甲基过氧自由基 (CH3O2) 和次氯酸甲酯 (CH3OCl) 反应与南极氯活化和臭氧损失的相关性,Tellus Series B: Chemical and Physical Meteorology

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甲基过氧自由基 (CH3O2) 和次氯酸甲酯 (CH3OCl) 反应与南极氯活化和臭氧损失的相关性
Tellus Series B: Chemical and Physical Meteorology ( IF 2.3 ) Pub Date : 2018-01-01 , DOI: 10.1080/16000889.2018.1507391
A. Mannan Zafar _{1,

2} , Rolf Müller ₁ , Jens-Uwe Grooss ₁ , Sabine Robrecht ₁ , Bärbel Vogel ₁ , Ralph Lehmann ₃

Affiliation

摘要南极泉水保持高浓度的活性氯会导致强烈的化学臭氧破坏。在极涡核心的平流层下部（约 16-18 公里，85-55 hPa，390-430 K），尽管会快速生成 HCl，但仍保持高水平的活性氯。维护是通过 HCl 无效循环实现的，其中 HCl 的产生通过立即重新激活来平衡。甲基过氧自由基 (CH3O2) 的化学性质对于这些 HCl 无效循环至关重要，因此对于极涡核心中平流层低层的南极氯和臭氧损失化学性质也是必不可少的。这里的关键反应是反应；在模拟极地臭氧损失时，不应忽视这一反应。在这里，我们研究了代表平流层低层极涡核心条件的箱模型模拟中 CH3O2 的完整化学成分。这些模拟包括反应 CH3O2 + Cl、反应 CH3O2 + ClO 的产物次氯酸甲酯 (CH3OCl) 以及随后的 CH3OCl 化学分解。我们发现，当考虑 CH3OCl 的形成时，重要的是还要考虑 CH3OCl 的主要损失通道，即光解和与 Cl 的反应。如果是这种情况，在我们的模拟中，CH3O2 + ClO 反应中 CH3OCl 的形成对极性氯化学只有中等影响。CH3OCl (ppb) 的模拟峰值混合比出现在臭氧混合比最低的时候。更远，我们的模型模拟表明反应 CH3O2 + Cl 对极性氯化学没有强烈影响。在 9 月下旬臭氧浓度最低期间，模拟了 CH3O2 的升高值，因此，甲醛（约 100 ppt）和甲醇（约 5 ppt）的值也升高了。

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The relevance of reactions of the methyl peroxy radical (CH3O2) and methylhypochlorite (CH3OCl) for Antarctic chlorine activation and ozone loss

Abstract The maintenance of large concentrations of active chlorine in Antarctic spring allows strong chemical ozone destruction to occur. In the lower stratosphere (approximately 16–18 km, 85–55 hPa, 390–430 K) in the core of the polar vortex, high levels of active chlorine are maintained, although rapid gas-phase production of HCl occurs. The maintenance is achieved through HCl null cycles in which the HCl production is balanced by immediate reactivation. The chemistry of the methyl peroxy radical (CH3O2) is essential for these HCl null cycles and thus for Antarctic chlorine and ozone loss chemistry in the lower stratosphere in the core of the polar vortex. The key reaction here is the reaction ; this reaction should not be neglected in simulations of polar ozone loss. Here we investigate the full chemistry of CH3O2 in box-model simulations representative for the conditions in the core of the polar vortex in the lower stratosphere. These simulations include the reaction CH3O2 + Cl, the product methylhypochlorite (CH3OCl) of the reaction CH3O2 + ClO, and the subsequent chemical decomposition of CH3OCl. We find that when the formation of CH3OCl is taken into account, it is important that also the main loss channels for CH3OCl, namely photolysis and reaction with Cl are considered. Provided that this is the case, there is only a moderate impact of the formation of CH3OCl in the reaction CH3O2 + ClO on polar chlorine chemistry in our simulations. Simulated peak mixing ratios of CH3OCl ( ppb) occur at the time of the lowest ozone mixing ratios. Further, our model simulations indicate that the reaction CH3O2 + Cl does not have a strong impact on polar chlorine chemistry. During the period of the lowest ozone concentrations in late September, enhanced values of CH3O2 are simulated and, as a consequence, also enhanced values of formaldehyde (about 100 ppt) and methanol (about 5 ppt).

更新日期：2018-01-01

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