Atmospheric new particle formation from sulfuric acid and amines in a Chinese megacity

被引:476
作者
Yao, Lei [1 ]
Garmash, Olga [2 ]
Bianchi, Federico [2 ,3 ]
Zheng, Jun [4 ]
Yan, Chao [2 ]
Kontkanen, Jenni [2 ,5 ,6 ]
Junninen, Heikki [2 ,7 ]
Mazon, Stephany Buenrostro [2 ]
Ehn, Mikael [2 ]
Paasonen, Pauli [2 ]
Sipila, Mikko [2 ]
Wang, Mingyi [1 ,16 ]
Wang, Xinke [1 ]
Xiao, Shan [1 ,17 ]
Chen, Hangfei [1 ]
Lu, Yiqun [1 ]
Zhang, Bowen [1 ]
Wang, Dongfang [8 ]
Fu, Qingyan [8 ]
Geng, Fuhai [9 ]
Li, Li [10 ]
Wang, Hongli [10 ]
Qiao, Liping [10 ]
Yang, Xin [1 ,11 ,12 ]
Chen, Jianmin [1 ,11 ,12 ]
Kerminen, Veli-Matti [2 ]
Petaja, Tuukka [2 ,13 ]
Worsnop, Douglas R. [2 ,14 ]
Kulmala, Markku [2 ,3 ]
Wang, Lin [1 ,11 ,12 ,15 ]
机构
[1] Fudan Univ, Dept Environm Sci & Engn, Shanghai Key Lab Atmospher Particle Pollut & Prev, Shanghai 200433, Peoples R China
[2] Univ Helsinki, Fac Sci, Inst Atmospher & Earth Syst Res Phys, FIN-00014 Helsinki, Finland
[3] Beijing Univ Chem Technol, Aerosol & Haze Lab, Beijing 100029, Peoples R China
[4] Nanjing Univ Informat Sci & Technol, Jiangsu Key Lab Atmospher Environm Monitoring & P, Nanjing 210044, Jiangsu, Peoples R China
[5] Stockholm Univ, Dept Environm Sci & Analyt Chem ACES, S-10691 Stockholm, Sweden
[6] Stockholm Univ, Bolin Ctr Climate Res, S-10691 Stockholm, Sweden
[7] Univ Tartu, Inst Phys, Lab Environm Phys, EE-50411 Tartu, Estonia
[8] Shanghai Environm Monitoring Ctr, Shanghai 200030, Peoples R China
[9] Shanghai Meteorol Bur, Shanghai 200135, Peoples R China
[10] Shanghai Acad Environm Sci, Shanghai 200233, Peoples R China
[11] Fudan Univ, Inst Atmospher Sci, Shanghai 200433, Peoples R China
[12] Collaborat Innovat Ctr Climate Change, Nanjing 210023, Jiangsu, Peoples R China
[13] Nanjing Univ, Joint Int Res Lab Atmospher & Earth Syst Sci JirL, Nanjing 210023, Jiangsu, Peoples R China
[14] Aerodyne Res, Billerica, MA 01821 USA
[15] Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China
[16] Carnegie Mellon Univ, Ctr Atmospher Particle Studies, Pittsburgh, PA 15213 USA
[17] Shanghai Qingning Environm Planning & Design, Shanghai 200052, Peoples R China
基金
瑞士国家科学基金会; 芬兰科学院; 欧洲研究理事会; 中国国家自然科学基金; 欧盟地平线“2020”;
关键词
YANGTZE-RIVER DELTA; NUMBER CONCENTRATION; SIZE DISTRIBUTION; NUCLEATION; AEROSOL; AMMONIA; GROWTH; TIME; EMISSIONS; MODEL;
D O I
10.1126/science.aao4839
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
Atmospheric new particle formation (NPF) is an important global phenomenon that is nevertheless sensitive to ambient conditions. According to both observation and theoretical arguments, NPF usually requires a relatively high sulfuric acid (H2SO4) concentration to promote the formation of new particles and a low preexisting aerosol loading to minimize the sink of new particles. We investigated NPF in Shanghai and were able to observe both precursor vapors (H2SO4) and initial clusters at a molecular level in a megacity. High NPF rates were observed to coincide with several familiar markers suggestive of H2SO4-dimethylamine (DMA)water (H2O) nucleation, including sulfuric acid dimers and H2SO4-DMA clusters. In a cluster kinetics simulation, the observed concentration of sulfuric acid was high enough to explain the particle growth to similar to 3 nanometers under the very high condensation sink, whereas the subsequent higher growth rate beyond this size is believed to result fromthe added contribution of condensing organic species. These findings will help in understanding urban NPF and its air quality and climate effects, as well as in formulating policies to mitigate secondary particle formation in China.
