Detailed Reaction Mechanism for the Combustion of Hydrogen and Syngas

A detailed reaction mechanism for the oxidation of hydrogen and syngas in freely propagating and burner-stabilized premixed flames as well as shock-tube, jet-stirred reactor, and plug-flow reactor experiments is developed. The H2/CO kinetic model is validated against experimental data from literature which include 87 sets of laminar flame speed, 39 sets of ignition delay times from shock tubes, 16 sets species concentrations in JSRs, 27 sets of species concentrations in PFRs, 8 sets of species concentrations in BSF and 4 sets of species concentrations in shock tube experiments. The rate parameters adopted to develop the detailed chemical kinetic mechanism of H2 and CO is mostly based on the recommendations of Baulch et al. 2005 (Journal of Physical and Chemical Reference Data 34, 757 (2005). https://doi.org/10.1063/1.1748524). This mechanism was developed in parallel to the ammonia mechanism (Detailed Kinetic Mechanism for the Oxidation of Ammonia Including the Formation and Reduction of Nitrogen Oxides. Energ Fuels 2018;32:10202−10217. doi:10.1021/acs.energyfuels.8b01056).

本研究开发了一套针对氢气与合成气（syngas）的详细氧化反应机理，适用场景涵盖自由传播预混火焰、燃烧器稳定预混火焰，以及激波管、射流搅拌反应器（jet-stirred reactor, JSR）、活塞流反应器（plug-flow reactor, PFR）的相关实验。本H2/CO动力学模型以已发表文献中的实验数据为基准进行验证，数据集包含87组层流火焰速度、39组激波管点火延迟时间、16组射流搅拌反应器内物种浓度、27组活塞流反应器内物种浓度、8组燃烧器稳定火焰（burner-stabilized flame, BSF）内物种浓度，以及4组激波管实验物种浓度数据。本H2与CO详细化学动力学机理所采用的速率参数，主要基于Baulch等人2005年发表于《物理与化学参考数据期刊》（Journal of Physical and Chemical Reference Data）第34卷第757页（2005年，DOI: 10.1063/1.1748524）的推荐结果。本机理与同期发表的氨氧化机理（包含氮氧化物生成与还原过程的氨详细氧化动力学机理，《能源与燃料》2018年；32卷：10202−10217，DOI: 10.1021/acs.energyfuels.8b01056）同步开发完成。