A surface-stabilized ozonide triggers bromide oxidation at the aqueous solution-vapour interface
<p dir="ltr">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 repo...
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2017
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| _version_ | 1864513556563623936 |
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| author | Luca Artiglia (1713652) |
| author2 | Jacinta Edebeli (10586622) Fabrizio Orlando (1701163) Shuzhen Chen (297742) Ming-Tao Lee (1568470) Pablo Corral Arroyo (5465684) Anina Gilgen (19479399) Thorsten Bartels-Rausch (4117720) Armin Kleibert (1270557) Mario Vazdar (1435945) Marcelo Andres Carignano (19725586) Joseph S. Francisco (1414543) Paul B. Shepson (1360947) Ivan Gladich (1442929) Markus Ammann (1600930) |
| author2_role | author author author author author author author author author author author author author author |
| author_facet | Luca Artiglia (1713652) Jacinta Edebeli (10586622) Fabrizio Orlando (1701163) Shuzhen Chen (297742) Ming-Tao Lee (1568470) Pablo Corral Arroyo (5465684) Anina Gilgen (19479399) Thorsten Bartels-Rausch (4117720) Armin Kleibert (1270557) Mario Vazdar (1435945) Marcelo Andres Carignano (19725586) Joseph S. Francisco (1414543) Paul B. Shepson (1360947) Ivan Gladich (1442929) Markus Ammann (1600930) |
| author_role | author |
| dc.creator.none.fl_str_mv | Luca Artiglia (1713652) Jacinta Edebeli (10586622) Fabrizio Orlando (1701163) Shuzhen Chen (297742) Ming-Tao Lee (1568470) Pablo Corral Arroyo (5465684) Anina Gilgen (19479399) Thorsten Bartels-Rausch (4117720) Armin Kleibert (1270557) Mario Vazdar (1435945) Marcelo Andres Carignano (19725586) Joseph S. Francisco (1414543) Paul B. Shepson (1360947) Ivan Gladich (1442929) Markus Ammann (1600930) |
| dc.date.none.fl_str_mv | 2017-09-26T03:00:00Z |
| dc.identifier.none.fl_str_mv | 10.1038/s41467-017-00823-x |
| dc.relation.none.fl_str_mv | https://figshare.com/articles/journal_contribution/A_surface-stabilized_ozonide_triggers_bromide_oxidation_at_the_aqueous_solution-vapour_interface/27088084 |
| dc.rights.none.fl_str_mv | CC BY 4.0 info:eu-repo/semantics/openAccess |
| dc.subject.none.fl_str_mv | Chemical sciences Organic chemistry Earth sciences Atmospheric sciences Oxidation of bromide Molecular halogen compounds Tropospheric ozone budget X-ray photoelectron spectroscopy Ozonide |
| dc.title.none.fl_str_mv | A surface-stabilized ozonide triggers bromide oxidation at the aqueous solution-vapour interface |
| dc.type.none.fl_str_mv | Text Journal contribution info:eu-repo/semantics/publishedVersion text contribution to journal |
| description | <p dir="ltr">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.</p><h2>Other Information</h2><p dir="ltr">Published in: Nature Communications<br>License: <a href="https://creativecommons.org/licenses/by/4.0" target="_blank">https://creativecommons.org/licenses/by/4.0</a><br>See article on publisher's website: <a href="https://dx.doi.org/10.1038/s41467-017-00823-x" target="_blank">https://dx.doi.org/10.1038/s41467-017-00823-x</a></p> |
| eu_rights_str_mv | openAccess |
| id | Manara2_e7246ac6802913b3c200c0ede79c244b |
| identifier_str_mv | 10.1038/s41467-017-00823-x |
| network_acronym_str | Manara2 |
| network_name_str | Manara2 |
| oai_identifier_str | oai:figshare.com:article/27088084 |
| publishDate | 2017 |
| repository.mail.fl_str_mv | |
| repository.name.fl_str_mv | |
| repository_id_str | |
| rights_invalid_str_mv | CC BY 4.0 |
| spelling | A surface-stabilized ozonide triggers bromide oxidation at the aqueous solution-vapour interfaceLuca Artiglia (1713652)Jacinta Edebeli (10586622)Fabrizio Orlando (1701163)Shuzhen Chen (297742)Ming-Tao Lee (1568470)Pablo Corral Arroyo (5465684)Anina Gilgen (19479399)Thorsten Bartels-Rausch (4117720)Armin Kleibert (1270557)Mario Vazdar (1435945)Marcelo Andres Carignano (19725586)Joseph S. Francisco (1414543)Paul B. Shepson (1360947)Ivan Gladich (1442929)Markus Ammann (1600930)Chemical sciencesOrganic chemistryEarth sciencesAtmospheric sciencesOxidation of bromideMolecular halogen compoundsTropospheric ozone budgetX-ray photoelectron spectroscopyOzonide<p dir="ltr">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.</p><h2>Other Information</h2><p dir="ltr">Published in: Nature Communications<br>License: <a href="https://creativecommons.org/licenses/by/4.0" target="_blank">https://creativecommons.org/licenses/by/4.0</a><br>See article on publisher's website: <a href="https://dx.doi.org/10.1038/s41467-017-00823-x" target="_blank">https://dx.doi.org/10.1038/s41467-017-00823-x</a></p>2017-09-26T03:00:00ZTextJournal contributioninfo:eu-repo/semantics/publishedVersiontextcontribution to journal10.1038/s41467-017-00823-xhttps://figshare.com/articles/journal_contribution/A_surface-stabilized_ozonide_triggers_bromide_oxidation_at_the_aqueous_solution-vapour_interface/27088084CC BY 4.0info:eu-repo/semantics/openAccessoai:figshare.com:article/270880842017-09-26T03:00:00Z |
| spellingShingle | A surface-stabilized ozonide triggers bromide oxidation at the aqueous solution-vapour interface Luca Artiglia (1713652) Chemical sciences Organic chemistry Earth sciences Atmospheric sciences Oxidation of bromide Molecular halogen compounds Tropospheric ozone budget X-ray photoelectron spectroscopy Ozonide |
| status_str | publishedVersion |
| title | A surface-stabilized ozonide triggers bromide oxidation at the aqueous solution-vapour interface |
| title_full | A surface-stabilized ozonide triggers bromide oxidation at the aqueous solution-vapour interface |
| title_fullStr | A surface-stabilized ozonide triggers bromide oxidation at the aqueous solution-vapour interface |
| title_full_unstemmed | A surface-stabilized ozonide triggers bromide oxidation at the aqueous solution-vapour interface |
| title_short | A surface-stabilized ozonide triggers bromide oxidation at the aqueous solution-vapour interface |
| title_sort | A surface-stabilized ozonide triggers bromide oxidation at the aqueous solution-vapour interface |
| topic | Chemical sciences Organic chemistry Earth sciences Atmospheric sciences Oxidation of bromide Molecular halogen compounds Tropospheric ozone budget X-ray photoelectron spectroscopy Ozonide |