Heterogeneous Nucleation Drives Particle Size Segregation in Sequential Ozone and Nitrate Radical Oxidation of Catechol,Environmental Science & Technology

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Heterogeneous Nucleation Drives Particle Size Segregation in Sequential Ozone and Nitrate Radical Oxidation of Catechol
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2021-11-23 , DOI: 10.1021/acs.est.1c02984
Lauren A Garofalo ₁ , Yicong He ₂ , Shantanu H Jathar ₂ , Jeffrey R Pierce ₃ , Carley D Fredrickson ₄ , Brett B Palm ₄ , Joel A Thornton ₄ , Fabian Mahrt _{5,

6} , Giuseppe V Crescenzo ₅ , Allan K Bertram ₅ , Danielle C Draper _{7,

8} , Juliane L Fry ₇ , John Orlando ₉ , Xuan Zhang _{9,

10} , Delphine K Farmer ₁

Affiliation

Department of Chemistry, Colorado State University, Fort Collins, Colorado 80523, United States.
Department of Mechanical Engineering, Colorado State University, Fort Collins, Colorado 80523, United States.
Department of Atmospheric Science, Colorado State University, Fort Collins, Colorado 80523, United States.
Department of Atmospheric Sciences, University of Washington, Seattle, Washington 98195, United States.
Department of Chemistry, University of British Columbia, Vancouver, British Columbia V6T 1Z4, Canada.
Laboratory of Environmental Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.
Department of Chemistry, Reed College, Portland, Oregon 97202, United States.
Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, California 91125, United States.
National Center for Atmospheric Research, Boulder, Colorado 80307, United States.
Department of Life and Environmental Sciences, University of California, Merced, California 95343, United States.

Secondary organic aerosol formation via condensation of organic vapors onto existing aerosol transforms the chemical composition and size distribution of ambient aerosol, with implications for air quality and Earth’s radiative balance. Gas-to-particle conversion is generally thought to occur on a continuum between equilibrium-driven partitioning of semivolatile molecules to the pre-existing mass size distribution and kinetic-driven condensation of low volatility molecules to the pre-existing surface area size distribution. However, we offer experimental evidence in contrast to this framework. When catechol is sequentially oxidized by O₃ and NO₃ in the presence of (NH₄)₂SO₄ seed particles with a single size mode, we observe a bimodal organic aerosol mass size distribution with two size modes of distinct chemical composition with nitrocatechol from NO₃ oxidation preferentially condensing onto the large end of the pre-existing size distribution (∼750 nm). A size-resolved chemistry and microphysics model reproduces the evolution of the two distinct organic aerosol size modes─heterogeneous nucleation to an independent, nitrocatechol-rich aerosol phase.

中文翻译：

非均相成核驱动邻苯二酚的连续臭氧和硝酸根自由基氧化中的粒度分离

通过有机蒸气冷凝到现有气溶胶上形成的二次有机气溶胶改变了环境气溶胶的化学成分和尺寸分布，对空气质量和地球辐射平衡产生影响。气体到颗粒的转化通常被认为发生在平衡驱动的半挥发性分子分配到预先存在的质量尺寸分布和低挥发性分子的动力学驱动冷凝到预先存在的表面积尺寸分布之间的连续体上。但是，我们提供了与此框架相反的实验证据。当邻苯二酚在 (NH ₄ ) ₂ SO ₄存在下被 O ₃和 NO ₃依次氧化时对于具有单一尺寸模式的种子颗粒，我们观察到双峰有机气溶胶质量尺寸分布，具有两种不同化学成分的尺寸模式，来自 NO ₃氧化的硝基儿茶酚优先冷凝到预先存在的尺寸分布的大端（~750 nm）。尺寸分辨化学和微物理学模型再现了两种不同的有机气溶胶尺寸模式的演变——异质成核到独立的、富含硝基儿茶酚的气溶胶相。

更新日期：2021-12-07

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