引用
收藏
页码:278 / +
页数:4
相关论文
共 38 条
[1]   Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere [J].
Almeida, Joao ;
Schobesberger, Siegfried ;
Kuerten, Andreas ;
Ortega, Ismael K. ;
Kupiainen-Maatta, Oona ;
Praplan, Arnaud P. ;
Adamov, Alexey ;
Amorim, Antonio ;
Bianchi, Federico ;
Breitenlechner, Martin ;
David, Andre ;
Dommen, Josef ;
Donahue, Neil M. ;
Downard, Andrew ;
Dunne, Eimear ;
Duplissy, Jonathan ;
Ehrhart, Sebastian ;
Flagan, Richard C. ;
Franchin, Alessandro ;
Guida, Roberto ;
Hakala, Jani ;
Hansel, Armin ;
Heinritzi, Martin ;
Henschel, Henning ;
Jokinen, Tuija ;
Junninen, Heikki ;
Kajos, Maija ;
Kangasluoma, Juha ;
Keskinen, Helmi ;
Kupc, Agnieszka ;
Kurten, Theo ;
Kvashin, Alexander N. ;
Laaksonen, Ari ;
Lehtipalo, Katrianne ;
Leiminger, Markus ;
Leppa, Johannes ;
Loukonen, Ville ;
Makhmutov, Vladimir ;
Mathot, Serge ;
McGrath, Matthew J. ;
Nieminen, Tuomo ;
Olenius, Tinja ;
Onnela, Antti ;
Petaja, Tuukka ;
Riccobono, Francesco ;
Riipinen, Ilona ;
Rissanen, Matti ;
Rondo, Linda ;
Ruuskanen, Taina ;
Santos, Filipe D. .
NATURE, 2013, 502 (7471) :359-+
[2]  
[Anonymous], 2013, INTERGOVERNMENTAL PA
[3]   New particle formation in the free troposphere: A question of chemistry and timing [J].
Bianchi, F. ;
Trostl, J. ;
Junninen, H. ;
Frege, C. ;
Henne, S. ;
Hoyle, C. R. ;
Molteni, U. ;
Herrmann, E. ;
Adamov, A. ;
Bukowiecki, N. ;
Chen, X. ;
Duplissy, J. ;
Gysel, M. ;
Hutterli, M. ;
Kangasluoma, J. ;
Kontkanen, J. ;
Kuerten, A. ;
Manninen, H. E. ;
Muench, S. ;
Perakyla, O. ;
Petaja, T. ;
Rondo, L. ;
Williamson, C. ;
Weingartner, E. ;
Curtius, J. ;
Worsnop, D. R. ;
Kulmala, M. ;
Dommen, J. ;
Baltensperger, U. .
SCIENCE, 2016, 352 (6289) :1109-1112
[4]   Insight into Acid-Base Nucleation Experiments by Comparison of the Chemical Composition of Positive, Negative, and Neutral Clusters [J].
Bianchi, Federico ;
Praplan, Arnaud P. ;
Sarnela, Nina ;
Dommen, Josef ;
Kuerten, Andreas ;
Ortega, Ismael K. ;
Schobesberger, Siegfried ;
Junninen, Heikki ;
Simon, Mario ;
Troestl, Jasmin ;
Jokinen, Tuija ;
Sipila, Mikko ;
Adamov, Alexey ;
Amorim, Antonio ;
Almeida, Joao ;
Breitenlechner, Martin ;
Duplissy, Jonathan ;
Ehrhart, Sebastian ;
Flagan, Richard C. ;
Franchin, Alessandro ;
Hakala, Jani ;
Hansel, Armin ;
Heinritzi, Martin ;
Kangasluoma, Juha ;
Keskinen, Helmi ;
Kim, Jaeseok ;
Kirkby, Jasper ;
Laaksonen, Ari ;
Lawler, Michael J. ;
Lehtipalo, Katrianne ;
Leiminger, Markus ;
Makhmutov, Vladimir ;
Mathot, Serge ;
Onnela, Antti ;
Petaja, Tuukka ;
Riccobono, Francesco ;
Rissanen, Matti P. ;
Rondo, Linda ;
Tome, Antonio ;
Virtanen, Annele ;
Viisanen, Yrjo ;
Williamson, Christina ;
Wimmer, Daniela ;
Winkler, Paul M. ;
Ye, Penglin ;
Curtius, Joachim ;
Kulmala, Markku ;
Worsnop, Douglas R. ;
Donahue, Neil M. ;
Baltensperger, Urs .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2014, 48 (23) :13675-13684
[5]   Acid-base chemical reaction model for nucleation rates in the polluted atmospheric boundary layer [J].
