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DOE OSTI2024

Transitory sensitivity in automatic chemical kinetic mechanism analysis

Abstract Detailed chemical kinetic mechanisms are necessary for resolving many important chemical processes. As the chemistry of smaller molecules has become better grounded and quantum chemistry calculations have become cheaper, kineticists have become interested in constructing progressively larger kinetic mechanisms to model increasingly complex chemical processes. These large kinetic mechanisms prove incredibly difficult to refine and time‐consuming to interpret. Traditional sensitivity analysis on a large mechanism can range from inconvenient to practically impossible without special techniques to reduce the computational cost. We first present a new time‐local sensitivity analysis we term transitory sensitivity analysis. Transitory sensitivity analysis is demonstrated in an example to accurately identify traditionally sensitive reactions at an 18,000x speed up over traditional sensitivities. By fusing transitory sensitivity analysis with more traditional time‐local branching, pathway, and cluster analyses, we develop an algorithm for efficient automatic mechanism analysis. This automatic mechanism analysis at a time point is able to identify the reactions a target is most sensitive to using transitory sensitivity analysis and then propose hypotheses why the reaction might be sensitive using branching, pathway, and cluster analyses. We implement these algorithms within the reaction mechanism simulator (RMS) package, which enables us to report the automatic mechanism analysis results in highly readable text formats and in molecular flux diagrams.

Johnson, Matthew S.↗

DOE OSTI2016

Heat exchanger selection and design analyses for metal hydride heat pump systems

This paper presents a design analysis for the development of highly efficient heat exchangers within stationary metal hydride heat pumps. The design constraints and selected performance criteria are applied to three representative heat exchangers. The proposed thermal model can be applied to select the most efficient heat exchanger design and provides outcomes generally valid in a pre-design stage. Heat transfer effectiveness is the principal performance parameter guiding the selection analysis, the results of which appear to be mildly (up to 13%) affected by the specific Nusselt correlation used. The thermo-physical properties of the heat transfer medium and geometrical parameters are varied in the sensitivity analysis, suggesting that the length of independent tubes is the physical parameter that influences the performance of the heat exchangers the most. The practical operative regions for each heat exchanger are identified by finding the conditions over which the heat removal from the solid bed enables a complete and continuous hydriding reaction. The most efficient solution is a design example that achieves the target effectiveness of 95%.

08 HYDROGEN↗

DOE OSTI2017

Direct Surface and Droplet Microsampling for Electrospray Ionization Mass Spectrometry Analysis with an Integrated Dual-Probe Microfluidic Chip

Ambient mass spectrometry (MS) has revolutionized the way of MS analysis and broadened its application in various fields. This paper describes the use of microfluidic techniques to simplify the setup and improve the functions of ambient MS by integrating the sampling probe, electrospray emitter probe, and online mixer on a single glass microchip. Two types of sampling probes, including a parallel-channel probe and a U-shaped channel probe, were designed for dryspot and liquid-phase droplet samples, respectively. We demonstrated that the microfabrication techniques not only enhanced the capability of ambient MS methods in analysis of dry-spot samples on various surfaces, but also enabled new applications in the analysis of nanoliter-scale chemical reactions in an array of droplets. The versatility of the microchip-based ambient MS method was demonstrated in multiple different applications including evaluation of residual pesticide on fruit surfaces, sensitive analysis of low-ionizable analytes using postsampling derivatization, and high-throughput screening of Ugi-type multicomponent reactions.

