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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 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Large scale synthesis of resorcinol-formaldehyde aerogel

A product includes an aerogel having a single bulk structure, the single bulk structure having at least one dimension greater than 10 millimeters. The single bulk structure includes a plurality of pores, where each pore has a largest diameter defined as a greatest distance between pore walls of the respective pore. In addition, an average of the largest diameters of a majority of the pores is within a specified range, and the plurality of pores are distributed substantially homogenously throughout the single bulk structure.

Loeb, Colin↗
DOE OSTI2022

An Improved Pathway to Ethylene Glycol via CO 2

This report describes our efforts to develop a partial electrochemical oxidation process to produce formaldehyde selectively from methanol. The effort examined numerous potential anode materials in pursuit of 70% Faradaic efficiency for conversion of methanol to formaldehyde. Among the various electrode materials tested herein both Pt and PtRu were identified as the most promising catalysts in this process as the Faradaic efficiency obtained in these cases are 40% and >70% respectively. Several other 3d transition metals, Pt group metals and their alloys were also studied in which the Faradaic efficiency was obtained within 5-30%. In case of Pt and PtRu bulk metal electrode shows higher selectivity to formaldehyde compared to their nanostructured materials. Based on the literature, nanostructured Pt and PtRu are considered as active catalysts for methanol fuel cells, thus, lower selectivity to formaldehyde with nano Pt and PtRu in our case was attributed to their preferential oxidation of methanol to CO 2 . Severe catalyst deactivation was noted when 0.5 (M) sulfuric acid was used as the electrolyte irrespective of catalyst formulation. On the other hand, much higher activity and selectivity for formaldehyde was noted when alkaline electrolyte was employed during oxidation. Considering selective electrochemical oxidation of methanol to formaldehyde is an area which is underexplored as of today, our findings about catalyst formulation and process condition is noteworthy in this direction. Both bulk metal electrodes of Pt and PtRu may be cost prohibitive and thus present challenges to the scale up this technology. Therefore, we recognize that additional efforts are needed to develop catalysts with high activities and Faradaic efficiencies similar to bulk electrodes for the electrooxidation of methanol to formaldehyde.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Methanol Partial Oxidation on Cu(111) and PtCu(111) Single-Atom Alloy Surfaces: Effect of Surface Oxygen Coverage on Selectivity

The selective oxidation of methanol to formaldehyde on Cu surfaces is an important and well-studied reaction. However, a systematic analysis of product selectivity as a function of oxygen coverage on Cu(111) and Cu-based single-atom alloys (SAAs) has not been previously reported. In this work, we present a comprehensive investigation of deuterated methanol (CD 3 OH) partial oxidation on Cu(111) and 1% PtCu(111) SAA surfaces as a function of preadsorbed oxygen coverage. Temperature-programmed desorption (TPD) and X-ray photoelectron spectroscopy (XPS) reveal that isolated Pt atoms inhibit the initial surface oxidation of Cu(111) under low oxygen exposures. Despite this difference in oxidation kinetics, the product selectivity remains largely unaffected: on both Cu(111) and PtCu(111), formaldehyde (CD 2 O) is the predominant partial oxidation product over a broad range of oxygen coverages. The selectivity toward formaldehyde peaks at intermediate oxygen coverages (∼0.3 monolayers, ML), indicating the existence of an optimal oxygen loading for partial oxidation. Notably, the similar product selectivities on Cu(111) and PtCu(111) over a range of surface oxygen coverage indicate that Pt single atoms do not significantly alter the reaction pathway or shift the optimal oxygen coverage for formaldehyde formation. Control experiments confirm that Cu(111) is unreactive toward methanol in the absence of oxygen, while PtCu(111) surfaces produce a small amount of formaldehyde even when oxygen is not preadsorbed, indicating that isolated Pt atoms facilitate O−H activation at below 150 K, leading to H 2 desorption, followed by C−D activation at higher temperatures (∼350 K). Density functional theory (DFT)-based calculations show that Pt atoms increase the O 2 dissociation barrier relative to Cu(111), consistent with the observed inhibition of oxidation at low exposures. Overall, this work provides the first detailed selectivity map for methanol oxidation on oxidized Cu(111) and PtCu(111) SAA surfaces. By linking classical mechanistic insights such as methoxy- and formate-mediated pathways with single-atom alloy catalyst design, this work demonstrates that while Pt substitution modulates the oxidation kinetics and oxygen binding, the overall selectivity toward formaldehyde is governed primarily by oxygen coverage. These findings underscore the potential of isolated dopants to tune surface oxidation behavior without compromising the intrinsic partial oxidation selectivity of copper-based catalysts.

