Investigation of Organic Nitrogen in Atmospheric Aerosols

大气气溶胶中有机氮的研究

• 批准号: NE/F01905X/1
• 负责人: Jacqueline Hamilton
• 金额: $ 36.58万
• 依托单位: University of York
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2008
• 资助国家: 英国
• 起止时间: 2008 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=NE%2FF01905X%2F1
• 关键词: Investigation; Organic; Nitrogen; Atmospheric; Aerosols

Organic nitrogen (ON) is ubiquitous in the atmosphere. Atmospheric particles typically have high concentrations of nitrogen and are a significant source of fixed nitrogen to the environment (though deposition processes), which may have an adverse impact on terrestrial and aquatic ecosystem. While the sources, formation and composition of oxygenated organics in the atmosphere have been extensively studied in recent years, ON has not received the same attention. Studies of atmospherically relevant processes (such as photo-chemical transformations) have been carried out on individual ON compounds but these studies are fundamentally limited since the bulk of ON in atmospheric particles is not characterized. The composition of ON within a particle may have an effect on its properties (such as hygroscopicity, toxicity and bio-availability) which will also change as the particle ages during long-range transport and may ultimately lead to the formation of humic-like substances. Studies have shown that when aqueous extracts of bulk ON from atmospheric aerosols were exposed to simulated sunlight and ozone, a significant portion of the ON was transformed into ammonium, nitrate and oxides of nitrogen. Atmospheric particles have been linked to increased mortality in the human population and a number of ON species are implicated in the toxicity of aerosols (e.g. nitrogentated polycyclic aromatic hydrocarbons, quinolines, nitroso-amines). The aim of this project is to build a novel, high resolution ON-Analyser capable of measuring the semi-volatile ON composition of atmospheric aerosols, for which there is currently very little known. It is based on a high resolution chromatographic technique (comprehensive two-dimensional gas chromatography - GCXGC) which is ideally suited to separating highly complex mixtures. This will be coupled to a highly selective nitrogen chemiluminescence detector, which provides a response for organic compounds containing nitrogen only. This removes interferences from the complex organic background found in aerosols. Aerosols will be samples onto filters and the ON content extracted using an Aerosol Thermal Desorption Injector. This novel instrument will be used to investigate the composition of ON species in aerosol in different environments, reflecting increasing photo-chemical age, from a polluted city centre roadside location (York) to a clean coastal rural site (Weybourne). Due to the complexity of the real atmosphere, linking the initial species emitted to the atmosphere to their reaction products in aerosol can be difficult. We will use the ON-Analyser to investigate the composition of ON in secondary organic aerosol formed in smog chamber simulations, allowing a direct link between pre-cursors and products. The outcomes of this project will increase our understanding of the composition, formation and transformation of organic nitrogen species in the atmosphere, providing valuable information across a range of disciplines including air quality, climate change and ecology.

有机氮（ON）在大气中无处不在。大气颗粒通常含有高浓度的氮，是环境中固定氮的重要来源（通过沉积过程），这可能对陆地和水生生态系统产生不利影响。尽管近年来人们对大气中含氧有机物的来源、形成和组成进行了广泛的研究，但ON并没有受到同样的关注。已经对单个 ON 化合物进行了与大气相关的过程（例如光化学转化）的研究，但这些研究从根本上受到限制，因为大气颗粒中的大部分 ON 尚未表征。颗粒内 ON 的组成可能会影响其特性（例如吸湿性、毒性和生物利用度），这些特性也会随着颗粒在长距离运输过程中的老化而发生变化，并可能最终导致腐殖质类物质的形成。研究表明，当从大气气溶胶中提取的大量 ON 的水提取物暴露于模拟阳光和臭氧时，很大一部分 ON 转化为铵、硝酸盐和氮氧化物。大气颗粒物与人类死亡率增加有关，并且许多 ON 物种与气溶胶的毒性有关（例如氮化多环芳烃、喹啉、亚硝基胺）。该项目的目的是构建一种新型高分辨率 ON 分析仪，能够测量大气气溶胶的半挥发性 ON 成分，目前对此知之甚少。它基于高分辨率色谱技术（全二维气相色谱 - GCXGC），非常适合分离高度复杂的混合物。它将与高选择性氮化学发光检测器耦合，该检测器为仅含氮的有机化合物提供响应。这消除了气溶胶中复杂有机背景的干扰。气溶胶将被采样到过滤器上，并使用气溶胶热解吸注射器提取 ON 含量。这种新颖的仪器将用于研究不同环境中气溶胶中 ON 物种的组成，反映从受污染的市中心路边位置（约克）到清洁的沿海乡村地点（韦伯恩）的光化学年龄的增加。由于真实大气的复杂性，将排放到大气中的初始物质与其气溶胶中的反应产物联系起来可能很困难。我们将使用 ON-Analyser 研究烟雾室模拟中形成的二次有机气溶胶中 ON 的成分，从而在前体和产品之间建立直接联系。该项目的成果将增进我们对大气中有机氮物种的组成、形成和转化的理解，为空气质量、气候变化和生态学等一系列学科提供有价值的信息。

项目成果

The import and export of organic nitrogen species at a Scottish ombrotrophic peatland

• DOI: 10.5194/bg-13-2353-2016
• 发表时间: 2015-01
• 期刊: Biogeosciences
• 影响因子: 4.9
• 作者: R. Mckenzie;M. Z. Ozel;J. Cape;J. Drewer;K. Dinsmore;E. Nemitz;Y. S. Tang;N. Dijk;M. Anderson;J. Hamilton;M. Sutton;M. Gallagher;U. Skiba

Comparative study of comprehensive gas chromatography-nitrogen chemiluminescence detection and gas chromatography-ion trap-tandem mass spectrometry for determining nicotine and carcinogen organic nitrogen compounds in thirdhand tobacco smoke.

气相色谱-氮化学发光综合检测法与气相色谱-离子阱-串联质谱法测定三手烟草烟气中尼古丁和致癌有机氮化合物的对比研究

• DOI: 10.1016/j.chroma.2015.11.035
• 发表时间: 2015
• 期刊: Journal of chromatography. A
• 作者: Ramírez N

Theoretical and Experimental Study on the Reaction of tert-Butylamine with OH Radicals in the Atmosphere.

• DOI: 10.1021/acs.jpca.8b01862
• 发表时间: 2018-04
• 期刊: The journal of physical chemistry. A
• 作者: Wen Tan;Liang Zhu;T. Mikoviny;C. Nielsen;A. Wisthaler;Philipp Eichler;M. Müller;B. d'Anna;Naomi J. Farren;J. Hamilton;J. Pettersson;M. Hallquist;S. Antonsen;Y. Stenstrøm