Ammonium-Induced Stabilization of Imidazoles in Aerosol Particles

IF 2.9 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY ACS Earth and Space Chemistry Pub Date : 2025-02-13 DOI:10.1021/acsearthspacechem.4c00378
Malsha Amugoda,  and , James F. Davies*, 
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Abstract

The chemical evolution of biomass burning aerosol occurs through reactive and nonreactive pathways, with both involving the partitioning of semivolatile organic compounds (SVOCs) between the gas and particle phase. Here, we explore the vapor pressure of imidazoles, a class of compounds characterized by an aromatic N-containing five-membered ring and commonly found in atmospheric particles. We estimate liquid phase vapor pressures of these compounds to be greater than 0.2 Pa, indicating that these compounds are highly volatile SVOCs. Despite this, ambient measurements identified imidazoles in the particle phase. In this work, we show that when imidazoles are internally mixed with certain inorganic salts, they are stabilized in the particle phase. In these mixed particles, we measure two distinct phases of evaporation, characterized by fast and slow changes. We analyze these regions separately, allowing the evolving composition of the particle to be determined from an evaporation model and identifying the characteristic composition at which stabilization occurs. Based on these observations, further supported by water uptake behavior and optical properties, we determine that the stabilization is driven by ammonium depletion due to protonation of the imidazole and evaporation of ammonia. This work highlights the importance of considering cosolutes and their stabilizing effect on SVOCs, with important implications for understanding and predicting the composition of biomass burning aerosol particles.

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氨诱导咪唑在气溶胶颗粒中的稳定作用
生物质燃烧气溶胶的化学演变通过反应性和非反应性途径发生,两者都涉及半挥发性有机化合物(SVOCs)在气相和颗粒相之间的分配。在这里,我们研究了咪唑的蒸汽压,咪唑是一类以芳香含n的五元环为特征的化合物,通常存在于大气颗粒中。我们估计这些化合物的液相蒸汽压大于0.2 Pa,表明这些化合物是高度挥发的SVOCs。尽管如此,环境测量发现咪唑处于颗粒相。在这项工作中,我们表明,当咪唑与某些无机盐内部混合时,它们在颗粒相中稳定。在这些混合粒子中,我们测量了蒸发的两个不同阶段,其特征是快速和缓慢的变化。我们分别分析这些区域,允许从蒸发模型确定粒子的演变组成,并确定稳定发生的特征组成。基于这些观察结果,并进一步得到水吸收行为和光学性质的支持,我们确定稳定化是由咪唑质子化和氨蒸发引起的铵耗竭驱动的。这项工作强调了考虑溶质及其对SVOCs的稳定作用的重要性,对理解和预测生物质燃烧气溶胶颗粒的组成具有重要意义。
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来源期刊
ACS Earth and Space Chemistry
ACS Earth and Space Chemistry Earth and Planetary Sciences-Geochemistry and Petrology
CiteScore
5.30
自引率
11.80%
发文量
249
期刊介绍: The scope of ACS Earth and Space Chemistry includes the application of analytical, experimental and theoretical chemistry to investigate research questions relevant to the Earth and Space. The journal encompasses the highly interdisciplinary nature of research in this area, while emphasizing chemistry and chemical research tools as the unifying theme. The journal publishes broadly in the domains of high- and low-temperature geochemistry, atmospheric chemistry, marine chemistry, planetary chemistry, astrochemistry, and analytical geochemistry. ACS Earth and Space Chemistry publishes Articles, Letters, Reviews, and Features to provide flexible formats to readily communicate all aspects of research in these fields.
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