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During this brief project period, we investigated the reactivity of nickel-substituted azurin and nickel-substituted ferredoxin as models of acetyl coenzyme A synthase (ACS) and carbon monoxide dehydrogenase (CODH).
Experimental intensity information is combined with numerically obtained vibrational wave functions in a nonlinear least squares fitting procedure to obtain the ground electronic state electric-dipole-moment function of carbon monoxide valid in the range of nuclear oscillation (0.87 to 1.01 A) of about the V = 38th vibrational level. Mechanical anharmonicity intensity factors, H, are computed from this function for delta V + = 1, 2, 3, with or = to 38.
Experimental intensity information is combined with numerically obtained vibrational wave functions in a nonlinear least-squares fitting procedure to obtain the ground electronic state electric dipole moment function of carbon monoxide valid in the range of nuclear oscillation (0.87-1.91 A) of about the V = 38th vibrational level. Vibrational transition matrix elements are computed from this function for Delta V = 1, 2, 3 with V not more than 38.
A new algorithm has been developed which permits, for the first time, real time data reduction of nadir measurements taken with a gas filter correlation radiometer to determine tropospheric carbon monoxide concentrations. The algorithm significantly reduces the complexity of the equations to be solved while providing accuracy comparable to line-by-line calculations. The method is based on a regression analysis technique using a truncated power series representation of the primary instrument output signals to infer directly a weighted average of trace gas concentration. The results produced by a microcomputer-based implementation of this technique are compared with those produced by the more rigorous line-by-line methods. This algorithm has been used in the reduction of Measurement of Air Pollution from Satellites, Shuttle, and aircraft data.
We present the progress toward an analytical performance model of a 2.3 micron infrared correlation radiometer (IRCRg) prototype subsystem for a future geostationary space-borne instrument. The prototype is designed specifically to measure carbon monoxide (CO) from geostationary orbit. NASA's Geostationary Coastal and Air Pollution Events (GEO-CAPE) mission, one of the United States Earth Science and Applications Decadal Survey missions, specifies the use of infrared correlation radiometry to measure CO in two spectral regions for this mission. GEO-CAPE will use the robust IRCR measurement technique at geostationary orbit, nearly 50 times farther away than the Terra/MOPITT orbit, to determine hourly changes in CO across a continental domain. The abundance of CO in Earth's troposphere directly affects the concentration of hydroxyl, which regulates the lifetimes of many tropospheric pollutants. In addition, CO is a precursor to ozone formation; CO is used as a tracer to study the transport of global and regional pollutants; and CO is used as an indicator of both natural and anthropogenic air pollution sources and sinks. We have structured our development project to enable rapid evaluation of future spaceborne instrument designs. The project is part of NASA's Instrument Incubator Program. We describe the architecture of the performance model and the planned evaluation of the performance model using laboratory test data.
The North Atlantic Ocean is bordered by continents which may each, under the influence of seasonal weather patterns, act as sources of natural and anthropogenic trace gas and particulate species. Photochemically active species such as carbon monoxide (CO) react to form ozone (O3), a species of critical importance in global climate change. CO is sparingly soluble in water, and the relatively long lifetime of CO in the troposphere makes this species an ideal tracer of air masses with origin over land. We have measured CO using a nondispersive infrared gas filter correlation analyzer at Mace Head on the west coast of Ireland nearly continuously since August 9, 1991. Measurements of CO were acquired at 20-sec resolution and recorded as 60-sec averages. Daily, monthly, and diurnal variation data characteristics of CO mixing ratios observed at this site are reported. Depending on source regions of air parcels passing over this site, 60-min concentrations of CO range from clean air values of approximately 90 ppbv to values in excess of 300 ppbv. Data characterizing the correlation between 60-min CO and O3 mixing ratio data observed at this site are reported also.
The goal of the MOPITT experiment is to enhance our knowledge of the lower atmosphere system and particularly how it interacts with the surface/ocean/biomass systems. The particular focus is the distribution, transport, sources and sinks of carbon monoxide and methane in the troposphere. The MOPITT instrument was launched on EOS TERRA satellite December 18, 1999. After the launch and until March 22, 2000 the MOPITT instrument was in engineering and calibration mode. Beginning March 23, 2000 through May 6, 2001 the instrument was in a science measurement mode with some calibration breaks. On May 7, 2001 a criocooler on a side B died and channels 1 - 4 became inoperational. The MOPITT resumed its scientific measurements on August 25, 2001 with channels 5 - 8. With some calibration breaks the instrument currently provides the data. The project has three elements to it: hardware, data analysis and modeling. The MOPITT instrument, on the NASA EOS Terra satellite, measures the upwelling infrared radiance. Using the technique of correlation spectroscopy, information regarding the distribution of atmospheric CO and CH4 can be extracted. By using appropriate data analysis techniques, concentration profiles of CO are currently obtained on a global basis at a reasonably high horizontal (approximately 22km) and vertical resolution (approximately 3km). Column amounts of methane will be derived over the sunlit side of the orbit. These profiles are assimilated into models to study the chemistry and dynamics of CO, CH4 and other constituents of the lower atmosphere.