Chen, Modi ;
Titcombe, Mari ;
Jiang, Jingkun ;
Jen, Coty ;
Kuang, Chongai ;
Fischer, Marc L. ;
Eisele, Fred L. ;
Siepmann, J. Ilja ;
Hanson, David R. ;
Zhao, Jun ;
McMurry, Peter H. .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2012, 109 (46) :18713-18718
[6]   Global atmospheric particle formation from CERN CLOUD measurements [J].
Dunne, Eimear M. ;
Gordon, Hamish ;
Kuerten, Andreas ;
Almeida, Joao ;
Duplissy, Jonathan ;
Williamson, Christina ;
Ortega, Ismael K. ;
Pringle, Kirsty J. ;
Adamov, Alexey ;
Baltensperger, Urs ;
Barmet, Peter ;
Benduhn, Francois ;
Bianchi, Federico ;
Breitenlechner, Martin ;
Clarke, Antony ;
Curtius, Joachim ;
Dommen, Josef ;
Donahue, Neil M. ;
Ehrhart, Sebastian ;
Flagan, Richard C. ;
Franchin, Alessandro ;
Guida, Roberto ;
Hakala, Jani ;
Hansel, Armin ;
Heinritzi, Martin ;
Jokinen, Tuija ;
Kangasluoma, Juha ;
Kirkby, Jasper ;
Kulmala, Markku ;
Kupc, Agnieszka ;
Lawler, Michael J. ;
Lehtipalo, Katrianne ;
Makhmutov, Vladimir ;
Mann, Graham ;
Mathot, Serge ;
Merikanto, Joonas ;
Miettinen, Pasi ;
Nenes, Athanasios ;
Onnela, Antti ;
Rap, Alexandru ;
Reddington, Carly L. S. ;
Riccobono, Francesco ;
Richards, Nigel A. D. ;
Rissanen, Matti P. ;
Rondo, Linda ;
Sarnela, Nina ;
Schobesberger, Siegfried ;
Sengupta, Kamalika ;
Simon, Mario ;
Sipila, Mikko .
SCIENCE, 2016, 354 (6316) :1119-1124
[7]   A large source of low-volatility secondary organic aerosol [J].
Ehn, Mikael ;
Thornton, Joel A. ;
Kleist, Einhard ;
Sipila, Mikko ;
Junninen, Heikki ;
Pullinen, Iida ;
Springer, Monika ;
Rubach, Florian ;
Tillmann, Ralf ;
Lee, Ben ;
Lopez-Hilfiker, Felipe ;
Andres, Stefanie ;
Acir, Ismail-Hakki ;
Rissanen, Matti ;
Jokinen, Tuija ;
Schobesberger, Siegfried ;
Kangasluoma, Juha ;
Kontkanen, Jenni ;
Nieminen, Tuomo ;
Kurten, Theo ;
Nielsen, Lasse B. ;
Jorgensen, Solvejg ;
Kjaergaard, Henrik G. ;
Canagaratna, Manjula ;
Dal Maso, Miikka ;
Berndt, Torsten ;
Petaja, Tuukka ;
Wahner, Andreas ;
Kerminen, Veli-Matti ;
Kulmala, Markku ;
Worsnop, Douglas R. ;
Wildt, Juergen ;
Mentel, Thomas F. .
NATURE, 2014, 506 (7489) :476-+
[8]   Elucidating severe urban haze formation in China [J].
Guo, Song ;
Hu, Min ;
Zamora, Misti L. ;
Peng, Jianfei ;
Shang, Dongjie ;
Zheng, Jing ;
Du, Zhuofei ;
Wu, Zhijun ;
Shao, Min ;
Zeng, Limin ;
Molina, Mario J. ;
Zhang, Renyi .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2014, 111 (49) :17373-17378
[9]   The role of relative humidity in continental new particle formation [J].
Hamed, Amar ;
Korhonen, Hannele ;
Sihto, Sanna-Liisa ;
Joutsensaari, Jorma ;
Jarvinen, Heikki ;
Petaja, Tuukka ;
Arnold, Frank ;
Nieminen, Tuomo ;
Kulmala, Markku ;
Smith, James N. ;
Lehtinen, Kari E. J. ;
Laaksonen, Ari .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2011, 116
[10]   Emission inventory of anthropogenic air pollutants and VOC species in the Yangtze River Delta region, China [J].
Huang, C. ;
Chen, C. H. ;
Li, L. ;
Cheng, Z. ;
Wang, H. L. ;
Huang, H. Y. ;
Streets, D. G. ;
Wang, Y. J. ;
Zhang, G. F. ;
Chen, Y. R. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (09) :4105-4120