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817 records · Page 46
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Degradation and fate of 2,4-dinitroanisole (DNAN) and its intermediates treated with Mg/Cu bimetal: Surface examination with XAS, DFT, and LDI-MS

In this article, a novel Mg-based bimetal reagent (Mg/Cu) was used as an enhanced reductive system to degrade insensitive munition 2,4-dinitroanisole (DNAN), a contaminant found in energetic-laden waste. Degradation of DNAN was significantly impacted by dissolved oxygen and studied in anoxic and oxic bimetal systems (i.e., purging with N 2 , air, or O 2 gas). Degradation occurred through sequential nitroreduction: first one nitro group was reduced (ortho or para) to form short-lived intermediates 2-amino-4-nitroanisole or 4-amino-2-nitroanisole (2-ANAN or 4-ANAN), and then subsequent reduction of the other nitro group formed 2,4-diaminoanisole (DAAN). The nitro-amino intermediates demonstrated regioselective reduction in the ortho position to 2-ANAN; Regioselectivity was also impacted by the anoxic/oxic environment. Under O 2 -purging DNAN degradation rate was slightly enhanced, but most notably O 2 significantly accelerated DAAN generation. DAAN also further degraded only in the oxygenated Mg/Cu system. Adsorption of DNAN byproducts to the reagent occurred regardless of anoxic/oxic condition, resulting in a partition of carbon mass between the adsorbed phase (27%-35%) and dissolved phase (59%-72%). Additional surface techniques were applied to investigate contaminant interaction with Cu. Density functional theory (DFT) calculations identified preferential adsorption structures for DNAN on Cu with binding through two O atoms of one or both nitro groups. X-ray absorption spectroscopy (XAS) measurements determined the oxidation state of catalytic metal Cu and formation of a Cu-O-N bond during treatment. Laser desorption ionization mass spectrometry (LDI-MS) measurements also identified intermediate 2-ANAN adsorbed to the bimetal surface.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2000

Global Warming Estimation from MSU: Correction for Drift and Calibration Errors

Microwave Sounding Unit (MSU) radiometer observations in Ch 2 (53.74 GHz), made in the nadir direction from sequential, sun-synchronous, polar-orbiting NOAA morning satellites (NOAA 6, 10 and 12 that have about 7am/7pm orbital geometry) and afternoon satellites (NOAA 7, 9, 11 and 14 that have about 2am/2pm orbital geometry) are analyzed in this study to derive global temperature trend from 1980 to 1998. In order to remove the discontinuities between the data of the successive satellites and to get a continuous time series, first we have used shortest possible time record of each satellite. In this way we get a preliminary estimate of the global temperature trend of 0.21 K/decade. However, this estimate is affected by systematic time-dependent errors. One such error is the instrument calibration error. This error can be inferred whenever there are overlapping measurements made by two satellites over an extended period of time. From the available successive satellite data we have taken the longest possible time record of each satellite to form the time series during the period 1980 to 1998 to this error. We find we can decrease the global temperature trend by about 0.07 K/decade. In addition there are systematic time dependent errors present in the data that are introduced by the drift in the satellite orbital geometry arises from the diurnal cycle in temperature which is the drift related change in the calibration of the MSU. In order to analyze the nature of these drift related errors the multi-satellite Ch 2 data set is partitioned into am and pm subsets to create two independent time series. The error can be assessed in the am and pm data of Ch 2 on land and can be eliminated. Observations made in the MSU Ch 1 (50.3 GHz) support this approach. The error is obvious only in the difference between the pm and am observations of Ch 2 over the ocean. We have followed two different paths to assess the impact of the errors on the global temperature trend. In one path the entire error is placed in the am data while in the other it is placed in the pm data. Global temperature trend is increased or decreased by about 0.03 K/decade depending upon this placement. Taking into account all random errors and systematic errors our analysis of MSU observations leads us to conclude that a conservative estimate of the global warming is 0. 11 (+-) 0.04 K/decade during 1980 to 1998.

Prabhakara, C.↗
DOE OSTI2021

Resonant amplification of enzymatic chemical oscillations by oscillating flow

Using theory and simulation, we analyzed the resonant amplification of chemical oscillations that occur due to externally imposed oscillatory fluid flows. The chemical reactions are promoted by two enzyme-coated patches located sequentially on the inner surface of a pipe that transports the enclosed chemical solution. In the case of diffusion-limited systems, the period of oscillations in chemical reaction networks is determined by the rate of the chemical transport, which is diffusive in nature and, therefore, can be effectively accelerated by the imposed fluid flows. In this work, we first identify the natural frequencies of the chemical oscillations in the unperturbed reaction–diffusion system and, then, use the frequencies as a forcing input to drive the system to resonance. We demonstrate that flow-induced resonance can be used to amplify the amplitude of the chemical oscillations and to synchronize their frequency to the external forcing. In particular, we show that even 10% perturbations in the flow velocities can double the amplitude of the resulting chemical oscillations. Particularly, effective control can be achieved for the two-step chemical reactions where during the first half-period, the fluid flow accelerates the chemical flux toward the second catalytic patch, while during the second half-period, the flow amplifies the flux to the first patch. The results can provide design rules for regulating the dynamics of coupled reaction–diffusion processes and can facilitate the development of chemical reaction networks that act as chemical clocks.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2000

