Chemical and toxicological properties of aerosol emissions subject to atmospheric processing

我们需要考虑大气气溶胶排放，不仅要考虑直接排放的颗粒物质，还要考虑通过大气处理可能形成次级颗粒物质的气体。然而，我们目前对这些气溶胶的化学形成和毒理学影响缺乏足够的基础科学认识。该项目旨在从EPSRC物理科学研究领域发展这一领域，但具有跨学科主题扩展休假（TBS）进入毒理学。氧化流反应器（OFR）可以提供一种标准化的方法来模拟排放源的大气过程，从而提供一种量化这些排放的气溶胶形成潜力的方法。这有助于为排放清单提供信息，并说明跨界污染的贡献。该博士学位将开发和应用使用新商业化的Dekati OFR产生这些气溶胶的新协议，并定量调查控制远程PM形成和人类健康影响的过程。这项工作将建立在NERC HIP-Tox联盟资助期间获得的先前经验的基础上，其中使用了许多标准化和可重复的来源（例如木炉，烹饪，柴油发动机）产生排放。将它们注入一个大型光化学反应室。这种复杂的方法不适合常规的排放评估，而且基础设施要求过于繁重，无法系统地探索跨排放源和大气条件的二次污染物范围。本博士的目标是使用Dekati OFR创建类似的大气处理模拟。OFR的操作条件将被优化，以模拟各种化学机制，并将使用曼彻斯特最先进的气溶胶仪器（包括气溶胶质谱仪）对气溶胶的质量和成分的影响进行量化。这种独特的先前工作的结合为这些真实世界来源的实验提供了化学和毒理学基础，将为基本过程提供新的重要见解。该项目旨在开发一种使用氧化流反应器（OFR）生成和量化二次和老化一次气溶胶的方案，适用于一系列重要的现实世界来源，并对这些气溶胶进行化学和毒理学分析。这些结果可用于为大气化学输送模型和空气污染的公共卫生影响模型提供信息。这将集中于以下具体目标：使用各种在线和离线化学分析技术，描述由OFR对以下气溶胶源引起的物理和化学转变。欧6柴油发动机。燃木炉（使用多种燃料）国内食品准备和进一步的机会主义探索一系列其他次要来源2。优化条件，使OFR最能代表区域大气老化，为污染源对空气质量的长期影响提供新的见解，重点关注气候变化对大气条件的可能变化。进一步开发一种方法，在对肺内膜液体进行详细成分分析的基础上，将气溶胶取样到生理相关的介质中，适用于毒理学评估，同时不捕获过量的气态氧化剂，以评估化学处理和二次气溶胶形成对健康的影响。

We need to account for atmospheric aerosol emissions not just in terms of directly emitted particulate matter but also gases that may form secondary particulate matter through atmospheric processing. However, we currently lack sufficient fundamental scientific understanding governing the chemical formation and toxicological impacts of these aerosols. This project seeks to develop this from the EPSRC physical sciences research area, but with an interdisciplinary thematic broadening sabbatical (TBS) crossing into toxicology.Oxidation flow reactors (OFR) can provide a standardised method of simulating atmospheric processes on sources of emission, and thus a method of quantifying the aerosol-forming potential of these emissions. This can help inform emission inventories and account for transboundary pollution contributions. This PhD will develop and apply a new protocol for the generation of these aerosols using the newly commercialised Dekati OFR and quantitatively investigate the processes governing long-range PM formation and human health impactsThis work will build on previous experience gained during the NERC HIP-Tox consortium grant, where a number of standardised and repeatable sources (e.g. wood stove, cooking, diesel engine) have been used to generate emissions, injecting them into a large photochemical reaction chamber. This complex methodology is unsuitable for routine emission evaluation, and the infrastructural requirements too burdensome to systematically explore the range of secondary pollutants across emission sources and atmospheric conditions. This PhD will aim to create similar atmospheric processing simulations using the Dekati OFR. The operating conditions of the OFR will be optimised to simulate various chemical regimes and the effect of this on the mass and the composition of the aerosol will be quantified using state of the art aerosol instrumentation at Manchester, including aerosol mass spectrometers. This unique combination of previous work to provide the chemical and toxicological basis for the experiments for these real-world sources will provide new important insights to the fundamental processes.The project aims to develop a protocol for the generation and quantification of secondary and aged primary aerosols using an oxidation flow reactor (OFR), applicable to a range of important real-world sources, and to subject these to chemical and toxicological analysis. These results can be used to inform models of atmospheric chemical transport models and public health impacts of air pollution. This will focus on the following specific objectives:1. Characterise the physical and chemical transformations induced by the OFR on the following aerosol sources, using a variety of on- and offline chemical analytical techniquesa. Euro 6 diesel engineb. Wood burning stove (using a variety of fuels)c. Domestic food preparationand further opportunistic exploration of a range of other secondary sources2. Optimise the conditions with the OFR to be most representative of regional atmospheric ageing, to provide new insight into long range impacts of pollution sources on air quality, with a focus on possible changes to atmospheric conditions in a changing climate.3. Further develop a method of sampling the aerosol into a physiologically relevant media, based on a detailed compositional analysis of lung lining fluids, suitable for toxicological assessment, without capturing excessive amounts of gaseous oxidants, for the purposes of evaluating the impacts of chemical processing and secondary aerosol formation on health.