Propionamide participating in H(2)SO(4)-based new particle formation: a theory study.
Propionamide participating in H(2)SO(4)-based new particle formation: a theory study.
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DOI：
10.1039/d0ra09323h
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发表时间：
2020-12-21
期刊：
影响因子：
3.9
通讯作者：
Wang W
中科院分区：
文献类型：
--
作者：
Zhao X;Li Y;Zuo C;Sun Y;Xu F;Nadykto AB;Du L;Xu Y;Zhang Q;Wang W
丙酰胺（PA）是一种重要的排放源，在世界范围内大量存在，并可能参与新粒子形成（NPF）。本研究利用计算化学和动力学模型研究了（PA）m(SA)n （m = 0-3和n = 0-3）簇的形成机理，评价了PA对H2SO4 （SA）基NPF的增强作用。我们的研究证明了所有含pa团簇的形成都是热力学有利的。此外，在PA多于SA的簇中，PA中的O基团起着重要的作用，并且随着SA量的增加，碱基的碱度的影响更大。研究表明，尽管PA的增强潜力低于甲胺（MA）和二甲胺（DMA）等最强的sa基NPF增强剂，但PA可以在十亿分之一（ppb）的水平上增强sa基NPF，这是典型的c3 -酰胺浓度，例如上海城市（中国）。单体蒸发是（PA）m(SA)n团簇的主要降解途径，与SA - dma体系的降解途径不同。含PA簇的形成速率与羟基（OH）自由基氧化PA的速率系数相当，表明参与基于sa的NPF是PA的关键sink。丙酰胺（PA）是一种重要的排放源，在世界范围内大量存在，并可能参与新粒子形成（NPF）。
Propionamide (PA), an important pollutant emitted into the atmosphere from a variety of sources, is abundant in many areas worldwide, and could be involved in new particle formation (NPF). In this study, the enhancement of the H2SO4 (SA)-based NPF by PA was evaluated through investigating the formation mechanism of (PA)m(SA)n (m = 0–3 and n = 0–3) clusters using computational chemistry and kinetics modeling. Our study proved that the formation of all the PA-containing clusters is thermodynamically favorable. Furthermore, the O group in PA plays an important role in the clusters with more PA than SA, and the basicity of bases exerts a greater influence with an increasing amount of SA. We demonstrate that although the enhancing potential of PA is lower than that of the strongest enhancers of SA-based NPF such as methylamine (MA) and dimethylamine (DMA), PA can enhance the SA-based NPF at the parts per billion (ppb) level, which is typical for concentrations of C3-amides in, for example, urban Shanghai (China). The monomer evaporation is the dominant degradation pathway for the (PA)m(SA)n clusters, which differs from that of the SA–DMA system. The formation rate of PA-containing clusters is comparable to the rate coefficients for PA oxidation by hydroxyl (OH) radicals, indicating that participating in the SA-based NPF is a crucial sink for PA. Propionamide (PA), an important pollutant emitted into the atmosphere from a variety of sources, is abundant in many areas worldwide, and could be involved in new particle formation (NPF).
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