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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Detection of Aliphatically Bridged Multi-Core Polycyclic Aromatic Hydrocarbons in Sooting Flames with Atmospheric-Sampling High-Resolution Tandem Mass Spectrometry
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Detection of Aliphatically Bridged Multi-Core Polycyclic Aromatic Hydrocarbons in Sooting Flames with Atmospheric-Sampling High-Resolution Tandem Mass Spectrometry

机译：用大气采样高分辨率串联质谱法检测氧化溅射的多核多环芳烃烃

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摘要

This paper provides experimental evidence for the chemical structures of aliphatically substituted and bridged polycyclic aromatic hydrocarbon (PAH) species in gas-physe combustion environments. The identification of these single-and multicore aromatic species, which have been hypothe-sized to be important in PAH growth and soot nucleation, was made possible through a combination of sampling gaseous constituents from an atmospheric pressure inverse coflow diffusion flame of ethylene and high-resolution tandem mass spectrometry (MS-MS). In these experiments, the flame-sampled components were ionized using a continuous VUV lamp at 10.0 eV and the ions were subsequently fragmented through collisions with Ar atoms in a collision-induced dissociation (CID) process. The resulting fragment ions, which were separated using a reflectron time-of-flight mass spectrometer, were used to extract structural information about the sampled aromatic compounds. The high-resolution mass spectra revealed the presence of alkylated single-core aromatic compounds and the fragment ions that were observed correspond to the loss of saturated and unsaturated units containing up to a total of 6 carbon atoms. Furthermore, the aromatic structures that form the foundational building blocks of the larger PAHs were identified to be smaller single-ring and pericondensed aromatic species with repetitive structural features. For demonstrative purposes, details are provided for the CID of molecular ions at masses 202 and 434. Insights into the role of the aliphatically substituted and bridged aromatics in the reaction network of PAH growth chemistry were obtained from spatially resolved measurements of the flame. The experimental results are consistent with a growth mechanism in which alkylated aromatics are oxidized to form pericondensed ring structures or react and recombine with other aromatics to form larger, potentially three-dimensional, aliphatically bridged multicore aromatic hydrocarbons.
机译：本文提供了脂族取代和桥接多环芳烃（PAH）物种中的化学结构的实验证据，包括气味燃烧环境。通过采样气态成分与大气压逆Coflow扩散火焰的乙烯和高 - 高型，使得在PAH生长和烟灰成核中具有沉淀至PAH生长和烟灰成核来鉴定这些单和多芯芳族物种。分辨率串联质谱（MS-MS）。在这些实验中，使用10.0eV的连续VUV灯电离火焰取样组分，随后通过碰撞诱导的解离（CID）方法与Ar原子的碰撞分段。使用反射飞行时间质谱仪分离的所得片段离子，用于提取有关采样芳族化合物的结构信息。高分辨率质谱显示出存在烷基化的单核芳族化合物和观察到的片段离子对应于含有高达6个碳原子的饱和和不饱和单元的损失。此外，鉴定形成较大PAHS的基础结构块的芳族结构，以重复结构特征是较小的单环和迭代芳香族物种。出于说明性目的，提供细节用于质量群体202和434的分子离子的CID。从空间分辨的火焰的测量中获得了在PAH生长化学的反应网络中的脂族取代和桥接芳族化合物的作用的见解。实验结果与一种生长机制一致，其中烷基化芳烃被氧化以形成迭代的环结构或与其他芳烃反应并重新结合形成更大，潜在的三维，脂桥桥的多芯芳烃。

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