Direct Link between Structure and Hydration in Ammonium and Aminium Bisulfate Clusters Implicated in Atmospheric New Particle Formation.

Autor: Yang Y; Department of Chemistry , Stony Brook University , 100 Nicolls Road , Stony Brook , New York 11794 , United States., Waller SE; Department of Chemistry , Stony Brook University , 100 Nicolls Road , Stony Brook , New York 11794 , United States., Kreinbihl JJ; Department of Chemistry , Stony Brook University , 100 Nicolls Road , Stony Brook , New York 11794 , United States., Johnson CJ; Department of Chemistry , Stony Brook University , 100 Nicolls Road , Stony Brook , New York 11794 , United States.
Jazyk: angličtina
Zdroj: The journal of physical chemistry letters [J Phys Chem Lett] 2018 Sep 20; Vol. 9 (18), pp. 5647-5652. Date of Electronic Publication: 2018 Sep 13.
DOI: 10.1021/acs.jpclett.8b02500
Abstrakt: The acid-base chemistry of amines and sulfuric acid promotes growth in the early stages of atmospheric new particle formation, with more basic amines enhancing growth rates. Hydration of these particles has been proposed to depend on acidity or basicity but is difficult to quantify; therefore, the role of water in this process is not well understood. Using tandem mass spectrometry coupled to a temperature-controlled ion trap, we show that water uptake by aminium bisulfate clusters depends on the total number of free hydrogen bond donors in the cluster and is unaffected by the interchange of amines featuring the same number of substituents but differing gas-phase basicity. Analyzing this trend reveals site-specific propensities for hydration. These results indicate that hydration is determined by structural factors and that reported dependences on acidity or basicity arise from the weaker correlation between the number of hydrogen bond donors of amines and their gas-phase basicity.
Databáze: MEDLINE