Clean Combustion Research Centre, Physical Sciences and Engineering Division, King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia.
Phys Chem Chem Phys. 2019 Mar 6;21(10):5510-5520. doi: 10.1039/c8cp07285j.
Pyrolytic kinetics of indene was studied in a flow reactor at 30 and 760 Torr. Indene and its decomposition products, as well as polycyclic aromatic hydrocarbons (PAHs), were measured with synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS). Five literature models were selected to reproduce the experimental data and analyze the reaction kinetics of indene. The experimental and predicted results illustrate that an indenyl radical is the dominant decomposition intermediate and also the main contributor to the further growth of aromatic rings in the pyrolysis of indene. The indene consumption process needs further precise characterization, especially the subsequent dissociation reactions of indanyl and indenyl radicals. A self-recombination reaction of the indenyl radical and the combination reactions between indenyl and other radicals are found to be necessary for the efficient formation of large PAHs. The absence of these pathways leads to the underprediction of experimental measurements. In contrast, literature models adopting indenyl global reactions for PAH formation generally overestimate the system reactivity. Proper radical combination pathways proposed in a future model should consider not only the PAH formation efficiency but also its impact on system reactivity.
在 30 和 760 托的流动反应器中研究了茚的热解动力学。使用同步加速器真空紫外光电离质谱（SVUV-PIMS）测量了茚及其分解产物以及多环芳烃（PAHs）。选择了五个文献模型来重现实验数据并分析茚的反应动力学。实验和预测结果表明，茚基自由基是主要的分解中间体，也是茚热解过程中芳香环进一步增长的主要贡献者。茚的消耗过程需要进一步精确表征，特别是茚基和茚基自由基的后续解离反应。发现茚基自由基的自重组反应和茚基与其他自由基之间的组合反应对于大 PAHs 的有效形成是必要的。这些途径的缺失导致对实验测量的低估。相比之下，采用茚基全局反应来形成 PAHs 的文献模型通常高估了系统的反应性。未来模型中提出的适当的自由基组合途径不仅应考虑 PAH 形成效率，还应考虑其对系统反应性的影响。