36 MATERIALS SCIENCE↗
NASA NTRS1986

Houseplants, Indoor Air Pollutants, and Allergic Reactions

The technology of using houseplant leaves for reducing volatile organics inside closed facilities has been demonstrated with formaldehyde and benzene. Philodendrons are among the most effective plants tested to date. Philodendron domesticum had demonstrated the ability to remove formaldehyde from small experimental chambers at a rate of 4.31 micro-g/sq cm leaf surface area with initial starting concentrations of 22 ppm. At initial starting concentrations of 2.3 ppm a formaldehyde removal rate of 0.57 micro-g/sq cm was achieved during a 24 hour test. Aleo vera demonstrated a much higher formaldehyde efficiency removal rate than Philodendron domesticum at low formaldehyde concentrations. During a 24 hour exposure period 5 ppm of formaldehyde were reduced to 0.5 ppm demonstrating a removal efficiency rate of 3.27 micro-g/sq cm. Removal efficiency rates can be expected to decrease with concentration levels because fewer molecules of chemicals come in contact with the leaf surface area. Several centimeters of small washed gravel should be used to cover the surface of pot plants when large numbers of plants are kept in the home. The reason for this is to reduce the exposed area of damp potting soil which encourages the growth of molds (fungi). The leaves of Philodendron domesticum and golden pothos (Scindapsus aureus) have also demonstrated their ability to remove benzene and carbon monoxide from closed chambers. A combination of activated carbon and plant roots have demonstrated the greatest potential for removing large volumes of volatile organics along with smoke and possible radon from closed systems. Although fewer plants are required for this concept a mechanical blower motor must be used to pull or push the air through the carbon-root filter. NASA studies on motor sizes and bioregeneration rates should be completed by 1988.

Wolverton, B. C.↗
NASA NTRS2018

Enantiomer Excesses in Meteoritic Organic Compounds: a Role for Radiation-Magnetism?

Carbonaceous chondrites contain an insoluble “macromolecular” carbon phase as well as discrete soluble organic compounds including amino acids and sugar derivatives. Both the macromolecular carbon and the sugar derivatives are thought to have formed through aqueous formaldehyde chemistry. Formaldehyde is a ubiquitous molecule in interstellar space environments and therefore its chemistry was likely important during the formation of the Earth and other planets. It was also likely delivered throughout Earth's history: it is found in comets and (asteroidal) meteorites. Among the reactions of formaldehyde, those in water are thought to be an important part of the primordial route to today’s nucleic acids, DNA and RNA. A plausible pre-biotic path to these biopolymers would begin with the "formose" reaction, the self-reaction of formaldehyde in an alkaline aqueous medium. Formaldehyde's inclusion in the young solar system’s planets would have provided a relatively fast route to a variety of hydroxylated compounds related to nucleic acids and metabolism, including sugars, sugar acids, sugar alcohols, and formaldehyde polymers.

