Abstract
AbstractThe combustion chambers of direct‐fired supercritical CO2 power plants operate at pressures of approximately 300 bar and CO2 dilutions of up to 96%. The rate coefficients used in existing chemical kinetic mechanisms are validated for much lower pressures and much smaller concentrations of CO2. Recently, the UoS sCO2 1.0 and UoS sCO2 2.0 mechanisms have been developed to better predict ignition delay time (IDT) data from shock tube studies at pressures from 1 to 260 bar in various CO2‐containing bath gas compositions. The chemistry of the methyldioxy radical (CH3O2) has been identified as an essential combustion intermediate for methane combustion above 100 bar, where mechanisms missing this species begin to vastly overpredict the IDT. The current literature available on CH3O2 is very limited and often concerned with atmospheric chemistry and low‐pressure, low‐temperature combustion. This means that the rate coefficients used in UoS sCO2 2.0 are commonly determined at sub‐atmospheric pressures and temperatures below 1000 K with some rate coefficients being over 30 years old. In this work, the rate coefficients of new potential CH3O2 reactions are added to the current mechanism to create UoS sCO2 2.1 It is shown that the influence of CH3O2 on the IDT is greatest at high pressures and low temperatures. It has also been demonstrated that CO2 has very little effect on the chemistry of CH3O2 at 300 bar meaning that CH3O2 rate coefficients can be determined in other bath gases, reducing the impact of non‐ideal effects such as bifurcation when studying in a CO2 bath gas. The updated UoS sCO2 2.1 mechanism is then compared to high‐pressure IDT data and the most important reactions which require reinvestigation have been identified as the essential next steps in understanding high‐pressure methane combustion.
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