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At least 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
NASA NTRS2012

Detection of Carbon Monoxide Using Polymer-Composite Films with a Porphyrin-Functionalized Polypyrrole

Post-fire air constituents that are of interest to NASA include CO and some acid gases (HCl and HCN). CO is an important analyte to be able to sense in human habitats since it is a marker for both prefire detection and post-fire cleanup. The need exists for a sensor that can be incorporated into an existing sensing array architecture. The CO sensor needs to be a low-power chemiresistor that operates at room temperature; the sensor fabrication techniques must be compatible with ceramic substrates. Early work on the JPL ElectronicNose indicated that some of the existing polymer-carbon black sensors might be suitable. In addition, the CO sensor based on polypyrrole functionalized with iron porphyrin was demonstrated to be a promising sensor that could meet the requirements. First, pyrrole was polymerized in a ferric chloride/iron porphyrin solution in methanol. The iron porphyrin is 5, 10, 15, 20-tetraphenyl-21H, 23Hporphine iron (III) chloride. This creates a polypyrrole that is functionalized with the porphyrin. After synthesis, the polymer is dried in an oven. Sensors were made from the functionalized polypyrrole by binding it with a small amount of polyethylene oxide (600 MW). This composite made films that were too resistive to be measured in the device. Subsequently, carbon black was added to the composite to bring the sensing film resistivity within a measurable range. A suspension was created in methanol using the functionalized polypyrrole (90% by weight), polyethylene oxide (600,000 MW, 5% by weight), and carbon black (5% by weight). The sensing films were then deposited, like the polymer-carbon black sensors. After deposition, the substrates were dried in a vacuum oven for four hours at 60 C. These sensors showed good response to CO at concentrations over 100 ppm. While the sensor is based on a functionalized pyrrole, the actual composite is more robust and flexible. A polymer binder was added to help keep the sensor material from delaminating from the electrodes, and carbon was added to improve the conductivity of the material.

Homer, Margie L.↗
NASA NTRS1989

The abundances of atomic carbon and carbon monoxide compared with visual extinction in the Ophiuchus molecular cloud complex

Emission from the 492 GHz lines of C I have been observed toward six positions in the Ophiuchus molecular cloud complex for which accurate visual extinctions are available. The column density of C I increases with A(V) to greater than 2 x 10 to the 17th/sq cm at 100 mag, the column-averaged fractional abundance reaches a peak of about 2.2 x 10 to the -5th for A(V) in the range 4-11 mag and the column-averaged abundance ratio of C I to CO decreases with A(V) from about 1 at 2 mag to greater that about 0.03 at 100 mag. These results imply that, while C I is not the primary reservoir of gaseous carbon even at cloud edges, its fractional abundance remains high for at least 10 mag into the cloud and may be significant at even greater depths.

Frerking, Margaret A.↗
NASA NTRS1975

A survey of carbon monoxide emission in dark clouds

Results are reported of a CO and (C-13)O survey of 68 dark clouds from the Lynds catalog. CO was detected in 63 of the 64 sources in which it was searched for, and the (C-13)O line was seen in 52 of 55 clouds. There is a rather narrow distribution of CO peak line radiation temperatures about a mean of 6 K; this may reflect the presence of a roughly uniform kinetic temperature of 9.5 K in the sources. Despite the probably subthermal excitation temperature of the (C-13)O transition observed, derived (C-13)O column densities are most likely good to within a factor of 2. Typical CO column densities for the clouds surveyed are 5 x 10 to the 17-th power per sq cm, assuming a terrestrial carbon isotope ratio. All 68 clouds have previously been studied by Dieter in 6-cm H2CO absorption; a comparison of line widths shows the (C-13)O lines to generally be wider than their formaldehyde counterparts. Possible explanations of this fact in terms of internal cloud motions are discussed.