Huang, Cong-Min↗

DOE OSTI2026

Dual-loop Solvent-based CCS for Net Negative CO 2 Emissions with Lower Cost

This final technical report details the successful design, construction, and operational validation of an innovative dual-loop CO 2 capture technology designed to achieve deep decarbonization (>99%) from Natural Gas Combined Cycle (NGCC) power plants that results in the electricity with carbon intensity of approximate 42 kg CO 2 -eq/MWh, less than the electricity produced by solar PV. The integrated process couples a primary aqueous solvent (in this project, a water lean solvent – WLS) absorption loop for bulk CO 2 removal with a secondary potassium hydroxide (KOH) polishing loop featuring electrochemical regeneration. This architecture leverages the higher exergy efficiency of the primary loop while utilizing the fastest kinetic of the secondary loop to capture dilute residual CO 2 , achieving an overall capture rate of 99.9% and co-producing pure hydrogen after moisture being condensed and dehydrated. Technical feasibility was established through a comprehensive 2,000-hour experimental campaign on a bench-scale fully-integrated unit (using 4” absorber and 4” stripper) with the feeding flue gas flowrate in the range of 8-20 cfm, confirming the attainment of Technology Readiness Level (TRL) 4. The project executed extensive parametric testing followed by 1,000 hours of continuous steady-state testing, demonstrating exceptional process stability with the electrochemical regenerator exhibiting less than a 10% reduction in electrical conductivity over the duration of the campaign. Operational characterization gathering on the bench unit revealed distinct energy profiles for the hybrid system: the primary loop required approximately 280 kJ mol -1 for bulk removal, while the polishing loop required approximately 1,600 kJ mol -1 specifically when reducing dilute CO 2 concentrations from ~740 ppm down to <50 ppm. (Please note those energy values/numbers can only be viewed as relative relationship and should not be extrapolated as absolute values required for CO 2 capture). Furthermore, dynamic testing validated the system’s flexibility for utility applications, demonstrating a rapid process response time of <30 minutes to changes in flue gas flowrate. Emission monitoring confirmed that the dual-loop architecture effectively mitigates solvent losses, utilizing a water wash to remove entrained aerosols to <1 ppm. The Techno-Economic Analysis (TEA) indicates a cost of capture of $\$$59.3/tonne and a Levelized Cost of Electricity (LCOE) of 71.7 $\$$/MWh at the overall capture efficiency of 99.8% of total carbon in the flue gas stream, with sensitivity analysis identifying an economic optimum when the primary loop captures 97% of the total CO 2 . A Life Cycle Assessment (LCA) confirms the technology’s potential for net-negative emissions, determining a Global Warming Potential (GWP) of 52 kg CO 2 -eq/MWh—significantly lower than the baseline—which further decreases to 42 kg CO 2 -eq/MWh when crediting the displacement of conventional hydrogen production.

03 NATURAL GAS↗

NASA NTRS1991

Thermal analysis of a conceptual design for a 250 We GPHS/FPSE space power system

A thermal analysis has been performed for a 250-We space nuclear power system which combines the US Department of Energy's general purpose heat source (GPHS) modules with a state-of-the-art free-piston Stirling engine (FPSE). The focus of the analysis is on the temperature of the indium fuel clad within the GPHS modules. The thermal analysis results indicate fuel clad temperatures slightly higher than the design goal temperature of 1573 K. The results are considered favorable due to numerous conservative assumptions used. To demonstrate the effects of the conservatism, a brief sensitivity analysis is performed in which a few of the key system parameters are varied to determine their effect on the fuel clad temperatures. It is shown that thermal analysis of a more detailed thermal mode should yield fuel clad temperatures below 1573 K.

Mccomas, Thomas J.↗

NASA NTRS1984

Inversion of vegetation canopy reflectance models for estimating agronomic variables. II - Use of angle transforms and error analysis as illustrated by Suits' model

The technique for inverting a vegetation canopy reflectance model described earlier (Goel and Strebel, 1983) is investigated further. The novel concept of an 'angle transform' is introduced. This concept allows the formation of functions of reflectances at different view zenith and azimuth angles, which are either sensitive or insensitive to a certain agronomic parameter. A proper combination of these functions can allow determination of all the important agronomic and spectral parameters from measured canopy reflectance data. The technique is demonstrated using Suits' (1972) model for homogeneous canopies. It is shown that leaf area index, leaf reflectance and transmittance, and average leaf angle all can be determined from the canopy reflectance at a set of selected view zenith and azimuth angles. A sensitivity analysis of the calculated values to the errors in the data is also carried out. Guidelines are formulated for the number and types of observations required to obtain the values of a particular canopy variable to within a given degree of accuracy for a given level of error in the measurement of canopy reflectance.

