Gas-Phase Nitrate Radical Production Using Irradiated Ceric Ammonium Nitrate: Insights into Secondary Organic Aerosol Formation from Biogenic and Biomass Burning Precursors

利用辐照铈铵硝酸盐生成气相硝酸自由基:深入了解生物质燃烧前体物中二次有机气溶胶的形成

阅读:1

Abstract

The importance of nitrate radicals (NO3) as a nighttime atmospheric oxidant is well-established. For decades, laboratory studies of multiphase NO3 chemistry have used the same methods - either NO2 + O3 reactions or N2O5 thermal decomposition - to generate NO3 as it occurs in the atmosphere. These methods, however, come with limitations, especially for N2O5 , which must be produced and stored under cold and dry conditions until use. Recently, we developed a new photolytic source of gas-phase NO3 by irradiating aerated aqueous solutions of ceric ammonium nitrate and nitric acid. In this study, we adapted the method to maintain stable NO3 concentrations for over 24 hr. We applied the method in laboratory oxidation flow reactor (OFR) experiments to measure the yield and chemical composition of oxygenated volatile organic compounds (OVOCs) and secondary organic aerosol (SOA) formed from NO3 oxidation of volatile organic compounds (VOCs) emitted by biogenic sources (isoprene, β -pinene, limonene and β -caryophyllene) and biomass burning sources (phenol, guaiacol and syringol). SOA yields and elemental ratios were typically within a factor of 2 and 10%, respectively, of those obtained in studies using conventional NO3 sources. Maximum SOA yields obtained in our studies ranged from 0.02 ( isoprene/NO3 ) to 0.96 ( β -caryophyllene/ NO3 ). The highest SOA oxygen-to-carbon ratios (O/C) ranged from 0.48 ( β -caryophyllene/ NO3 ) to 1.61 ( syringol/NO3 ). Additionally, we characterized novel condensed-phase oxidation products from syringol/NO3 reactions. Overall, the use of irradiated aqueous cerium nitrate as a source of gas-phase NO3 may enable more widespread studies of NO3 -initiated oxidative aging, which has been less explored compared to hydroxyl radical chemistry.

特别声明

1、本页面内容包含部分的内容是基于公开信息的合理引用;引用内容仅为补充信息,不代表本站立场。

2、若认为本页面引用内容涉及侵权,请及时与本站联系,我们将第一时间处理。

3、其他媒体/个人如需使用本页面原创内容,需注明“来源:[生知库]”并获得授权;使用引用内容的,需自行联系原作者获得许可。

4、投稿及合作请联系:info@biocloudy.com。