Cooper, G.↗
DOE OSTI2023

Synthesis of Carbohydrates from Methanol Using Electrochemical Partial Oxidation over Palladium with the Integrated Formose Reaction

Electrochemically derived multicarbon products are a golden target for valorization of captured carbon dioxide due to the potential of turning a waste product into useful commodity chemicals with renewable energy sources. As a tantalizing approach toward their synthesis, the formose reaction utilizes catalytic condensation of formaldehyde to generate carbohydrates. Furthermore, while a sustainable approach to artificial carbohydrate production through electrochemical generation of formaldehyde is desirable, to date, it has not been fully realized. Here, we study the electrocatalytic conversion of methanol to formaldehyde on palladium with faradaic efficiency of over 90% at 0.9 V vs Ag/AgCl and with the partial current density of nearly 3 mA cm -2 at 1.6 V vs Ag/AgCl. We observe the concurrent generation of palladium oxides as a consequence of the high overpotentials employed, which may partially explain the higher selectivity toward the partial oxidation product. Moreover, we demonstrate that formaldehyde produced electrochemically from methanol is feasible for formose reactions without the need for further purification, achieving 21-28% carbon conversion to carbohydrates. This process, therefore, represents a potential avenue for the electrochemical generation of formaldehyde and its utilization in generating multicarbon products inaccessible by other electrocatalytic means.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2003

STS-113/11A: Assessment of Air Quality in the International Space Station (ISS) and Space Shuttle Based on Samples Returned in December 2002 and in May 2003 aboard Soyuz 5

The toxicological assessments of grab sample canisters (GSCs) returned aboard STS-l13 and Soyuz 5 are reported. Analytical methods have not changed from earlier reports. Surrogate standard recoveries from the GSCs were 79-120% except as noted in the table. One sample was returned with the valve opened. The two general criteria used to assess air quality are the total-non-methane-volatile organic hydrocarbons (NMVOCs) and the total T-value (minus the CO2 and formaldehyde contributions). Control of atmospheric alcohols is important to the water recovery system engineers, hence total alcohols (including acetone) are also shown for each sample. Octafluoropropane (OFP) has leaked from heat-exchange units in large quantities, so its concentration is tracked separately. Because formaldehyde is quantified from sorbent badges, its concentration is also listed separately. The table shows that the air quality in general was acceptable for crew respiration through the middle of December 2002. No conclusions can be made about the air quality after that date due to NASA's inability to return air samples from the ISS . Alcohols are not being controlled to the recently lowered guideline of 5 mg/m3, which was recommended to protect the water recovery systems. The airlock sample was taken during the regeneration of Met ox canisters in the adjacent Node. The trace pollutants were not increased above background; however, inspection of table 1 in the appendix shows a CO2 concentration of 17,000 mg/cu m, which is a relatively high concentration, but still below the 24-hour SMAC of23,000 mg/cu m. The control of OFP continues to be adequate at least through December 2002. Formaldehyde concentrations suggest that the high levels that were being found in the Lab atmosphere have subsided. This is probably attributable to the restoration of IMV in early February 2003 . Before the obstructing material was removed from ducts the Lab formaldehyde concentrations approached 0.06 mg/cu m, whereas after the repair the levels were near 0.04 mg/m3 . This does not mean that local sources in the Lab have been reduced, only that the excess of formaldehyde produced in the Lab is distributed into the whole volume of the ISS.

James, John T.↗
NASA NTRS2003

Assessment of Air Quality in the International Space Station (ISS) and Space Shuttle Based on Samples Returned Aboard STS-ll1 (UF2) in June 2002

