Impacts of HOx regeneration and recycling in the oxidation of isoprene: Consequences for the composition of past, present and future atmospheres

被引:68
作者
Archibald, A. T. [1 ,6 ]
Levine, J. G. [5 ]
Abraham, N. L. [1 ,6 ]
Cooke, M. C. [2 ]
Edwards, P. M. [3 ]
Heard, D. E. [1 ,3 ]
Jenkin, M. E. [1 ,2 ]
Karunaharan, A. [4 ]
Pike, R. C. [6 ]
Monks, P. S. [1 ,4 ]
Shallcross, D. E. [2 ]
Telford, P. J. [1 ,6 ]
Whalley, L. K. [1 ,3 ]
Pyle, J. A. [1 ,6 ]
机构
[1] Natl Ctr Atmospher Sci, Cambridge, England
[2] Univ Bristol, Atmospher Chem Res Grp, Sch Chem, Bristol BS8 1TS, Avon, England
[3] Univ Leeds, Sch Chem, Leeds LS2 9JT, W Yorkshire, England
[4] Univ Leicester, Dept Chem, Leicester LE1 7RH, Leics, England
[5] British Antarctic Survey, Cambridge CB3 0ET, England
[6] Univ Cambridge, Dept Chem, Cambridge CB2 1EW, England
关键词
TROPICAL OZONE CLIMATOLOGY; TROPOSPHERIC OZONE; EMISSIONS; FOREST; CHEMISTRY; CAMPAIGN; BUDGETS; SUMMER; MODEL;
D O I
10.1029/2010GL046520
中图分类号
P [天文学、地球科学];
学科分类号
07 ;
摘要
A global chemistry-climate model is used to assess the impact on atmospheric composition of the regeneration and recycling of HOx in the photo-oxidation of isoprene. The impact is explored subject to present-day, pre-industrial and future climate/emission scenarios. Our calculations show that, in all cases, the inclusion of uni-molecular iso-merisations of the isoprene hydroxy-peroxy radicals leads to enhanced production of HOx radicals and ozone. The global burden of ozone increases by 25-36 Tg (8-18%), depending on the climate/emissions scenario, whilst the changes in OH lead to decreases in the methane lifetime of between 11% in the future and 35% in the pre-industrial. Critically the size of the change in methane lifetime depends on the VOC/NOx emission ratio. The results of the present-day calculations suggest a certain amount of parameter refinement is still needed to reconcile the updated chemistry with field observations (particularly for HO2+RO2). However, the updated chemistry could have far-reaching implications for: future-climate predictions; projections of future oxidising capacity; and our understanding of past changes in oxidising capacity. Citation: Archibald, A. T., et al. (2011), Impacts of HOx regeneration and recycling in the oxidation of isoprene: Consequences for the composition of past, present and future atmospheres, Geophys. Res. Lett., 38, L05804, doi: 10.1029/2010GL046520.
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页数:6
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