Dickman, R. L.↗
DOE OSTI2024

Catalytic Reduction of Carbon Monoxide to Liquid Fuels with Recyclable Hydride Donors

Solar light absorption and catalysis are physically separated processes in natural photosynthesis. Natural cofactors, such as nicotinamide adenine dinucleotides (NADH), transport electrons and hydrogen to regulate and activate enzymes at remote locations. The physical separation of light absorption from catalysis provides some inspiration for artificial photosynthesis. One rather extreme implementation is to use copper wires to transport carriers from photovoltaic cells to dark electrodes, where catalysis occurs. Indeed, with a futuristic electrical grid powered solely by photovoltaics, solar capture could be separated from catalysis by hundreds of miles. An alternative approach, that bares more similarity to natural photosynthesis, employs mobile NADH/NAD + -like species that shuttle between the light absorber and a proximate, yet unilluminated, location where catalysis occurs. Additionally, such a remote approach to solar photocatalysis was recently proposed for the reduction of carbon oxides, CO 2 and CO, to methanol by cascade catalysis. This developing artificial photosynthetic approach offers the promise of catalytic generation of methanol and oxygen gas with sunlight as the sole energy source and CO 2 and water as the only chemical feedstocks. This Viewpoint evaluates the strengths and weaknesses of this approach with an emphasis on CO reduction catalysis with photorecyclable hydride donors while looking forward to what might reasonably be achieved with continued research.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1978

The ratio of carbon monoxide to molecular hydrogen in interstellar dark clouds

LTE (C-13)O column densities are compared with the corresponding values of beam-convolved visual extinction at more than 100 locations within 38 different interstellar dark clouds. A roughly linear correlation is found to exist between these two quantities for visual extinctions in the range from about 1.5 to 5 mag. It is argued that this correlation can be extended up to about 10 mag and that the standard gas-to-extinction ratio can be expected to remain valid in the sources studied. The correlation of LTE (C-13)O column density with visual extinction is used to obtain an equation for the H2 column density associated with a given (C-13)O column density. It is shown that if the clouds studied are assumed to be chemically homogeneous, the equation obtained implies that at least 12% of all gas-phase carbon is in the form of CO. Comparison of the observational data with various theories proposed for molecule formation in dark clouds indicates that Langer's (1977) ion-molecule scheme accounts well for the observations when the fractionation channel of Watson et al. (1976) is included.

Dickman, R. L.↗
NASA NTRS2011

Daily and Hourly Variability in Global Fire Emissions and Consequences for Atmospheric Model Predictions of Carbon Monoxide

Attribution of the causes of atmospheric trace gas and aerosol variability often requires the use of high resolution time series of anthropogenic and natural emissions inventories. Here we developed an approach for representing synoptic- and diurnal-scale temporal variability in fire emissions for the Global Fire Emissions Database version 3 (GFED3). We distributed monthly GFED3 emissions during 2003-2009 on a daily time step using Moderate Resolution Imaging Spectroradiometer (MODIS)-derived measurements of active fires from Terra and Aqua satellites. In parallel, mean diurnal cycles were constructed from Geostationary Operational Environmental Satellite (GOES) active fire observations. We found that patterns of daily variability in fires varied considerably across different biomes, with short but intense periods of daily emissions in boreal ecosystems and lower intensity (but more continuous) periods of bunting in savannas. On diurnal timescales, our analysis of the GOES active fires indicated that fires in savannas, grasslands, and croplands occurred earlier in the day as compared to fires in nearby forests. Comparison with Total Carbon Column Observing Network (TCCON) and Measurements of Pollution in the Troposphere (MOPITT) column CO observations provided evidence that including daily variability in emissions moderately improved atmospheric model simulations, particularly during the fire season and near regions with high levels of biomass burning. The high temporal resolution estimates of fire emissions developed here may ultimately reduce uncertainties related to fire contributions to atmospheric trace gases and aerosols. Important future directions include reconciling top-down and bottom up estimates of fire radiative power and integrating burned area and active fire time series from multiple satellite sensors to improve daily emissions estimates.

Mu, M.↗
NASA NTRS2011

Daily and 3-hourly Variability in Global Fire Emissions and Consequences for Atmospheric Model Predictions of Carbon Monoxide

