Clustering mechanism of oxocarboxylic acids involving hydration reaction

Implications for the atmospheric models

Ling Liu, Oona Kupiainen-Maatta, Haijie Zhang, Hao Li, Jie Zhong, Theo Kurten, Hanna Vehkamaki, Shaowen Zhang, Yunhong Zhang, Maofa Ge, Xiuhui Zhang, Zesheng Li

Forskningsoutput: TidskriftsbidragArtikelVetenskapligPeer review

Sammanfattning

The formation of atmospheric aerosol particles from condensable gases is a dominant source of particulate matter in the boundary layer, but the mechanism is still ambiguous. During the clustering process, precursors with di↵erent reactivities can induce various chemical reactions in addition to the formation of hydrogen bonds. However, the clustering mechanism involving chemical reactions is rarely considered in most of the nucleation process models. Oxocarboxylic acids are common compositions of secondary organic aerosol, but the role of oxocarboxylic acids in secondary organic aerosol formation is still not fully understood. In this paper, glyoxylic acid, the simplest and the most abundant atmospheric oxocarboxylic acids, has been selected as a representative example of oxocarboxylic acids in order to study the clustering mechanism involving hydration reaction using Density Functional Theory combined with the Atmospheric Clusters Dynamic Code. The hydration reaction of glyoxylic acid
can occur either in the gas phase or during the clustering process. In atmospheric
conditions, the total conversion ratio of glyoxylic acid to its hydration reaction product (2,2-dihydroxyacetic acid) in both gas phase and clusters can be up to 85%, andthe product can further participate in the clustering process. The di↵erences in cluster structures and properties induced by the hydration reaction lead to significant di↵erences in cluster formation rates and pathways at relatively low temperatures.
Originalspråkengelska
Artikelnummer214303
TidskriftJournal of Chemical Physics
Volym148
Utgåva21
Antal sidor10
ISSN0021-9606
DOI
StatusPublicerad - 7 jun 2018
MoE-publikationstypA1 Tidskriftsartikel-refererad

Vetenskapsgrenar

  • 114 Fysik
  • 116 Kemi

Citera det här

Liu, Ling ; Kupiainen-Maatta, Oona ; Zhang, Haijie ; Li, Hao ; Zhong, Jie ; Kurten, Theo ; Vehkamaki, Hanna ; Zhang, Shaowen ; Zhang, Yunhong ; Ge, Maofa ; Zhang, Xiuhui ; Li, Zesheng. / Clustering mechanism of oxocarboxylic acids involving hydration reaction : Implications for the atmospheric models. I: Journal of Chemical Physics. 2018 ; Vol. 148, Nr. 21.
@article{9d940b6b8fba4d0db0440ce57fd11e8d,
title = "Clustering mechanism of oxocarboxylic acids involving hydration reaction: Implications for the atmospheric models",
abstract = "The formation of atmospheric aerosol particles from condensable gases is a dominant source of particulate matter in the boundary layer, but the mechanism is still ambiguous. During the clustering process, precursors with di↵erent reactivities can induce various chemical reactions in addition to the formation of hydrogen bonds. However, the clustering mechanism involving chemical reactions is rarely considered in most of the nucleation process models. Oxocarboxylic acids are common compositions of secondary organic aerosol, but the role of oxocarboxylic acids in secondary organic aerosol formation is still not fully understood. In this paper, glyoxylic acid, the simplest and the most abundant atmospheric oxocarboxylic acids, has been selected as a representative example of oxocarboxylic acids in order to study the clustering mechanism involving hydration reaction using Density Functional Theory combined with the Atmospheric Clusters Dynamic Code. The hydration reaction of glyoxylic acidcan occur either in the gas phase or during the clustering process. In atmosphericconditions, the total conversion ratio of glyoxylic acid to its hydration reaction product (2,2-dihydroxyacetic acid) in both gas phase and clusters can be up to 85{\%}, andthe product can further participate in the clustering process. The di↵erences in cluster structures and properties induced by the hydration reaction lead to significant di↵erences in cluster formation rates and pathways at relatively low temperatures.",
keywords = "PRE-NUCLEATION CLUSTERS, CARBON ISOTOPIC COMPOSITION, DENSITY-FUNCTIONAL THEORY, BEE COLONY ALGORITHM, SULFURIC-ACID, PARTICLE FORMATION, MOLECULAR CLUSTERS, DICARBOXYLIC-ACIDS, EARTHS ATMOSPHERE, ALPHA-DICARBONYLS, 114 Physical sciences, 116 Chemical sciences",
author = "Ling Liu and Oona Kupiainen-Maatta and Haijie Zhang and Hao Li and Jie Zhong and Theo Kurten and Hanna Vehkamaki and Shaowen Zhang and Yunhong Zhang and Maofa Ge and Xiuhui Zhang and Zesheng Li",
year = "2018",
month = "6",
day = "7",
doi = "10.1063/1.5030665",
language = "English",
volume = "148",
journal = "Journal of Chemical Physics",
issn = "0021-9606",
publisher = "AVS",
number = "21",

