| Zugriffsnummer | 49585 |
| Dokumenttyp | Zeitschriftenartikel |
| Peer Review | mit Peer Review |
| Sprache | Englisch |
| Titel | Interactions in ammonia and hydrogen oxidation examined in a flow reactor and a shock tube |
| Autor(in); Institution |
Ruwe, Lena; 3.7, Grundlagen des Explosionsschutzes, PTB-Braunschweig
Schmitt, Steffen; Universität Bielefeld, Bielefeld, GERMANY
Kohse-Höingthaus, Katharina; Universität Bielefeld, Bielefeld, GERMANY
|
| Quelle/Jahr | Journal of Physical Chemistry A: 127 (2023), 10, 2351 - 2366 |
| ISSN | 1089-5639 (print) ; 1520-5215 (online) |
| DOI | |
| Verlag | Washington, DC: American Chemical Society (ACS) |
| Freie Schlagworte | ammonia ; hydrogen ; flow reactor ; MBMS ; NO ; TDLAS ; shock tube ; mechanism |
| Zusammenfassung | Ammonia (NH3) is a promising fuel as it is carbon-free and easier to store and transport than hydrogen (H2). However, an ignition enhancer such as H2 might be needed for technical applications due to the rather poor ignition properties of NH3. The combustion of pure NH3 and H2 has been explored widely. However, for mixtures of both gases, mostly only global parameters such as ignition delay times or flame speeds were reported. Studies with extensive experimental species profiles are scarce. Therefore, we experimentally investigated the interactions in the oxidation of different NH3/H2 mixtures in the temperature range of 750-1173 K at 0.97 bar in a plug-flow reactor (PFR), as well as in the temperature range of 1615-2358 K with an average pressure of 3.16 bar in a shock tube. In the PFR, temperature-dependent mole fraction profiles of the main species were obtained via electron ionization molecular-beam mass spectrometry (EI-MBMS). Additionally, for the first time, tunable diode laser absorption spectroscopy (TDLAS) with a scanned-wavelength method was adapted to the PFR for the quantification of nitric oxide (NO). In the shock tube, time-resolved NO profiles were also measured by TDLAS using a fixed-wavelength approach. The experimental results both in PFR and shock tube reveal the reactivity enhancement by H2 on ammonia oxidation. The extensive sets of results were compared with predictions by four NH3-related reaction mechanisms. None of the mechanisms can well predict all experimental results, but the Stagni et al. (React. Chem. Eng. 2020, 5, 696-711) and Zhu et al. (Combust. Flame 2022, 246, 115389) mechanisms perform best for the PFR and shock tube conditions, respectively. Exploratory kinetic analysis was conducted to identify the effect of H2 addition on ammonia oxidation and NO formation, as well as sensitive reactions in different temperature regimes. The results presented in this study can provide valuable information for further model development and highlight relevant properties of H2-assisted NH3 combustion. |
| Themenbereich der Metrologie | Metrologie in der Chemie und Stoffeigenschaften |
| Förderinformationen (1) |
Förderername: Alexander von Humboldt-Stiftung (AvH)
Förderer ID: 0000 0001 1034 1691 Förderer ID Typ: ISNI Förderprogramm: Postdoc Program Titel der Förderung: H2−WaVe Förderungsnummer: ZN3772 URI der Förderung: https://www.humboldt-foundation.de |
Zitierung
Zhu, D., Ruwe, L., Schmitt, S., Shu, B., Kohse-Höingthaus, K., & Lucassen, A. (2023). Interactions in ammonia and hydrogen oxidation examined in a flow reactor and a shock tube. Journal of Physical Chemistry A, 127(10), 2351–2366. https://doi.org/10.1021/acs.jpca.2c07784