The toxicological assessments of grab sample canisters (GSCs) and 2 solid sorbent air samplers (SSASs) returned aboard STS-111 are reported. Analytical methods have not changed from earlier reports. Surrogate standard recoveries from the GSCs were 86-106% and 62% to 136 % from the SSASs; 2 tubes with low surrogate recoveries were not reported. Pressure tracking indicated no leaks in the canisters during analysis. Recoveries from lab and trip controls for formaldehyde analyses ranged from 87 to 96%. The two general criteria used to assess air quality are the total-non-methane-volatile organic hydrocarbons (NMVOCs) and the total T-value (minus the CO2 and formaldehyde contributions). Because of the inertness of Freon 218 (octafluoropropane, OFP), Its contribution to the NMVOC is subtracted and tabulated separately. Control of atmospheric alcohols is important to the water recovery system engineers, hence total alcohols (including acetone) are also shown for each sample. Because formaldehyde is quantified from sorbent badges, its concentration is listed separately. The table shows that the air quality in general was acceptable for crew respiration; however, certain values shown in bold require further explanation. The 1.05 T value on 2/28/02 was caused by an unusually high measurement ofhexamethylcyc1otrisiloxane (T value = 0.50), which is not a concern. The MPLM T value of 1.42 and the alcohol level of 7.5 mg/cu m were due to an overall polluted atmosphere, which was expected at first entry. The major T-value component was carbon monoxide at a contribution of 0.44 units. Since the crew was only exposed momentarily to the polluted atmosphere, no health effects are expected. The formaldehyde value of 0.060 mg/cu m found in the Lab sample from 3/27/02 is cause for concern because the Lab consistently shows higher concentrations of formaldehyde than the SM and occasionally the concentrations are above the acceptable guideline. Levels of OFP have remained low, suggesting that no further leaks of the SM air conditioner have occurred.

James, John T.↗
DOE OSTI2023

AMORE-Isoprene v1.0: a new reduced mechanism for gas-phase isoprene oxidation

Abstract. Gas-phase oxidation of isoprene by ozone (O3) and the hydroxyl (OH) and nitrate (NO3) radicals significantly impacts tropospheric oxidant levels and secondary organic aerosol formation. The most comprehensive and up-to-date chemical mechanism for isoprene oxidation consists of several hundred species and over 800 reactions. Therefore, the computational expense of including the entire mechanism in large-scale atmospheric chemical transport models is usually prohibitive, and most models employ reduced isoprene mechanisms ranging in size from ∼ 10 to ∼ 200 species. We have developed a new reduced isoprene oxidation mechanism using a directed-graph path-based automated model reduction approach, with minimal manual adjustment of the output mechanism. The approach takes as inputs a full isoprene oxidation mechanism, the environmental parameter space, and a list of priority species which are protected from elimination during the reduction process. Our reduced mechanism, AMORE-Isoprene (where AMORE stands for Automated Model Reduction), consists of 12 species which are unique to the isoprene mechanism as well as 22 reactions. We demonstrate its performance in a box model in comparison with experimental data from the literature and other current isoprene oxidation mechanisms. AMORE-Isoprene's performance with respect to predicting the time evolution of isoprene oxidation products, including isoprene epoxydiols (IEPOX) and formaldehyde, is favorable compared with other similarly sized mechanisms. When AMORE-Isoprene is included in the Community Regional Atmospheric Chemistry Multiphase Mechanism 1.0 (CRACMM1AMORE) in the Community Multiscale Air Quality Model (CMAQ, v5.3.3), O3 and formaldehyde agreement with Environmental Protection Agency (EPA) Air Quality System observations is improved. O3 bias is reduced by 3.4 ppb under daytime conditions for O3 concentrations over 50 ppb. Formaldehyde bias is reduced by 0.26 ppb on average for all formaldehyde measurements compared with the base CRACMM1. There was no significant change in computation time between CRACMM1AMORE and the base CRACMM. AMORE-Isoprene shows a 35 % improvement in agreement between simulated IEPOX concentrations and chamber data over the base CRACMM1 mechanism when compared in the Framework for 0-D Atmospheric Modeling (F0AM) box model framework. This work demonstrates a new highly reduced isoprene mechanism and shows the potential value of automated model reduction for complex reaction systems.

