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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 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Vapor-Phase Cyclohexene Epoxidation by Single-Ion Fe(III) Sites in Metal–Organic Frameworks

Heterogeneous catalysts supported on metal–organic frameworks (MOFs), which possess uniform porosity and crystallinity, have attracted significant interest for recent years due to the ease of active-site characterization via X-ray diffraction and the subsequent relation of the active site structure to the catalytic activity. We report the syntheses, structures, and oxidation catalytic activities of single-ion iron catalysts incorporated into the zirconium MOF NU-1000. Single-ion iron catalysts with different counteranions were anchored onto the Zr node through postsynthetic solvothermal deposition. Crystallographic characterization of the resulting MOFs (NU-1000-Fe-Cl and NU-1000-Fe-NO 3 ) revealed that, while both frameworks have similar Fe coordination, the distance between Fe and the Zr 6 node differs significantly between the two. Lastly, the product rate profiles of the two catalysts for vapor-phase cyclohexene epoxidation demonstrate different initial rates and product formations, likely originating from the different Fe–O distances.

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

Generalized synthesis of high surface area mesoporous metal titanates as efficient heterogeneous catalysts

A novel metal dissolution coupled with reverse micelle formation approach is used as a generalized synthesis method for a series of high surface area metal titanates where the metals used are Bi, Mg, V, Mn, Fe, Co, Ni, Cu, Zn, Mo, W, and Ce. This study reports the highest surface areas published so far. The homogeneous distributions of the metals and titanium are observed in SEM-EDX and TEM mapping. The synthesized materials were comprehensively characterized using PXRD, Raman, nitrogen adsorption isotherms, SEM; EDX, TEM, TEM mapping, TGA, and XPS. The green catalytic oxidation of aniline to nitrosobenzene occurs within 30 min at room temperature when mesoporous W/Ti binary metal oxide is used as the catalyst. The radical mediated catalytic reaction gives excellent yields and the catalyst is reusable up to 4 reaction cycles without losing significant activity.

36 MATERIALS SCIENCE↗
NASA NTRS1990

CO-oxidation catalysts: Low-temperature CO oxidation over Noble-Metal Reducible Oxide (NMRO) catalysts

Oxidation of CO to CO2 is an important reaction technologically and environmentally and a complex and interesting reaction scientifically. In most cases, the reaction is carried out in order to remove CO as an environmental hazard. A major application of heterogeneous catalysts is catalytic oxidation of CO in the exhaust of combustion devices. The reaction over catalysts in exhaust gas is fast and often mass-transfer-limited since exhaust gases are hot and O2/CO ratios are high. The main challenges to catalyst designers are to control thermal sintering and chemical poisoning of the active materials. The effect of the noble metal on the oxide is discussed, followed by the effect of the oxide on the noble metal, the interaction of the noble metal and oxide to form unique catalytic sites, and the possible ways in which the CO oxidation reaction is catalyzed by the NMRO materials.

Herz, Richard K.↗
NASA NTRS1987

CO oxidation studies over supported noble metal catalysts and single crystals: A review

The catalytic oxidation of CO over noble metal catalysts is reviewed. Results obtained on supported noble metal catalysts and single crystals both at high pressures and under UHV conditions are compared. The underlying causes which result in surface instabilities and multiple steady-state oscillations are considered, in particular, the occurrence of hot spots. CO islands of reactivity, surface oxide formation and phase transformations under oscillatory conditions are discussed.

Boecker, Dirk↗
DOE OSTI2025

Backbone editing and deconstruction of polyethylene by Beckmann rearrangement and hydrogenolysis

Polyethylene is the most widely produced commodity plastic and is used in many applications, including packaging, insulation, and medical devices. However, the inertness of polyethylene makes chemical recycling inefficient and challenging. We report the conversion of oxidized high-density and low-density polyethylene, formed by direct, catalytic oxidation, to polyamides by Beckmann rearrangement of the corresponding oximes. These polyamides have enhanced surface properties over those of unmodified polyethylene, while maintaining the same, favorable mechanical profiles. The amide sites were reductively cleaved by hydrogenolysis with ruthenium-based catalysts to furnish alcohol- and amine-terminated fragments, which were used for the synthesis of polyurea-urethanes with poly(tetrahydrofuran) and methylene diphenyl diisocyanate. These experiments show how to install cleavable moieties into the backbone of polyethylene to facilitate deconstruction and the generation of new materials to affect greater sustainability in polyolefins.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2010

