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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...
Autores principales: | , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
The Royal Society of Chemistry
2022
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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. |
format | Online Article Text |
id | pubmed-9714771 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | The Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
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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