4.8 Article

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

期刊

ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 48, 期 23, 页码 13675-13684

出版社

AMER CHEMICAL SOC
DOI: 10.1021/es502380b

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资金

  1. EC [215072, 316662, 57360, 227463]
  2. German Federal Ministry of Education and Research [01LK0902A, 01LK1222A]
  3. Swiss National Science Foundation [200020_135307, 206620_141278]
  4. Academy of Finland (Center of Excellence) [1118615, 135054, 133872, 251427, 139656, 139995, 137749, 141217, 141451, 138951]
  5. Finnish Funding Agency for Technology and Innovation
  6. V.is.l. Foundation
  7. Nessling Foundation
  8. Austrian Science Fund (FWF) [J3198-N21]
  9. Portuguese Foundation for Science and Technology [CERN/FP/116387/2010]
  10. Swedish Research Council, Vetenskapsradet [2011-5120]
  11. Presidium of the Russian Academy of Sciences and Russian
  12. Foundation for Basic Research [08-02-91006-CERN, 12-02-91522-CERN]
  13. U.S. National Science Foundation [AGS1136479, CHE1012293]
  14. PEGASOS project by European Commission [FP7-ENV-2010-265148]
  15. Davidow Foundation
  16. Div Atmospheric & Geospace Sciences
  17. Directorate For Geosciences [1136479] Funding Source: National Science Foundation
  18. Swiss National Science Foundation (SNF) [206620_141278] Funding Source: Swiss National Science Foundation (SNF)

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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.

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