Testing radical assay by nitrite chemical entrapment (TRANCE)
通过亚硝酸盐化学包埋法 (TRANCE) 测试自由基测定
基本信息
- 批准号:NE/H002502/1
- 负责人:
- 金额:$ 7.28万
- 依托单位:
- 依托单位国家:英国
- 项目类别:Research Grant
- 财政年份:2010
- 资助国家:英国
- 起止时间:2010 至 无数据
- 项目状态:已结题
- 来源:
- 关键词:
项目摘要
Radicals play a pivotal role in the atmosphere even though their concentrations are extremely small. The hydroxyl radical (OH) controls the oxidation of most atmospheric pollutants, including many important greenhouse gases, whilst the nature and fate of peroxy radicals (RO2) has a major impact on tropospheric ozone chemistry. It is therefore extremely important that global chemistry models accurately simulate the OH and peroxy radical concentrations. Current radical measurement methods, whilst sensitive, fast and well proven, are large, expensive and complicated and therefore observations of radicals are very limited in space and time. A consequence of this is that OH estimations in global models are often tested against long-lived tracers (e.g. methyl chloroform) even though the emissions of these tracers themselves are not necessarily accurately known. Further, the existing techniques for measuring peroxy radicals are unable to provide a measure of individual organic RO2 with which to validate the models. Therefore it would be of immense benefit if there were extensive, long term measurements of radicals with which to assess and improve models, but this would need small, easily-deployable systems which are not currently available. Hydroxyl and peroxy radicals almost certainly play a key role in other important processes such as photochemically induced emissions from snowpacks which have a great influence on the chemistry of the polar troposphere. Detailed radical measurements within the snowpack would be hugely beneficial in understanding this chemistry, but are not currently possible. Currently available kinetic data suggests that small organic peroxy radicals can be converted rapidly and quantitatively into stable organic nitrites by reaction with high concentrations of NO. This project will examine the feasibility of quantifying organic peroxy radicals by this conversion into distinct organic nitrite compounds which can be measured by highly sensitive negative ion gas chromatography-mass spectrometry (NI-GCMS). Additionally, if OH is allowed to react with a hydrocarbon to produce a distinct peroxy radical, then the nitrite conversion method offers the opportunity to measure OH as well. This novel method offers more information on individual organic peroxy radicals than current technology affords, should be able to measure OH and organic peroxy radicals concurrently, and has the potential to also measure Cl and NO3 radicals. The radical conversion and sampling is distinct from the analysis instrument which should allow the future development of a small, low-cost sampling device suitable for the large scale deployments required to test global chemistry models, as well as a sampling system well suited to measuring radicals in snowpack experiments.
自由基在大气中起着关键作用,尽管它们的浓度非常小。羟基自由基(OH)控制着大多数大气污染物的氧化,包括许多重要的温室气体,而过氧自由基(RO 2)的性质和命运对对流层臭氧化学有重大影响。因此,全球化学模型准确地模拟OH和过氧自由基浓度是极其重要的。目前的自由基测量方法,虽然灵敏,快速和良好的证明,是大,昂贵和复杂的,因此自由基的观察是非常有限的空间和时间。其结果是,全球模型中的OH估计值往往是针对长寿命示踪剂(如甲基氯仿)进行测试的,即使这些示踪剂本身的排放量不一定是准确的。此外,用于测量过氧自由基的现有技术不能提供用于验证模型的单个有机RO 2的测量。因此,如果有广泛的,长期的自由基测量,以评估和改进模型,这将是巨大的好处,但这将需要小,易于部署的系统,目前还没有。羟基和过氧自由基几乎肯定在其他重要过程中发挥关键作用,如积雪的光化学诱导排放,对极地对流层的化学性质有很大影响。在积雪中进行详细的自由基测量将对理解这种化学性质非常有益,但目前还不可能。目前可用的动力学数据表明,小的有机过氧自由基可以快速和定量地转化为稳定的有机亚硝酸盐与高浓度的NO反应。本项目将研究量化有机过氧自由基的可行性,通过这种转换成不同的有机亚硝酸盐化合物,可以测量高灵敏度的负离子气相色谱-质谱(NI-GCMS)。此外,如果允许OH与烃反应以产生独特的过氧自由基,则亚硝酸盐转化方法也提供了测量OH的机会。这种新的方法提供了更多的信息,个别有机过氧自由基比目前的技术提供,应该能够同时测量OH和有机过氧自由基,并有可能也测量Cl和NO3自由基。自由基转换和采样与分析仪器不同,分析仪器应允许未来开发适合于测试全球化学模型所需的大规模部署的小型低成本采样设备,以及非常适合于测量积雪实验中的自由基的采样系统。
项目成果
期刊论文数量(0)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
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David Oram其他文献
David Oram的其他文献
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