TY - JOUR
T1 - Structures and reactivity of peroxy radicals and dimeric products revealed by online tandem mass spectrometry
AU - Tomaz, Sophie
AU - Wang, Dongyu
AU - Zabalegui, Nicolás
AU - Li, Dandan
AU - Lamkaddam, Houssni
AU - Bachmeier, Franziska
AU - Vogel, Alexander
AU - Monge, María Eugenia
AU - Perrier, Sébastien
AU - Baltensperger, Urs
AU - George, Christian
AU - Rissanen, Matti
AU - Ehn, Mikael
AU - El Haddad, Imad
AU - Riva, Matthieu
N1 - Funding Information:
This work was financially supported by the University of Lyon through the Breakthrough grant WANTED, the French National program LEFE (Les Enveloppes Fluides et l’En-vironnement), the Academy of Finland (grants 317380 & 320094), the Swiss National Science Foundation (no. 200020_172602), the European Union’s Horizon 2020 research and innovation program under Marie Skłodowska-Curie grant agreement (no. 690958 & no. 701647), ERC-StG COALA (no. 638703), and ERC-StG MAARvEL (no. 852161). M.E.M. is a Research Staff member from CONICET. The authors thank Frederic Bourgain for technical support.
Publisher Copyright:
© 2021, The Author(s).
Copyright:
Copyright 2021 Elsevier B.V., All rights reserved.
PY - 2021
Y1 - 2021
N2 - Organic peroxy radicals (RO2) play a pivotal role in the degradation of hydrocarbons. The autoxidation of atmospheric RO2 radicals produces highly oxygenated organic molecules (HOMs), including low-volatility ROOR dimers formed by bimolecular RO2 + RO2 reactions. HOMs can initiate and greatly contribute to the formation and growth of atmospheric particles. As a result, HOMs have far-reaching health and climate implications. Nevertheless, the structures and formation mechanism of RO2 radicals and HOMs remain elusive. Here, we present the in-situ characterization of RO2 and dimer structure in the gas-phase, using online tandem mass spectrometry analyses. In this study, we constrain the structures and formation pathway of several HOM-RO2 radicals and dimers produced from monoterpene ozonolysis, a prominent atmospheric oxidation process. In addition to providing insights into atmospheric HOM chemistry, this study debuts online tandem MS analyses as a unique approach for the chemical characterization of reactive compounds, e.g., organic radicals.
AB - Organic peroxy radicals (RO2) play a pivotal role in the degradation of hydrocarbons. The autoxidation of atmospheric RO2 radicals produces highly oxygenated organic molecules (HOMs), including low-volatility ROOR dimers formed by bimolecular RO2 + RO2 reactions. HOMs can initiate and greatly contribute to the formation and growth of atmospheric particles. As a result, HOMs have far-reaching health and climate implications. Nevertheless, the structures and formation mechanism of RO2 radicals and HOMs remain elusive. Here, we present the in-situ characterization of RO2 and dimer structure in the gas-phase, using online tandem mass spectrometry analyses. In this study, we constrain the structures and formation pathway of several HOM-RO2 radicals and dimers produced from monoterpene ozonolysis, a prominent atmospheric oxidation process. In addition to providing insights into atmospheric HOM chemistry, this study debuts online tandem MS analyses as a unique approach for the chemical characterization of reactive compounds, e.g., organic radicals.
U2 - 10.1038/s41467-020-20532-2
DO - 10.1038/s41467-020-20532-2
M3 - Article
AN - SCOPUS:85099202577
SN - 2041-1723
VL - 12
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 300
ER -