The effect of combustor operating conditions on the conversion of fuel-bound nitrogen (FBN) to nitrogen oxides NO sub x was analytically determined. The effect of FBN and of operating conditions on carbon monoxide (CO) formation was also studied. For these computations, the combustor was assumed to be a two stage, adiabatic, perfectly-stirred reactor. Propane-air was used as the combustible mixture and fuel-bound nitrogen was simulated by adding nitrogen atoms to the mixture. The oxidation of propane and formation of NO sub x and CO were modeled by a fifty-seven reaction chemical mechanism. The results for NO sub x and CO formation are given as functions of primary and secondary stage equivalence ratios and residence times.
Evidence is presented that many of the weak features observed with International Ultraviolet Explorer (IUE) in the far-ultraviolet (1150-2000 A) spectrum of the archetype red giant Arcturus (K2 III) are A-X fourth positive bands of carbon monoxide excited by chromospheric emissions of O I, C I, and H I. The appearance of fluorescent CO bands near the wavelength of commonly used indicators of high-temperature (T greater than 20,000 K) plasma, such as C II at wavelength 1335 and C IV at wavelength 1548, introduces a serious ambiguity in diagnosing the presence of hot material in the outer atmospheres of the cool giants by means of low-dispersion IUE spectra.
Faint, diffuse emissions near 1380 A in deeply exposed IUE spectrograms of the red giant Arcturus very likely are associated with bands of the A-X fourth-positive system of carbon monoxide, fluoresced by multiplet UV2 of neutral oxygen near 1305 A. Numerical simulations indicate that the strength of the CO bands is exceedingly sensitive, in the best available one-dimensional model of the chromosphere of Arcturus, to a delicate balance between the rapid inward attenuation of the oxygen radiation field and the rapid outward decline of the molecular absorptivity. The fortuitous character of the overlap region in the single-component model argues that one should also consider the possibility that the pumping occurs in a highly inhomogeneous chromosphere, of the type proposed in previous studies of Arcturus based on observations of the infrared absorption bands of CO.
Water solvation plays a critical role in a wide range of electrochemical transformations, but its role is often convoluted since water is typically used as both a solvent and a proton source. Here, we experimentally control water speciation and activity using aprotic solvent media during the carbon monoxide reduction reaction (CORR). Remarkably, we show that aprotic solvents that support microheterogeneous water–water clusters lead to significant amounts of CORR products (methane and ethylene) with a maximum ethylene Faradaic efficiency of 22% in acetonitrile (χ H 2 O = 0.2). In contrast, microhomogeneous systems–where water integrates into the solvents’ intermolecular binding network and has lower activity–primarily support the undesired hydrogen evolution reaction (HER). As a result, insights gained expand our understanding of water activity and nonaqueous electrolyte design for other important transformation reactions beyond CO reduction, such as CO2RR and HER.
The Single Field-of-View (SFOV) retrieval products from CrIS on SNPP have a spatial resolution of 14 km. These products include temperature, water vapor, clouds and trace gases, such as ozone (O3) and carbon monoxide (CO). Such high-resolution sounder products enable us to make process-oriented analysis of CO emission and transport from Australia’s unprecedented wildfires as well as the O3 production along the transport of fire plumes in the end of 2019 to early 2020. Comparisons of CO with other satellite products, such as AIRS, TROPOMI and MOPPIT, show a good agreement of CO from these space-borne observations. The mean difference SFOV total CO with TROPOMI CO is 0.22%14.0% (R=0.92) and 1.1%17.6% (R=0.87) using data on December, 30, 2019 and January 1, 2020, respectively. This study also demonstrates the advantage of the SFOV CO in capturing the feature of CO transport for air quality study.
A vertically and zonally averaged model of the troposphere has been constructed which calculates photochemical interactions and diffusive North-South transport of trace species. The model can be used to calculate the latitudinal distribution of the source function of a species if its concentration distribution is known. This procedure has been applied to carbon monoxide and large sources have been found outside the industrialized belt in the Northern Hemisphere.