Advanced Catalysts for the Ambient Temperature Oxidation of Carbon Monoxide and Formaldehyde

The primary applications for ambient temperature carbon monoxide (CO) oxidation catalysts include emergency breathing masks and confined volume life support systems, such as those employed on the Shuttle. While Hopcalite is typically used in emergency breathing masks for terrestrial applications, in the 1970s, NASA selected a 2% platinum (Pt) on carbon for use on the Shuttle since it is more active and also more tolerant to water vapor. In the last 10-15 years there have been significant advances in ambient temperature CO oxidation catalysts. Langley Research Center developed a monolithic catalyst for ambient temperature CO oxidation operating under stoichiometric conditions for closed loop carbon dioxide (CO2) laser applications which is also advertised as having the potential to oxidize formaldehyde (HCHO) at ambient temperatures. In the last decade it has been discovered that appropriate sized nano-particles of gold are highly active for CO oxidation, even at sub-ambient temperatures, and as a result there has been a wealth of data reported in the literature relating to ambient/low temperature CO oxidation. In the shorter term missions where CO concentrations are typically controlled via ambient temperature oxidation catalysts, formaldehyde is also a contaminant of concern, and requires specially treated carbons such as Calgon Formasorb as untreated activated carbon has effectively no HCHO capacity. This paper examines the activity of some of the newer ambient temperature CO and formaldehyde (HCHO) oxidation catalysts, and measures the performance of the catalysts relative to the NASA baseline Ambient Temperature Catalytic Oxidizer (ATCO) catalyst at conditions of interest for closed loop trace contaminant control systems.

Nalette, Tim↗
DOE OSTI2022

Mechanistic Investigation of Enhanced Catalytic Selectivity toward Alcohol Oxidation with Ce Oxysulfate Clusters

Ceria-based materials have been highly desired in photocatalytic reactions due to their easily redox property and strong oxygen storage and transfer ability. Herein, we report the structures of one CeCe 70 oxysulfate cluster and four MCe 70 clusters (M = Cu, Ni, Co, Fe) with the same Ce 70 core. As noted, single crystal X-ray diffraction confirmed the structures of CeCe 70 and the MCe 70 series, while Raman spectroscopy indicated an increase in oxygen defects upon the introduction of Cu and Fe ions. The clusters catalyzed the oxidation of 4-methoxybenzyl alcohol under ultraviolet light. CuCe 70 and FeCe 70 exhibited enhanced reactivity compared to CeCe 70 and improved aldehyde selectivity compared to control experiments. In comparison with their homogeneous congeners, the CeCe 70 /MCe 70 clusters altered the location of radical generation from the bulk solution to the clusters’ surfaces. Mechanistic studies highlight the role of oxygen defects and specific transition metal introduction for efficient photocatalysis. Furthermore, the mechanistic pathway in this study provides insight on how to select or design a highly selective catalyst for photocatalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1999

Enhanced Oxidation Catalysts for Water Reclamation

This effort seeks to develop and test high-performance, long operating life, physically stable catalysts for use in spacecraft water reclamation systems. The primary goals are to a) reduce the quantity of expendable water filters used to purify water aboard spacecraft, b) to extend the life of the oxidation catalysts used for eliminating organic contaminants in the water reclamation systems, and c) reduce the weight/volume of the catalytic oxidation systems (e.g. VRA) used. This effort is targeted toward later space station utilization and will consist of developing flight-qualifiable catalysts and long-term ground tests of the catalyst prior to their utilization in flight. Fixed -bed catalytic reactors containing 5% platinum on granular activated carbon have been subjected to long-term dynamic column tests to measure catalyst stability vs throughput. The data generated so far indicate that an order of magnitude improvement can be obtained with the treated catalysts vs the control catalyst, at only a minor loss (approx 10%) in the initial catalytic activity.

Jolly, Clifford D.↗
NASA NTRS1990

Advanced air revitalization system modeling and testing

To support manned lunar and Martian exploration, an extensive evaluation of air revitalization subsystems (ARS) is being conducted. The major operations under study include carbon dioxide removal and reduction; oxygen and nitrogen production, storage, and distribution; humidity and temperature control; and trace contaminant control. A comprehensive analysis program based on a generalized block flow model was developed to facilitate the evaluation of various processes and their interaction. ASPEN PLUS was used in modelling carbon dioxide removal and reduction. Several life support test stands were developed to test new and existing technologies for their potential applicability in space. The goal was to identify processes which use compact, lightweight equipment and maximize the recovery of oxygen and water. The carbon dioxide removal test stands include solid amine/vacuum desorption (SAVD), regenerative silver oxide chemisorption, and electrochemical carbon dioxide concentration (EDC). Membrane-based carbon dioxide removal and humidity control, catalytic reduction of carbon dioxide, and catalytic oxidation of trace contaminants were also investigated.

