Investigation of nitric oxide formation in methane, methane/propane, and methane/hydrogen flames under condensing gas boiler conditions

In this study, NOx formation in lean premixed burner-stabilized flames was investigated under condensing gas boiler operating conditions for pure methane, methane/propane, and methane/hydrogen mixtures. Temperature and NOx species profiles were experimentally obtained from thermocouple and wet chemi...

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Main Authors: Jörn Hinrichs, Maximilian Hellmuth, Felix Meyer, Stephan Kruse, Marco Plümke, Heinz Pitsch
Format: Article
Language:English
Published: Elsevier 2021-03-01
Series:Applications in Energy and Combustion Science
Subjects:
Online Access:http://www.sciencedirect.com/science/article/pii/S2666352X20300145
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author Jörn Hinrichs
Maximilian Hellmuth
Felix Meyer
Stephan Kruse
Marco Plümke
Heinz Pitsch
author_facet Jörn Hinrichs
Maximilian Hellmuth
Felix Meyer
Stephan Kruse
Marco Plümke
Heinz Pitsch
author_sort Jörn Hinrichs
collection DOAJ
description In this study, NOx formation in lean premixed burner-stabilized flames was investigated under condensing gas boiler operating conditions for pure methane, methane/propane, and methane/hydrogen mixtures. Temperature and NOx species profiles were experimentally obtained from thermocouple and wet chemiluminescence detector measurements using in-situ extracted gas samples. Resolved simulations utilizing different NO sub-mechanisms from the GRI 2.11, the GRI 3.0, the CRECK mechanism, and a recent mechanism from Glarborg and co-workers were performed, where the mechanism from Glarborg showed the best agreement with the measured NOx concentrations. While the other mechanisms also agreed fairly well with the experiments, a pathway analysis revealed that this results from error compensation, where the prompt pathway was underestimated, which was balanced by an overestimated contribution of the NNH pathway. Interestingly, the prompt pathway was found to be the major NOx formation route for condensing gas boiler conditions despite the lean mixture. While the temperature level in the post-flame region was too low for the thermal pathway to become dominant, the NNH and N2O pathways reached their chemical equilibrium just downstream of the flame front and therefore did not further contribute to the overall NOx emissions.The partial substitution of methane by hydrogen slightly reduced NOx emissions, which was similarly found in experiment and simulation. The post-flame temperature for methane/hydrogen remained nearly unchanged, because the higher adiabatic flame temperature compared to pure methane was compensated by increased heat losses due to a higher laminar burning velocity. The addition of hydrogen decreased the amount of CH radicals in the flame front, which led to a lower contribution of the most important prompt pathway.Substituting methane by propane increased the temperature level due to a higher adiabatic flame temperature and a slightly smaller laminar burning velocity. While increasing NOx emissions were found in the experiment, the simulation predicted a minimally smaller NOx level compared to pure methane. The higher temperature caused increasing contributions of the thermal, NNH, and N2O pathways. For the prompt pathway, which is again the most important NOx formation route, the temperature trend was superimposed by a decreasing CH concentration in the flame front.
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spelling doaj.art-445a18f0cd654563b29c0fb5cf82c8592022-12-21T22:01:28ZengElsevierApplications in Energy and Combustion Science2666-352X2021-03-015100014Investigation of nitric oxide formation in methane, methane/propane, and methane/hydrogen flames under condensing gas boiler conditionsJörn Hinrichs0Maximilian Hellmuth1Felix Meyer2Stephan Kruse3Marco Plümke4Heinz Pitsch5Corresponding author.; Rheinisch-Westfalische Technische Hochschule Aachen, Aachen, GermanyRheinisch-Westfalische Technische Hochschule Aachen, Aachen, GermanyRheinisch-Westfalische Technische Hochschule Aachen, Aachen, GermanyRheinisch-Westfalische Technische Hochschule Aachen, Aachen, GermanyRheinisch-Westfalische Technische Hochschule Aachen, Aachen, GermanyRheinisch-Westfalische Technische Hochschule Aachen, Aachen, GermanyIn this study, NOx formation in lean premixed burner-stabilized flames was investigated under condensing gas boiler operating conditions for pure methane, methane/propane, and methane/hydrogen mixtures. Temperature and NOx species profiles were experimentally obtained from thermocouple and wet chemiluminescence detector measurements using in-situ extracted gas samples. Resolved simulations utilizing different NO sub-mechanisms from the GRI 2.11, the GRI 3.0, the CRECK mechanism, and a recent mechanism from Glarborg and co-workers were performed, where the mechanism from Glarborg showed the best agreement with the measured NOx concentrations. While the other mechanisms also agreed fairly well with the experiments, a pathway analysis revealed that this results from error compensation, where the prompt pathway was underestimated, which was balanced by an overestimated contribution of the NNH pathway. Interestingly, the prompt pathway was found to be the major NOx formation route for condensing gas boiler conditions despite the lean mixture. While the temperature level in the post-flame region was too low for the thermal pathway to become dominant, the NNH and N2O pathways reached their chemical equilibrium just downstream of the flame front and therefore did not further contribute to the overall NOx emissions.The partial substitution of methane by hydrogen slightly reduced NOx emissions, which was similarly found in experiment and simulation. The post-flame temperature for methane/hydrogen remained nearly unchanged, because the higher adiabatic flame temperature compared to pure methane was compensated by increased heat losses due to a higher laminar burning velocity. The addition of hydrogen decreased the amount of CH radicals in the flame front, which led to a lower contribution of the most important prompt pathway.Substituting methane by propane increased the temperature level due to a higher adiabatic flame temperature and a slightly smaller laminar burning velocity. While increasing NOx emissions were found in the experiment, the simulation predicted a minimally smaller NOx level compared to pure methane. The higher temperature caused increasing contributions of the thermal, NNH, and N2O pathways. For the prompt pathway, which is again the most important NOx formation route, the temperature trend was superimposed by a decreasing CH concentration in the flame front.http://www.sciencedirect.com/science/article/pii/S2666352X20300145Burner-stabilized flamesNOx formationHydrogen combustionCondensing gas boiler conditionsResolved simulationExperimental measurements
spellingShingle Jörn Hinrichs
Maximilian Hellmuth
Felix Meyer
Stephan Kruse
Marco Plümke
Heinz Pitsch
Investigation of nitric oxide formation in methane, methane/propane, and methane/hydrogen flames under condensing gas boiler conditions
Applications in Energy and Combustion Science
Burner-stabilized flames
NOx formation
Hydrogen combustion
Condensing gas boiler conditions
Resolved simulation
Experimental measurements
title Investigation of nitric oxide formation in methane, methane/propane, and methane/hydrogen flames under condensing gas boiler conditions
title_full Investigation of nitric oxide formation in methane, methane/propane, and methane/hydrogen flames under condensing gas boiler conditions
title_fullStr Investigation of nitric oxide formation in methane, methane/propane, and methane/hydrogen flames under condensing gas boiler conditions
title_full_unstemmed Investigation of nitric oxide formation in methane, methane/propane, and methane/hydrogen flames under condensing gas boiler conditions
title_short Investigation of nitric oxide formation in methane, methane/propane, and methane/hydrogen flames under condensing gas boiler conditions
title_sort investigation of nitric oxide formation in methane methane propane and methane hydrogen flames under condensing gas boiler conditions
topic Burner-stabilized flames
NOx formation
Hydrogen combustion
Condensing gas boiler conditions
Resolved simulation
Experimental measurements
url http://www.sciencedirect.com/science/article/pii/S2666352X20300145
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