Abstract:
:Oxidation of bromide in aqueous environments initiates the formation of molecular halogen compounds, which is important for the global tropospheric ozone budget. In the aqueous bulk, oxidation of bromide by ozone involves a [Br•OOO-] complex as intermediate. Here we report liquid jet X-ray photoelectron spectroscopy measurements that provide direct experimental evidence for the ozonide and establish its propensity for the solution-vapour interface. Theoretical calculations support these findings, showing that water stabilizes the ozonide and lowers the energy of the transition state at neutral pH. Kinetic experiments confirm the dominance of the heterogeneous oxidation route established by this precursor at low, atmospherically relevant ozone concentrations. Taken together, our results provide a strong case of different reaction kinetics and mechanisms of reactions occurring at the aqueous phase-vapour interface compared with the bulk aqueous phase.Heterogeneous oxidation of bromide in atmospheric aqueous environments has long been suspected to be accelerated at the interface between aqueous solution and air. Here, the authors provide spectroscopic, kinetic and theoretical evidence for a rate limiting, surface active ozonide formed at the interface.
journal_name
Nat Communjournal_title
Nature communicationsauthors
Artiglia L,Edebeli J,Orlando F,Chen S,Lee MT,Corral Arroyo P,Gilgen A,Bartels-Rausch T,Kleibert A,Vazdar M,Andres Carignano M,Francisco JS,Shepson PB,Gladich I,Ammann Mdoi
10.1038/s41467-017-00823-xsubject
Has Abstractpub_date
2017-09-26 00:00:00pages
700issue
1issn
2041-1723pii
10.1038/s41467-017-00823-xjournal_volume
8pub_type
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