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DOE OSTI2017

Butanol Separation from Humid CO 2 -Containing Multicomponent Vapor Mixtures by Zeolitic Imidazolate Frameworks

Butanol is a promising renewable fuel and feedstock. A major challenge in fermentative butanol production is to find a cost-effective butanol separation process from dilute aqueous solutions, usually an acetone-butanol-ethanol (ABE) mixture. Nanoporous zeolitic imidazolate frameworks (ZIFs) have shown potential for alcohol separation from dilute solutions. However, little is known about butanol separation from multicomponent mixtures using ZIFs, including the effects of the humid acid gas (CO 2 ) used to sparge the fermenter and generate the vapor product stream. We present a study of butanol separation by ZIF-8, ZIF-90, ZIF-71 and hybrid ZIF-8–90 and ZIF-8–71 adsorbents with binary butanol/water and multicomponent ABE feeds. To obtain reliable structure–property relations for ZIF adsorbents in realistic conditions, we combine multicomponent vapor breakthrough with structural, textural, and stability characterization techniques in humid CO 2 environments. In the absence of CO 2 , more hydrophobic materials such as ZIF-8, ZIF-8 55 -71 45 , ZIF-8 70 -90 30 , and ZIF-71 are found to be excellent candidates with butanol/water selectivities >10 and butanol capacities >3.5 mmol/g. However, in the presence of humid CO 2 , all the materials except ZIF-71 are found to degrade. The mechanistic aspects of this degradation are studied by FTIR spectroscopy and explained based upon acid gas attack of Zn–N coordinate bonds. ZIF-71 emerges as an excellent candidate owing to its acid gas stability, good butanol adsorption capacity, and selectivity. Vapor breakthrough with a model ABE solution demonstrates the high butanol selectivity of ZIF-71 relative to acetone, ethanol, and water and the recovery of a 65 mol % butanol product by desorption at 453 K. Finally, this study highlights the importance of determining structure–property relationships of MOF/ZIF materials in realistic multicomponent conditions, and the importance of acid gas stability in their applications.

09 BIOMASS FUELS↗

NASA NTRS1981

Calculation of two-dimensional inlet flow fields by an implicit method including viscous effects: User's manual

Inlet flow fields for airbreathing missiles are calculated by the adaptation of a two dimensional computational method developed for the flow around airfoils. A supersonic free stream is assumed to allow the forebody calculation to be uncoupled from the inlet calculation. The inlet calculation employs an implicit, time marching finite difference procedure to solve the thin layer Navier-Stokes equations formulated in body fitted coordinates. The mathematical formulation of the problem and the solution algorithm are given. Numerical stability and accuracy as well as the initial and boundary conditions used are discussed. Instructions for program use and operation along with the overall program logic are also given.

Biringen, S.↗

NASA NTRS1993

Relationship between transition and modes of instability in supersonic boundary layers

The relationship between the predicted transition location and the first and second modes of instability in two-dimensional supersonic boundary-layer flow on a flat plate is examined. Linear stability theory and the N-factor criterion are used to predict transition location. The effect of heat transfer is also studied; the results demonstrate that the transition reversal phenomenon can be explained by the opposite effect of cooling on the first and second modes of instability. Compressibility of destabilizing at free-stream Mach numbers of 2 to 3.5. The predicted transition location is due to the oblique first modes of instability, up to free-stream Mach numbers between 6 and 6.5. At higher Mach numbers, the predicted transition location is due to a combination of two-dimensional first and second modes of instability.