Attribution of the causes of atmospheric trace gas and aerosol variability often requires the use of high resolution time series of anthropogenic and natural emissions inventories. Here we developed an approach for representing synoptic- and diurnal-scale temporal variability in fire emissions for the Global Fire Emissions Database version 3 (GFED3). We disaggregated monthly GFED3 emissions during 2003.2009 to a daily time step using Moderate Resolution Imaging Spectroradiometer (MODIS) ]derived measurements of active fires from Terra and Aqua satellites. In parallel, mean diurnal cycles were constructed from Geostationary Operational Environmental Satellite (GOES) Wildfire Automated Biomass Burning Algorithm (WF_ABBA) active fire observations. Daily variability in fires varied considerably across different biomes, with short but intense periods of daily emissions in boreal ecosystems and lower intensity (but more continuous) periods of burning in savannas. These patterns were consistent with earlier field and modeling work characterizing fire behavior dynamics in different ecosystems. On diurnal timescales, our analysis of the GOES WF_ABBA active fires indicated that fires in savannas, grasslands, and croplands occurred earlier in the day as compared to fires in nearby forests. Comparison with Total Carbon Column Observing Network (TCCON) and Measurements of Pollution in the Troposphere (MOPITT) column CO observations provided evidence that including daily variability in emissions moderately improved atmospheric model simulations, particularly during the fire season and near regions with high levels of biomass burning. The high temporal resolution estimates of fire emissions developed here may ultimately reduce uncertainties related to fire contributions to atmospheric trace gases and aerosols. Important future directions include reconciling top ]down and bottom up estimates of fire radiative power and integrating burned area and active fire time series from multiple satellite sensors to improve daily emissions estimates.

Mu, M.↗
NASA NTRS1977

Carbon monoxide observations of a rotating dust globule

Results are presented for observations of the J = 1-0 rotational lines of (C-12)(O-16), (C-13)(O-16), and (C-12)(O-18) at rest frequencies of 115.2712, 110.2014, and 109.7822 GHz, respectively, in the direction of the small dust cloud B361. For a distance of 350 pc, the cloud is found to have an overall radius of about 1.2 pc and a core radius of about 0.4 pc. The core density is estimated to be about 10,000 per cu cm, and it is shown that the density at the center is high enough for the CO to be collisionally thermalized. A cloud temperature of 8.5 K is determined, a lower limit of 125 solar masses is placed on the core mass, and it is suggested that most of the mass is contained within the inner 6% of the cloud volume. The dense inner core is found to be rotating with a velocity gradient of 2.9 km/s per pc. A n(CO)/n(H) ratio that is no more than 0.07 of the solar n(C)/n(H) ratio is derived, indicating that most of the carbon present in the cloud is not in the form of CO.

Milman, A. S.↗
DOE OSTI2025

Cryogenic Carbon Monoxide Oxidation on Cuprous Oxide

Performing oxidation reactions at low temperatures using earth-abundant materials is crucial for advancing solutions for sustainable chemistry. CO oxidation serves as a benchmark reaction to characterize oxidation and to advance fundamental concepts in surface chemistry. While there are several examples of CO oxidation occurring on metal oxides at low temperatures, from 300 K to ∼200 K, reactivity in the cryogenic temperature regime typically requires a metal nanoparticle on a metal oxide. Here, we show oxygen atoms on the (111) facet of Cu 2 O react with CO to form CO 2 at temperatures below 100 K. Combining spectroscopic experimental evidence with calculations, we propose a low barrier path for CO oxidation at reconstructed surface sites on Cu 2 O(111). This finding is a rare example of an earth-abundant metal oxide, in this case copper, that can provide highly reactive multifunctional sites, enabling both adsorption and reaction fundamental steps toward the efficient heterogeneous oxidation of chemicals.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Enhancing the Carbon Monoxide Oxidation Performance through Surface Defect Enrichment of Ceria-Based Supports for Platinum Catalyst

Effective synthesis and application of single-atom catalysts on supports lacking enough defects remain a significant challenge in environmental catalysis. Herein, we present a universal defect-enrichment strategy to increase the surface defects of CeO 2 -based supports through H 2 reduction pretreatment. The Pt catalysts supported by defective CeO 2 -based supports, including CeO 2 , CeZrO x , and CeO 2 /Al 2 O 3 (CA), exhibit much higher Pt dispersion and CO oxidation activity upon reduction activation compared to their counterpart catalysts without defect enrichment. Specifically, Pt is present as embedded single atoms on the CA support with enriched surface defects (CA-HD) based on which the highly active catalyst showing embedded Pt clusters (Pt C ) with the bottom layer of Pt atoms substituting the Ce cations in the CeO 2 surface lattice can be obtained through reduction activation. Embedded PtC can better facilitate CO adsorption and promote O 2 activation at Pt C –CeO 2 interfaces, thereby contributing to the superior low-temperature CO oxidation activity of the Pt/CA-HD catalyst after activation.

36 MATERIALS SCIENCE↗