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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Support Effect and Surface Reconstruction in In 2 O 3 / m- ZrO 2 Catalyzed CO 2 Hydrogenation

Here, we investigate the chemical and structural dynamics at the interface of In 2 O 3 /m-ZrO 2 and their consequences on the CO 2 hydrogenation reaction (CO 2 HR) under reaction conditions. While acting to enrich CO 2 , monoclinic zirconia (m-ZrO 2 ) was also found to serve as a chemical and structural modifier of In 2 O 3 that directly governs the outcome of the CO 2 HR. These modifying effects include the following: (1) Under reaction conditions (above 623 K), partially reduced In 2 O 3 , i.e., InO x (0 < x < 1.5), was found to migrate in and out of the subsurface of m-ZrO 2 in a semireversible manner, where m-ZrO 2 accommodates and stabilizes InO x by serving as a reservoir. The decreased concentration of surface InO x under elevated temperatures coincides with significantly decreased selectivity toward methanol and a sharp increase of the reverse water–gas shift reaction. The reconstruction-induced variation of InO x concentration appears to be one of the most important factors contributing to the altered catalytic performance of CO 2 HR at different reaction conditions. (2) The strong interactions and reactions between m-ZrO 2 and In 2 O 3 result in the activation of a pool of In–O bonds at the In 2 O 3 /m-ZrO 2 interface to form oxygen vacancies. On the other hand, the high dispersity of In 2 O 3 nanostructures onto m-ZrO 2 prevents their over-reduction under catalytically relevant conditions (up to 673 K), when bare In 2 O 3 is unavoidably reduced into the metallic phase (In 0 ). The relationship between the extent of reduction of In 2 O 3 and catalytic performance (CO 2 conversion, CH 3 OH selectivity, or yield of CH 3 OH) suggests the presence of an optimum coverage of surface InO x and oxygen vacancies under reaction conditions. The conventional model that links catalytic performance solely to the coverage of oxygen vacancies appears invalid in the present case. In situ analysis also allows the observation of surface reaction intermediates and their interconversions, including the reduction of CO 3 * into formate, a precursor for the formation of methanol and CO. The combinative ex situ and in situ study sheds light on the reaction mechanism of the CO 2 HR on In 2 O 3 /m-ZrO 2 -based catalysts. Our findings on the large-scale surface reconstructions, support effect, and the reaction mechanism of In 2 O 3 /m-ZrO 2 for CO 2 HR may apply to other related metal oxide catalyzed CO 2 reduction reactions.

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

Mechanistic understanding of support effect on the activity and selectivity of indium oxide catalysts for CO 2 hydrogenation

Herein we present a mechanistic study on the support effect (ZrO 2 and CeO 2 ) of In 2 O 3 catalysts in CO 2 hydrogenation by a combined experimental and computational approach. Kinetic experiments and surface characterization suggested that the activity of In 2 O 3 catalysts cannot be simply correlated with the abundance of surface oxygen vacancies (O v ) formed by either H 2 -reduction or thermal treatment, which has been frequently invoked in previous studies. The support effect should originate from the electronic interactions between In 2 O 3 and the support oxide, rather than geometric factors or the difference in the particle size of In 2 O 3 . Theoretical modelling revealed that surface O v facilitate the formation and stabilization of the formate (HCOO*) intermediate. While a carbonate-like structure is favored for CO 2 adsorption on CeO 2 -supported or unsupported In 2 O 3 catalysts, CO 2 tends to bind strongly in a bent configuration on the O v site at the In 2 O 3 -ZrO 2 interface. The distinct CO 2 adsorption structures on different supported In 2 O 3 catalysts may account for the different reaction energy profiles in the subsequent hydrogenation reactions, especially the rate-limiting step, i.e., hydrogenation of HCOO* to CH 2 O* and methoxy (CH 3 O*). The relatively higher methanol selectivity of In 2 O 3 catalyst supported on ZrO 2 with respect to that on CeO 2 are suggested to stem from the greater energy difference (Δ$E_a$) between the parallel hydrogenation and C-O bond cleavage of HCOO*, which leads to the formation of methanol and CO, respectively. We report this study underlines the important role of metal-oxide-interface in determining the catalytic behavior of oxide-supported In 2 O 3 catalysts in CO 2 conversion.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2023

