Enhanced uptake of glyoxal at the acidic nanoparticle interface: implications for secondary organic aerosol formation
Enhanced uptake of glyoxal at the acidic nanoparticle interface: implications for secondary organic aerosol formation
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酸性纳米颗粒界面乙二醛的吸收增强：对二次有机气溶胶形成的影响
DOI：
10.1039/d0en00016g
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发表时间：
2020
影响因子：
7.3
通讯作者：
An Taicheng
中科院分区：
文献类型：
--
作者：
Shi Qiuju;Zhang Weina;Ji Yuemeng;Wang Jiaxin;Qin D;an;Chen Jiangyao;Gao Yanpeng;Li Guiying;An Taicheng
乙二醛（GL）是二次有机气溶胶（SOA）的重要前体物质，具有广泛的生物和人为来源，但其界面化学对SOA形成的贡献尚不确定。在这里，我们进行了分子动力学（MD）模拟和量子化学（QC）计算，以检查的界面过程中的气态GL对水性纳米粒子，包括探测GL吸引的纳米粒子，在空气-纳米粒子界面的吸收，以及在中性和酸性条件下的纳米粒子内的水合反应。分子动力学模拟结果表明，GL的羰基O原子在空气-纳米颗粒界面上具有择优取向。酸性纳米颗粒界面相对于中性纳米颗粒界面显示出对气态GL吸收的偏好，表明硫酸（SA）的存在增强了对GL的吸附和容纳。此外，SA加速了GL在纳米颗粒内部区域内的水反应，这间接促进了在纳米颗粒界面处的摄取。我们的研究结果揭示了显着增强的酸性纳米粒子界面处的GL的摄取，强调了评估SOA形成时考虑界面过程的必要性。
Glyoxal (GL) represents an important precursor of a secondary organic aerosol (SOA) and has broad biogenic and anthropogenic sources, but the interfacial chemistry of GL contributing to SOA formation is uncertain. Here, we performed molecular dynamics (MD) simulations and quantum chemical (QC) calculations to examine the interfacial process of gaseous GL on aqueous nanoparticles, including probing the GL attraction to the nanoparticles, uptake at the air–nanoparticle interface, and the hydration reaction within the nanoparticles under neutral and acidic conditions. The MD simulations show that the carbonyl O-atom of GL exhibits a preferential orientation to the air–nanoparticle interface. The acidic nanoparticle interface displays a preference for the uptake of gaseous GL relative to the neutral nanoparticle interface, showing that the presence of sulfuric acid (SA) enhances the adsorption and accommodation for GL. In addition, SA accelerates the aqueous reaction of GL inside the interior region of the nanoparticle, which indirectly promotes the uptake at the nanoparticle interface. Our results reveal the significantly enhanced uptake of GL at the acidic nanoparticle interface, highlighting the necessity to account for the interfacial process when assessing SOA formation.