Global Warming Estimation from MSU: Correction for Drift and Calibration Errors

Microwave Sounding Unit (MSU) radiometer observations in Ch 2 (53.74 GHz), made in the nadir direction from sequential, sun-synchronous, polar-orbiting NOAA morning satellites (NOAA 6, 10 and 12 that have approximately 7am/7pm orbital geometry) and. afternoon satellites (NOAA 7, 9, 11 and 14 that have approximately 2am/2pm orbital geometry) are analyzed in this study to derive global temperature trend from 1980 to 1998. In order to remove the discontinuities between the data of the successive satellites and to get a continuous time series, first we have used shortest possible time record of each satellite. In this way we get a preliminary estimate of the global temperature trend of 0.21 K/decade. However, this estimate is affected by systematic time-dependent errors. One such error is the instrument calibration error eo. This error can be inferred whenever there are overlapping measurements made by two satellites over an extended period of time. From the available successive satellite data we have taken the longest possible time record of each satellite to form the time series during the period 1980 to 1998 to this error eo. We find eo can decrease the global temperature trend by approximately 0.07 K/decade. In addition there are systematic time dependent errors ed and ec present in the data that are introduced by the drift in the satellite orbital geometry. ed arises from the diurnal cycle in temperature and ec is the drift related change in the calibration of the MSU. In order to analyze the nature of these drift related errors the multi-satellite Ch 2 data set is partitioned into am and pm subsets to create two independent time series. The error ed can be assessed in the am and pm data of Ch 2 on land and can be eliminated. Observation made in the MSU Ch 1 (50.3 GHz) support this approach. The error ec is obvious only in the difference between the pm and am observations of Ch 2 over the ocean. We have followed two different paths to assess the impact of the error ec on the global temperature trend. In one path the entire error ec is placed in the am data while in the other it is placed in the pm data. Global temperature trend is increased or decreased by approximately 0.03 K/decade depending upon this placement. Taking into account all random errors and systematic errors our analysis of MSU observations leads us to conclude that a conservative estimate of the global warming is 0. 11 (+/-) 0.04 K/decade during 1980 to 1998.

Prabhakara, C.↗
NASA NTRS2017

Imaging a Free-Geometry Magma Reservoir Using FEM-Based Linear Inverse Modeling of InSAR Data: Application to Rabaul Caldera, Papua New Guinea

We test an innovative inversion scheme using Green’s functions from an array of pressure sources embedded in finite-element method (FEM) models to image, without assuming an a-priori geometry, the composite and complex shape of a volcano deformation source. We invert interferometric synthetic aperture radar (InSAR) data to estimate the pressurization and shape of the magma reservoir of Rabaul caldera, Papua New Guinea. The results image the extended shallow magmatic system responsible for a broad and long-term subsidence of the caldera between 2007 February and 2010 December. Elastic FEM solutions are integrated into the regularized linear inversion of InSAR data of volcano surface displacements in order to obtain a 3-D image of the source of deformation. The Green’s function matrix is constructed from a library of forward line-of-sight displacement solutions for a grid of cubic elementary deformation sources. Each source is sequentially generated by removing the corresponding cubic elements from a common meshed domain and simulating the injection of a fluid mass flux into the cavity, which results in a pressurization and volumetric change of the fluidfilled cavity. The use of a single mesh for the generation of all FEM models avoids the computationally expensive process of non-linear inversion and remeshing a variable geometry domain. Without assuming an a-priori source geometry other than the configuration of the 3-D grid that generates the library of Green’s functions, the geodetic data dictate the geometry of the magma reservoir as a 3-D distribution of pressure (or flux of magma) within the source array. The inversion of InSAR data of Rabaul caldera shows a distribution of interconnected sources forming an amorphous, shallow magmatic system elongated under two opposite sides of the caldera. The marginal areas at the sides of the imaged magmatic system are the possible feeding reservoirs of the ongoing Tavurvur volcano eruption of andesitic products on the east side and of the past Vulcan volcano eruptions of more evolved materials on the west side. The interconnection and spatial distributions of sources correspond to the petrography of the volcanic products described in the literature and to the dynamics of the single and twin eruptions that characterize the caldera. The ability to image the complex geometry of deformation sources in both space and time can improve our ability to monitor active volcanoes, widen our understanding of the dynamics of active volcanic systems and improve the predictions of eruptions.

