Lamkaddam Houssni, Dommen Josef, Ranjithkumar Ananth, Gordon Hamish, Wehrle Günther, Krechmer Jordan, Majluf Francesca, Salionov Daniil, Schmale Julia, Bjelić Saša, Carslaw Kenneth S, El Haddad Imad, Baltensperger Urs
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.
School of Earth and Environment, University of Leeds, Leeds LS2 9JT, UK.
Sci Adv. 2021 Mar 24;7(13). doi: 10.1126/sciadv.abe2952. Print 2021 Mar.
Aerosols still present the largest uncertainty in estimating anthropogenic radiative forcing. Cloud processing is potentially important for secondary organic aerosol (SOA) formation, a major aerosol component: however, laboratory experiments fail to mimic this process under atmospherically relevant conditions. We developed a wetted-wall flow reactor to simulate aqueous-phase processing of isoprene oxidation products (iOP) in cloud droplets. We find that 50 to 70% (in moles) of iOP partition into the aqueous cloud phase, where they rapidly react with OH radicals, producing SOA with a molar yield of 0.45 after cloud droplet evaporation. Integrating our experimental results into a global model, we show that clouds effectively boost the amount of SOA. We conclude that, on a global scale, cloud processing of iOP produces 6.9 Tg of SOA per year or approximately 20% of the total biogenic SOA burden and is the main source of SOA in the mid-troposphere (4 to 6 km).
在估算人为辐射强迫时,气溶胶仍然存在最大的不确定性。云处理对于二次有机气溶胶(SOA)的形成可能很重要,SOA是一种主要的气溶胶成分;然而,实验室实验未能在与大气相关的条件下模拟这一过程。我们开发了一种湿壁流动反应器,以模拟云滴中异戊二烯氧化产物(iOP)的水相处理过程。我们发现,50%至70%(摩尔)的iOP会分配到云水相中,在那里它们会与羟基自由基迅速反应,云滴蒸发后产生摩尔产率为0.45的SOA。将我们的实验结果整合到一个全球模型中,我们表明云有效地增加了SOA的量。我们得出结论,在全球范围内,iOP的云处理每年产生6.9太克的SOA,约占生物源SOA总负担的20%,并且是对流层中部(4至6公里)SOA的主要来源。