Masad, Jamal A.↗

NASA NTRS1996

Hypersonic Boundary Layer Stability over a Flared Cone in a Quiet Tunnel

Hypersonic boundary layer measurements were conducted over a flared cone in a quiet wind tunnel. The flared cone was tested at a freestream unit Reynolds number of 2.82x106/ft in a Mach 6 flow. This Reynolds number provided laminar-to-transitional flow over the model in a low-disturbance environment. Point measurements with a single hot wire using a novel constant voltage anemometry system were used to measure the boundary layer disturbances. Surface temperature and schlieren measurements were also conducted to characterize the laminar-to-transitional state of the boundary layer and to identify instability modes. Results suggest that the second mode disturbances were the most unstable and scaled with the boundary layer thickness. The integrated growth rates of the second mode compared well with linear stability theory in the linear stability regime. The second mode is responsible for transition onset despite the existence of a second mode sub-harmonic. The sub-harmonic wavelength also scales with the boundary layer thickness. Furthermore, the existence of higher harmonics of the fundamental suggests that non-linear disturbances are not associated with high free stream disturbance levels.

Lachowicz, Jason T.↗

DOE OSTI2019

Improving Alkylamine Incorporation in Porous Polymer Networks through Dopant Incorporation

The industrial scale capture of CO 2 from flue gas streams is becoming an increasingly important environmental issue. However, many of the existing CO 2 capture systems either have regenerative energy demands that are too high or are cost prohibitive. A promising solution is the utilization of functionalized solid sorbents, such as porous polymer networks (PPNs). PPNs are attractive due to their inherent structural stability, flexibility, high surface areas, and ability to incorporate various functional groups within the chemical scaffold. Herein, a low cost, scalable alternative to common carbon capture systems using a series of robust mesoporous melamine-formaldehyde resins (mPMFs) loaded with active alkylamine sorbents is presented, which is dubbed as the PPN-150 family. The variants within this material class are differentiated based on the incorporation of functionalized dopants; small molecules added at low molar percent concentrations to impart additional functionality into the PPN in order to achieve low cost noncovalent tethering of alkylamines. The cyanuric acid doped PPN-151-DETA (DETA = diethylenetriamine) demonstrate unique features such as improved cycling capacity and heat of adsorption. To show its scalability, PPN-151-DETA is successfully synthesized at the 250 g scale without loss of the sorbent properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2015

Lifecycle assessment of microalgae to biofuel: Comparison of thermochemical processing pathways

Microalgae are currently being investigated as a renewable transportation fuel feedstock based on various advantages that include high annual yields, utilization of poor quality land, does not compete with food, and can be integrated with various waste streams. This study focuses on directly assessing the impact of two different thermochemical conversion technologies on the microalgae to biofuel process through life cycle assessment. A system boundary of a “well to pump” (WTP) is defined and includes sub-process models of the growth, dewatering, thermochemical bio-oil recovery, bio-oil stabilization, conversion to renewable diesel, and transport to the pump. Models were validated with experimental and literature data and are representative of an industrial-scale microalgae to biofuel process. Two different thermochemical bio-oil conversion systems are modeled and compared on a systems level, hydrothermal liquefaction (HTL) and pyrolysis. The environmental impact of the two pathways were quantified on the metrics of net energy ratio (NER), defined here as energy consumed over energy produced, and greenhouse gas (GHG) emissions. Results for WTP biofuel production through the HTL pathway were determined to be 1.23 for the NER and GHG emissions of -11.4 g CO 2-eq (MJ renewable diesel) -1 . WTP biofuel production through the pyrolysis pathway results in a NER of 2.27 and GHG emissions of 210 g CO2 eq (MJ renewable diesel)-1. The large environmental impact associated with the pyrolysis pathway is attributed to feedstock drying requirements and combustion of co-products to improve system energetics. Discussion focuses on a detailed breakdown of the overall process energetics and GHGs, impact of modeling at laboratory- scale compared to industrial-scale, environmental impact sensitivity to engineering systems input parameters for future focused research and development and a comparison of results to literature.