Dall-Baumann, Liese↗
DOE OSTI2022

Amine Oxidation Catalyzed by NO 2

Amine oxidation is a major risk in the deployment of amine scrubbing for CO2 capture from post-combustion flue gas. Oxidation probably occurs by dissolved oxygen at elevated temperature, Fe(III)/Fe(II) shuttling between the absorber and the stripper, and by NO2 in the absorber. Amine selection, dissolved oxygen removal, and solvent reclaiming mitigate oxidation due to dissolved oxygen and iron shuttle mechanism, but not by NO2. This work examines piperazine (PZ) oxidation by NO2 in a bench-scale high gas flow reactor (HGF). PZ is an effective second-generation solvent with high CO2 capacity, fast capture rate, good thermal stability, and good resistance to oxidation. Flue gas typically contains 0.5–5 ppm NO2 and 10–100 ppm NO. NO2 at 1 ppm in the flue gas appears to cause significant amine oxidation in pilot plant testing. PZ solution can easily absorb NO2, and it is hypothesized that NO2 can catalytically oxidize PZ through free-radical propagation. The issue may not be solved by a NO2 pre-scrubber since the coexistence of NO and O2 in the flue gas will keep producing non-negligible amounts of NO2 in the ductwork and the absorber after the NO2 incoming with the flue gas has been scrubbed. In addition, NO2 may not only oxidize PZ but also the intermediate degradation products, and it is unknown if the existence of dissolved iron influences the oxidation by NO2. Previous workers have also shown that NO2 is the stoichiometric source of nitrosamine. A comprehensive analysis of NO2 oxidation is needed to address solvent management and its health/environmental impact. The new high gas flow (HGF) reactor focuses only on the absorber environment and is simpler to interpret because it does not include oxidation at high temperatures and by dissolved metal catalysts from corrosion. This paper presents the results of HGF experiments and shows evidence to support a hypothesis of amine oxidation catalyzed by NO2, presents the synergic effect of NO2 and iron on amine oxidation, points out the different effects of NO2 in clean and degraded solvents, and demonstrates that NO2 not only can oxidize amines but also their degradation products.

NO2, iron, piperazine (PZ), solvent oxidation, sol↗
DOE OSTI2022

Formation Mechanisms, Crystal Structure, and Interfacial Reactivity of (Mixed) Metal Sulfide Nanoparticles Produced via Biological versus Abiotic Systems

The primary goals of this project were to understand the formation mechanisms and reactivity of mix-metal sulfide nanophases (Cu-Fe, Ni-Fe, Co-Fe sulfides) produced via biological and abiotic pathways that are relevant to low-temperature aqueous environments. These mix-metal sulfide nanophases have been identified in a range of natural and anthropogenic systems and are considered to play key roles in the biogeochemical cycling of elements, biomineralization, environmental remediation, resource recovery, eco-toxicity, and the origin and evolution of life. Using a comparative approach, we aimed to elucidate: (i) if these mix-metal sulfides tend to form nanoscale phases regardless of their formation pathways; (ii) what mechanisms are involved in the biological and abiotic crystallization processes; (iii) what phases form that have been otherwise expected; and (iv) if we can combine the experimental results with what we see and surmise from field studies to facilitate a more comprehensive understanding regarding the origin and biogeochemical roles of these mix-metal sulfides. Along a related pathway of electron transfer in nano-systems, in this case dealing with Fe-oxides instead of Fe-sulfides, we have continued to explore the reactions and solid products of heterogeneous catalytic oxidation of aqueous Mn(II) by dissolved oxygen in the presence of iron oxides (hematite) nanoparticles. The nano-Mn-oxides produced are known to be efficient sorbents of transition metal elements, including Cu, Ni, and Co studied in our sulfide work.

