Volatility of Secondary Organic Aerosol from β-Caryophyllene Ozonolysis over a Wide Tropospheric Temperature Range,Environmental Science & Technology

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Volatility of Secondary Organic Aerosol from β-Caryophyllene Ozonolysis over a Wide Tropospheric Temperature Range
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2023-06-07 , DOI: 10.1021/acs.est.3c01151
Linyu Gao _{1,

2} , Angela Buchholz ₃ , Zijun Li _{3,

4} , Junwei Song _{1,

2} , Magdalena Vallon ₁ , Feng Jiang _{1,

2} , Ottmar Möhler ₁ , Thomas Leisner _{1,

5} , Harald Saathoff ₁

Affiliation

We investigated secondary organic aerosol (SOA) from β-caryophyllene oxidation generated over a wide tropospheric temperature range (213–313 K) from ozonolysis. Positive matrix factorization (PMF) was used to deconvolute the desorption data (thermograms) of SOA products detected by a chemical ionization mass spectrometer (FIGAERO-CIMS). A nonmonotonic dependence of particle volatility (saturation concentration at 298 K, C_298K^*) on formation temperature (213–313 K) was observed, primarily due to temperature-dependent formation pathways of β-caryophyllene oxidation products. The PMF analysis grouped detected ions into 11 compound groups (factors) with characteristic volatility. These compound groups act as indicators for the underlying SOA formation mechanisms. Their different temperature responses revealed that the relevant chemical pathways (e.g., autoxidation, oligomer formation, and isomer formation) had distinct optimal temperatures between 213 and 313 K, significantly beyond the effect of temperature-dependent partitioning. Furthermore, PMF-resolved volatility groups were compared with volatility basis set (VBS) distributions based on different vapor pressure estimation methods. The variation of the volatilities predicted by different methods is affected by highly oxygenated molecules, isomers, and thermal decomposition of oligomers with long carbon chains. This work distinguishes multiple isomers and identifies compound groups of varying volatilities, providing new insights into the temperature-dependent formation mechanisms of β-caryophyllene-derived SOA particles.

中文翻译：

宽对流层温度范围内 β-石竹烯臭氧分解产生的二次有机气溶胶的挥发性

我们研究了臭氧分解在宽对流层温度范围 (213–313 K) 内产生的 β-石竹烯氧化产生的二次有机气溶胶 (SOA)。使用正矩阵分解 (PMF) 对化学电离质谱仪 (FIGAERO-CIMS) 检测到的 SOA 产物的解吸数据（热分析图）进行解卷积。观察到颗粒挥发度（298 K 时的饱和浓度， C _298K ^* ）对形成温度（213-313 K）的非单调依赖性，这主要是由于 β-石竹烯氧化产物的温度依赖性形成途径。 PMF 分析将检测到的离子分为 11 个具有特征挥发性的化合物组（因子）。这些复合组充当底层 SOA 形成机制的指标。它们不同的温度响应表明，相关的化学途径（例如，自氧化、低聚物形成和异构体形成）在213至313 K之间具有不同的最佳温度，明显超出了温度依赖性分配的影响。此外，将 PMF 解析的挥发性组与基于不同蒸气压估计方法的挥发性基组 (VBS) 分布进行比较。不同方法预测的挥发性变化受到高含氧分子、异构体和长碳链低聚物热分解的影响。这项工作区分了多种异构体并识别了不同挥发性的化合物组，为 β-石竹烯衍生的 SOA 颗粒的温度依赖性形成机制提供了新的见解。

更新日期：2023-06-07

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