4.7 Article

Heterogeneous formation of EPFRs from aromatic adsorbates on the carbonaceous particulate matter

期刊

APPLIED SURFACE SCIENCE
卷 602, 期 -, 页码 -

出版社

ELSEVIER
DOI: 10.1016/j.apsusc.2022.154316

关键词

Particulate matter; Density functional theory; Graphene oxide; Reaction route; Surface groups; Carbon vacancy

资金

  1. NSFC (National Natural Science Foundation of China) [21876102]
  2. Taishan Scholars

向作者/读者索取更多资源

This study investigates the formation mechanism of environmentally persistent free radicals (EPFRs) on carbonaceous particulate matter. The results reveal that aromatic precursors tend to undergo homolytic fission on the surface of carbonaceous PM to form EPFRs, with surface OH groups and water playing essential roles. This study unveils the formation mechanism of EPFRs on carbonaceous particulate matter and highlights the differences from the mechanism on metal oxide surfaces.
Pyrogenic carbonaceous materials of atmospheric particulate matter (PM) have recently aroused intensive interest, due to their critical role in the formation of environmentally persistent free radicals (EPFRs). This study focuses on the heterogeneous formation of EPFRs on the graphene oxide (GO), the dominant component of carbonaceous PM. First-principles calculations have been performed to investigate the interaction between 2-chlorophenol (2-CP), an important precursor of EPFRs, and GO to find the stable adsorption configurations. The climbing image nudged elastic band (CI-NEB) method and Dimer method were employed to explore the decomposition route of 2-CP to generate different types of EPFRs on the GO surface. The results indicate that aromatic precursors tend to undergo homolytic fission rather than heterolytic splitting to form EPFRs induced by surface oxygen-containing groups and carbon defects on the carbonaceous PM. Surface OH groups and water, both of which are related to ambient humidity, play essential roles in producing EPFRs. The formation mechanism of EPFRs over GO unveiled in this study, which represents dramatic differences from the conventional mechanism on the metal oxide surfaces, may account for a previously overlooked source of EPFRs encountered in atmospheric PM.

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。

评论

主要评分

4.7
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

暂无数据
暂无数据