@inproceedings{ShresthaSeidelMauss, author = {Shrestha, Krishna Prasad and Seidel, Lars and Mauß, Fabian}, title = {Kinetic study of methanol and ethanol oxidation in presence of NOx}, series = {Workshop on Gas-phase reaction kinetics of biofuels oxygenated molecules}, booktitle = {Workshop on Gas-phase reaction kinetics of biofuels oxygenated molecules}, language = {en} } @misc{ShresthaSeidelZeuchetal., author = {Shrestha, Krishna Prasad and Seidel, Lars and Zeuch, Thomas and Mauß, Fabian}, title = {Detailed Kinetic Mechanism for the Oxidation of Ammonia Including the Formation and Reduction of Nitrogen Oxides}, series = {Energy \& Fuels}, volume = {32}, journal = {Energy \& Fuels}, number = {10}, issn = {1520-5029}, doi = {10.1021/acs.energyfuels.8b01056}, pages = {10202 -- 10217}, abstract = {This work introduces a newly developed reaction mechanism for the oxidation of ammonia in freely propagating and burner-stabilized premixed flames as well as shock-tube, jet-stirred reactor, and plug-flow reactor experiments. The paper mainly focuses on pure ammonia and ammonia-hydrogen fuel blends. The reaction mechanism also considers the formation of nitrogen oxides as well as the reduction of nitrogen oxides depending upon the conditions of the surrounding gas phase. Doping of the fuel blend with NO2 can result in acceleration of H2 autoignition via the reaction NO2 + HO2 ⇋ HONO + O2, followed by the thermal decomposition of HONO, or deceleration of H2 oxidation via NO2 + OH ⇋ NO + HO2. The concentration of HO2 is decisive for the active reaction pathway. The formation of NO in burner-stabilized premixed flames is shown to demonstrate the capability of the mechanism to be integrated …}, language = {en} } @inproceedings{ShresthaSeidelMaussetal., author = {Shrestha, Krishna Prasad and Seidel, Lars and Mauß, Fabian and Zeuch, Thomas}, title = {Development of a kinetic mechanism for NOx fuel interaction}, series = {Proceedings, Joint Meeting of the German and Italian Sections of the Combustion Institute, 41st Meeting on Combustion, Sorrento, May 2018}, booktitle = {Proceedings, Joint Meeting of the German and Italian Sections of the Combustion Institute, 41st Meeting on Combustion, Sorrento, May 2018}, editor = {Bockhorn, Henning and Scala, F. and Commodo, M. and Tregrossi, A.}, publisher = {Associazione Sezione Italiana del Combustion Institute}, address = {Napoli}, isbn = {978-88-88104-22-5}, pages = {6}, abstract = {This work introduces a newly developed reaction mechanism to predict fuel/NOx interaction in freely propagating, burner stabilized premixed flames, shock tubes, jet stirred reactors and plug flow reactors experiments. The study focuses on pure ammonia as fuel as well as H₂,H₂/CO, CH₄ doped with NO, NO₂ and N₂O. The kinetic scheme also focuses on the formation and consumption of nitrogen oxides at different experimental conditions. It is found that the doping with N₂O has almost no sensitivity on the H₂ chemistry, while small amount of NO₂ is enough to change the pressure dependence of H₂ auto ignition. The experiments with N₂O still show the significant influence of the chain breaking reaction H+O₂(+M)⇋HO₂(+M) on the H₂ ignition delay times, resulting in the crossing lines for the ignition delay times, which are moved at higher pressure to higher temperature. The concentration of HO₂ is decisive for the active reaction pathway in shock tube oxidation as well as in jet stirred and flow reactor. Reaction NO+HO₂⇋NO₂+OH and NO₂+H⇋NO+OH are very important because they strongly influence the inter conversion process of NO and NO₂ in jet stirred reactor and flow reactor for cases studied herein. The formation of NO in burner stabilized premixed flames is shown to demonstrate the capability of the mechanism to be integrated into mechanisms for hydrocarbon oxidation.}, language = {en} } @misc{ShresthaSeidelZeuchetal., author = {Shrestha, Krishna Prasad and Seidel, Lars and Zeuch, Thomas and Mauß, Fabian}, title = {Kinetic Modeling of NOx Formation and Consumption during Methanol and Ethanol Oxidation}, series = {Combustion Science and Technology}, volume = {191}, journal = {Combustion Science and Technology}, number = {9}, issn = {1563-521X}, doi = {10.1080/00102202.2019.1606804}, pages = {1628 -- 1660}, language = {en} } @misc{ShresthaVinHerbinetetal., author = {Shrestha, Krishna Prasad and Vin, Nicolas and Herbinet, Olivier and Seidel, Lars and Battin-Leclerc, Fr{\´e}d{\´e}rique and Zeuch, Thomas and Mauß, Fabian}, title = {Insights into nitromethane combustion from detailed kinetic modeling - Pyrolysis experiments in jet-stirred and flow reactors}, series = {Fuel}, volume = {261}, journal = {Fuel}, issn = {0016-2361}, doi = {https://doi.org/10.1016/j.fuel.2019.116349}, pages = {19}, abstract = {The pyrolysis of nitromethane highly diluted in helium was studied in a plug flow reactor and in a jet-stirred reactor at 1.07 bar and over the temperature range from 500 to 1100 K. Mole fraction profiles of major products and of intermediates were identified with gas chromatography and Fourier transform infrared spectroscopy. Using these experimental data, as well as published ones, we have developed a newly compiled model for the prediction of the pyrolysis and of the oxidation of nitromethane in jet-stirred and flow reactors, freely propagating, and burner-stabilized premixed flames, as well as in shock-tubes. The experimental results from the present work and from the literature are interpreted with the help of the kinetic model derived here. This study mainly focuses on the analysis of speciation in different reactors. Among the nitrogenous species, NO is found to be a major product for pyrolysis and oxidation. The model suggests that for nitromethane pyrolysis and oxidation the thermal dissociation channel to CH3 and NO2 is the main reaction path for the nitromethane degradation followed by the H-atom abstraction channel. The most sensitive reactions for nitromethane pyrolysis in a flow reactor and during pyrolysis and oxidation in a jet-stirred reactor are found to be CH3NO2(+M) ⇋ CH3 + NO2(+M) and CH3 + NO2 ⇋ CH3O + NO. The reaction CH3 + NO2 ⇋ CH3O + NO is found to be the most important reaction for all conditions studied. In a burner-stabilized premixed flame, as the mixture gets richer, the thermal dissociation channel CH3NO2(+M) ⇋ CH3 + NO2(+M) becomes more important as the contribution of the H-atom abstraction channel is decreased. Furthermore, in the burner-stabilized premixed flames, it was found that NO is mainly formed via NO2: NO2 + H ⇋ NO + OH, NO2 + CH3 ⇋ CH3O + NO. The model provided an overall reasonable agreement with the experimental data. However, for pyrolysis conditions, future work is desirable to improve predictions of intermediate species. This work extends the kinetic database and helps to improve the understanding of nitromethane chemistry. The kinetic model presented in this work can serve as a base model for hydrocarbons and oxygenated fuels higher than C2 and nitrogen-containing compounds higher than C1 as well as for pure nitrogen compounds.}, language = {en} } @misc{ShresthaSeidelZeuchetal., author = {Shrestha, Krishna Prasad and Seidel, Lars and Zeuch, Thomas and Mauß, Fabian}, title = {Modeling for Nitromethane oxidation}, series = {1st International Conference on Smart Energy Carriers Napoli, 2019}, journal = {1st International Conference on Smart Energy Carriers Napoli, 2019}, abstract = {The diminishing availability of conventional fuels and stricter regulations on pollution control and CO2 emission targets have led scientist and engineers to look for alternative fuels. Recently nitromethane has slowly gained interest as alternative fuel over conventional fuel for internal combustion engines. In the past, it was mostly used as rocket propellant or as an explosives [1,2]. Nitromethane is an energetic compound with a wide variety of applications, including its use as a monopropellant, a liquid explosive, a solvent for chemical processing and analysis, and a highperformance fuel additive for internal combustion engines and pulsed detonation engines [3]. The chemical formula of nitromethane is CH3NO2. As the name suggests, the molecule is essentially methane with one of the four hydrogens replaced by a nitro group. In essence, it is the simplest of possible energetic CHON molecules that contain nitro groups, which is why it is often used in reaction studies as a prototype for more complex energetic materials. There is no reliable kinetic model for nitromethane combustion, which is validated over a wide range of experimental conditions. There are a few published studies [4-8] both numerically and experimentally focusing often on a single reactor at very specific conditions. The aim of the present work is to extend our recently published mechanism [9] for syngas, methane and ammonia oxidation to include CH3NO2 as fuel and validate against the available experimental data from the literature. The development and compilation strategy for our mechanism is described in our recent work [9] and this study is conducted in a similar manner. Rates are taken mainly from [7,10-16]. This makes the kinetic model more robust and reliable for combustion modelling.