Support Effect Studied on Thin-Film Perovskites

Some functional oxides exhibit strong support effects but typically have low surface areas and stabilities that negate the promotional effects. The primary goal of our work in the past three years was to develop high-surface-area versions of these supports by Atomic Layer Deposition onto stable supports, then use these to understand how the oxide supports affect the metal catalytic properties. The primary application targeted for these materials was methane oxidation and related reactions for emissions control. Systems of particular interest were supported, precious metals on thin-film perovskites in order to develop “intelligent” catalysts in which the metal can reversibly ex-solve from perovskite lattices. This following report lists the papers that were published with the support of this DOE grant, together with a brief summary of the results from each paper.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2001

Investigating Uncertainty in Predicting Carbon Dynamics in North American Biomes: Putting Support-Effect Bias in Perspective

A fundamental strategy in NASA's Earth Observing System's (EOS) monitoring of vegetation and its contribution to the global carbon cycle is to rely on deterministic, process-based ecosystem models to make predictions of carbon flux over large regions. These models are parameterized (that is, the input variables are derived) using remotely sensed images such as those from the Moderate Resolution Imaging Spectroradiometer (MODIS), ground measurements and interpolated maps. Since early applications of these models, investigators have noted that results depend partly on the spatial support of the input variables. In general, the larger the support of the input data, the greater the chance that the effects of important components of the ecosystem will be averaged out. A review of previous work shows that using large supports can cause either positive or negative bias in carbon flux predictions. To put the magnitude and direction of these biases in perspective, we must quantify the range of uncertainty on our best measurements of carbon-related variables made on equivalent areas. In other words, support-effect bias should be placed in the context of prediction uncertainty from other sources. If the range of uncertainty at the smallest support is less than the support-effect bias, more research emphasis should probably be placed on support sizes that are intermediate between those of field measurements and MODIS. If the uncertainty range at the smallest support is larger than the support-effect bias, the accuracy of MODIS-based predictions will be difficult to quantify and more emphasis should be placed on field-scale characterization and sampling. This talk will describe methods to address these issues using a field measurement campaign in North America and "upscaling" using geostatistical estimation and simulation.

Dungan, Jennifer L.↗
DOE OSTI2020

Heterolytic Hydrogen Activation: Understanding Support Effects in Water–Gas Shift, Hydrodeoxygenation, and CO Oxidation Catalysis

Identifying the role of oxide supports in transition metal catalysis is critical toward our understanding of heterogeneous catalysis. The water-gas shift (WGS) reaction is a prototypical example where oxide support dictates catalytic activity, yet the cause for this remains uncertain. Herein, we show that a single descriptor—the equilibrium constant for hydroxyl formation—relates the WGS turnover frequency across disparate oxide supports. The dissimilar equilibrium constant, or oxophilicity, between early and late transition metals exemplify the utility of metal-support interfacial sites to circumvent adsorption-energy scaling restrictions, thereby providing bifunctional gains for the WGS reaction class. In relation, the equilibrium constant for hydroxyl formation is equivalent to the equilibrium constant for the formal heterolytic dissociation of hydrogen, and therefore, reflects the ability of the metal-support interface to participate in hydrogen heterolysis. The ubiquitous coexistence, yet divergent chemical behavior of homo- and heterolytically activated hydrogen renders oxide support identity central toward our understanding of hydrogenation catalysis. This work was supported by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences and performed at the Environmental Molecular Sciences Laboratory in (EMSL), which is a DOE Office of Science User Facility located at the Pacific Northwest National Laboratory (PNNL). PNNL is a multiprogram national laboratory operated for DOE by Battelle. Computational resources were provided by a user proposal at the National Energy Research Scientific Computing Center (NERSC), a DOE Office of Science User Facility. N.N. would like to thank Oliver Y. Gutierrez for critical feedback during the final stage of manuscript preparation.

