No Evidence for a Significant Impact of Heterogeneous Chemistry on Radical Concentrations in the North China Plain in Summer 2014

2014年夏季华北平原非均相化学反应对自由基浓度无显著影响的证据

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Abstract

The oxidation of nitric oxide to nitrogen dioxide by hydroperoxy (HO(2)) and organic peroxy radicals (RO(2)) is responsible for the chemical net ozone production in the troposphere and for the regeneration of hydroxyl radicals, the most important oxidant in the atmosphere. In Summer 2014, a field campaign was conducted in the North China Plain, where increasingly severe ozone pollution has been experienced in the last years. Chemical conditions in the campaign were representative for this area. Radical and trace gas concentrations were measured, allowing for calculating the turnover rates of gas-phase radical reactions. Therefore, the importance of heterogeneous HO(2) uptake on aerosol could be experimentally determined. HO(2) uptake could have suppressed ozone formation at that time because of the competition with gas-phase reactions that produce ozone. The successful reduction of the aerosol load in the North China Plain in the last years could have led to a significant decrease of HO(2) loss on particles, so that ozone-forming reactions could have gained importance in the last years. However, the analysis of the measured radical budget in this campaign shows that HO(2) aerosol uptake did not impact radical chemistry for chemical conditions in 2014. Therefore, reduced HO(2) uptake on aerosol since then is likely not the reason for the increasing number of ozone pollution events in the North China Plain, contradicting conclusions made from model calculations reported in the literature.

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