09 BIOMASS FUELS↗

DOE OSTI2015

Technetium incorporation into goethite (α-FeOOH): An atomic-scale investigation

During the processing of low-activity radioactive waste to generate solid waste forms (e.g., glass), technetium-99 (Tc) is of concern because of its volatility. A variety of materials are under consideration to capture Tc from waste streams, including the iron oxyhydroxide, goethite (α-FeOOH), which was experimentally shown to sequester Tc(IV). This material could ultimately be incorporated into glass or other low-temperature waste form matrices. However, questions remain regarding the incorporation mechanism for Tc(IV) in goethite, which has implications for predicting the long-term stability of Tc in waste forms under changing conditions. Here, quantum-mechanical calculations were used to evaluate the energy of five different charge-compensated Tc(IV) incorporation scenarios in goethite. The two most stable incorporation mechanisms involve direct substitution of Tc(IV) onto Fe(III) lattice sites and charge balancing either by removing one nearby H+ (i.e., within 5 Å), or by creating an Fe(III) vacancy when substituting 3 Tc(IV) for 4 Fe(III), with the former being preferred over the latter relative to gas-phase ions. When corrections for hydrated references phases are applied, the Fe(III)-vacancy mechanism becomes more energetically competitive. Calculated incorporation energies and optimized bond-lengths are presented. Proton movement is observed to satisfy under-coordinated bonds surrounding vacancies in the goethite structure.

atomic-scale modeling↗

NASA NTRS1975

Viscous flow solutions with a cubic spline approximation

A cubic spline approximation is used for the solution of several problems in fluid mechanics. This procedure provides a high degree of accuracy even with a nonuniform mesh, and leads to a more accurate treatment of derivative boundary conditions. The truncation errors and stability limitations of several typical integration schemes are presented. For two-dimensional flows a spline-alternating-direction-implicit (SADI) method is evaluated. The spline procedure is assessed and results are presented for the one-dimensional nonlinear Burgers' equation, as well as the two-dimensional diffusion equation and the vorticity-stream function system describing the viscous flow in a driven cavity. Comparisons are made with analytic solutions for the first two problems and with finite-difference calculations for the cavity flow.

Rubin, S. G.↗

NASA NTRS1978

The effect of cycle variables on the emissions and performance of lean premixed gas turbine primary zone combustor

Experiments were conducted in which a stream of premixed propane and air was burned under conditions representative of gas-turbine operation. Emissions of NOx, CO, and unburned hydrocarbons were measured over a range of combustor inlet temperature (600-1000 K), pressure (5-30 atm), and residence time (1-3 msec) at equivalence ratios from 0.7 down to the lean stability limit. At inlet temperatures of 800 and 1000 K, NOx emissions displayed little sensitivity to pressure. At an inlet temperature of 600 K, observed NOx levels dropped markedly with decreasing pressure for pressures below 20 atm. NOx levels were proportional to combustor residence time, and formation rate was principally a function of adiabatic flame temperature. For adiabatic flame temperatures of 2050 K and higher, CO reached chemical equilibrium within 2 msec. Unburned hydrocarbon species dropped to a negligible level within 2 msec regardless of inlet temperature, pressure, or equivalence ratio. For a combustor residence time of 2.5 msec, combustion inefficiency became less than 0.01% at an adiabatic flame temperature of 2050 K. The maximum combustion inefficiency observed was of the order of 1% and corresponded to conditions near the lean stability limit.

Roffe, G.↗

NASA NTRS1985

Electromagnetic hot ion beam instabilities - Quasi-linear theory and simulation

This paper considers the quasi-linear theory of the right- and left-hand resonant electromagnetic instabilities driven by a hot ion beam streaming parallel to a magnetic field in a homogeneous Vlasov plasma. Using the single-mode approximation, the time evolutions of important parameters are obtained to show that for the range of parameters considered, reduction of the beam speed and formation of temperature anisotropies are the most significant factors in the quasi-linear stabilization process. Combining both instabilities in a quasi-linear study is found to produce a roughly equal mixture of both polarizations and relatively isotropic conditions for tenuous beam densities and low initial beam drift speeds. Computer simulations are used to compare with the quasi-linear results. The simulations justify the single-mode assumption, verify that quasi-linear changes are the means of saturation for the parameter range of concern, and check the nonlinear evolution of the system when both modes are present.