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

Identifying Support Effects in Au-Catalyzed CO Oxidation

Some catalytic oxide supports are more equal than others, with numerous variable properties ranging from crystal symmetry to surface chemistry and electronic structure. As a consequence, it is often very difficult to determine which of these act as the driver of performance changes observed in catalysis. In this work, we hold many of these variable properties constant with structurally similar LnScO 3 (Ln = La, Sm, and Nd) nanoparticle supports with cuboidal shapes and a common Sc-rich surface termination. Using CO oxidation over supported Au nanoparticles as a probe reaction, we observe higher activation energy and a slower rate using NdScO 3 as the support material. This change is found to correlate to the strength of CO 2 binding to the support surface, identified by temperature-programmed desorption measurements. Furthermore, the change is due to differences in the 4f electrons of the lanthanide cations, the cations’ Lewis acidity, and the inductive effect they impose.

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

A Study of Support Effects for the Water-Gas-Shift Reaction over Cu

The water–gas-shift (WGS) reaction was studied on a series of supported Cu catalysts in which the MgAl 2 O 4 (MAO) support was modified by depositing ZnO, CeO 2 , Mn2O 3 and CoO using Atomic Layer Deposition (ALD). Addition of Cu by one ALD cycle gave rise to catalysts with nominally 1-wt% Cu. A 1.1-wt% Cu/MAO catalyst prepared by ALD exhibited twice the dispersion but ten times the WGS activity of a 1-wt% Cu/MAO catalyst prepared by impregnation, implying that the reaction is structure sensitive. However, Cu catalysts prepared with the ZnO, CeO 2 , and Mn 2 O 3 films showed negligible differences from that of the Cu/MAO catalyst, implying that these oxides did not promote the reaction. Cu catalysts prepared on the CoO film showed a slightly lower activity, possibly due to alloy formation. The implications of these results for the development of better WGS catalysts is discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Understanding Support Effects of ZnO-Promoted Co Catalysts for Syngas Conversion to Alcohols Using Atomic Layer Deposition

Co 2 C, an emerging catalyst for the conversion of syngas to oxygenates, shows support-sensitive behavior that has not yet been fully explained. In this work, we characterize Co catalysts modified with ZnO atomic layer deposition on SiO 2 , carbon, CeO 2 , and Al 2 O 3 supports. We find that under syngas conditions, ZnO-promoted Co transforms into Co 2 C on SiO 2 , carbon, and CeO 2 , but not on Al 2 O 3 . Moreover, the support affects the extent of carburization: while the SiO 2 -supported catalyst carburizes completely, carbon- and CeO 2 -supported catalysts show incomplete conversion of Co to Co 2 C. These three catalysts also exhibit different oxygenate selectivities. In contrast, the modified Al 2 O 3 -supported catalyst retains the Fischer-Tropsch catalytic properties of metallic Co. By depositing increasing amounts of Al 2 O 3 by ALD on the SiO 2 support, decreasing Co 2 C formation and oxygenate selectivity occurs. In-situ XANES reveals that Al 2 O 3 prevents Co 2 C formation by enabling the ZnO to restructure into ZnAl 2 O 4 during reduction. Thus, in addition to modifying the active catalyst phase, the promoter can also strongly interact with the support, significantly impacting catalyst performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Unveiling the support effect in Pt-based catalysts for the selective catalytic oxidation of NH 3 under realistic diesel engine conditions