Goel, N. S.↗

NASA NTRS2014

Generalized Linear Covariance Analysis

This talk presents a comprehensive approach to filter modeling for generalized covariance analysis of both batch least-squares and sequential estimators. We review and extend in two directions the results of prior work that allowed for partitioning of the state space into solve-for'' and consider'' parameters, accounted for differences between the formal values and the true values of the measurement noise, process noise, and textita priori solve-for and consider covariances, and explicitly partitioned the errors into subspaces containing only the influence of the measurement noise, process noise, and solve-for and consider covariances. In this work, we explicitly add sensitivity analysis to this prior work, and relax an implicit assumption that the batch estimator's epoch time occurs prior to the definitive span. We also apply the method to an integrated orbit and attitude problem, in which gyro and accelerometer errors, though not estimated, influence the orbit determination performance. We illustrate our results using two graphical presentations, which we call the variance sandpile'' and the sensitivity mosaic,'' and we compare the linear covariance results to confidence intervals associated with ensemble statistics from a Monte Carlo analysis.

Navagation↗

NASA NTRS2014

Generalized Linear Covariance Analysis

n/a↗

DOE OSTI2025

Optimal design of power constrained bipolar membrane electrodialysis over a wide brine range

Bipolar membrane electrodialysis enables the in-situ production of high value products (e.g., acid and base) from clean brine, which is essential for a sustainable future. A technoeconomic assessment (TEA) was conducted on extraction of value from brine using the WaterTAP framework to identify optimal cost across a wide design space. Here, in the power constrained regime, increasing supplied salt concentration does not necessarily result in reduced cost or increased NaOH concentration. A detailed analysis elucidates the critical roles of water dissociation, limiting currents, and sodium diffusion play in shaping the landscape of levelized cost. Among these, water splitting predominantly influences the TEA outcomes across most of the optimal design space. Sensitivity analysis further demonstrates that membrane properties controlling water dissociation significantly impact the unit cost. The results indicate that innovations targeting improvements in water disassociation should be prioritised to effectively reduce the levelized cost of product production.

Bipolar membrane electrodialysis↗

DOE OSTI2024

Technoeconomic Analysis of a Direct Air Capture System Utilizing a Looped CaCO3/Ca(OH)2 Process

This presentation reports preliminary results from a screening level techno-economic analysis of a looped CaCO3/Ca(OH)2 direct air capture process. Preliminary results reveal that the looped CaCO3/Ca(OH)2 process may be cost competitive with solvent- and sorbent-based DAC technologies. Results from a detailed sensitivity analysis revealing multiple avenues for system optimization and cost reduction are presented.

Homsy, Sally↗

DOE OSTI2018

Microtopographic control on the ground thermal regime in ice wedge polygons

The goal of this research is to constrain the influence of ice wedge polygon microtopography on near-surface ground temperatures. Ice wedge polygon microtopography is prone to rapid deformation in a changing climate, and cracking in the ice wedge depends on thermal conditions at the top of the permafrost; therefore, feedbacks between microtopography and ground temperature can shed light on the potential for future ice wedge cracking in the Arctic. We first report on a year of sub-daily ground temperature observations at 5 depths and 9 locations throughout a cluster of low-centered polygons near Prudhoe Bay, Alaska, and demonstrate that the rims become the coldest zone of the polygon during winter, due to thinner snowpack. We then calibrate a polygon-scale numerical model of coupled thermal and hydrologic processes against this dataset, achieving an RMSE of less than 1.1 °C between observed and simulated ground temperature. Finally, we conduct a sensitivity analysis of the model by systematically manipulating the height of the rims and the depth of the troughs and tracking the effects on ice wedge temperature. The results indicate that winter temperatures in the ice wedge are sensitive to both rim height and trough depth, but more sensitive to rim height. Rims act as preferential outlets of subsurface heat; increasing rim size decreases winter temperatures in the ice wedge. Deeper troughs lead to increased snow entrapment, promoting insulation of the ice wedge. The potential for ice wedge cracking is therefore reduced if rims are destroyed or if troughs subside, due to warmer conditions in the ice wedge. These findings can help explain the origins of secondary ice wedges in modern and ancient polygons. The findings also imply that the potential for re-establishing rims in modern thermokarst-affected terrain will be limited by reduced cracking activity in the ice wedges, even if regional air temperatures stabilize.