Rogers, B.↗

NASA NTRS1986

Stability analysis of double-peaked proton distribution functions in the solar wind

Twelve proton velocity distribution functions as measured for different solar wind speeds by the plasma analyzer at the Helios spacecraft are modeled analytically by a superposition of two bi-Maxwellians. The stability of these distributions is investigated by solving the linear dispersion equation for parallel propagation of both left- and right-hand polarized modes. Due to the temperature anisotropy of the main proton component the presence of the resonant left-hand ion cyclotron instability is found to be typical for high-speed streams and is independent of an ion beam. The results indicate that the ratio of the beam density to total particle density and the beam drift velocity are generally close to the threshold values necessary to drive a highly unstable nonresonant right-hand mode. This instability is found for one proton distribution and is a consequence of the beam particles. It is concluded that both the ion cyclotron instability and the ion beam instability act as a regulating mechanism on the shape of solar wind double humped proton distribution functions.

Leubner, Manfred P.↗

NASA NTRS1989

Calculations of rotational flows using stream function

The stream function equation is solved for steady two-dimensional (and axisymmetric) rotational flows. Both finite differences and finite volumes discretization techniques are studied, using generalized body fitted coordinates and unstructured staggered grids, respectively. For inviscid transonic flows, a new artificial viscosity scheme which does not produce any artificial vorticity is introduced, for the stability of the mixed flow calculations and for capturing shocks. The solution of Euler equations, in primitive variables, are also considered. The effects of the artificial viscosity and numerical boundary conditions on the total enthalpy and the vorticity distributions are demonstrated.

Hafez, M.↗

NASA NTRS1992

Streamwise vortices in heated boundary layers

The nonlinear instability of the boundary layer on a heated flat plate placed in an oncoming flow is investigated. Such flows are unstable to stationary vortex instabilities and inviscid traveling wave disturbances governed by the Taylor-Goldstein equation. For small temperature differences the Taylor-Goldstein equation reduces to Rayleigh's equation. When the temperature difference between the wall and free stream is small the preferred mode of instability is a streamwise vortex. It is shown in this case that the vortex, assumed to be of small wavelength, restructures the underlying mean flow to produce a profile which can be massively unstable to inviscid traveling waves. The mean state is shown to be destabilized or stabilized to inviscid waves depending on whether the Prandtl number is less or greater than unity.

Hall, Philip↗

NASA NTRS2004

Experimental Investigation of Diffuser Hub Injection to Improve Centrifugal Compressor Stability

Results from a series of experiments to investigate whether centrifugal compressor stability could be improved by injecting air through the diffuser hub surface are reported. The research was conducted in a 4:1 pressure ratio centrifugal compressor configured with a vane-island diffuser. Injector nozzles were located just upstream of the leading edge of the diffuser vanes. Nozzle orientations were set to produce injected streams angled at 8, 0 and +8 degrees relative to the vane mean camber line. Several injection flow rates were tested using both an external air supply and recirculation from the diffuser exit. Compressor flow range did not improve at any injection flow rate that was tested. Compressor flow range did improve slightly at zero injection due to the flow resistance created by injector openings on the hub surface. Leading edge loading and semi-vaneless space diffusion showed trends similar to those reported earlier from shroud surface experiments that did improve compressor flow range. Opposite trends are seen for hub injection cases where compressor flow range decreased. The hub injection data further explain the range improvement provided by shroud-side injection and suggest that different hub-side techniques may produce range improvement in centrifugal compressors.