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

A Review on the Impact of SO 2 on the Oxidation of NO, Hydrocarbons, and CO in Diesel Emission Control Catalysis

A high-efficiency after-treatment technology has been required to meet the increasingly stringent regulations on the emissions of nitrogen oxides (NO x ), hydrocarbons (HCs), and carbon monoxide (CO) exhausts from diesel engine vehicles throughout the world. The diesel oxidation catalyst (DOC) is an indispensable part of a diesel-fueled exhaust system, which mainly functions in the oxidation of unburned HCs and CO to CO 2 and H 2 O (in the case of HCs) and a proportion of NO to NO 2 . However, the DOC will unavoidably be poisoned by trace gaseous SO 2 or accumulated sulfur on the catalyst under real operational conditions and hence impair the overall purification efficiency of the aftertreatment system. There have been significant research efforts from both academia and industry involving sulfur-relevant diesel oxidation chemistry and development of robust sulfur-resistant oxidation catalysts. In this review, we focus on recent advances in the study of SO 2 effects on the catalytic oxidation of NO, HCs, and CO over DOCs, with particular attention to the fundamentals beneath apparent observations of sulfur influence on PGM-based and non-noble metal-based catalysts in the different oxidation reactions. Regeneration methods and design rationale for sulfur-resistant catalysts are also covered. Several challenges in the future research regarding microscopic insights into the SO 2 -influencing mechanism and next-generation sulfur-resistant DOC design are highlighted toward real-world practice.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Engineered Glucose Oxidase‐Carbon Nanotube Conjugates for Tissue‐Translatable Glucose Nanosensors

Abstract Continuous and non‐invasive glucose monitoring and imaging is important for disease diagnosis, treatment, and management. However, glucose monitoring remains a technical challenge owing to the dearth of tissue‐transparent glucose sensors. In this study, we present the development of near‐infrared fluorescent single‐walled carbon nanotube (SWCNT) based nanosensors directly functionalized with glucose oxidase (GOx) capable of immediate and reversible glucose imaging in biological fluids and tissues. We prepared GOx‐SWCNT nanosensors by facile sonication of SWCNT with GOx in a manner that—surprisingly—does not compromise the ability of GOx to detect glucose. Importantly, we find by using denatured GOx that the fluorescence modulation of GOx‐SWCNT is not associated with the catalytic oxidation of glucose but rather triggered by glucose‐GOx binding. Leveraging the unique response mechanism of GOx‐SWCNT nanosensors, we developed catalytically inactive apo‐GOx‐SWCNT that enables both sensitive and reversible glucose imaging, exhibiting a ΔF/F 0 of up to 40 % within 1 s of exposure to glucose without consuming the glucose analyte. We finally demonstrate the potential applicability of apo‐GOx‐SWCNT in biomedical applications by glucose quantification in human plasma and glucose imaging in mouse brain slices.

Chemistry↗
NASA NTRS2011

Development and Progress in Enabling the Photocatalyst Ti02 Visible-Light-Active

Photocatalytic oxidation (PCO) of organic contaminants is a promising air and water quality management approach which offers energy and cost savings compared to thermal catalytic oxidation (TCO). The most widely used photocatalyst, anatase TiO2, has a wide band gap (3.2 eV) and is activated by UV photons. Since solar radiation consists of less than 4% UV, but contains 45% visible light, catalysts capable of utilizing these visible photons need to be developed to make peo approaches more efficient, economical, and safe. Researchers have attempted various approaches to enable TiO2 to be visible-light-active with varied degrees of success'. Strategies attempted thus far fall into three categories based on their electrochemical' mechanisms: 1) narrowing the band gap of TiO2 by implantation of transition metal elements or nonmetal elements such as N, S, and C, 2) modifying electron-transfer processes during PCO by adsorbing sensitizing dyes, and 3) employing light-induced interfacial electron transfer in the heteronanojunction systems consisting of narrow band gap semiconductors represented by metal sulfides and TiO2. There are diverse technical approaches to implement each of these strategies. This paper presents a review of these approaches and results of the photocatalytic activity and photonic efficiency of the end .products under visible light. Although resulting visible-light-active (VLA) photocatalysts show promise, there is often no comparison with unmodified TiO2 under UV. In a limited number of studies where such comparison was provided, the UV-induced catalytic activity of bare TiO2 is much greater than the visible-light-induced catalytic activity of the VLA catalyst. Furthermore, VLA-catalysts have much lower quantum efficiency compared to the approx.50% quantum efficiency of UV-catalysts. This stresses the need for continuing research in this area.