58 GEOSCIENCES↗

NASA NTRS1984

Topics in the optimization of millimeter-wave mixers

This report is in three parts: 1. In the first part a user-oriented computer program for the analysis of single-ended Schottky diode mixers is described. The program is used to compute the performance of a 140-220 GHz mixer and excellent agreement with measurements at 150 and 180 GHz is obtained. A sensitivity analysis indicates the importance of various diode and mount characteristics on the mixer performance. 2. The second part of this report describes a computer program for the analysis of varactor diode multipliers. The diode may operate in either the reverse biased varactor mode or with substantial forward current flow where the conversion mechanism is predominantly resistive. In addition, a design for a varactor diode doubler, tunable over an output frequency range of 150-220 GHz, is given. The doubler has 10-20% conversion efficiency with an instantaneous bandwidth of 3%. 3. The third section of this report contains a description and analysis of i new H-plane rectangular waveguide transformer. The transformer can be made luckily and easily in split-block waveguide using a standard slitting saw. It is particularly suited for use in the millimeter-wave band, replacing conventional electroformed stepped transformers. A theoretical analysis of the transformer is given, and good agreement is obtained with measurements made at X-band. Design curves are included for transitions which have a VSWR <1.2 over a full waveguide band when the impedance ratio is as high as 4 to 1.

Millimeter-wave↗

DOE OSTI2024

Measurement of Stark-split beam and carbon charge exchange emissions for simultaneous B-field and temperature/rotation analysis at DIII-D

A set of two newly designed, single-channel Czerny–Turner spectrometers has been deployed at the DIII-D tokamak for measurements of the motional Stark effect (MSE) split beam emission and the C6+ (CVI) carbon charge exchange recombination (CER) emission at high spectral (δλ = 0.13 nm) and temporal (1–5 kHz) resolution. High throughput optics (f/# = 2.8) allow for good signal-to-noise at high time resolution using fast EMCCD detectors. The MSE emission allows for spectral fitting of the magnitude and direction of the local B-field, while the carbon emission yields local ion temperature and toroidal rotation information. To reduce so-called Doppler broadening of the MSE emission, a new channel-specific variable lens-masking approach has been developed. Experimental data collected from the 2023 DIII-D experimental campaign demonstrate the signal quality and instrument fidelity for both diagnostic measurements. Moreover, initial CER data analysis shows a clear evolution of the toroidal rotation during edge localized modes. Initial progress on the advanced MSE model, including a new validated ray-trace model of the DIII-D collection optics, is shown via sensitivity analysis.

Instruments & Instrumentation↗

DOE OSTI2017

Thermal Analysis of Disposal of High-Level Nuclear Waste in a Generic Bedded Salt repository using the Semi-Analytical Method.

An example case is presented for testing analytical thermal models. The example case represents thermal analysis of a generic repository in bedded salt at 500 m depth. The analysis is part of the study reported in Matteo et al. (2016). Ambient average ground surface temperature of 15°C, and a natural geothermal gradient of 25°C/km, were assumed to calculate temperature at the near field. For generic salt repository concept crushed salt backfill is assumed. For the semi-analytical analysis crushed salt thermal conductivity of 0.57 W/m-K was used. With time the crushed salt is expected to consolidate into intact salt. In this study a backfill thermal conductivity of 3.2 W/m-K (same as intact) is used for sensitivity analysis. Decay heat data for SRS glass is given in Table 1. The rest of the parameter values are shown below. Results of peak temperatures at the waste package surface are given in Table 2.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

RAVEN Template for Dynamic Representativity Analysis of the High Temperature Test Facility

These slides present a walkthrough of the template that has been developed for using RAVEN to perform representativity analysis using models of the High Temperature Test Facility and the General Atomics Modular High Temperature Gas-cooled Reactor. The presentation provides participants in the HTTF benchmark with a walkthrough on how to use RAVEN for their sensitivity analysis and how to read results from the MHTGR-350 to perform representativity

22 - GENERAL STUDIES OF NUCLEAR REACTORS↗

NASA NTRS1992

Numerical analysis of the sensitivity of crystal growth experiments to spacecraft residual acceleration

An analysis is conducted of the sensitivity of the Bridgman-Stockbarger crystal growth method, using an idealized model for a range of operating and boundary conditions over a variety of accelerations. Attention is given to the dopant nonuniformity at the melt-crystal interface. The largest compositional nonuniformities are found to occur for disturbances whose amplitudes are greater than 10 exp 6 g, and frequencies below 0.1 Hz.

