期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 22, 期 9, 页码 5314-5331出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0cp00116c
关键词
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资金
- US Department of Energy, Basic Energy Sciences [DE-FG02-04ER15570]
- Ministry of Higher Education and Science of the Russian Federation [14.Y26.31.0020]
The mechanism of carbon particulate (soot) inception has been a subject of numerous studies and debates. The article begins with a critical review of prior proposals, proceeds to the analysis of factors enabling the development of a meaningful nucleation flux, and then introduces new ideas that lead to the fulfillment of these requirements. In the new proposal, a rotationally-activated dimer is formed in the collision of an aromatic molecule and an aromatic radical; the two react during the lifetime of the dimer to form a stable, doubly-bonded bridge between them, with the reaction rooted in a five-member ring present on the molecule edge. Several such reactions were examined theoretically and the most promising one generated a measurable nucleation flux. The consistency of the proposed model with known aspects of soot particle nanostructure is discussed. The foundation of the new model is fundamentally the H-Abstraction-Carbon-Addition (HACA) mechanism with the reaction affinity enhanced by rotational excitation.
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