}, language = {en} } @misc{ShresthaSeidelMaussetal., author = {Shrestha, Krishna Prasad and Seidel, Lars and Mauß, Fabian and Zeuch, Thomas}, title = {Kinetic Modeling for NOx prediction with improved base Chemistry}, series = {COST 1404, SMARTCATs, Chemistry of smart energy carriers and technologies, 3rd General Meeting and Workshop on SECs in Industry of SMARTCATs Action}, journal = {COST 1404, SMARTCATs, Chemistry of smart energy carriers and technologies, 3rd General Meeting and Workshop on SECs in Industry of SMARTCATs Action}, language = {en} } @misc{LeonRuweMoshammeretal., author = {Le{\´o}n, Larisa and Ruwe, Lena and Moshammer, Kai and Seidel, Lars and Shrestha, Krishna Prasad and Wang, Xiaoxiao and Mauß, Fabian and Kohse-H{\"o}inghaus, Katharina and Hansen, Nils}, title = {Chemical insights into the larger sooting tendency of 2-methyl-2-butene compared to n-pentane}, series = {Combustion and Flame}, volume = {208}, journal = {Combustion and Flame}, issn = {0010-2180}, doi = {10.1016/j.combustflame.2019.06.029}, pages = {182 -- 197}, abstract = {A comprehensive, chemically detailed mechanism for the combustion of 2-methyl-2-butene and n-pentane is presented to provide insights into the different sooting tendencies of these two structurally different C5 hydrocarbons. A hierarchically assembled mechanism has been developed to specifically target speciation data from low-pressure premixed flames of 2-methyl-2-butene [Ruwe et al., Combust. Flame, 175, 34-46, 2017] and newly measured mole fraction data for a fuel-rich (ɸ=1.8) n-pentane flame, in which species profiles up to phenol were quantified. The partially isomer-resolved chemical composition of this flame was determined using flame-sampling molecular-beam mass spectrometry with single-photon ionization by tunable, synchrotron-generated vacuum-ultraviolet radiation. The presented model, which includes a newly determined, consistent set of the thermochemistry data for the C5 species, presents overall satisfactory capabilities to predict the mole fraction profiles of common combustion intermediates. The analysis of the model predictions revealed the fuel-structure dependencies (i.e. saturated vs. unsaturated and linear vs. branched) of the formation of small aromatic species that are considered as soot precursors. The propensity of the 2-methyl-2-butene flame to form larger concentrations of aromatic species was traced back to the readily available formation routes of several small precursor molecules and the efficient formation of "first aromatic rings" beyond benzene.}, language = {en} } @misc{ShresthaEckartElbazetal., author = {Shrestha, Krishna Prasad and Eckart, Sven and Elbaz, Ayman M. and Giri, Binod Raj and Fritsche, Chris and Seidel, Lars and Roberts, William L. and Krause, Hartmut and Mauß, Fabian}, title = {A comprehensive kinetic model for dimethyl ether and dimethoxymethane oxidation and NOx interaction utilizing experimental laminar flame speed measurements at elevated pressure and temperature}, series = {Combustion and Flame}, volume = {218}, journal = {Combustion and Flame}, issn = {1556-2921}, doi = {10.1016/j.combustflame.2020.04.016}, pages = {57 -- 74}, abstract = {Laminar flame speeds of dimethyl ether and dimethoxymethane at pressures from 1 to 5 bar and initial temperatures from 298 to 373 K were determined experimentally using a constant volume spherical vessel and a heat flux burner setup. This study is the first to report dimethoxymethane laminar flame speeds at a pressure higher than 1 bar. Using these experimental data along with data available in the literature, a new kinetic model for the prediction of the oxidation behavior of dimethyl ether and dimethoxymethane in freely propagating and burner stabilized premixed flames, in shock tubes, rapid compression machines, flow reactors, and a jet-stirred reactor has been developed. The experimental results from the present work and literature are interpreted with the help of the derived kinetic model. This newly developed reaction mechanism considers the redox chemistry of NOx to accommodate the influence of the oxygen level on the onset of fuel conversion and interconversion of NO and NO2. The current model suggests that an increased O2 level promotes the HO2 production, which in turn leads to the formation of OH radicals, which promotes the combustion of the fuel/air mixture under lean conditions. The increase of OH radical concentrations is mainly via the NO/NO2 interconversion reaction channel, NO+HO2=NO2+OH, NO2+H=NO+OH, CH3OCH3+NO2=CH3OCH2+HONO, followed by the thermal decomposition of HONO. This work extends the kinetic database and helps to improve the understanding of dimethyl ether and dimethoxymethane combustion behavior. The kinetic model presented in this work can serve as a base model for hydrocarbons and oxygenated fuels higher than C2.