The C5 chemistry preceding the formation of polycyclic aromatic hydrocarbons in a premixed 1-pentene flame
The C5 chemistry preceding the formation of polycyclic aromatic hydrocarbons in a premixed 1-pentene flame
复制标题
DOI：
10.1016/j.combustflame.2019.05.013
复制
发表时间：
2019-08
影响因子：
4.4
通讯作者：
L. Ruwe;L. Cai;K. Moshammer;N. Hansen;H. Pitsch;K. Kohse-Höinghaus
中科院分区：
文献类型：
--
作者：
L. Ruwe;L. Cai;K. Moshammer;N. Hansen;H. Pitsch;K. Kohse-Höinghaus
小分子多环芳烃（PAHs）及其前体物的生成受到C5物种反应的强烈影响。为了改善现有的燃烧机制，小PAH的形成，因此，它是有价值的，以了解燃料特定的化学C5燃料。为此，我们提供了定量异构体分辨物种配置文件中测量的层流预混（λ = 1.8）低压（4千帕）火焰的1-戊烯与光电离分子束质谱（PI-MBMS）使用可调谐同步真空紫外（VUV）辐射。这些实验结果伴随着数值模拟，从Wang等人[JetSurF版本2.0（2010）]和Healy等人[Energy Fuels 24（2010）1521-1528]的文献模型开始，其针对不同燃料开发，但包括1-戊烯作为中间体，以及Narayanaswamy等人[Combust. Flame 157（2010）1879-1898]，关注小PAH化学。考虑到实验结果和模拟结果之间的差异，C5化学的新机制，包括PAH的形成途径，其性能进行了详细的分析。特别强调了1-戊烯的初始燃料消耗以及小芳烃的形成途径。关于燃料分解和碳氢化合物生长反应的机制显示出差异。这些一方面导致不同模型的模拟之间存在明显差异，另一方面也导致模型预测与实验结果之间存在偏差。虽然新的模型提出了总体上令人满意的能力来预测常见的燃烧中间产物的摩尔分数分布，但文献模型的预测能力对于一些中间物种（包括C4 H6、C7 H8和C10 H8）并不完全令人满意。研究结果表明，C5燃料特性的反应路线以及小分子PAH的生成机理有待进一步研究.
The formation of small polycyclic aromatic hydrocarbons (PAHs) and their precursors can be strongly affected by reactions of C5species. For improving existing combustion mechanisms for small PAH formation, it is therefore valuable to understand the fuel-specific chemistry of C5fuels. To this end, we provide quantitative isomer-resolved species profiles measured in a laminar premixed (ϕ= 1.8) low-pressure (4 kPa) flame of 1-pentene with photoionization molecular-beam mass spectrometry (PI-MBMS) using tunable synchrotron vacuum-ultraviolet (VUV) radiation. These experimental results are accompanied with numerical simulations, starting from models from the literature by Wang et al. [JetSurF version 2.0 (2010)] and Healy et al. [Energy Fuels 24 (2010) 1521–1528] that were developed for different fuels, but which include 1-pentene as an intermediate, and by Narayanaswamy et al. [Combust. Flame 157 (2010) 1879–1898] focusing on the small PAH chemistry. Taking observed discrepancies between experimental results and simulations into consideration, a mechanism for C5chemistry was newly developed including PAH formation pathways, and its performance analyzed in detail. Special emphasis was placed on the initial fuel consumption of 1-pentene as well as on formation pathways of small aromatics. The mechanisms show differences regarding fuel decomposition and hydrocarbon growth reactions. These contribute to noticeable differences between the simulations with different models on one hand, and deviations between model predictions and experimental results on the other. While the new model presents overall satisfactory capabilities to predict the mole fraction profiles of common combustion intermediates, the predictive capability of the literature models was not fully satisfying for some intermediate species, including C4H6, C7H8, and C10H8. The results indicate that the fuel-specific C5reaction routes as well as the mechanism for small PAH formation need further investigation.