}

Clustering mechanism of oxocarboxylic acids involving hydration reaction : Implications for the atmospheric models. / Liu, Ling; Kupiainen-Maatta, Oona; Zhang, Haijie; Li, Hao; Zhong, Jie; Kurten, Theo; Vehkamaki, Hanna; Zhang, Shaowen; Zhang, Yunhong; Ge, Maofa; Zhang, Xiuhui; Li, Zesheng.

I: Journal of Chemical Physics, Vol. 148, Nr. 21, 214303, 07.06.2018.

Forskningsoutput: TidskriftsbidragArtikelVetenskapligPeer review

TY - JOUR

T1 - Clustering mechanism of oxocarboxylic acids involving hydration reaction

T2 - Implications for the atmospheric models

AU - Liu, Ling

AU - Kupiainen-Maatta, Oona

AU - Zhang, Haijie

AU - Li, Hao

AU - Zhong, Jie

AU - Kurten, Theo

AU - Vehkamaki, Hanna

AU - Zhang, Shaowen

AU - Zhang, Yunhong

AU - Ge, Maofa

AU - Zhang, Xiuhui

AU - Li, Zesheng

PY - 2018/6/7

Y1 - 2018/6/7

N2 - The formation of atmospheric aerosol particles from condensable gases is a dominant source of particulate matter in the boundary layer, but the mechanism is still ambiguous. During the clustering process, precursors with di↵erent reactivities can induce various chemical reactions in addition to the formation of hydrogen bonds. However, the clustering mechanism involving chemical reactions is rarely considered in most of the nucleation process models. Oxocarboxylic acids are common compositions of secondary organic aerosol, but the role of oxocarboxylic acids in secondary organic aerosol formation is still not fully understood. In this paper, glyoxylic acid, the simplest and the most abundant atmospheric oxocarboxylic acids, has been selected as a representative example of oxocarboxylic acids in order to study the clustering mechanism involving hydration reaction using Density Functional Theory combined with the Atmospheric Clusters Dynamic Code. The hydration reaction of glyoxylic acidcan occur either in the gas phase or during the clustering process. In atmosphericconditions, the total conversion ratio of glyoxylic acid to its hydration reaction product (2,2-dihydroxyacetic acid) in both gas phase and clusters can be up to 85%, andthe product can further participate in the clustering process. The di↵erences in cluster structures and properties induced by the hydration reaction lead to significant di↵erences in cluster formation rates and pathways at relatively low temperatures.

AB - The formation of atmospheric aerosol particles from condensable gases is a dominant source of particulate matter in the boundary layer, but the mechanism is still ambiguous. During the clustering process, precursors with di↵erent reactivities can induce various chemical reactions in addition to the formation of hydrogen bonds. However, the clustering mechanism involving chemical reactions is rarely considered in most of the nucleation process models. Oxocarboxylic acids are common compositions of secondary organic aerosol, but the role of oxocarboxylic acids in secondary organic aerosol formation is still not fully understood. In this paper, glyoxylic acid, the simplest and the most abundant atmospheric oxocarboxylic acids, has been selected as a representative example of oxocarboxylic acids in order to study the clustering mechanism involving hydration reaction using Density Functional Theory combined with the Atmospheric Clusters Dynamic Code. The hydration reaction of glyoxylic acidcan occur either in the gas phase or during the clustering process. In atmosphericconditions, the total conversion ratio of glyoxylic acid to its hydration reaction product (2,2-dihydroxyacetic acid) in both gas phase and clusters can be up to 85%, andthe product can further participate in the clustering process. The di↵erences in cluster structures and properties induced by the hydration reaction lead to significant di↵erences in cluster formation rates and pathways at relatively low temperatures.

KW - PRE-NUCLEATION CLUSTERS

KW - CARBON ISOTOPIC COMPOSITION

KW - DENSITY-FUNCTIONAL THEORY

KW - BEE COLONY ALGORITHM

KW - SULFURIC-ACID

KW - PARTICLE FORMATION

KW - MOLECULAR CLUSTERS

KW - DICARBOXYLIC-ACIDS

KW - EARTHS ATMOSPHERE

KW - ALPHA-DICARBONYLS

KW - 114 Physical sciences

KW - 116 Chemical sciences

U2 - 10.1063/1.5030665

DO - 10.1063/1.5030665

M3 - Article

VL - 148

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

SN - 0021-9606

IS - 21

M1 - 214303

ER -