Skoch, Gary J.↗

NASA NTRS2020

Mechanisms of Stationary Crossflow Instability Growth and Breakdown Induced by Forward-Facing Steps

An experimental study is performed to determine the mechanisms by which a forward-facing step impacts the growth and breakdown to turbulence of the stationary cross-flow instability. Particle image velocimetry measurements are obtained in the boundary layer of a 30◦swept flat plate with a pressure body. Step heights range from 53 % to 71 % of the boundary-layer thickness. The critical step height is approximately 60 % of the boundary-layer thickness for the current study, although it is also shown that the critical step height depends on the initial amplitude of the stationary cross-flow vortices. For the critical cases, the stationary cross-flow amplitude grows sharply downstream of the step, decays for a short region and then grows again. The initial growth region is linear, and can be explained primarily through the impact of the step on the mean flow. Namely, the step causes abrupt changes to the mean flow, resulting in large values of wall-normal shear, as well as highly inflectional profiles, due to either cross-flow reversal, separation or both. These inflectional profiles are highly unstable for the stationary cross-flow. Additionally,the reversed flow regions are significantly modulated by the stationary cross-flow vortices. The second region of growth occurs due to the stationary-cross-flow-induced modulation of the shear layer, which leads to multiple smaller wavelength stream wise vortices. High-frequency fluctuations indicate that the unsteady transition mechanism for the critical cases relates to the shedding of vortices downstream of reattachment of the modulated separated regions.

boundary layer stability↗

DOE OSTI2020

High-loading single Pt atom sites [Pt-O(OH) x ] catalyze the CO PROX reaction with high activity and selectivity at mild conditions

The preferential oxidation of CO (PROX) in hydrogen-rich fuel gas streams is an attractive option to remove CO while effectively conserving energy and H 2 . However, high CO conversion with concomitant high selectivity to CO 2 but not H 2 O is challenging. Here, we report the synthesis of high-loading single Pt atom (2.0 weight %) catalysts with oxygen-bonded alkaline ions that stabilize the cationic Pt. The synthesis is performed in aqueous solution and achieves high Pt atom loadings in a single-step incipient wetness impregnation of alumina or silica. Promisingly, these catalysts have high CO PROX selectivity even at high CO conversion (~99.8% conversion, 70% selectivity at 110°C) and good stability under reaction conditions. These findings pave the way for the design of highly efficient single-atom catalysts, elucidate the role of –OH species in CO oxidation, and confirm the absence of a support effect for our case.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1975

A cubic spline approximation for problems in fluid mechanics

A cubic spline approximation is presented which is suited for many fluid-mechanics problems. This procedure provides a high degree of accuracy, even with a nonuniform mesh, and leads to an accurate treatment of derivative boundary conditions. The truncation errors and stability limitations of several implicit and explicit integration schemes are presented. For two-dimensional flows, a spline-alternating-direction-implicit method is evaluated. The spline procedure is assessed, and results are presented for the one-dimensional nonlinear Burgers' equation, as well as the two-dimensional diffusion equation and the vorticity-stream function system describing the viscous flow in a driven cavity. Comparisons are made with analytic solutions for the first two problems and with finite-difference calculations for the cavity flow.

Rubin, S. G.↗

NASA NTRS1986

Transition to unstable ion flow in parallel electric fields

The stability of ionospheric O(+)-H(+) outflows accelerated by a nonambipolar parallel electric field is considered under conditions where the ion motion initially develops adiabatically and the ambient plasma is vertically stratified with an effective temperature that increases with altitude. Such conditions are expected near the bottom of the auroral acceleration region where ion and electron streaming instabilities first develop. It is shown for a particular equilibrium profile that the differentially accelerated ion flows become unstable within about 100 km from their entry point in the acceleration region. At O(+)/H(+) density ratios less than about 9, the instability is dominated by a violent H(+)-O(+) two-stream interaction which couples the O(+) and H(+) acoustic modes, and which mediates a transition to nonadiabatic acceleration. At higher altitudes and/or larger O(+)/H(+) density ratios, a much weaker resonant instability exists, which is driven by the relative drift between electrons and O(+) or H(+) ions. The results suggest that the H(+)-O(+) two-stream instability may be a viable mechanism for heating upflowing auroral ions.

Bergmann, R.↗