Alexander, J. I. D.↗

NASA NTRS2012

Pulsed Lidar Measurements of Atmospheric CO2 Column Absorption and Range During the ASCENDS 2009-2011 Airborne Campaigns

We have developed a pulsed lidar technique for measuring the tropospheric CO2 concentrations as a candidate for NASA's ASCENDS mission and have demonstrated the CO2 and O2 measurements from aircraft. Our technique uses two pulsed lasers allowing simultaneous measurement of a single CO2 absorption line near 1572 nm, O2 extinction in the Oxygen A-band, surface height and backscatter profile. The lasers are stepped in wavelength across the CO2 line and an O2 line doublet during the measurement. The column densities for the CO2 and O2 are estimated from the differential optical depths (DOD) of the scanned absorption lines via the IPDA technique. For the 2009 ASCENDS campaign we flew the CO2 lidar only on a Lear-25 aircraft, and measured the absorption line shapes of the CO2 line using 20 wavelength samples per scan. Measurements were made at stepped altitudes from 3 to 12.6 km over the Lamont OK, central Illinois, North Carolina, and over the Virginia Eastern Shore. Although the received signal energies were weaker than expected for ASCENDS, clear C02 line shapes were observed at all altitudes. Most flights had 5-6 altitude steps with 200-300 seconds of recorded measurements per step. We averaged every 10 seconds of measurements and used a cross-correlation approach to estimate the range to the scattering surface and the echo pulse energy at each wavelength. We then solved for the best-fit CO2 absorption line shape, and calculated the DOD of the fitted CO2 line, and computed its statistics at the various altitude steps. We compared them to CO2 optical depths calculated from spectroscopy based on HITRAN 2008 and the column number densities calculated from the airborne in-situ readings. The 2009 measurements have been analyzed in detail and they were similar on all flights. The results show clear CO2 line shape and absorption signals, which follow the expected changes with aircraft altitude from 3 to 13 km. They showed the expected nearly the linear dependence of DOD vs altitude. The measurements showed -1 ppm random errors for 8-10 km altitudes and -30 sec averaging times. For the 2010 ASCENDS campaigns we flew the CO2 lidar on the NASA DC-8 and added an O2 lidar channel. During July 2010 we made measurements of CO2 and O2 column absorption during longer flights over Railroad Valley NV, the Pacific Ocean and over Lamont OK. CO2 measurements were made with 30 steps/scan, 300 scans/sec and improved line resolution and receiver sensitivity. Analysis of the 2010 CO2 measurements shows the expected -linear change of DOD with altitude. For measurements at altitudes> 6 km the random errors were 0.3 ppm for 80 sec averaging times. For the summer 2011 ASCENDS campaigns we made further improvements to the lidar's CO2 line scan and receiver sensitivity. The seven flights in the 2011 Ascends campaign were flown over a wide variety of surface and cloud conditions in the US, which produced a wide variety of lidar signal conditions. Details of the lidar measurements and their analysis will be described in the presentation.

Abshire, J. B.↗

DOE OSTI2020

"Sintering" Models and In-Situ Experiments: Data Assimilation for Microstructure Prediction in SLS Additive Manufacturing of Nylon Components

Selective laser sintering methods are workhorses for additively manufacturing polymer-based components. The ease of rapid prototyping also means it is easy to produce illicit components. It is necessary to have a data-calibrated in-situ physical model of the build process in order to predict expected and defective microstructure characteristics that inform component provenance. Toward this end, sintering models are calibrated and characteristics such as component defects are explored. This is accomplished by assimilating multiple data streams, imaging analysis, and computational model predictions in an adaptive Bayesian parameter estimation algorithm. From these data sources, along with a phase-field model, bulk porosity distributions are inferred. Model parameters are constrained to physically-relevant search directions by sensitivity analysis, and then matched to predictions using adaptive sampling. Using this feedback loop, data-constrained estimates of sintering model parameters along with uncertainty bounds are obtained.

3D printing, Additive Manufacturing, polymer, sint↗