free ion or labile complexes likely to be bioavailable through respiratory surfaces. Modeled concentrations of free and inorganically bound Cu and Pb were lower than the DGT fraction indicating that DGT accumulated some organically bound Cu and Pb that might not have been bioavailable. DGT-exposure times in excess of 5 days may have contributed to the accumulation of partly labile organic–metal complexes and were associated with substantial biofouling that caused metal uptake by DGT to depart from linearity.

54 ENVIRONMENTAL SCIENCES↗