The Aarhus Chamber Campaign on Highly Oxygenated Organic Molecules and Aerosols (ACCHA): particle formation, organic acids, and dimer esters from α-pinene ozonolysis at different temperatures
The Aarhus Chamber Campaign on Highly Oxygenated Organic Molecules and Aerosols (ACCHA): particle formation, organic acids, and dimer esters from α-pinene ozonolysis at different temperatures
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奥尔胡斯高含氧有机分子和气溶胶室运动 (ACCHA)：不同温度下 α-蒎烯臭氧分解产生的颗粒形成、有机酸和二聚酯
DOI：
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发表时间：
2020
期刊：
影响因子：
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通讯作者：
M. Bilde
中科院分区：
文献类型：
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作者：
K. Kristensen;Louise J. N. Jensen;L. Quéléver;S. Christiansen;B. Rosati;J. Elm;R. Teiwes;Henrik B Pedersen;M. Glasius;M. Ehn;M. Bilde
抽象的。关于零度以下的温度对地层的影响，
二次有机气溶胶（SOA）的α -蒎烯。在当前
工作，臭氧引发的氧化α -蒎烯在初始
浓度分别为10和50 ppb，在
温度为20、0和−15摄氏度，
奥胡斯大学研究气溶胶（AURA）烟雾室在奥胡斯商会运动的高含氧
有机分子和气溶胶（ACCHA）。在这里，我们展示了温度如何影响
α -蒎烯衍生的SOA的形成和化学组成
具体侧重于有机酸和二聚体酯的形成。与
关于颗粒形成，结果显示，
颗粒形成率、颗粒数浓度和颗粒质量
低温下的浓度。特别是，
在较低的0和-15 ° C温度下，10 nm以下颗粒的数量显著增加。温度也影响
形成SOA的化学成分。在这里，详细的离线化学
分析表明有机酸占15 - 30质量%，
在最低温度下观察到的贡献最大，
这些半挥发性物质的浓缩作用。相比之下，A
发现总共30种鉴定的二聚体酯占总SOA质量的4%至11%。化学成分无显著差异
α -蒎烯衍生的SOA颗粒的组成（即有机酸和二聚体酯）在以下条件下进行的实验之间观察到：
10和50 ppb的初始α -蒎烯浓度，从而表明
反应温度对SOA化学组成的影响大于α -蒎烯负载量。有趣的是，
温度对二聚体酯形成的影响不同，
个别物种。较少氧化的二聚体酯的形成-与
氧碳比（O：C）0.4 -显示出在低
温度，而更多的氧化物种（O：C > 0.4）的形成受到抑制，因此导致
α -蒎烯衍生的SOA的温度调制组合物。
将α -蒎烯衍生的SOA暴露于
温度变化（加热和冷却）表明，
相对于二聚体酯的SOA的组成几乎
仅仅由氧化开始时的温度决定，
随后的温度变化。同样，由此产生的SOA质量
浓度被发现是更多的影响，由初始α -蒎烯氧化温度，从而表明，形成
条件在很大程度上决定了形成的SOA的类型，而不是
这是SOA后来暴露的条件。本文首次讨论了已鉴定的二聚体
酯和高度氧化的有机分子（HOM），
化学电离-大气压界面-飞行时间质谱仪（CI-APi-ToF）在ACCHA实验期间。我们提出
尽管化学结构和O：C比例非常不同，但许多
二聚体酯和HOM可以通过类似的RO 2反应连接
二聚体酯和HOM仅仅代表两种不同的途径，
RO 2自由基的命运
Abstract. Little is known about the effects of subzero temperatures on the formation
of secondary organic aerosol (SOA) from α -pinene. In the current
work, ozone-initiated oxidation of α -pinene at initial
concentrations of 10 and 50 ppb, respectively, is performed at
temperatures of 20, 0, and −15 ∘ C in
the Aarhus University Research on Aerosol (AURA) smog chamber during the Aarhus Chamber Campaign on Highly Oxygenated
Organic Molecules and Aerosols (ACCHA). Herein, we show how temperature influences the
formation and chemical composition of α -pinene-derived SOA with a
specific focus on the formation of organic acids and dimer esters. With
respect to particle formation, the results show significant increase in
particle-formation rates, particle number concentrations, and particle mass
concentrations at low temperatures. In particular, the number concentrations
of sub-10 nm particles were significantly increased at the lower 0 and −15 ∘ C temperatures. Temperature also affects
the chemical composition of formed SOA. Here, detailed offline chemical
analyses show that organic acids contribute from 15 % to 30 % by mass,
with highest contributions observed at the lowest temperatures, indicative
of enhanced condensation of these semivolatile species. In comparison, a
total of 30 identified dimer esters were seen to contribute between 4 % and 11 % to the total SOA mass. No significant differences in the chemical
composition (i.e. organic acids and dimer esters) of the α -pinene-derived SOA particles are observed between experiments performed at
10 and 50 ppb initial α -pinene concentrations, thus suggesting a
higher influence of reaction temperature compared to that of α -pinene loading on the SOA chemical composition. Interestingly, the effect
of temperature on the formation of dimer esters differs between the
individual species. The formation of less oxidized dimer esters – with
oxygen-to-carbon ratio ( O : C ) 0.4 – is shown to increase at low
temperatures, while the formation of the more oxidized species ( O : C > 0.4 ) is suppressed, consequently resulting in
temperature-modulated composition of the α -pinene-derived SOA.
Temperature ramping experiments exposing α -pinene-derived SOA to
changing temperatures (heating and cooling) reveal that the chemical
composition of the SOA with respect to dimer esters is governed almost
solely by the temperature at which oxidization started and is insusceptible to
subsequent changes in temperature. Similarly, the resulting SOA mass
concentrations were found to be more influenced by the initial α -pinene oxidation temperatures, thus suggesting that the formation
conditions to a large extent govern the type of SOA formed, rather than the
conditions to which the SOA is later exposed. For the first time, we discuss the relation between the identified dimer
ester and the highly oxygenated organic molecules (HOMs) measured by
chemical ionization–atmospheric pressure interface–time-of-flight mass spectrometer (CI-APi-ToF) during the ACCHA experiments. We propose
that, although very different in chemical structures and O:C ratios, many
dimer esters and HOMs may be linked through similar RO2 reaction
pathways and that dimer esters and HOMs merely represent two different
fates of the RO2 radicals.
影响因子：
6.3
作者：
Ying Li;M. Shiraiwa
通讯作者：
Ying Li;M. Shiraiwa
DOI：
10.1073/pnas.1517742112
发表时间：
2015-11
期刊：
Proceedings of the National Academy of Sciences
影响因子：
--
作者：
Xuan Zhang;Renee McVay;D. Huang;N. Dalleska;B. Aumont;R. Flagan;J. Seinfeld
通讯作者：
Xuan Zhang;Renee McVay;D. Huang;N. Dalleska;B. Aumont;R. Flagan;J. Seinfeld
影响因子：
3.4
作者：
Claflin, Megan S.;Krechmer, Jordan E.;Ziemann, Paul J.
通讯作者：
Ziemann, Paul J.