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Spontaneous generation of hydrogen peroxide from aqueous microdroplets

We show H(2)O(2) is spontaneously produced from pure water by atomizing bulk water into microdroplets (1 μm to 20 µm in diameter). Production of H(2)O(2), as assayed by H(2)O(2)-sensitve fluorescence dye peroxyfluor-1, increased with decreasing microdroplet size. Cleavage of 4-carboxyphenylboronic a...

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Autores principales: Lee, Jae Kyoo, Walker, Katherine L., Han, Hyun Soo, Kang, Jooyoun, Prinz, Fritz B., Waymouth, Robert M., Nam, Hong Gil, Zare, Richard N.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: National Academy of Sciences 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6765303/
https://www.ncbi.nlm.nih.gov/pubmed/31451646
http://dx.doi.org/10.1073/pnas.1911883116
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author Lee, Jae Kyoo
Walker, Katherine L.
Han, Hyun Soo
Kang, Jooyoun
Prinz, Fritz B.
Waymouth, Robert M.
Nam, Hong Gil
Zare, Richard N.
author_facet Lee, Jae Kyoo
Walker, Katherine L.
Han, Hyun Soo
Kang, Jooyoun
Prinz, Fritz B.
Waymouth, Robert M.
Nam, Hong Gil
Zare, Richard N.
author_sort Lee, Jae Kyoo
collection PubMed
description We show H(2)O(2) is spontaneously produced from pure water by atomizing bulk water into microdroplets (1 μm to 20 µm in diameter). Production of H(2)O(2), as assayed by H(2)O(2)-sensitve fluorescence dye peroxyfluor-1, increased with decreasing microdroplet size. Cleavage of 4-carboxyphenylboronic acid and conversion of phenylboronic acid to phenols in microdroplets further confirmed the generation of H(2)O(2). The generated H(2)O(2) concentration was ∼30 µM (∼1 part per million) as determined by titration with potassium titanium oxalate. Changing the spray gas to O(2) or bubbling O(2) decreased the yield of H(2)O(2) in microdroplets, indicating that pure water microdroplets directly generate H(2)O(2) without help from O(2) either in air surrounding the droplet or dissolved in water. We consider various possible mechanisms for H(2)O(2) formation and report a number of different experiments exploring this issue. We suggest that hydroxyl radical (OH) recombination is the most likely source, in which OH is generated by loss of an electron from OH(−) at or near the surface of the water microdroplet. This catalyst-free and voltage-free H(2)O(2) production method provides innovative opportunities for green production of hydrogen peroxide.
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spelling pubmed-67653032019-10-29 Spontaneous generation of hydrogen peroxide from aqueous microdroplets Lee, Jae Kyoo Walker, Katherine L. Han, Hyun Soo Kang, Jooyoun Prinz, Fritz B. Waymouth, Robert M. Nam, Hong Gil Zare, Richard N. Proc Natl Acad Sci U S A Physical Sciences We show H(2)O(2) is spontaneously produced from pure water by atomizing bulk water into microdroplets (1 μm to 20 µm in diameter). Production of H(2)O(2), as assayed by H(2)O(2)-sensitve fluorescence dye peroxyfluor-1, increased with decreasing microdroplet size. Cleavage of 4-carboxyphenylboronic acid and conversion of phenylboronic acid to phenols in microdroplets further confirmed the generation of H(2)O(2). The generated H(2)O(2) concentration was ∼30 µM (∼1 part per million) as determined by titration with potassium titanium oxalate. Changing the spray gas to O(2) or bubbling O(2) decreased the yield of H(2)O(2) in microdroplets, indicating that pure water microdroplets directly generate H(2)O(2) without help from O(2) either in air surrounding the droplet or dissolved in water. We consider various possible mechanisms for H(2)O(2) formation and report a number of different experiments exploring this issue. We suggest that hydroxyl radical (OH) recombination is the most likely source, in which OH is generated by loss of an electron from OH(−) at or near the surface of the water microdroplet. This catalyst-free and voltage-free H(2)O(2) production method provides innovative opportunities for green production of hydrogen peroxide. National Academy of Sciences 2019-09-24 2019-08-26 /pmc/articles/PMC6765303/ /pubmed/31451646 http://dx.doi.org/10.1073/pnas.1911883116 Text en Copyright © 2019 the Author(s). Published by PNAS. https://creativecommons.org/licenses/by-nc-nd/4.0/ https://creativecommons.org/licenses/by-nc-nd/4.0/This open access article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND) (https://creativecommons.org/licenses/by-nc-nd/4.0/) .
spellingShingle Physical Sciences
Lee, Jae Kyoo
Walker, Katherine L.
Han, Hyun Soo
Kang, Jooyoun
Prinz, Fritz B.
Waymouth, Robert M.
Nam, Hong Gil
Zare, Richard N.
Spontaneous generation of hydrogen peroxide from aqueous microdroplets
title Spontaneous generation of hydrogen peroxide from aqueous microdroplets
title_full Spontaneous generation of hydrogen peroxide from aqueous microdroplets
title_fullStr Spontaneous generation of hydrogen peroxide from aqueous microdroplets
title_full_unstemmed Spontaneous generation of hydrogen peroxide from aqueous microdroplets
title_short Spontaneous generation of hydrogen peroxide from aqueous microdroplets
title_sort spontaneous generation of hydrogen peroxide from aqueous microdroplets
topic Physical Sciences
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6765303/
https://www.ncbi.nlm.nih.gov/pubmed/31451646
http://dx.doi.org/10.1073/pnas.1911883116
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