Chapter 6 Optimization of Reaction Models with Solution Mapping

Frenklach, Michael; Packard, Andrew; Feeley, Ryan

doi:10.1016/s0069-8040(07)42006-4

Cited by 28 publications

(29 citation statements)

References 39 publications

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“…A system of four and five coupled differential equations was numerically solved (Frenklach et al 1992(Frenklach et al , 2007 for the respective pathways A and B, resulting in the corresponding set of rate constants derived (Table 3).…”

Section: Reaction Mechanismsmentioning

confidence: 99%

Abiotic Formation of Carboxylic Acids (Rcooh) in Interstellar and Solar System Model Ices

Kim

Kaiser

2010

ApJ

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The present laboratory study simulated the abiotic formation of carboxylic acids (RCOOH) in interstellar and solar system model ices of carbon dioxide (CO 2 )-hydrocarbon mix C n H 2n+2 (n = 1-6). The pristine model ices were irradiated at 10 K under contamination-free, ultrahigh vacuum conditions with energetic electrons generated in the track of galactic cosmic-ray particles. The chemical processing of the ices was monitored by a Fourier transform infrared spectrometer and a quadrupole mass spectrometer during the irradiation phase and subsequent warm-up phases on line and in situ in order to extract qualitative (carriers) and quantitative (rate constants and yields) information on the newly synthesized species. Carboxylic acids were identified to be the main carrier, together with carbon monoxide (CO) and a trace of formyl (HCO) and hydroxycarbonyl (HOCO) radicals at 10 K. The upper limit of acid column density at 10 K was estimated as much as (1.2 ± 0.1) × 10 17 molecules cm −2 at doses of 17 ± 2 eV molecule −1 , or the yield of 39% ± 4% from the initial column density of carbon dioxide. The temporal column density profiles of the products were then numerically fit using two independent kinetic schemes of reaction mechanisms. Finally, we transfer this laboratory simulation to star-forming regions of the interstellar medium, wherein cosmic-ray-induced processing of icy grains at temperatures as low as 10 K could contribute to the current level of chemical complexity as evidenced in astronomical observations and in extracts of carbonaceous meteorites.

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Section: Reaction Mechanismsmentioning

confidence: 99%

Abiotic Formation of Carboxylic Acids (Rcooh) in Interstellar and Solar System Model Ices

Kim

Kaiser

2010

ApJ

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“…For reaction O + OH + M → HO 2 + M, we took the value from Saxena and Williams [40] and uncertainty bounds from Burke et al [41], who showed that this reaction impacted significantly the mass burning rate of lean high-pressure hydrogen flames. In the present study, variables are defined as the normalized forms of rate preexponential factors, as multipliers to the overall rate coefficients (see the description and equations in Appendix A of [5] and [12]). …”

Section: Kinetic Model Of Hydrogen Combustionmentioning

confidence: 99%

“…The one on the left shows ranked sensitivity coefficients, displayed also as a list on the left panel of the figure. The second bar chart shows corresponding impact factors, computed as a product of the absolute value of sensitivity coefficient and the corresponding span; the latter being the square root of the ratio of the upper and lower bounds of the reaction rate-coefficient preexponential factors, listed in the left panel of the figure (further details of this definition can be found in [5] and [12]). The surrogate models are built on the fly, similar to the sensitivity analysis, by performing a series of computational runs according to a design matrix.…”

Section: Creation Of a Datasetmentioning

confidence: 99%

“…Numerical efficiency is attained through the use of surrogate models in numerical algorithms of DataCollaboration. The surrogate models are developed by Solution Mappingapproximation of model responses via computer experiments and regression [2,11,12]. Building surrogate models and organizing data are not simple tasks and, as experience showed [3], become error prone with the increase in the (reaction) system size.…”

Section: Introductionmentioning

confidence: 99%

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Process informatics tools for predictive modeling: Hydrogen combustion

You

Packard

Frenklach

2011

Int J of Chemical Kinetics

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Predictive modeling of chemical reaction systems is facilitated through development of an automated data-centric infrastructure, Process Informatics Model (PrIMe). Modeling and analysis tools were built to bridge the PrIMe Data infrastructure with DataCollaboration, a framework designed to make inferences from experimental observations in the context of an underlying model. The developed tools were integrated with the PrIMe Workflow Application, allowing users to create and run drag-and-drop applications on the fly. Organizing the data, linking the data to scientific methods, and automating the analysis offer new venues of scientific inquiry, such as evaluating the consistency of heterogeneous data records, making uncertainty-quantified predictions, quantifying the contribution of newly obtained or even hypothetical data to the question of interest, or testing similar "what-if" scenarios. The developed system is demonstrated for the chemical kinetics of hydrogen combustion. C

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“…Further analysis of the origin of such ''controversies'' can be found in Refs. [40,53,54] and examples of feasible sets encountered in combustion kinetics in Refs. [47,53,[55][56][57].…”

Section: Artificial Controversiesmentioning

confidence: 99%