The Tropospheric Oxidation Capacity Research Group

Biosphere-Atmosphere-Human Interactions

3216 Croul Hall Irvine CA 92627 (email)

A new atmospherically relevant oxidant of sulphur dioxide

Mauldin, RL, Berndt T, Sipila M, Paasonen P, Petaja T, Kim S, Kurten T, Stratmann F, Kerminen VM, Kulmala M.  2012.  

Journal:

Nature

Volume Number:

488

Issue Number:

7410

Pages:

193-+

Abstract:

Atmospheric oxidation is a key phenomenon that connects atmospheric chemistry with globally challenging environmental issues, such as climate change(1), stratospheric ozone loss(2), acidification of soils and water(3), and health effects of air quality(4). Ozone, the hydroxyl radical and the nitrate radical are generally considered to be the dominant oxidants that initiate the removal of trace gases, including pollutants, from the atmosphere. Here we present atmospheric observations from a boreal forest region in Finland, supported by laboratory experiments and theoretical considerations, that allow us to identify another compound, probably a stabilized Criegee intermediate (a carbonyl oxide with two free-radical sites) or its derivative, which has a significant capacity to oxidize sulphur dioxide and potentially other trace gases. This compound probably enhances the reactivity of the atmosphere, particularly with regard to the production of sulphuric acid, and consequently atmospheric aerosol formation. Our findings suggest that this new atmospherically relevant oxidation route is important relative to oxidation by the hydroxyl radical, at least at moderate concentrations of that radical. We also find that the oxidation chemistry of this compound seems to be tightly linked to the presence of alkenes of biogenic origin.

Notes:

ISI Document Delivery No.: 985LETimes Cited: 1Cited Reference Count: 34Mauldin, R. L., III Berndt, T. Sipilae, M. Paasonen, P. Petaja, T. Kim, S. Kurten, T. Stratmann, F. Kerminen, V-M Kulmala, M.European Commission Sixth Framework programme project EUCAARI[036833-2]; Academy of Finland[251427, 139656, 141135]; European Research Council (ATMNUCLE); Kone Foundation; Vaisala Foundation; Maj and Tor Nessling Foundation[2010212]; Otto Malm Foundation; US National Science FoundationWe thank K. Pielok and A. Rohmer for technical assistance. This work was partially funded by the European Commission Sixth Framework programme project EUCAARI, contract no. 036833-2 (EUCAARI), the Academy of Finland (251427, 139656, Finnish centre of excellence 141135), the European Research Council (ATMNUCLE), the Kone Foundation, the Vaisala Foundation, the Maj and Tor Nessling Foundation (2010212), the Otto Malm Foundation and the US National Science Foundation.NATURE PUBLISHING GROUPLONDON

Related External URL:

<Go to ISI>://WOS:000307267000029
Citation:
Mauldin, RL, Berndt T, Sipila M, Paasonen P, Petaja T, Kim S, Kurten T, Stratmann F, Kerminen VM, Kulmala M.  2012.  A new atmospherically relevant oxidant of sulphur dioxide. Nature. 488(7410):193-+.