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Peters, L. K.

Publications and source records attributed to Peters, L. K..

An Eulerian transport/transformation/removal model for SO2 and sulfate. I - Model development. II - Model calculation of SO(x) transport in the eastern United States

A three-dimensional, time dependent Eulerian atmospheric SO2 and sulfate transport/transformation/removal model is described and applied to the eastern U.S. The model was developed in anticipation of increased input to the atmospheric sulfur content by coal-burning power plants in the near future and is intended as an aid in identifying sources of SO2. The Eulerian transport model incorporates functions for chemical transformations, dry deposition, spatial topographical variations, spatial and temporal variations of mixing layer heights, the wind field, eddy diffusivities, deposition velocities, and temperature and water concentration profiles. Attention is also given to the SO2 photochemical oxidation mechanism and rates. Results from a 72-hr simulation of SO(x) transport over the eastern U.S., using actual 1974 meteorological data, illustrate the model's capability to depict interactions between emissions, transport, chemistry and removal. Concentration distributions are demonstrated to have significant spatial and temporal variations.

Carmichael, G. R.↗

Analysis of the error associated with grid representation of point sources

The steady-state, three-dimensional transport equation for inert pollutant dispersion in the atmosphere is solved analytically to obtain expressions for pollutant concentrations from both a point source and a rectangular area source. The results of this analysis have application to numerical grid models in which the smallest resolvable source is the size of a single grid. The concentrations at ground level along the plume centerline from the two types of sources are in close agreement with each other at distances greater than 10 km downwind when the horizontal dimension of the rectangular source is not less than 100 m. The dimension of the source in the vertical direction is held constant at 50 m. Similar results are obtained for concentrations along the plume centerline at the effective stack height. When the size of the source in the crosswind direction is increased to 1 km, good agreement between the two concentrations is obtained for downwind distances over 60 km for the ground level case and over 140 km for the concentration at stack height level. For the horizontal dimension equal to 10 km, good agreement between the two cases is only obtained at extremely large downwind distances at both the stack height and ground levels.

Karamchandani, P.↗

A modeling study of SO(x)-NO(x)-hydrocarbon plumes and their transport to the background troposphere

The behavior of a complex urban plume and its transport to the background troposphere are analyzed in terms of a model including sulfur oxide, nitrogen oxide and hydrocarbon (HC) photochemistry. A reaction mechanism consisting of 73 NO(x), SO(x) and HC reactions is employed in a model taking account of plume dilution, entrainment, deposition and the development of a diurnal mixing layer from a ground-based nocturnal inversion. When simulation results are compared with field measurements of the urban plumes leaving St. Louis and Milwaukee, and a power plant within the Milwaukee plume, the predicted concentration profiles of NO(x), SO2 and O3 are found to be in close agreement with the measurement, although agreement with the rate of transformation of SO2 to SO4(2-) is less good. Simulations made for a hypothetical urban location under a range of background concentrations and initial HC concentrations show particulate sulfate concentrations to depend strongly on the HC/NO(x) ratio, indicating that the homogeneous gas-phase transformation may occur at night.

Balko, J. A.↗

The possible role of heterogeneous aerosol processes in the chemistry of CH4 and CO in the troposphere

The effect of particle-gas interactions on the CH4 to CO oxidation sequence in the troposphere is investigated by developing rate expressions for the heterogeneous removal of gaseous species based on the absorption of the species by aerosol particles. The results of this analysis indicate that the homogeneous models describe the tropospheric chemistry of CO and CH4 more accurately than heterogeneous models, which suggests that heterogeneous processes may not be significant in this sequence of chemical reactions. Estimates of the CO and CH4 emission rates are not found to provide a conclusive basis on which to compare the significance of the homogeneous and heterogeneous processes. In addition, the time period during which an aerosol particle is effective in removing a trace gaseous species from the troposphere is determined to vary according to the tropospheric concentration and solubility of the particular gaseous species.

Luther, C. J.↗

An algorithm to generate input data from meteorological and space shuttle observations to validate a CH4-CO model

Objective procedures to analyze data from meteorological and space shuttle observations to validate a three dimensional model were investigated. The transport and chemistry of carbon monoxide and methane in the troposphere were studied. Four aspects were examined: (1) detailed evaluation of the variational calculus procedure, with the equation of continuity as a strong constraint, for adjustment of global tropospheric wind fields; (2) reduction of the National Meteorological Center (NMC) data tapes for data input to the OSTA-1/MAPS Experiment; (3) interpolation of the NMC Data for input to the CH4-CO model; and (4) temporal and spatial interpolation procedures of the CO measurements from the OSTA-1/MAPS Experiment to generate usable contours of the data.

Peters, L. K.↗

The transport of photochemical pollutants to the background troposphere

The considered investigation is concerned with the phenomena occurring as a chemically reacting plume, with specific initial concentrations of NO, NO2, O3, and hydrocarbons, emerges from an urban area and is advected to the background troposphere. A better understanding of the global NOx and hydrocarbon budgets can be realized by determining the fractions of NOx and hydrocarbons that are transported to distances far enough to be considered background. The investigation makes use of a 56-step, lumped kinetic mechanism for photochemical smog, which includes current information on pertinent chemical reactions and rate constants for the reactions.

