Towards a common C0-C2 mechanism: a critical evaluation of rate constants for syngas combustion kinetics
| Main Authors: | Pelucchi, Matteo, Burke, Ultan, Cai, Limin, Somers, K.P., Glarborg, Peter, Turanyi, Tamas, Pitsch, Heinz, Curran, Henry J., Faravelli, Tiziano, Klippenstein, Stephen J. |
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| Format: | Proceeding |
| Bahasa: | eng |
| Terbitan: |
, 2019
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| Online Access: |
https://zenodo.org/record/3587865 |
Daftar Isi:
- Since the pioneering studies of Tsang and Hampson [1], and of Baulch and co-workers [2, 3], the knowledge of elementary combustion kinetics has increased, largely due to more accurate theories, advanced computing facilities and progresses in experimental measurements [4]. However, no effort has been devoted to the collection and reinterpretation of this knowledge after the early 2000s. Starting in February 2017, we have collected and interpreted a very large number of direct and indirect rate constant measurements from the literature, as well as every state of the art theo-retical calculation available for 50 elementary reaction steps involved in H2/CO pyrolysis and combustion. A strong need for reconciling rate constant measurements and theory has emerged from this analysis. A significant number of the indirect measurements of rate constants and theoretical determinations seem, in fact, to disagree beyond the expected accuracy of parame-ters in the syngas subset. This is mostly due to the need for reconciliation of data and theory and the reinterpretation of the raw signals of the measurements with more accurate and better constrained models according to a careful iterative procedure. The joint effort of SMARTCAT partners at Politecnico di Milano, NUI Galway, ELTE Buda-pest and Denmark Technical University together with RWTH Aachen University (DE) and Argonne National Laboratory (USA), aims to propose a fundamentally based state of the art mechanism for syngas combustion, to serve as a reference for the entire combustion kinetics community. Due to many different reasons, models for real fuels available in the literature rely on more or less different C0-C2 subsets. These differences often do not have substantial im-pacts on the overall performances as different rates in the core mechanism are often counter-balanced by different rates in the model subset relating to heavier fuels. This leads to very sim-ilar radical distributions and therefore in similar macroscopic behavior. However, the adoption of a fundamentally based common core mechanism will constitute a substantial thrust to in-crease the robustness of higher molecular weight fuel’s kinetics.