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Dust-Catalyzed Oxidative Polymerization of Catechol and Its Impacts on Ice Nucleation Efficiency and Optical Properties
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2020-06-08 , DOI: 10.1021/acsearthspacechem.0c00107
Nicole Link 1 , Nicole Removski 1 , Jingwei Yun 1 , Lauren T. Fleming 2 , Sergey A. Nizkorodov 2 , Allan K. Bertram 1 , Hind A. Al-Abadleh 3
Affiliation  

Dust is the major source of iron in atmospheric aerosols but little is known about its role in catalyzing polymerization reactions of organics in particles. Using Arizona Test Dust (AZTD) and hematite nanoparticles as laboratory standards and proxies for hematite-rich natural dust, respectively, we show that their reactions with catechol in aqueous slurries lead to the formation of black polycatechol. This observation is in contrast to oxalate and sulfate which form surface complexes promoting the dissolution of iron from the dust particles. Results from ultraviolet–visible spectroscopy and microscopy/elemental mapping show that the formation of polycatechol changed the optical properties of the dust particles and surface chemical composition. Results from ice nucleation studies using a droplet freezing technique show that polycatechol did not significantly impact ice nucleation or block ice nucleation sites on AZTD. In contrast, increasing pH decreased the ice nucleation ability of AZTD. These results highlight the complexity of iron’s role in aerosol aging processes, brown carbon formation, and ice nucleation.

中文翻译:

邻苯二酚的粉尘催化氧化聚合及其对冰成核效率和光学性质的影响

灰尘是大气气溶胶中铁的主要来源,但对其催化颗粒中有机物聚合反应的作用知之甚少。分别使用Arizona Test Dust(AZTD)和赤铁矿纳米粒子作为实验室标准品和富含赤铁矿的天然粉尘的代理,我们证明了它们与水性浆液中邻苯二酚的反应会导致黑色聚儿茶酚的形成。该观察结果与草酸盐和硫酸盐形成表面复合物相反,草酸盐和硫酸盐形成表面络合物,促进铁从尘埃颗粒中溶解。紫外可见光谱和显微镜/元素图谱的结果表明,聚儿茶酚的形成改变了尘埃颗粒的光学性质和表面化学成分。使用液滴冷冻技术进行冰核研究的结果表明,聚儿茶酚不会显着影响冰成核或阻止AZTD上的冰成核部位。相反,增加pH会降低AZTD的冰核能力。这些结果凸显了铁在气溶胶老化过程,褐碳形成和冰核化中作用的复杂性。
更新日期:2020-07-16
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