Levine, Lanfang H.↗
NASA NTRS1981

Evolution of the atmosphere of Venus

The photochemistry of the stratosphere of Venus was modeled using an updated and expanded chemical scheme, and the results of recent laboratory studies. The model satisfactorily accounts for the observations of CO, O2, (1) and SO2 in the stratosphere. Oxygen, derived from CO2 photolysis, is primarily consumed by CO2 recombination and oxidation of SO2 to H2SO4. Photolysis of HCl in the upper stratosphere provides a major source of odd hydrogen radicals essential for the catalytic oxidation of CO. Oxidation of SO2 by O occurs in the lower stratosphere, with the O-O bond broken by S + O2 and SO + HO2. The sensitivity of stratospheric chemistry to ambient H2 abundance was studied and the model prefers the high value (1 10 ppm) recently inferred from the Pioneer Venus ionospheric measurements. The importance of the photochemical production of S2O, (SO)2, S2, H2S2O2 and H2S2O3 is speculated. A number of previously unsuspected similarities between the chemistry of the stratospheres of Venus and the Earth, presented and discussed.

Yung, Y. L.↗
NASA NTRS1984

Mechanism of the atmospheric oxidation of sulfur dioxide - Catalysis by hydroxyl radicals

A flash photolysis/resonance fluorescence technique was used to investigate the decay of OH due to the reaction OH + SO2 (+M) to HOSO2 (+M). In the presence of small amounts of NO (10 to the 14th per cu cm), the decays deviated from the normal semilogarithmic linearity due to reformation of OH. On the basis of computer simulations of the decay curves, it is suggested that the reactions HOSO2 + O2 to HO2 + SO3 (k3), and HO2 + HO to OH + NO2 are the likely subsequent steps in SO2 oxidation. The upper limit for the binding energy of HOSO2 relative to OH + SO2 is estimated to be 32 kcal/mol. The atmospheric implications of a catalytic oxidation mechanism are briefly discussed.

Margitan, J. J.↗
NASA NTRS2009

Reactive Distillation and Air Stripping Processes for Water Recycling and Trace Contaminant Control

Reactive distillation designs are considered to reduce the presence of volatile organic compounds in the purified water. Reactive distillation integrates a reactor with a distillation column. A review of the literature in this field has revealed a variety of functional reactive columns in industry. Wastewater may be purified by a combination of a reactor and a distiller (e.g., the EWRS or VPCAR concepts) or, in principle, through a design which integrates the reactor with the distiller. A review of the literature in reactive distillation has identified some different designs in such combinations of reactor and distiller. An evaluation of reactive distillation and reactive air stripping is presented with regards to the reduction of volatile organic compounds in the contaminated water and air. Among the methods presented, an architecture is presented for the evaluation of the simultaneous oxidation of organics in air and water. These and other designs are presented in light of potential improvements in power consumptions and air and water purities for architectures which include catalytic activity integrated into the water processor. In particular, catalytic oxidation of organics may be useful as a tool to remove contaminants that more traditional distillation and/or air stripping columns may not remove. A review of the current leading edge at the commercial level and at the research frontier in catalytically active materials is presented. Themes and directions from the engineering developments in catalyst design are presented conceptually in light of developments in the nanoscale chemistry of a variety of catalyst materials.

Boul, Peter J.↗
NASA NTRS2010

Air Stripping Designs and Reactive Water Purification Processes for the Lunar Surface

Air stripping designs are considered to reduce the presence of volatile organic compounds in the purified water. Components of the wastewater streams are ranked by Henry's Law Constant and the suitability of air stripping in the purification of wastewater in terms of component removal is evaluated. Distillation processes are modeled in tandem with air stripping to demonstrate the potential effectiveness and utility of these methods in recycling wastewater on the Moon. Scaling factors for distillation and air stripping columns are presented to account for the difference in the lunar gravitation environment. Commercially available distillation and air stripping units which are considered suitable for Exploration Life Support are presented. The advantages to the various designs are summarized with respect to water purity levels, power consumption, and processing rates. An evaluation of reactive distillation and air stripping is presented with regards to the reduction of volatile organic compounds in the contaminated water and air. Among the methods presented, an architecture is presented for the evaluation of the simultaneous oxidation of organics in air and water. These and other designs are presented in light of potential improvements in power consumptions and air and water purities for architectures which include catalytic activity integrated into the water processor. In particular, catalytic oxidation of organics may be useful as a tool to remove contaminants that more traditional distillation and/or air stripping columns may not remove. A review of the current leading edge at the commercial level and at the research frontier in catalytically active materials is presented. Themes and directions from the engineering developments in catalyst design are presented conceptually in light of developments in the nanoscale chemistry of a variety of catalyst materials.

Boul, Peter J.↗