Inverse theory↗
NASA NTRS2017

Imaging the Complex Geometry of a Magma Reservoir Using Fem-Based Linear Inverse Modeling of InSAR Data: Application to Rabaul Caldera, Papua New Guinea

We test an innovative inversion scheme using Green’s functions from an array of pressure sources embedded in finite-element method (FEM) models to image, without assuming an a-priori geometry, the composite and complex shape of a volcano deformation source. We invert interferometric synthetic aperture radar (InSAR) data to estimate the pressurization and shape of the magma reservoir of Rabaul caldera, Papua New Guinea. The results image the extended shallow magmatic system responsible for a broad and long-term subsidence of the caldera between 2007 February and 2010 December. Elastic FEM solutions are integrated into the regularized linear inversion of InSAR data of volcano surface displacements in order to obtain a 3-D image of the source of deformation. The Green’s function matrix is constructed from a library of forward line-of-sight displacement solutions for a grid of cubic elementary deformation sources. Each source is sequentially generated by removing the corresponding cubic elements from a common meshed domain and simulating the injection of a fluid mass flux into the cavity, which results in a pressurization and volumetric change of the fluid-filled cavity. The use of a single mesh for the generation of all FEM models avoids the computationally expensive process of non-linear inversion and remeshing a variable geometry domain. Without assuming an a-priori source geometry other than the configuration of the 3-D grid that generates the library of Green’s functions, the geodetic data dictate the geometry of the magma reservoir as a 3-D distribution of pressure (or flux of magma) within the source array. The inversion of InSAR data of Rabaul caldera shows a distribution of interconnected sources forming an amorphous, shallow magmatic system elongated under two opposite sides of the caldera. The marginal areas at the sides of the imaged magmatic system are the possible feeding reservoirs of the ongoing Tavurvur volcano eruption of andesitic products on the east side and of the past Vulcan volcano eruptions of more evolved materials on the west side. The interconnection and spatial distributions of sources correspond to the petrography of the volcanic products described in the literature and to the dynamics of the single and twin eruptions that characterize the caldera. The ability to image the complex geometry of deformation sources in both space and time can improve our ability to monitor active volcanoes, widen our understanding of the dynamics of active volcanic systems and improve the predictions of eruptions.

Inverse theory↗
NASA NTRS1996

Unsteady, Transonic Flow Around Delta Wings Undergoing Coupled and Natural Modes Response: A Multidisciplinary Problem

The unsteady, three-dimensional Navier-Stokes equations coupled with the Euler equations of rigid-body dynamics are sequentially solved to simulate and analyze the aerodynamic response of a high angle of attack delta wing undergoing oscillatory motion. The governing equations of fluid flow and dynamics of the multidisciplinary problem are solved using a time-accurate solution of the laminar, unsteady, compressible, full Navier- Stokes equations with the implicit, upwind, Roe flux-difference splitting, finite-volume scheme and a four-stage Runge-Kutta scheme, respectively. The primary model under consideration consists of a 65 deg swept, sharp-edged, cropped delta wing of zero thickness at 20 deg angle of attack. In a freestream of Mach 0.85 and Reynolds number of 3.23 x 10(exp 6), the flow over the upper surface of the wing develops a complex shock system which interacts with the leading-edge primary vortices producing vortex breakdown. The effect of the oscillatory motion of the wing on the vortex breakdown and overall aerodynamic response is detailed to provide insight to the complicated physics associated with unsteady flows and the phenomenon of wing rock. Forced sinusoidal single and coupled mode rolling and pitching motion is presented for the wing in a transonic freestream. The Reynolds number, frequency of oscillation, and the phase angle are varied. Comparison between the single and coupled mode forced rolling and pitching oscillation cases illustrate the effects of coupling the motion. This investigation shows that even when coupled, forced rolling oscillation at a reduced frequency of 2(pi) eliminates the vortex breakdown which results in an increase in lift. The coupling effect for in phase forced oscillations show that the lift coefficient of the pitching-alone case and the rolling-moment coefficient of the rolling-alone case dominate the resulting response. However, with a phase lead in the pitching motion, the coupled motion results in a non-periodic response of the rolling moment. The second class of problems involve releasing the wing in roll to respond to the flowfield. Two models of sharp-edged delta wings, the previous 65 deg swept model and an 80 deg swept, sharp-edged delta wing, are used to observe the aerodynamic response of a wing free to roll in a transonic and subsonic freestream, respectively. These cases demonstrate damped oscillations, self-sustained limit cycle oscillations, and divergent rolling oscillations. Ultimately, an active control model using a mass injection system was applied on the surface of the wing to suppress the self-sustained limit cycle oscillation known as wing rock. Comparisons with experimental investigations complete this study, validating the analysis and illustrating the complex details afforded by computational investigations.

Menzies, Margaret Anne↗