}, language = {en} } @misc{ShresthaLhuillierBarbosaetal., author = {Shrestha, Krishna Prasad and Lhuillier, Charles and Barbosa, Amanda Alves and Brequigny, Pierre and Contino, Francesco and Mouna{\"i}m-Rousselle, Christine and Seidel, Lars and Mauß, Fabian}, title = {An experimental and modeling study of ammonia with enriched oxygen content and ammonia/hydrogen laminar flame speed at elevated pressure and temperature}, series = {Proceedings of the Combustion Institute}, volume = {2020}, journal = {Proceedings of the Combustion Institute}, issn = {1540-7489}, doi = {10.1016/j.proci.2020.06.197}, pages = {1 -- 12}, abstract = {Laminar flame speeds of ammonia with oxygen-enriched air (oxygen content varying from 21 to 30 vol.\%) and ammonia-hydrogen-air mixtures (fuel hydrogen content varying from 0 to 30 vol.\%) at elevated pressure (1-10 bar) and temperature (298-473 K) were determined experimentally using a constant volume combustion chamber. Moreover, ammonia laminar flame speeds with helium as an inert were measured for the first time. Using these experimental data along with published ones, we have developed a newly compiled kinetic model for the prediction of the oxidation of ammonia and ammonia-hydrogen blends in freely propagating and burner stabilized premixed flames, as well as in shock tubes, rapid compression machines and a jet-stirred reactor. The reaction mechanism also considers the formation of nitrogen oxides, as well as the reduction of nitrogen oxides depending on the conditions of the surrounding gas phase. The experimental results from the present work and the literature are interpreted with the help of the kinetic model derived here. The experiments show that increasing the initial temperature, fuel hydrogen content, or oxidizer oxygen content causes the laminar flame speed to increase, while it decreases when increasing the initial pressure. The proposed kinetic model predicts the same trends than experiments and a good agreement is found with measurements for a wide range of conditions. The model suggests that under rich conditions the N2H2 formation path is favored compared to stoichiometric condition. The most important reactions under rich conditions are: NH2+NH=N2H2+H, NH2+NH2=N2H2+H2, N2H2+H=NNH+H2 and N2H2+M=NNH+H+M. These reactions were also found to be among the most sensitive reactions for predicting the laminar flame speed for all the cases investigated.}, language = {en} } @misc{IssayevGiriElbazetal., author = {Issayev, Gani and Giri, Binod Raj and Elbaz, Ayman M. and Shrestha, Krishna Prasad and Mauß, Fabian and Roberts, William L. and Farooq, Aamir}, title = {Combustion behavior of ammonia blended with diethyl ether}, series = {Proceedings of the Combustion Institute}, volume = {38 (2021)}, journal = {Proceedings of the Combustion Institute}, number = {1}, issn = {1540-7489}, doi = {10.1016/j.proci.2020.06.337}, pages = {499 -- 506}, abstract = {Ammonia (NH3) is recognized as a carbon-free hydrogen-carrier fuel with a high content of hydrogen atoms per unit volume. Recently, ammonia has received increasing attention as a promising alternative fuel for internal combustion engine and gas turbine applications. However, the viability of ammonia fueling future combustion devices has several barriers to overcome. To overcome the challenge of its low reactivity, it is proposed to blend it with a high-reactivity fuel. In this work, we have investigated the combustion characteristics of ammonia/diethyl ether (NH3/DEE) blends using a rapid compression machine (RCM) and a constant volume spherical reactor (CVSR). Ignition delay times (IDTs) of NH3/DEE blends were measured using the RCM over a temperature range of 620 to 942 K, pressures near 20 and 40 bar, equivalence ratios (Φ) of 1 and 0.5, and a range of mole fractions of DEE, χDEE, from 0.05 to 0.2 (DEE/NH3 = 5 - 20\%). Laminar burning velocities of NH3/DEE premixed flames were measured using the CVSR at 298 K, 1 bar, Φ of 0.9 to 1.3, and χDEE from 0.1 to 0.4. Our results indicate that DEE promotes the reactivity of fuel blends resulting in significant shortening of the ignition delay times of ammonia under RCM conditions. IDTs expectedly exhibited strong dependence on pressure and equivalence ratio for a given blend. Laminar burning velocity was found to increase with increasing fraction of DEE. The burnt gas Markstein length increased with equivalence ratio for χDEE = 0.1 as seen in NH3-air flames, while the opposite evolution of Markstein length was observed with Φ for 0.1 < χDEE ≤ 0.4, as observed in isooctane-air flames. A detailed chemical kinetics model was assembled to analyze and understand the combustion characteristics of NH3/DEE blends.}, language = {en} }