Pt catalysts have been widely used for the selective catalytic oxidation of NH 3 (NH 3 -SCO) in practical applications due to their high activity at low temperatures. However, more stringent regulations require further enhancement of low-temperature NH 3 -SCO activity. In this study, we investigated the influence of different supports, including aluminum oxide (Al 2 O 3 ), silica (SiO 2 ), and chabazite (CHA), on the NH 3 -SCO performance of Pt catalysts. Furthermore, our findings demonstrate that the Pt/CHA catalyst exhibited superior NH 3 -SCO performance under realistic diesel engine conditions, characterized by high space velocity and the presence of water vapor. Notably, the Pt/CHA catalyst achieved a significantly lower T 50 (temperature at which 50% NH 3 conversion is achieved) of 218 °C under conditions with both CO 2 and H 2 O, with a 56 °C reduction compared to the state-of-the-art Pt/Al 2 O 3 catalyst. The exceptional NH 3 -SCO performance is attributed to the high abundance of metallic Pt 0 species and the presence of rich and stable acid sites that facilitate NH 3 adsorption and activation. Furthermore, these results highlight CHA as a promising support for the Pt catalyst in NH 3 -SCO applications for diesel engine emission control.

36 MATERIALS SCIENCE↗
NASA NTRS1956

An Experimental Investigation of Sting-Support Effects on Drag and a Comparison with Jet Effects at Transonic Speeds

This paper presents the results of an investigation of sting-support interference on afterbody drag at transonic speeds. Stings with varying diameter, cone angle, and cylindrical length were tested at the rea r of a model with various afterbody shapes. The data were obtained at an angle of attack of O deg. and at Mach numbers from 0.80 to 1.10. It was found that, in general, the addition of a sting caused a drag reduction. A method is presented whereby approximate sting-interferen ce corrections may be made to models with afterbodies and sting suppo rts of similar size and scale to those of this paper provided the bou ndary layer is turbulent at the model base and the Reynolds numbers a re of the same order of magnitude. Reynolds number of the tests prese nted varied from 15.0 x 10 (exp 6) to 17.4 x 10 (exp 6) based on body length. Sting effects from this investigation are compared with data of jet effects on the same afterbodies. The results of this comparis on indicate that for the more gradually contoured afterbodies, a stin g shape can be found which will duplicate the jet effects, but that f or blunt afterbodies no solid sting shape will duplicate the jet effe cts.

Cahn, Maurice S.↗
NASA NTRS1988

Periodic weight support effects on rat soleus fibers after hindlimb suspension

The morphological and histochemical properties of rat soleus muscles were investigated following one week of hindlimb suspension. Short-duration daily weight support activity is shown to ameliorate, but not prevent, soleus atrophy induced by hindlimb suspension. The results indicate that fiber cross-sectional area is more responsive to periodic weight support in dark than light ATPas fibers, and that muscle fiber atrophy need not be associated with a loss in succinate dehydrogenase activity.

Hauschka, Edward O.↗
DOE OSTI2025

Pt Particles on a Dynamic TiO 2 Support in Near-Ambient Conditions−Disentangling Size, Pressure, and Support Effects

Platinum particles on reducible oxides are known to form complex and highly dynamic catalyst systems at elevated pressures and temperatures, often adopting active structures that differ from those found at room temperature and under ultrahigh vacuum (UHV). Here, we study the oxidation and structural evolution of subnanometer Pt clusters and nanoparticles supported on rutile TiO 2 (110) across an oxygen pressure range from UHV to 0.1 mbar, using near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS), scanning tunneling microscopy (STM) under UHV and NAP conditions, and low-energy ion scattering (LEIS). Our results reveal distinct differences in oxidation behavior and thermal stability between Pt nanoparticles and clusters, which are further modulated by the support stoichiometry and oxygen pressure. Small Pt clusters become oxidized even at room temperature but are susceptible to accelerated sintering in 0.1 mbar O 2 at elevated temperatures. In contrast, well-crystallized Pt nanoparticles on near-stoichiometric TiO 2 show weaker oxidation. On a reduced, defective TiO 2 support, Pt instead quickly becomes deeply buried by new titania layers, which are formed during support reoxidation. This process appears to result primarily from interactions of the support with the gas phase, unlike the classical, selflimited encapsulation that is induced by the strong metal−support interaction (SMSI). Finally, we address the full complexity of real catalysts in a direct side-by-side comparison of the single-crystalline model system with a Pt-loaded TiO 2 powder catalyst (P25). We conclude that the stoichiometry of the model supports must be carefully chosen and controlled to accurately reproduce the expected state of powder supports during redox reactions.

