Mineral dust photochemistry induces nucleation events in the presence of SO2

被引:109
作者
Dupart, Yoan [1 ,2 ]
King, Stephanie M. [1 ,2 ]
Nekat, Bettina [3 ]
Nowak, Andreas [3 ]
Wiedensohler, Alfred [3 ]
Herrmann, Hartmut [3 ]
David, Gregory [4 ]
Thomas, Benjamin [4 ]
Miffre, Alain [4 ]
Rairoux, Patrick [4 ]
D'Anna, Barbara [1 ,2 ]
George, Christian [1 ,2 ]
机构
[1] Univ Lyon 1, F-69365 Lyon, France
[2] Inst Rech Catalyse & Environm Lyon, CNRS, UMR 5256, F-69626 Villeurbanne, France
[3] Leibniz Inst Tropospher Res, D-04318 Leipzig, Germany
[4] Univ Lyon 1, CNRS, UMR5306, Inst Lumiere Mat, F-69622 Villeurbanne, France
关键词
OH production; photocatalysis; SO2; nucleation; LIDAR; atmospheric optics; REMOTE PHOTOCATALYTIC OXIDATION; SULFUR-DIOXIDE; PARTICLES; AEROSOL; ACID; ADSORPTION; MECHANISM;
D O I
10.1073/pnas.1212297109
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Large quantities of mineral dust particles are frequently ejected into the atmosphere through the action of wind. The surface of dust particles acts as a sink for many gases, such as sulfur dioxide. It is well known that under most conditions, sulfur dioxide reacts on dust particle surfaces, leading to the production of sulfate ions. In this report, for specific atmospheric conditions, we provide evidence for an alternate pathway in which a series of reactions under solar UV light produces first gaseous sulfuric acid as an intermediate product before surface-bound sulfate. Metal oxides present in mineral dust act as atmospheric photocatalysts promoting the formation of gaseous OH radicals, which initiate the conversion of SO2 to H2SO4 in the vicinity of dust particles. Under low dust conditions, this process may lead to nucleation events in the atmosphere. The laboratory findings are supported by recent field observations near Beijing, China, and Lyon, France.
引用
收藏
页码:20842 / 20847
页数:6
相关论文
共 36 条
[1]   Adsorption of sulfur dioxide on hematite and goethite particle surfaces [J].
Baltrusaitis, Jonas ;
Cwiertny, David M. ;
Grassian, Vicki H. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2007, 9 (41) :5542-5554
[2]   Sulfur Dioxide Adsorption on TiO2 Nanoparticles: Influence of Particle Size, Coadsorbates, Sample Pretreatment, and Light on Surface Speciation and Surface Coverage [J].
Baltrusaitis, Jonas ;
Jayaweera, Pradeep M. ;
Grassian, Vicki H. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (02) :492-500
[3]  
Berndt T., 2008, Atmos. Chem. Phys. Discuss, V8, P9761
[4]   Quantitative Assessment of the Sulfuric Acid Contribution to New Particle Growth [J].
Bzdek, Bryan R. ;
Zordan, Christopher A. ;
Pennington, M. Ross ;
Luther, George W., III ;
Johnston, Murray V. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2012, 46 (08) :4365-4373
[5]   Chemistry and photochemistry of mineral dust aerosol [J].
Cwiertny, David M. ;
Young, Mark A. ;
Grassian, Vicki H. .
ANNUAL REVIEW OF PHYSICAL CHEMISTRY, 2008, 59 :27-51
[6]   Sensitive and accurate dual-wavelength UV-VIS polarization detector for optical remote sensing of tropospheric aerosols [J].
David, G. ;
Miffre, A. ;
Thomas, B. ;
Rairoux, P. .
APPLIED PHYSICS B-LASERS AND OPTICS, 2012, 108 (01) :197-216
[7]   Estimates of the direct and indirect radiative forcing due to tropospheric aerosols: A review [J].
Haywood, J ;
Boucher, O .
REVIEWS OF GEOPHYSICS, 2000, 38 (04) :513-543
[8]   Detection of S(IV) Species in Aerosol Particles Using XANES Spectroscopy [J].
Higashi, Masayuki ;
Takahashi, Yoshio .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2009, 43 (19) :7357-7363
[9]   Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation [J].
Kirkby, Jasper ;
Curtius, Joachim ;
Almeida, Joao ;
Dunne, Eimear ;
Duplissy, Jonathan ;
Ehrhart, Sebastian ;
Franchin, Alessandro ;
Gagne, Stephanie ;
Ickes, Luisa ;
Kuerten, Andreas ;
Kupc, Agnieszka ;
Metzger, Axel ;
Riccobono, Francesco ;
Rondo, Linda ;
Schobesberger, Siegfried ;
Tsagkogeorgas, Georgios ;
Wimmer, Daniela ;
Amorim, Antonio ;
Bianchi, Federico ;
Breitenlechner, Martin ;
David, Andre ;
Dommen, Josef ;
Downard, Andrew ;
Ehn, Mikael ;
Flagan, Richard C. ;
Haider, Stefan ;
Hansel, Armin ;
Hauser, Daniel ;
Jud, Werner ;
Junninen, Heikki ;
Kreissl, Fabian ;
Kvashin, Alexander ;
Laaksonen, Ari ;
Lehtipalo, Katrianne ;
Lima, Jorge ;
Lovejoy, Edward R. ;
Makhmutov, Vladimir ;
Mathot, Serge ;
Mikkila, Jyri ;
Minginette, Pierre ;
Mogo, Sandra ;
Nieminen, Tuomo ;
Onnela, Antti ;
Pereira, Paulo ;
Petaja, Tuukka ;
Schnitzhofer, Ralf ;
Seinfeld, John H. ;
Sipila, Mikko ;
Stozhkov, Yuri ;
Stratmann, Frank .
NATURE, 2011, 476 (7361) :429-U77
[10]   Heterogeneous nucleation as a potential sulphate-coating mechanism of atmospheric mineral dust particles and implications of coated dust on new particle formation -: art. no. 4546 [J].
Korhonen, H ;
Napari, I ;
Timmreck, C ;
Vehkamäki, H ;
Pirjola, L ;
Lehtinen, KEJ ;
Lauri, A ;
Kulmala, M .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2003, 108 (D17)