Laboratory and modelling studies of the reactions of peroxy radicals with XO (where X = Cl, Br or I).

卤素化学可以在整个对流层中控制臭氧、氮氧化物、硝态氮和HOx的预算方面发挥至关重要的作用，这些家族在确定大气成分、地球辐射平衡和任何未来气候变化方面的重要性怎么强调都不为过。然而，动力学数据库中有一个主要的空白，因为亚环境温度的数据很少或没有数据，而在有数据的地方，情况远不清楚，因此不能充分评估卤素化学与过氧自由基耦合的大气重要性。提出了一个综合的实验室和模型研究方案，以研究一组关键的过氧自由基反应，即RO2 + XO。一个最先进的实验系统，一个湍流化学电离质谱仪，可以直接实验到大气相关的温度和压力，将用于确定动力学和机械参数。实验结果将使用最先进的初始计算进行合理化，然后纳入全球大气模型，该模型允许评估过氧自由基与XO自由基相互作用的大气重要性。提出的工作对于使卤素化学对大气污染和气候变化的影响合理化将是非常宝贵的

Halogen chemistry can play a vital role in controlling the budgets of ozone, NOx, NOy and HOx throughout the troposphere and the importance of these families in determining atmospheric composition, the earth's radiative balance and any future change in climate can not be over-emphasised. However, there is a major gap in the kinetic database, in that there is little or no data for sub ambient temperatures and where data is available the picture is far from clear, and thus does not allow the full atmospheric importance of the coupling of halogen chemistry with peroxy radicals to be assessed. An integrated programme of laboratory and modelling studies is proposed to study a key set of peroxy radical reactions, namely RO2 + XO. A state of the art experimental system, a turbulent flow chemical ionisation mass spectrometer, that enables direct experimental acess to atmospherically relevant teperatures and pressures will be used to determine kinetic and mechanistic parameters. The experimental results will be raionalised using state of the art ab - intio calculations and then be incorporated into a global atmospheric model which allows the atmospheric importance of the interacttion of peroxy radicals with XO radicals to be assessed. The proposed work will be invaluable for the rationalisation of the effect of halogen chemistry on atmospheric pollution and climate change