Bazzell, C. C.↗

Application of the mixing-reaction in series model to NO/x/-O3 plume chemistry

The mixing-reaction in series model developed by Ghodsizadem (1978) is successfully applied to the study of NO oxidation in the near-source portion of the Potomac Electric Company's Morgantown, Maryland power plant plume. The model employs a single parameter. With initial conditions consistent with the plume data measured by Davis et al. (1974) and utilizing the mixing parameter estimated from the study by Shu et al. (1978), the predicted temporal profiles of the ratio of the concentration of NO2 to NO, of NO2 to NO plus NO2, in-plume concentrations of NO and O3, and fraction of NO remaining are consistent with field study data. In addition, the model predicts large deviations from the photostationary state in the near-source portion of the plume, also consistent with field study data. In the far field region of this plume (t greater than approximately 20 min), the mixing processes are essentially complete over much of the plume cross-section.

Carmichael, G. R.↗

Application of a Galerkin finite element method to atmospheric transport problems

Numerical simulation of the movement of a contaminant within the atmosphere presents difficulties due to the multidimensionality of the problem and the fact that the horizontal transport is usually convection dominated, that the boundary conditions are mixed, and that both slow and fast atmospheric chemical reactions can be important. In this study, numerical experiments using a Crank-Nicolson Galerkin finite element method to solve the time-dependent partial differential equations demonstrate the applicability and accuracy of this method for the variety of conditions encountered in atmospheric pollutant modeling. The Crank-Nicolson Galerkin method using piecewise linear, piecewise cubic Hermite polynomials, and upwind finite elements is shown to accurately model the pure convection of initial wave forms. Numerical results studying the interactions of convection, diffusion, chemical reaction, pollutant removal, and the effects of contaminant emission source strength, source location and multiple sources are also presented.

Carmichael, G. R.↗

A model of CO-CH4 global transport/chemistry. I - Chemistry model

A simplified chemistry model was developed to incorporate the CO-CH4 chemistry into the global transport model of these compounds. CO is important because of its effects on atmospheric chemistry and is partly responsible for controlling the hydroxyl radical (OH) concentration in the troposphere. The model includes the photodissociation rate coefficients expressed as functions of solar zenith angle and altitude, and it was applied to determine the sensitivity of the OH concentration to trace gaseous species, such as NOx, O3, and H2O. Also, the concentrations and diurnal variations of OH and HO2, and the contribution of individual reactions to OH generation and consumption were calculated.

Peters, L. K.↗

A model of CO-CH4 global transport/chemistry. II - Preliminary calculation by 1 dimensional model

Calculations of the one-dimensional CO-CH4 transport/chemistry model were performed to investigate the sensitivity of the OH vertical profile to various factors. The boundary conditions at the earth's surface and the tropopause are discussed. The results show that the liquid-phase or soil-phase resistance dominates the mass transfer of both CO and CH4 between the atmosphere and the earth's surface. At the tropopause, the CO and CH4 fluxes are set approximately equal to the value at the previous time step in the numerical calculation. Photolysis rate coefficients that increase with altitude modified the OH vertical profile so that the maximum value was at midtroposphere altitudes. Increasing the CO concentration caused a decrease of the OH concentration, and the OH profile was very sensitive to the NO(x) profiles. The calculated OH profiles are compared with those from other investigations and also with some available measurements. Although the available measurements of the OH profiles are limited, the calculated OH profiles agree fairly well with them.

Kitada, T.↗

The chemistry and transport of methane and carbon monoxide in the troposphere

The present understanding of the physical and chemical behavior of methane, carbon monoxide and the chemical species involved in the conversion of CH4 to CO in the troposphere is reviewed. Following a brief summary of CO and CH4 emission and reactions in urban areas, attention is given to measurements of the spatial and temporal distributions of CO and CH4 in the rural atmosphere, the contribution of the oceans to atmospheric CO and CH4 concentrations, and interactions of CH4 and CO with soils and vegetation. Estimates of the transport of CH4 and CO from the troposphere to the stratosphere are discussed, and photochemical reactions of the constituents are examined. Two- and three-dimensional models for CH4 and CO transport are presented, and possible future variations in atmospheric abundances of the molecules are considered. Finally, present estimates of the global methane and carbon dioxide budgets are summarized, and it is pointed out that, despite the large contribution of anthropogenic sources, the budgets appear to be in balance.

Peters, L. K.↗

Further development of a global pollution model for CO, CH4, and CH2 O

Global tropospheric pollution models are developed that describe the transport and the physical and chemical processes occurring between the principal sources and sinks of CH4 and CO. Results are given of long term static chemical kinetic computer simulations and preliminary short term dynamic simulations.

Peters, L. K.↗

Development of a global pollution model for CO, CH4, and CH2O

The current status of a global pollution model for carbon monoxide, methane, and formaldehyde is described. The physico-chemical action is considered of these three pollutants in the troposphere. This geographic restriction is convenient since the tropopause provides a natural boundary across which little transport occurs. The data on sources and sinks for these pollutants is based on available information and assumptions relative to the major man-made and natural contributions. The distributions and concentrations of methane, formaldehyde, and carbon monoxide in the atmosphere are interrelated by the chemical reactions in which they participate. A chemical kinetic model based on the pseudo-steady state approximation for the intermediate species was developed to account for these reactions. The numerical procedure used to mathematically describe the pollution transport is a mass conservative scheme employing an integral flux approach.

Peters, L. K.↗