Does Ozonolysis Chemistry affect Atmospheric Marine Boundary Layer Sulphur Cycling ?

臭氧分解化学是否影响大气海洋边界层硫循环？

• 批准号: NE/N013654/1
• 负责人: William Bloss
• 金额: $ 4.95万
• 依托单位: University of Birmingham
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2016
• 资助国家: 英国
• 起止时间: 2016 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=NE%2FN013654%2F1
• 关键词: Does; Ozonolysis; Chemistry; affect; Atmospheric

This Pump-Priming project will initiate a new collaboration with a leading Chinese research group (Prof Xinming Wang, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences). Our aim is to assess the importance of a new atmospheric reaction, recently discovered by the UK team through a current NERC research grant, using the unique simulation chamber facility available in Guangzhou.The wider project context is the atmospheric processing of sulphur species. Well understood atmospheric chemical processes break down the sulphur species - molecules such as dimethylsulphide (DMS) or SO2 - these reactions are driven by OH radicals in the gas phase, and form sulphate aerosol particles, which scatter sunlight and can catalyse the formation of cloud droplets - so the processing of sulphur species exerts a major influence upon climate. Sulphur processing leading to sulphuric acid also contributes to rainwater acidity.Our current NERC project aimed to investigate the impact of a new set of chemical reactants upon sulphur processing - the Stabilised Criegee Intermediates (SCIs). SCIs are formed from alkene-ozone reactions (found throughout the boundary layer) and alkyl iodide photolysis (in the marine boundary layer), and can act as atmospheric oxidants, like OH, initiating the processing of species such as SO2. Our current project was motivated by the recent discovery that the SCI + SO2 reaction was three orders of magnitude faster than previously thought - but SCI behaviour had not been tested under realistic atmospheric conditions. Our approach was to use the EUPHORE atmospheric simulation chamber (a 200 m3 reactor in Spain, in which an artificial atmosphere may be introduced - containing, for example, alkenes, ozone and SO2 - and fitted with instruments to monitor the evolving chemical composition). In EUPHORE, we have studied reactions of SCIs with SO2, H2O and their thermal decomposition - leading to five papers so far - and also discovered that SCIs, formed from isoprene-ozone reactions, react with DMS.DMS is the dominant natural sulphur emission (with volcanic SO2), so any enhancement in DMS oxidation (e.g. by SCIs, alongside OH) will increase the rate and change the spatial distribution of sulphate aerosol formation, of potentially substantial importance for atmospheric composition and climate. However, the instruments in EUPHORE could not determine the products of the SCI + DMS reaction; nor were we able to assess their dependence upon the alkene used to form the SCI. In this project, we propose to use the newly developed chamber in Guangzhou to resolve these uncertainties - the GIG chamber instrumentation can detect the gas- and condensed-phase DMS oxidation products, and has recently been used for a study of SCI chemistry in vehicle exhausts. The project will consist of PI / research staff exchanges to plan and model the chamber experiments in detail, followed by simulation chamber measurements to probe the SCI - DMS system in Guangzhou. These experiments will definitively determine the importance of this new reaction, under realistic atmospheric boundary layer conditions.This proposal has developed following discussions between Bloss and Wang at meetings in Beijing, and a visit by Bloss to the GIG facility in March 2015. In addition to the specific science goals, it will nurture a developing collaboration between UK groups (with substantial expertise in the conduct of simulation chamber experiments) and leading Chinese researchers at GIG (with unique chamber facilities) in atmospheric chemistry, with potential for future links, for example in the context of forthcoming NERC-Newton-NSFC "Urban Air Pollution in a Chinese Megacity" projects. China is rapidly emerging as a research-leading nation, and this engagement links to top scientists (i.e., within the Chinese Academy of Sciences) thereby supporting the UK's international reputation in atmospheric science.

这个泵送项目将与中国领先的研究小组（Xinming Wang教授，广州地球化学研究所，中国科学院）启动新的合作。我们的目的是评估英国团队最近通过当前的NERC研究赠款发现了一种新的大气反应的重要性，使用广州可用的独特模拟室设施。更广泛的项目环境是硫种类的大气加工。 Well understood atmospheric chemical processes break down the sulphur species - molecules such as dimethylsulphide (DMS) or SO2 - these reactions are driven by OH radicals in the gas phase, and form sulphate aerosol particles, which scatter sunlight and can catalyse the formation of cloud droplets - so the processing of sulphur species exerts a major influence upon climate.导致硫酸的硫加工也有助于雨水酸度。我们当前的NERC项目旨在研究一组新的化学反应物对硫加工的影响 - 稳定的Criegee中间体（SCIS）。 SCI是由烷烃反应（在整个边界层中发现）和碘化烷基光解（在海洋边界层中）形成的，并且可以像OH一样充当大气氧化剂，启动了SO2等物种的加工。我们当前的项目是由于最近发现的，即SCI + SO2反应比以前想象的要快三个数量级 - 但是在现实的大气条件下，SCI行为尚未进行测试。我们的方法是使用大气模拟室（西班牙的200 M3反应堆，其中可能引入人造大气 - 其中包含例如烯烃，臭氧和SO2，并配备了仪器来监视演变的化学成分）。 In EUPHORE, we have studied reactions of SCIs with SO2, H2O and their thermal decomposition - leading to five papers so far - and also discovered that SCIs, formed from isoprene-ozone reactions, react with DMS.DMS is the dominant natural sulphur emission (with volcanic SO2), so any enhancement in DMS oxidation (e.g. by SCIs, alongside OH) will increase the rate and change the spatial distribution硫酸盐气溶胶的形成，对大气成分和气候具有潜在的重要性。但是，Euphore中的仪器无法确定SCI + DMS反应的产物。我们也无法评估它们对形成SCI的烯烃的依赖性。在这个项目中，我们建议使用广州新开发的室解决这些不确定性 - 演出室仪器可以检测气体和冷凝相DMS DMS氧化产物，并且最近已用于对车辆排气中的SCI化学研究。该项目将包括PI /研究人员交换，以详细规划和建模室内实验，然后进行模拟室测量，以探测广州的Sci -DMS系统。 These experiments will definitively determine the importance of this new reaction, under realistic atmospheric boundary layer conditions.This proposal has developed following discussions between Bloss and Wang at meetings in Beijing, and a visit by Bloss to the GIG facility in March 2015. In addition to the specific science goals, it will nurture a developing collaboration between UK groups (with substantial expertise in the conduct of simulation chamber experiments) and leading Chinese researchers at GIG (with unique chamber facilities) in atmospheric化学，具有未来联系的潜力，例如，在即将到来的NERC-NEWTON-NSFC“中国大型城市空气污染”项目的背景下。中国正在迅速成为一个研究领导的国家，这种参与与顶级科学家（即中国科学院内）的联系，从而支持英国在大气科学方面的国际声誉。