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Early dynamics of the emission of solvated electrons from nanodiamonds in water

Solvated electrons are among the most reductive species in an aqueous environment. Diamond materials have been proposed as a promising source of solvated electrons, but the underlying emission process in water remains elusive so far. Here, we show spectroscopic evidence for the emission of solvated...

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Autores principales: Buchner, Franziska, Kirschbaum, Thorren, Venerosy, Amélie, Girard, Hugues, Arnault, Jean-Charles, Kiendl, Benjamin, Krueger, Anke, Larsson, Karin, Bande, Annika, Petit, Tristan, Merschjann, Christoph
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9714771/
https://www.ncbi.nlm.nih.gov/pubmed/36394505
http://dx.doi.org/10.1039/d2nr03919b
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author Buchner, Franziska
Kirschbaum, Thorren
Venerosy, Amélie
Girard, Hugues
Arnault, Jean-Charles
Kiendl, Benjamin
Krueger, Anke
Larsson, Karin
Bande, Annika
Petit, Tristan
Merschjann, Christoph
author_facet Buchner, Franziska
Kirschbaum, Thorren
Venerosy, Amélie
Girard, Hugues
Arnault, Jean-Charles
Kiendl, Benjamin
Krueger, Anke
Larsson, Karin
Bande, Annika
Petit, Tristan
Merschjann, Christoph
author_sort Buchner, Franziska
collection PubMed
description Solvated electrons are among the most reductive species in an aqueous environment. Diamond materials have been proposed as a promising source of solvated electrons, but the underlying emission process in water remains elusive so far. Here, we show spectroscopic evidence for the emission of solvated electrons from detonation nanodiamonds upon excitation with both deep ultraviolet (225 nm) and visible (400 nm) light using ultrafast transient absorption. The crucial role of surface termination in the emission process is evidenced by comparing hydrogenated, hydroxylated and carboxylated nanodiamonds. In particular, a transient response that we attribute to solvated electrons is observed on hydrogenated nanodiamonds upon visible light excitation, while it shows a sub-ps recombination due to trap states when excited with deep ultraviolet light. The essential role of surface reconstructions on the nanodiamonds in these processes is proposed based on density functional theory calculations. These results open new perspectives for solar-driven emission of solvated electrons in an aqueous phase using nanodiamonds.
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spelling pubmed-97147712022-12-20 Early dynamics of the emission of solvated electrons from nanodiamonds in water Buchner, Franziska Kirschbaum, Thorren Venerosy, Amélie Girard, Hugues Arnault, Jean-Charles Kiendl, Benjamin Krueger, Anke Larsson, Karin Bande, Annika Petit, Tristan Merschjann, Christoph Nanoscale Chemistry Solvated electrons are among the most reductive species in an aqueous environment. Diamond materials have been proposed as a promising source of solvated electrons, but the underlying emission process in water remains elusive so far. Here, we show spectroscopic evidence for the emission of solvated electrons from detonation nanodiamonds upon excitation with both deep ultraviolet (225 nm) and visible (400 nm) light using ultrafast transient absorption. The crucial role of surface termination in the emission process is evidenced by comparing hydrogenated, hydroxylated and carboxylated nanodiamonds. In particular, a transient response that we attribute to solvated electrons is observed on hydrogenated nanodiamonds upon visible light excitation, while it shows a sub-ps recombination due to trap states when excited with deep ultraviolet light. The essential role of surface reconstructions on the nanodiamonds in these processes is proposed based on density functional theory calculations. These results open new perspectives for solar-driven emission of solvated electrons in an aqueous phase using nanodiamonds. The Royal Society of Chemistry 2022-11-01 /pmc/articles/PMC9714771/ /pubmed/36394505 http://dx.doi.org/10.1039/d2nr03919b Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by/3.0/
spellingShingle Chemistry
Buchner, Franziska
Kirschbaum, Thorren
Venerosy, Amélie
Girard, Hugues
Arnault, Jean-Charles
Kiendl, Benjamin
Krueger, Anke
Larsson, Karin
Bande, Annika
Petit, Tristan
Merschjann, Christoph
Early dynamics of the emission of solvated electrons from nanodiamonds in water
title Early dynamics of the emission of solvated electrons from nanodiamonds in water
title_full Early dynamics of the emission of solvated electrons from nanodiamonds in water
title_fullStr Early dynamics of the emission of solvated electrons from nanodiamonds in water
title_full_unstemmed Early dynamics of the emission of solvated electrons from nanodiamonds in water
title_short Early dynamics of the emission of solvated electrons from nanodiamonds in water
title_sort early dynamics of the emission of solvated electrons from nanodiamonds in water
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9714771/
https://www.ncbi.nlm.nih.gov/pubmed/36394505
http://dx.doi.org/10.1039/d2nr03919b
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