58 GEOSCIENCES↗
NASA NTRS1995

Oligonucleotides as probes for studying polymerization reactions in dilute aqueous solution. 2: Polycondensations

We have prepared a (P-32)-labeled oligonucleotide probe carrying a ureido (-NH-CO-NH2) function at its 3'-terminus. This labeled oligomer was used to study polycondensations of urea and formaldehyde and of various phenols and formaldehyde in aqueous solution. The formation of formaldehyde copolymers attached to the amido-function of the probe was monitored by gel electrophoresis. Our results are generally in agreement with those obtained using conventional techniques. Our method is suitable for monitoring potentially prebiotic polycondensation reactions involving formaldehyde.

Kolb, Vera↗
NASA NTRS2001

The sugar model: catalysis by amines and amino acid products

Ammonia and amines (including amino acids) were shown to catalyze the formation of sugars from formaldehyde and glycolaldehyde, and the subsequent conversion of sugars to carbonylcontaining products under the conditions studied (pH 5.5 and 50 degrees C). Sterically unhindered primary amines were better catalysts than ammonia, secondary amines, and sterically hindered primary amines (i.e. alpha-aminoisobutyric acid). Reactions catalyzed by primary amines initially consumed formaldehyde and glycolaldehyde about 15-20 times faster than an uncatalyzed control reaction. The amine-catalyzed reactions yielded aldotriose (glyceraldehyde), ketotriose (dihydroxyacetone), aldotetroses (erythrose and threose), ketotetrose (erythrulose), pyruvaldehyde, acetaldehyde, glyoxal, pyruvate, glyoxylate, and several unindentified carbonyl products. The concentrations of the carbonyl products, except pyruvate and ketotetrose, initially increased and then declined during the reaction, indicating their ultimate conversion to other products (like larger sugars or pyruvate). The uncatalyzed control reaction yielded no pyruvate or glyoxylate, and only trace amounts of pyruvaldehyde, acetaldehyde and glyoxal. In the presence of 15 mM catalytic primary amine, such as alanine, the rates of triose and pyruvaldehyde of synthesis were about 15-times and 1200-times faster, respectively, than the uncatalyzed reaction. Since previous studies established that alanine is synthesized from glycolaldehyde and formaldehyde via pyruvaldehyde as its direct precursor, the demonstration that the alanine catalyzes the conversion of glycolaldehyde and formaldehyde to pyruvaldehyde indicates that this synthetic pathway is capable of autocatalysis. The relevance of this synthetic process, named the Sugar Model, to the origin of life is discussed.

Acetaldehyde/analogs & derivatives/chemistry↗
NASA NTRS1995

Oligonucleotides as probes for studying polymerization reactions in dilute aqueous solution: II. Polycondensations

We have prepared a [32P]-labeled oligonucleotide probe carrying a ureido (-NH-CO-NH2) function at its 3'-terminus. This labeled oligomer was used to study polycondensations of urea and formaldehyde and of various phenols and formaldehyde in aqueous solution. The formation of formaldehyde copolymers attached to the amido-function of the probe was monitored by gel electrophoresis. Our results are generally in agreement with those obtained using conventional techniques. Our method is suitable for monitoring potentially prebiotic polycondensation reactions involving formaldehyde.

NASA Discipline Exobiology↗
NASA NTRS2007

STS 118 Return Samples: Assessment of Air Quality aboard the Shuttle (STS-118) and International Space Station

The toxicological assessments of 2 grab sample canisters (GSCs) and one pair of formaldehyde badges from the Shuttle are reported. Analytical methods have not changed from earlier reports. The recoveries of the 3 surrogates (C-13-acetone, fluorobenzene, and chlorobenzene) from the 2 GSCs averaged 120, 117, and 122 %, respectively. Three formaldehyde controls averaged 98% recovery. The Shuttle atmosphere was acceptable for human respiration. The toxicological assessment of 8 GSCs and 6 pairs of formaldehyde badges from the ISS is shown. The recoveries of the 3 standards (as listed above) from the GSCs averaged 99, 99 and 99%, respectively. Three formaldehyde control badges averaged 98% recovery. Based on these limited samples, the ISS atmosphere is acceptable for human respiration. The alcohol levels were well controlled throughout the period of sampling.

James, John T.↗