期刊
PROCEEDINGS OF THE COMBUSTION INSTITUTE
卷 38, 期 1, 页码 1525-1532出版社
ELSEVIER SCIENCE INC
DOI: 10.1016/j.proci.2020.09.029
关键词
Soot formation; Molecular dynamics; Localized pi-radical; Aromatic rim-bonded hydrocarbons; Aromatic penta-linked hydrocarbons
资金
- National Research Foundation (NRF) , Prime Minister's Office, Singapore under its Campus for Research Excellence and Technological Enterprise (CREATE) programme
- European Union [724145]
- EPSRC [EP/R029369/1]
- ARCHER
- EPSRC [EP/R029369/1] Funding Source: UKRI
- H2020 Societal Challenges Programme [724145] Funding Source: H2020 Societal Challenges Programme
A new crosslinking reaction between two pentagonal rings around pericondensed aromatic molecules is proposed, leading to the formation of a stable aromatic molecule that may play a role in soot nucleation.
A new crosslinking reaction between two pentagonal rings around the periphery of planar pericondensed aromatic molecules is proposed and its impact on soot nanoparticle formation explored. The reaction mechanism was computed, using density functional theory, between an aryl-type sigma-radical on a rim-based pentagonal ring attacking another rim-based pentagonal ring. A hydrogen migration allowed for the formation of a double bond forming a planar aromatic penta-linked hydrocarbon (APLH) complex, recently experimentally observed. The clustering of this planar species is compared with a pericondensed polyaromatic hydrocarbon (PCAH) and an aromatic aryl-linked hydrocarbon (AALH) using molecular dynamics and metadynamics. Similar clustering is found for the investigated species compared with a pericondensed structure of similar mass indicating enhanced physical interactions after forming the crosslink. Finally, a further crosslink is possible between the unsaturated pentagonal ring sites forming an aromatic rim-linked hydrocarbon (ARLH) complex of considerable stability. This was confirmed by simulating the stable molecular dynamics of such a complex with on-the-fly quantum forces from a quantum semi-empirical method, revealing possible reactions under flame conditions that might play a role in soot nucleation. (C) 2020 The Combustion Institute. Published by Elsevier Inc. All rights reserved.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据