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Mechanistic Insights on the Photosensitized Chemistry of a Fatty Acid at the Air/Water Interface
[Image: see text] Interfaces are ubiquitous in the environment and many atmospheric key processes, such as gas deposition, aerosol, and cloud formation are, at one stage or another, strongly impacted by physical and chemical processes occurring at interfaces. Here, the photoinduced chemistry of an a...
Autores principales: | , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American
Chemical Society
2016
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5072107/ https://www.ncbi.nlm.nih.gov/pubmed/27611489 http://dx.doi.org/10.1021/acs.est.6b03165 |
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author | Tinel, Liselotte Rossignol, Stéphanie Bianco, Angelica Passananti, Monica Perrier, Sébastien Wang, Xinming Brigante, Marcello Donaldson, D. James George, Christian |
author_facet | Tinel, Liselotte Rossignol, Stéphanie Bianco, Angelica Passananti, Monica Perrier, Sébastien Wang, Xinming Brigante, Marcello Donaldson, D. James George, Christian |
author_sort | Tinel, Liselotte |
collection | PubMed |
description | [Image: see text] Interfaces are ubiquitous in the environment and many atmospheric key processes, such as gas deposition, aerosol, and cloud formation are, at one stage or another, strongly impacted by physical and chemical processes occurring at interfaces. Here, the photoinduced chemistry of an air/water interface coated with nonanoic acid—a fatty acid surfactant we use as a proxy for chemically complex natural aqueous surface microlayers—was investigated as a source of volatile and semivolatile reactive organic species. The carboxylic acid coating significantly increased the propensity of photosensitizers, chosen to mimic those observed in real environmental waters, to partition to the interface and enhance reactivity there. Photochemical formation of functionalized and unsaturated compounds was systematically observed upon irradiation of these coated surfaces. The role of a coated interface appears to be critical in providing a concentrated medium allowing radical–radical reactions to occur in parallel with molecular oxygen additions. Mechanistic insights are provided from extensive analysis of products observed in both gas and aqueous phases by online switchable reagent ion-time of flight-mass spectrometry and by off-line ultraperformance liquid chromatography coupled to a Q Exactive high resolution mass spectrometer through heated electrospray ionization, respectively. |
format | Online Article Text |
id | pubmed-5072107 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2016 |
publisher | American
Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-50721072016-10-21 Mechanistic Insights on the Photosensitized Chemistry of a Fatty Acid at the Air/Water Interface Tinel, Liselotte Rossignol, Stéphanie Bianco, Angelica Passananti, Monica Perrier, Sébastien Wang, Xinming Brigante, Marcello Donaldson, D. James George, Christian Environ Sci Technol [Image: see text] Interfaces are ubiquitous in the environment and many atmospheric key processes, such as gas deposition, aerosol, and cloud formation are, at one stage or another, strongly impacted by physical and chemical processes occurring at interfaces. Here, the photoinduced chemistry of an air/water interface coated with nonanoic acid—a fatty acid surfactant we use as a proxy for chemically complex natural aqueous surface microlayers—was investigated as a source of volatile and semivolatile reactive organic species. The carboxylic acid coating significantly increased the propensity of photosensitizers, chosen to mimic those observed in real environmental waters, to partition to the interface and enhance reactivity there. Photochemical formation of functionalized and unsaturated compounds was systematically observed upon irradiation of these coated surfaces. The role of a coated interface appears to be critical in providing a concentrated medium allowing radical–radical reactions to occur in parallel with molecular oxygen additions. Mechanistic insights are provided from extensive analysis of products observed in both gas and aqueous phases by online switchable reagent ion-time of flight-mass spectrometry and by off-line ultraperformance liquid chromatography coupled to a Q Exactive high resolution mass spectrometer through heated electrospray ionization, respectively. American Chemical Society 2016-09-09 2016-10-18 /pmc/articles/PMC5072107/ /pubmed/27611489 http://dx.doi.org/10.1021/acs.est.6b03165 Text en Copyright © 2016 American Chemical Society This is an open access article published under an ACS AuthorChoice License (http://pubs.acs.org/page/policy/authorchoice_termsofuse.html) , which permits copying and redistribution of the article or any adaptations for non-commercial purposes. |
spellingShingle | Tinel, Liselotte Rossignol, Stéphanie Bianco, Angelica Passananti, Monica Perrier, Sébastien Wang, Xinming Brigante, Marcello Donaldson, D. James George, Christian Mechanistic Insights on the Photosensitized Chemistry of a Fatty Acid at the Air/Water Interface |
title | Mechanistic
Insights on the Photosensitized Chemistry
of a Fatty Acid at the Air/Water Interface |
title_full | Mechanistic
Insights on the Photosensitized Chemistry
of a Fatty Acid at the Air/Water Interface |
title_fullStr | Mechanistic
Insights on the Photosensitized Chemistry
of a Fatty Acid at the Air/Water Interface |
title_full_unstemmed | Mechanistic
Insights on the Photosensitized Chemistry
of a Fatty Acid at the Air/Water Interface |
title_short | Mechanistic
Insights on the Photosensitized Chemistry
of a Fatty Acid at the Air/Water Interface |
title_sort | mechanistic
insights on the photosensitized chemistry
of a fatty acid at the air/water interface |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5072107/ https://www.ncbi.nlm.nih.gov/pubmed/27611489 http://dx.doi.org/10.1021/acs.est.6b03165 |
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