Radiative analysis of luminescence in photoreactive systems: Application to photosensitizers for solar fuel production.

Most chemical reactions promoted by light and using a photosensitizer (a dye) are subject to the phenomenon of luminescence. Redistribution of light in all directions (isotropic luminescence emission) and in a new spectral range (luminescence emission spectrum) makes experimental and theoretical stu...

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Autores principales: Caroline Supplis, Jérémi Dauchet, Victor Gattepaille, Fabrice Gros, Thomas Vourc'h, Jean-François Cornet
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Publicado: Public Library of Science (PLoS) 2021
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spelling oai:doaj.org-article:830e70676ee144c3bfc9a84e4ee5fa762021-12-02T20:06:35ZRadiative analysis of luminescence in photoreactive systems: Application to photosensitizers for solar fuel production.1932-620310.1371/journal.pone.0255002https://doaj.org/article/830e70676ee144c3bfc9a84e4ee5fa762021-01-01T00:00:00Zhttps://doi.org/10.1371/journal.pone.0255002https://doaj.org/toc/1932-6203Most chemical reactions promoted by light and using a photosensitizer (a dye) are subject to the phenomenon of luminescence. Redistribution of light in all directions (isotropic luminescence emission) and in a new spectral range (luminescence emission spectrum) makes experimental and theoretical studies much more complex compared to a situation with a purely absorbing reaction volume. This has a significant impact on the engineering of photoreactors for industrial applications. Future developments associated with photoreactive system optimization are therefore extremely challenging, and require an in-depth description and quantitative analysis of luminescence. In this study, a radiative model describing the effect of luminescence radiation on the calculation of absorptance is presented and analyzed with the multiple inelastic-scattering approach, using Monte Carlo simulations. The formalism of successive orders of scattering expansion is used as a sophisticated analysis tool which provides, when combined with relevant physical approximations, convenient analytical approximate solutions. Its application to four photosensitizers that are representative of renewable hydrogen production via artificial photosynthesis indicates that luminescence has a significant impact on absorptance and on overall quantum yield estimation, with the contribution of multiple scattering and important spectral effects due to inelastic scattering. We show that luminescence cannot be totally neglected in that case, since photon absorption lies at the root of the chemical reaction. We propose two coupled simple and appropriate analytical approximations enabling the estimation of absorptance with a relative error below 6% in every tested situation: the zero-order scattering approximation and the gray single-scattering approximation. Finally, this theoretical approach is used to determine and discuss the overall quantum yield of a bio-inspired photoreactive system with Eosin Y as a photosensitizer, implemented in an experimental setup comprising a photoreactor dedicated to hydrogen production.Caroline SupplisJérémi DauchetVictor GattepailleFabrice GrosThomas Vourc'hJean-François CornetPublic Library of Science (PLoS)articleMedicineRScienceQENPLoS ONE, Vol 16, Iss 7, p e0255002 (2021)
institution DOAJ
collection DOAJ
language EN
topic Medicine
R
Science
Q
spellingShingle Medicine
R
Science
Q
Caroline Supplis
Jérémi Dauchet
Victor Gattepaille
Fabrice Gros
Thomas Vourc'h
Jean-François Cornet
Radiative analysis of luminescence in photoreactive systems: Application to photosensitizers for solar fuel production.
description Most chemical reactions promoted by light and using a photosensitizer (a dye) are subject to the phenomenon of luminescence. Redistribution of light in all directions (isotropic luminescence emission) and in a new spectral range (luminescence emission spectrum) makes experimental and theoretical studies much more complex compared to a situation with a purely absorbing reaction volume. This has a significant impact on the engineering of photoreactors for industrial applications. Future developments associated with photoreactive system optimization are therefore extremely challenging, and require an in-depth description and quantitative analysis of luminescence. In this study, a radiative model describing the effect of luminescence radiation on the calculation of absorptance is presented and analyzed with the multiple inelastic-scattering approach, using Monte Carlo simulations. The formalism of successive orders of scattering expansion is used as a sophisticated analysis tool which provides, when combined with relevant physical approximations, convenient analytical approximate solutions. Its application to four photosensitizers that are representative of renewable hydrogen production via artificial photosynthesis indicates that luminescence has a significant impact on absorptance and on overall quantum yield estimation, with the contribution of multiple scattering and important spectral effects due to inelastic scattering. We show that luminescence cannot be totally neglected in that case, since photon absorption lies at the root of the chemical reaction. We propose two coupled simple and appropriate analytical approximations enabling the estimation of absorptance with a relative error below 6% in every tested situation: the zero-order scattering approximation and the gray single-scattering approximation. Finally, this theoretical approach is used to determine and discuss the overall quantum yield of a bio-inspired photoreactive system with Eosin Y as a photosensitizer, implemented in an experimental setup comprising a photoreactor dedicated to hydrogen production.
format article
author Caroline Supplis
Jérémi Dauchet
Victor Gattepaille
Fabrice Gros
Thomas Vourc'h
Jean-François Cornet
author_facet Caroline Supplis
Jérémi Dauchet
Victor Gattepaille
Fabrice Gros
Thomas Vourc'h
Jean-François Cornet
author_sort Caroline Supplis
title Radiative analysis of luminescence in photoreactive systems: Application to photosensitizers for solar fuel production.
title_short Radiative analysis of luminescence in photoreactive systems: Application to photosensitizers for solar fuel production.
title_full Radiative analysis of luminescence in photoreactive systems: Application to photosensitizers for solar fuel production.
title_fullStr Radiative analysis of luminescence in photoreactive systems: Application to photosensitizers for solar fuel production.
title_full_unstemmed Radiative analysis of luminescence in photoreactive systems: Application to photosensitizers for solar fuel production.
title_sort radiative analysis of luminescence in photoreactive systems: application to photosensitizers for solar fuel production.
publisher Public Library of Science (PLoS)
publishDate 2021
url https://doaj.org/article/830e70676ee144c3bfc9a84e4ee5fa76
work_keys_str_mv AT carolinesupplis radiativeanalysisofluminescenceinphotoreactivesystemsapplicationtophotosensitizersforsolarfuelproduction
AT jeremidauchet radiativeanalysisofluminescenceinphotoreactivesystemsapplicationtophotosensitizersforsolarfuelproduction
AT victorgattepaille radiativeanalysisofluminescenceinphotoreactivesystemsapplicationtophotosensitizersforsolarfuelproduction
AT fabricegros radiativeanalysisofluminescenceinphotoreactivesystemsapplicationtophotosensitizersforsolarfuelproduction
AT thomasvourch radiativeanalysisofluminescenceinphotoreactivesystemsapplicationtophotosensitizersforsolarfuelproduction
AT jeanfrancoiscornet radiativeanalysisofluminescenceinphotoreactivesystemsapplicationtophotosensitizersforsolarfuelproduction
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