metal nanoparticles↗
NASA NTRS1958

An experimental investigation of sting-support effects on drag and a comparison with jet effects at transonic speeds

Various dummy stings were tested on the rear of a related series of afterbody shapes for Mach numbers from 0.80 to 1.10 and Reynolds numbers based on body length from 15.0 x 16 to the 6th power to 17.4 x 10 to the 6th power. A method is presented whereby approximate sting interference corrections can be made to models having afterbody shapes and sting supports similar to those of these tests if the Reynolds numbers are of the same order of magnitude and a turbulent boundary layer exists at the model base. Also presented is an analysis of jet duplication by use of a sting.

Cahn, Maurice S↗
NASA NTRS2010

Weighting Statistical Inputs for Data Used to Support Effective Decision Making During Severe Emergency Weather and Environmental Events

National Aeronautical and Space Administration (NASA) weather and atmospheric environmental organizations are insatiable consumers of geophysical, hydrometeorological and solar weather statistics. The expanding array of internet-worked sensors producing targeted physical measurements has generated an almost factorial explosion of near real-time inputs to topical statistical datasets. Normalizing and value-based parsing of such statistical datasets in support of time-constrained weather and environmental alerts and warnings is essential, even with dedicated high-performance computational capabilities. What are the optimal indicators for advanced decision making? How do we recognize the line between sufficient statistical sampling and excessive, mission destructive sampling ? How do we assure that the normalization and parsing process, when interpolated through numerical models, yields accurate and actionable alerts and warnings? This presentation will address the integrated means and methods to achieve desired outputs for NASA and consumers of its data.

Gardner, Adrian↗
NASA NTRS1994

Use of a multimission system for cost effective support of planetary science data processing

JPL's Multimission Operations Systems Office (MOSO) provides a multimission facility at JPL for processing science instrument data from NASA's planetary missions. This facility, the Multimission Image Processing System (MIPS), is developed and maintained by MOSO to meet requirements that span the NASA family of planetary missions. Although the word 'image' appears in the title, MIPS is used to process instrument data from a variety of science instruments. This paper describes the design of a new system architecture now being implemented within the MIPS to support future planetary mission activities at significantly reduced operations and maintenance cost.

Green, William B.↗
NASA NTRS2015

Unified User Interface to Support Effective and Intuitive Data Discovery, Dissemination, and Analysis at NASA GES DISC

Goddard Earth Sciences Data and Information Services Center (GES DISC) has been providing access to scientific data sets since 1990s. Beginning as one of the first Earth Observing System Data and Information System (EOSDIS) archive centers, GES DISC has evolved to offer a wide range of science-enabling services. With a growing understanding of needs and goals of its science users, GES DISC continues to improve and expand on its broad set of data discovery and access tools, sub-setting services, and visualization tools. Nonetheless, the multitude of the available tools, a partial overlap of functionality, and independent and uncoupled interfaces employed by these tools often leave the end users confused as of what tools or services are the most appropriate for a task at hand. As a result, some the services remain underutilized or largely unknown to the users, significantly reducing the availability of the data and leading to a great loss of scientific productivity. In order to improve the accessibility of GES DISC tools and services, we have designed and implemented UUI, the Unified User Interface. UUI seeks to provide a simple, unified, and intuitive one-stop shop experience for the key services available at GES DISC, including sub-setting (Simple Subset Wizard), granule file search (Mirador), plotting (Giovanni), and other services. In this poster, we will discuss the main lessons, obstacles, and insights encountered while designing the UUI experience. We will also present the architecture and technology behind UUI, including NodeJS, Angular, and Mongo DB, as well as speculate on the future of the tool at GES DISC as well as in a broader context of the Space Science Informatics.

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