Electrochemical reduction of CO 2 gas is a novel CO 2 utilization technique that has the potential to mitigate the global climate crisis caused by anthropogenic CO 2 emissions, and enable the large-scale storage of energy generated from renewable sources in the form of carbon-based chemicals and fuels. However, due to the complexity of the electrochemical reactions, the explicit first-principles models for CO2 reduction are not available yet, and there has been a limited effort to develop process modeling, optimization and control of CO 2 electrochemical reactors. To this end, a rotating cylinder electrode (RCE) reactor has been constructed at UCLA to understand the mass transfer and reaction kinetics effects separately on the productivity. In the RCE reactor, the applied potential strongly influences the reaction energetics and the electrode rotation speed affects the hydrodynamic boundary layer and modifies the film mass transfer coefficient, which involves convective and diffusive transport. Further, the present work aims to develop a multi-input multi-output (MIMO) control scheme for the RCE reactor that integrates techniques from artificial and recurrent neural network modeling, nonlinear optimization, and process controller design. Specifically, production rates of two products from the experimental reactor, ethylene and carbon monoxide, are controlled by manipulating two inputs, applied potential and catalyst rotation speed. Process dynamics and controllability are analyzed, a feedback control strategy is designed and the controllers are tuned accordingly. The experimental electrochemical cell is employed to gather data for process modeling and implement the multivariable control system. Finally, the experimental results are presented which demonstrate excellent closed-loop performance by the control system and regulation of the outputs at three different set-points including an economically-optimal set-point.
It is noted that the Global Atmospheric Sampling Program (GASP) was intended to establish global baseline values of selected atmospheric constituents that could be used for studies of the dynamics of the sampled region as well as for modeling purposes. Instrument packages were carried on four Boeing 747 aircraft in routine commercial service. Carbon monoxide and ozone data were collected simultaneously from early 1977 to early 1979 when GASP terminated. CO was measured with an infrared absorption analyzer using dual isotope fluorescence. Ozone was measured via absorption of UV light. Correlations between the CO and the O3 are tabulated; they are clearly negative for both troposphere and stratosphere in middle latitudes, indicating that transport processes between the stratosphere and troposphere (discussed) dominate. But in the low latitude troposphere the correlations are positive, indicating the possible influence of photochemical effects.
Computational Fluid Dynamics (CFD) technology has been used to assess the exhaust plume pollutant environment of the RD-170 engine hot-firing on the F1 Test Stand at Marshall Space Flight Center. Researchers know that rocket engine hot-firing has the potential for forming thermal nitric oxides (NOx), as well as producing carbon monoxide (CO) when hydrocarbon fuels are used. Because of the complicated physics involved, however, little attempt has been made to predict the pollutant emissions from ground-based engine testing, except for simplified methods which can grossly underpredict and/or overpredict the pollutant formations in a test environment. The objective of this work, therefore, has been to develop a technology using CFD to describe the underlying pollutant emission physics from ground-based rocket engine testing. This resultant technology is based on a three-dimensional, viscous flow, pressure-based CFD formulation, where wet CO and thermal NOx finite-rate chemistry mechanisms are solved with a Penalty function method.
Fires play a crucial role in several ecosystems. They are routinely used to burn forests in order to accommodate the needs of the expanding population, clear land for agricultural purposes, eliminate weeds and pests, regenerate nutrients in grazing and crop lands and produce energy for cooking and heating purposes. Most of the fires on earth are related to biomass burning in the tropics, although they are not confined to these latitudes. The boreal and tundra regions also experience fires on a yearly basis. The current study examines global fire patterns, Aerosol Optical Thickness (AOT) and carbon monoxide concentrations during April 9-19, 1994. Recently, global Advanced Very High Resolution Radiometer (AVHRR) data at nadir ground spatial resolution of 1 km are made available through the NASA/NOAA Pathfinder project. These data from April 9-19, 1994 are used to map fires over the earth. In summary, our analysis shows that fires from biomass burning appear to be the dominant factor for increased tropospheric CO concentrations as measured by the MAPS. The vertical transport of CO by convective activities, along with horizontal transport due to the prevailing winds, are responsible for the observed spatial distribution of CO.
The characteristics of the Southeastern Virginia urban plume were defined with emphasis on the photon-oxidant species. The measurement area was a rectangle, approximately 150 km by 100 km centered around Cape Charles, Virginia. Included in this area are the cities of Norfolk, Virginia Beach, Chesapeake, Newport News, and Hampton. The area is bounded on the north by Wallops Island, Virginia, and on the south by the Hampton Roads area of Tidewater Virginia. The major axis of the rectangle is oriented in the southwest-northeast direction. The data set includes aircraft measurements for carbon monoxide, methane, nonmethane hydrocarbons, and ozone. The experiment shows that CO can be successfully measured as a tracer gas and used as an index for determining localized and urban plumes. The 1978 data base provided sufficient data to assess an automated chromatograph with flame ionization detection used for measuring methane and nonmethane hydrocarbons in flight.