煤烟上NO2转化为HONO的新机理:元素碳和有机碳的协同作用

IF 8.8 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL
Jianhua Chen, Hongyu Jiang, Xiaoran Chen, Jinzhao Wang, Di Huang, Chaofan Lian, Weigang Wang, Markus Ammann, Fengxia Bao*, Chuncheng Chen* and Jincai Zhao, 
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引用次数: 0

摘要

煤烟主要由元素碳(EC)和有机碳(OC)组成,在大气中通过与二氧化氮(NO2)的非均相反应形成亚硝酸(HONO)的过程中发挥着重要作用。在这项研究中,我们发现新鲜烟灰表现出比其单独的EC或OC成分高得多的HONO产率。这不支持先前提出的在烟灰表面的单个还原位点形成HONO的氢提取机制。基于我们对红外(IR)光谱和流管实验的观察,我们提出了一种新的机制,该机制涉及两个位点的协同参与:一个位于OC,另一个位于EC。它们通过质子耦合电子转移途径分别提供NO2还原为HONO所需的质子和电子。这一机制突出了OC和EC在烟灰释放HONO中的重要作用,并强调了烟灰成分对大气氧化能力的重要影响。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

A Novel Mechanism for NO2-to-HONO Conversion on Soot: Synergistic Effect of Elemental Carbon and Organic Carbon

A Novel Mechanism for NO2-to-HONO Conversion on Soot: Synergistic Effect of Elemental Carbon and Organic Carbon

Soot, mainly composed of elemental carbon (EC) and organic carbon (OC), plays an important role in the formation of atmospheric nitrous acid (HONO) through the heterogeneous reaction with nitrogen dioxide (NO2). In this study, we found that fresh soot exhibits a much higher HONO yield than its EC or OC components alone. This does not support the previously proposed hydrogen-abstraction mechanism for HONO formation at a single reductive site on the soot surface. Based on our observations of infrared (IR) spectroscopy and flow tube experiments, we propose a new mechanism that involves the synergistic participation of two sites: one located at OC and the other at EC. They provide a proton and an electron necessary for NO2 reduction to HONO, respectively, via a proton-coupled electron transfer pathway. This mechanism highlights the important roles of OC and EC in HONO release from soot and underscores the significant implications of soot compositions in atmospheric oxidative capacity.

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来源期刊
Environmental Science & Technology Letters Environ.
Environmental Science & Technology Letters Environ. ENGINEERING, ENVIRONMENTALENVIRONMENTAL SC-ENVIRONMENTAL SCIENCES
CiteScore
17.90
自引率
3.70%
发文量
163
期刊介绍: Environmental Science & Technology Letters serves as an international forum for brief communications on experimental or theoretical results of exceptional timeliness in all aspects of environmental science, both pure and applied. Published as soon as accepted, these communications are summarized in monthly issues. Additionally, the journal features short reviews on emerging topics in environmental science and technology.
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