Laboratory studies of Criegee radical reactions

Criegee自由基反应的实验室研究

• 批准号: NE/I014381/1
• 负责人: Dudley Shallcross
• 金额: $ 11.93万
• 依托单位: University of Bristol
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2011
• 资助国家: 英国
• 起止时间: 2011 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=NE%2FI014381%2F1
• 关键词: Laboratory; studies; Criegee; radical; reactions

Chemicals entering the atmosphere come from a number of sources, but in broad terms are either from human activity or from the biosphere (natural systems). What happens to these chemicals once in the atmosphere is very important of course. If they are toxic they can impact on the health of humans, animals and natural ecosystems. Therefore, it is vital that we understand how pollutants are removed by the atmosphere. One very important removal process involves the so called hydroxyl radical. This is an extremely reactive species that acts like a chemical detergent, destroying pollutants and cleaning up the atmosphere. It has emerged in recent investigations that an important source of the hydroxyl radical must be coming from Criegee radicals. However, these Criegee radicals have been impossible to measure until recently. Work carried out by us, using a facility in the USA, has allowed us to observe a Criegee radical for the first time. In this project we will develop a state-of-the-art experimental system that will allow us to investigate the chemistry of Criegee radicals and therefore to help us to understand how they affect the amount of hydroxyl radical is present in the atmosphere. Such work will not only improve our understanding of the urban environment but will also have implications for climate studies as well. Reactions of Criegee intermediates, over a wide range of pressure and temperature, are of importance in atmospheric chemistry. The proposed UV-PE apparatus will be the first of its kind and will enable us to carry out a range of experiments to study reactions of these radicals that, as far as we are aware, no one else in the world can do. To demonstrate how versatile the apparatus is we propose a carefully designed set of experiments to look at the source and fate of Criegee radicals in the troposphere. Quantum chemistry calculations of the reactions studied will provide detailed understanding of their mechanisms and the kinetic data will be incorporated into models describing the troposphere and compared with available measurements.

进入大气的化学物质来自许多来源，但总的来说是来自人类活动或生物圈（自然系统）。这些化学物质曾经在大气中发生的事情当然非常重要。如果它们有毒，它们可能会影响人类，动物和自然生态系统的健康。因此，至关重要的是，我们了解如何通过大气去除污染物。一个非常重要的去除过程涉及所谓的羟基自由基。这是一种极其反应性的物种，其作用像化学洗涤剂，破坏污染物并清理大气。在最近的研究中，它已经出现了，羟基自由基的重要来源必须来自Criegee自由基。但是，直到最近才无法衡量这些Criegee激进分子。我们在美国使用设施进行的工作使我们首次观察Criegee激进分子。在这个项目中，我们将开发一个最先进的实验系统，该系统将使我们能够研究Criegee激进分子的化学反应，从而帮助我们了解它们如何影响大气中的羟基自由基的数量。这样的工作不仅会改善我们对城市环境的理解，而且还将对气候研究产生影响。 Criegee中间体的反应在广泛的压力和温度范围内在大气化学中至关重要。提出的UV-PE设备将是同类产品中的第一个，将使我们能够进行一系列实验，以研究这些激进分子的反应，据我们所知，世界上没有其他人可以做。为了证明该设备多功能，我们提出了一组精心设计的实验集，以查看对流层中Criegee自由基的来源和命运。研究反应的量子化学计算将提供对其机制的详细了解，并且动力学数据将纳入描述对流层的模型，并将其与可用的测量结果进行比较。

项目成果

The first UK measurements of nitryl chloride using a chemical ionization mass spectrometer in central London in the summer of 2012, and an investigation of the role of Cl atom oxidation

• DOI: 10.1002/2014jd022629
• 发表时间: 2015-06
• 期刊: Journal of Geophysical Research: Atmospheres
• 作者: T. Bannan;A. M. Booth;A. Bacak;J. Muller;K. Leather;Michael Le Breton;B. Jones;D. Young;H. Coe;J. Allan;S. Visser;J. Slowik;M. Furger;A. Prevot;James D. Lee;R. Dunmore;J. Hopkins;J. Hamilton;A. Lewis;L. Whalley;T. Sharp;D. Stone;D. Heard;Z. Fleming;R. Leigh;D. Shallcross;C. Percival

Impact of Criegee Intermediate Reactions with Peroxy Radicals on Tropospheric Organic Aerosol

• DOI: 10.1021/acsearthspacechem.0c00147
• 发表时间: 2020-10-15
• 期刊: ACS EARTH AND SPACE CHEMISTRY
• 影响因子: 3.4
• 作者: Chhantyal-Pun, Rabi;Khan, M. Anwar H.;Orr-Ewing, Andrew J.
• 通讯作者: Orr-Ewing, Andrew J.

The effect of the novel HO 2 + NO ? HNO 3 reaction channel at South Pole, Antarctica

新型 HO 2 NO 的效果？

• DOI: 10.1017/s0954102012000144
• 发表时间: 2012
• 期刊: Antarctic Science
• 影响因子: 1.6
• 作者: Boxe C

The reaction of hydroxyl and methylperoxy radicals is not a major source of atmospheric methanol.

• DOI: 10.1038/s41467-018-06716-x
• 发表时间: 2018-10-19
• 期刊: Nature communications
• 影响因子: 16.6
• 作者: Caravan RL;Khan MAH;Zádor J;Sheps L;Antonov IO;Rotavera B;Ramasesha K;Au K;Chen MW;Rösch D;Osborn DL;Fittschen C;Schoemaecker C;Duncianu M;Grira A;Dusanter S;Tomas A;Percival CJ;Shallcross DE;Taatjes CA
• 通讯作者: Taatjes CA

Importance of direct anthropogenic emissions of formic acid measured by a chemical ionisation mass spectrometer (CIMS) during the Winter ClearfLo Campaign in London, January 2012

• DOI: 10.1016/j.atmosenv.2013.10.029
• 发表时间: 2014-02-01
• 期刊: ATMOSPHERIC ENVIRONMENT
• 影响因子: 5
• 作者: Bannan, Thomas J.;Bacak, Asan;Percival, Carl J.
• 通讯作者: Percival, Carl J.