Inception of Carbonaceous Nanostructures via Hydrogen-Abstraction Phenylacetylene-Addition Mechanism,Journal of the American Chemical Society

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Inception of Carbonaceous Nanostructures via Hydrogen-Abstraction Phenylacetylene-Addition Mechanism
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-11-16 , DOI: 10.1021/jacs.1c08230
Hanfeng Jin ₁ , Lili Ye ₂ , Jiuzhong Yang ₃ , Yu Jiang ₄ , Long Zhao ₃ , Aamir Farooq ₁

Affiliation

Sufficient experimental evidence has suggested that polycyclic aromatic hydrocarbons are the building blocks of carbonaceous nanostructures in combustion and circumstellar envelops of carbon-rich stars, but their fundamental formation mechanisms remain elusive. By exploring the reaction kinetics of phenylacetylene with 1-naphthyl/4-phenanthryl radicals, we provide compelling theoretical and experimental evidence for a novel and self-consistent hydrogen-abstraction phenylacetylene-addition (HAPaA) mechanism. HAPaA operates efficiently at both low and high temperatures, leading to the formation, expansion, and nucleation of peri-condensed aromatic hydrocarbons (PCAHs), which are otherwise difficult to synthesis via traditional hydrogen-abstraction acetylene/vinylacetylene-addition pathways. The HAPaA mechanism can be generalized to other α-alkynyl PCAHs and thus provides an alternative covalent bond bridge for PCAH combination via an acetylene linker. The proposed HAPaA mechanism may contribute toward a comprehensive understanding of soot formation, carbonaceous nanomaterials synthesis, and the origin and evolution of carbon in our galaxy.

中文翻译：

通过提氢苯乙炔加成机制形成碳质纳米结构

充分的实验证据表明，多环芳烃是燃烧过程中碳质纳米结构和富碳恒星环绕恒星的基石，但它们的基本形成机制仍然难以捉摸。通过探索苯乙炔与 1-萘基/4-菲基自由基的反应动力学，我们为新颖且自洽的吸氢苯乙炔加成 (HAPaA) 机制提供了令人信服的理论和实验证据。HAPaA 在低温和高温下均能有效运行，从而导致环缩合芳烃 (PCAH) 的形成、膨胀和成核，否则这些烃很难通过传统的提氢乙炔/乙烯基乙炔加成途径合成。HAPaA 机制可以推广到其他 α-炔基 PCAH，从而通过乙炔连接体为 PCAH 结合提供替代的共价键桥。所提出的 HAPaA 机制可能有助于全面了解烟灰的形成、碳质纳米材料的合成以及我们银河系中碳的起源和演化。

更新日期：2021-12-15

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