Insight into Acid-Base Nucleation Experiments by Comparison of the Chemical Composition of Positive, Negative, and Neutral Clusters

被引：53

作者：

Bianchi, Federico ^{[1
]}

Praplan, Arnaud P. ^{[2
]}

Sarnela, Nina ^{[2
]}

Dommen, Josef ^{[1
]}

Kuerten, Andreas ^{[3
]}

Ortega, Ismael K. ^{[4
]}

Schobesberger, Siegfried ^{[2
]}

Junninen, Heikki ^{[2
]}

Simon, Mario ^{[3
]}

Troestl, Jasmin ^{[1
]}

Jokinen, Tuija ^{[2
]}

Sipila, Mikko ^{[2
]}

Adamov, Alexey ^{[2
]}

Amorim, Antonio ^{[5
,6
]}

Almeida, Joao ^{[7
]}

Breitenlechner, Martin ^{[8
,9
]}

Duplissy, Jonathan ^{[2
,7
,10
]}

Ehrhart, Sebastian ^{[7
]}

Flagan, Richard C. ^{[11
]}

Franchin, Alessandro ^{[2
]}

Hakala, Jani ^{[2
]}

Hansel, Armin ^{[8
,9
]}

Heinritzi, Martin ^{[3
,8
]}

Kangasluoma, Juha ^{[2
]}

Keskinen, Helmi ^{[12
]}

Kim, Jaeseok ^{[12
]}

Kirkby, Jasper ^{[3
,7
]}

Laaksonen, Ari ^{[12
,16
]}

Lawler, Michael J. ^{[12
,13
]}

Lehtipalo, Katrianne ^{[2
,14
]}

Leiminger, Markus ^{[3
]}

Makhmutov, Vladimir ^{[15
]}

Mathot, Serge ^{[7
]}

Onnela, Antti ^{[7
]}

Petaja, Tuukka ^{[2
]}

Riccobono, Francesco ^{[1
]}

Rissanen, Matti P. ^{[2
]}

Rondo, Linda ^{[3
]}

Tome, Antonio ^{[5
,6
]}

Virtanen, Annele ^{[12
]}

Viisanen, Yrjo ^{[16
]}

Williamson, Christina ^{[3
]}

Wimmer, Daniela ^{[2
,3
]}

Winkler, Paul M. ^{[17
]}

Ye, Penglin ^{[18
]}

Curtius, Joachim ^{[3
]}

Kulmala, Markku ^{[2
]}

Worsnop, Douglas R. ^{[2
,19
]}

Donahue, Neil M. ^{[18
]}

Baltensperger, Urs ^{[1
]}

机构：

[1] Paul Scherrer Inst, Lab Atmospher Chem, CH-5232 Villigen, Switzerland

[2] Univ Helsinki, Dept Phys, Helsinki 00014, Finland

[3] Goethe Univ Frankfurt, Inst Atmospher & Environm Sci, D-60438 Frankfurt, Germany

[4] Univ Lille 1 Sci & Technol, Lab Phys Lasers Atomes & Mol, F-59655 Villeneuve Dascq, France

[5] Univ Lisbon, CENTRA SIM, P-1749 Lisbon, Portugal

[6] Univ Beira Interior, P-1749 Lisbon, Portugal

[7] CERN, CH-1211 Geneva, Switzerland

[8] Univ Innsbruck, A-6020 Innsbruck, Austria

[9] IONICON Analyt GmbH, A-6020 Innsbruck, Austria

[10] Helsinki Inst Phys, Helsinki 00014, Finland

[11] CALTECH, Pasadena, CA 91125 USA

[12] Univ Eastern Finland, Dept Appl Phys, Kuopio 70211, Finland

[13] Natl Ctr Atmospher Res, Div Atmospher Chem, Boulder, CO 80301 USA

[14] Airmodus Ltd, Helsinki 00560, Finland

[15] RAS, Lebedev Phys Inst, Moscow 119991, Russia

[16] Finnish Meteorol Inst, FIN-00101 Helsinki, Finland

[17] Univ Vienna, Fac Phys, A-1090 Vienna, Austria

[18] Carnegie Mellon Univ, Ctr Atmospher Particle Studies, Pittsburgh, PA 15213 USA

[19] Aerodyne Res Inc, Billerica, MA 01821 USA

来源：

ENVIRONMENTAL SCIENCE & TECHNOLOGY | 2014年 / 48卷 / 23期

基金：

奥地利科学基金会; 美国国家科学基金会; 瑞典研究理事会; 瑞士国家科学基金会; 芬兰科学院;

关键词：

SULFURIC-ACID; PARTICLE NUCLEATION; OXIDATION-PRODUCTS; AMMONIA; DIMETHYLAMINE; ENERGETICS; GROWTH; H2SO4; CONTRIBUTE; AMBIENT;

D O I：

10.1021/es502380b

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

We investigated the nucleation of sulfuric acid together with two bases (ammonia and dimethylamine), at the CLOUD chamber at CERN. The chemical composition of positive, negative, and neutral clusters was studied using three Atmospheric Pressure interface-Time Of Flight (APi-TOF) mass spectrometers: two were operated in positive and negative mode to detect the chamber ions, while the third was equipped with a nitrate ion chemical ionization source allowing detection of neutral clusters. Taking into account the possible fragmentation that can happen during the charging of the ions or within the first stage of the mass spectrometer, the cluster formation proceeded via essentially one-to-one acid-base addition for all of the clusters, independent of the type of the base. For the positive clusters, the charge is carried by one excess protonated base, while for the negative clusters it is carried by a deprotonated acid; the same is true for the neutral clusters after these have been ionized. During the experiments involving sulfuric acid and dimethylamine, it was possible to study the appearance time for all the clusters (positive, negative, and neutral). It appeared that, after the formation of the clusters containing three molecules of sulfuric acid, the clusters grow at a similar speed, independent of their charge. The growth rate is then probably limited by the arrival rate of sulfuric acid or cluster-cluster collision.

引用

页码：13675 / 13684

页数：10

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