دورية أكاديمية
Confined water radiolysis in aluminosilicate nanotubes: The importance of charge separation effects
| العنوان: | Confined water radiolysis in aluminosilicate nanotubes: The importance of charge separation effects |
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| المؤلفون: | Pignie, Marie-Claire, Shcherbakov, Viacheslav, Charpentier, Thibault, Moskura, Mélanie, Carteret, Cedric, Denisov, Sergey, Mostafavi, Mehran, Thill, Antoine, Le Caer, Sophie |
| المساهمون: | Laboratoire Interdisciplinaire sur l'Organisation Nanométrique et Supramoléculaire (LIONS), Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M) (NIMBE UMR 3685), Institut Rayonnement Matière de Saclay (DRF) (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie - CNRS Chimie (INC-CNRS)-Centre National de la Recherche Scientifique (CNRS)-Institut Rayonnement Matière de Saclay (DRF) (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut de Chimie - CNRS Chimie (INC-CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie Physique (ICP), Institut de Chimie - CNRS Chimie (INC-CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Laboratoire Structure et Dynamique par Résonance Magnétique (LCF) (LSDRM), Laboratoire de Chimie Physique et Microbiologie pour les Matériaux et l'Environnement (LCPME), Institut de Chimie - CNRS Chimie (INC-CNRS)-Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), DIM RESPORE (GRANITE Project) |
| المصدر: | ISSN: 2040-3364. |
| بيانات النشر: | HAL CCSD Royal Society of Chemistry |
| سنة النشر: | 2021 |
| مصطلحات موضوعية: | [CHIM.MATE]Chemical Sciences/Material chemistry |
| الوصف: | International audience ; Imogolite nanotubes are potentially promising co-photocatalysts because they are predicted to have curvature-induced, efficient electron-hole pair separation. This prediction has however not yet been experimentally proven. Here, we investigated the behavior upon irradiation of these inorganic nanotubes as a function of their water content to understand the fate of the generated electrons and holes. Two types of aluminosilicate nanotubes were studied: one was hydrophilic on its external and internal surfaces (IMO-OH) and the other had a hydrophobic internal cavity due to Si-CH$_3$ bonds (IMO-CH$_3$), with the external surface remaining hydrophilic. Picosecond pulse radiolysis experiments demonstrated that the electrons are efficiently driven outward. For imogolite samples with very few external water molecules (around 1% of the total mass), quasi-free electrons were formed. They were able to attach to a water molecule, generating a water radical anion, which ultimately led to dihydrogen. When more external water molecules were present, solvated electrons, precursors of dihydrogen, were formed. In contrast, holes moved towards the internal surface of the tubes. They mainly led to the formation of dihydrogen and of methane in irradiated IMO-CH$_3$. The attachment of the quasi-free electron to water was a very efficient process and accounted for the high dihydrogen production at low relative humidity values. When the water content increased, 2 electron solvation dominated over attachment to water molecules. Electron solvation led to dihydrogen production, albeit to a lesser extent than quasi-free electrons. Our experiments demonstrated the spontaneous curvature-induced charge separation in these inorganic nanotubes, making them very interesting potential co-photocatalysts. |
| نوع الوثيقة: | article in journal/newspaper |
| اللغة: | English |
| العلاقة: | cea-03125779; https://cea.hal.science/cea-03125779Test; https://cea.hal.science/cea-03125779/documentTest; https://cea.hal.science/cea-03125779/file/Nanoscale_leCaer2021_V0.pdfTest |
| DOI: | 10.1039/D0NR08948F |
| الإتاحة: | https://doi.org/10.1039/D0NR08948FTest https://cea.hal.science/cea-03125779Test https://cea.hal.science/cea-03125779/documentTest https://cea.hal.science/cea-03125779/file/Nanoscale_leCaer2021_V0.pdfTest |
| حقوق: | info:eu-repo/semantics/OpenAccess |
| رقم الانضمام: | edsbas.8688293D |
| قاعدة البيانات: | BASE |
| DOI: | 10.1039/D0NR08948F |
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