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Title: Theory and modeling of relevance to prompt-NO formation at high pressure

An improved understanding of NO x formation at high pressures would be of considerable utility to efforts to develop advanced combustion devices. Here a combination of theoretical and modeling studies are implemented in an effort to improve the accuracy of models for the prompt NO process, which is the dominant source of NO under many conditions, and to improve our understanding of the role of this process at high pressures. The theoretical effort implements state-of-the-art treatments of NCN thermochemistry, the interrelated CH + N 2 and NCN + H kinetics, and the kinetics of the NCN + OH reaction. For both reaction systems, we implement high level ab initio transition state theory based master equation simulations paying particular attention to the role of stabilization processes. For the NCN + H kinetics we include a treatment of inter-system crossing. The modeling effort focuses on exploring the role of pressure and prompt NO for premixed laminar flames at pressures ranging from 1 to 15 atm, via a comparison with the available experimental data. Additional simulations at higher pressures further explore the mechanistic changes at the pressures of relevance to applied combustion devices (e.g., 100 atm).
Authors:
ORCiD logo [1] ; ORCiD logo [1] ;  [1] ;  [2]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  2. Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Chemical and Biochemical Engineering
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Combustion and Flame
Additional Journal Information:
Journal Volume: 195; Journal Issue: C; Journal ID: ISSN 0010-2180
Publisher:
Elsevier
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; Innovation Fund Denmark
Country of Publication:
United States
Language:
English
Subject:
03 NATURAL GAS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Flame Modeling; NOx; Theoretical Chemical Kinetics; High pressure; Prompt NOx; NCN kinetics
OSTI Identifier:
1462738

Klippenstein, Stephen J., Pfeifle, Mark, Jasper, Ahren W., and Glarborg, Peter. Theory and modeling of relevance to prompt-NO formation at high pressure. United States: N. p., Web. doi:10.1016/j.combustflame.2018.04.029.
Klippenstein, Stephen J., Pfeifle, Mark, Jasper, Ahren W., & Glarborg, Peter. Theory and modeling of relevance to prompt-NO formation at high pressure. United States. doi:10.1016/j.combustflame.2018.04.029.
Klippenstein, Stephen J., Pfeifle, Mark, Jasper, Ahren W., and Glarborg, Peter. 2018. "Theory and modeling of relevance to prompt-NO formation at high pressure". United States. doi:10.1016/j.combustflame.2018.04.029.
@article{osti_1462738,
title = {Theory and modeling of relevance to prompt-NO formation at high pressure},
author = {Klippenstein, Stephen J. and Pfeifle, Mark and Jasper, Ahren W. and Glarborg, Peter},
abstractNote = {An improved understanding of NOx formation at high pressures would be of considerable utility to efforts to develop advanced combustion devices. Here a combination of theoretical and modeling studies are implemented in an effort to improve the accuracy of models for the prompt NO process, which is the dominant source of NO under many conditions, and to improve our understanding of the role of this process at high pressures. The theoretical effort implements state-of-the-art treatments of NCN thermochemistry, the interrelated CH + N2 and NCN + H kinetics, and the kinetics of the NCN + OH reaction. For both reaction systems, we implement high level ab initio transition state theory based master equation simulations paying particular attention to the role of stabilization processes. For the NCN + H kinetics we include a treatment of inter-system crossing. The modeling effort focuses on exploring the role of pressure and prompt NO for premixed laminar flames at pressures ranging from 1 to 15 atm, via a comparison with the available experimental data. Additional simulations at higher pressures further explore the mechanistic changes at the pressures of relevance to applied combustion devices (e.g., 100 atm).},
doi = {10.1016/j.combustflame.2018.04.029},
journal = {Combustion and Flame},
number = C,
volume = 195,
place = {United States},
year = {2018},
month = {5}
}