Dihydrogen H$_2$ steady state in $\alpha$-radiolysis of water adsorbed on PuO$_2$ surface
| Autor: | Jackie Vermeulen, Philippe Moisy, Nicolas Vigier, Jérémy Gaillard, Natalia Budanova, Laurent Venault, Arnaud Deroche, Olivier Lemaire, Jérôme Maurin |
|---|---|
| Přispěvatelé: | Département de recherche sur les procédés pour la mine et le recyclage du combustible (DMRC), CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), ORANO, the Orano Group, CEA- Saclay (CEA), Commissariat à l'énergie atomique et aux énergies alternatives (CEA) |
| Jazyk: | angličtina |
| Rok vydání: | 2019 |
| Předmět: |
Radiation
Hydrogen 010308 nuclear & particles physics Kinetics chemistry.chemical_element Thermal treatment 01 natural sciences 030218 nuclear medicine & medical imaging 03 medical and health sciences 0302 clinical medicine Adsorption chemistry 13. Climate action Chemical physics Specific surface area 0103 physical sciences Radiolysis [CHIM]Chemical Sciences Relative humidity Hydrogen production |
| Zdroj: | Radiation Physics and Chemistry Radiation Physics and Chemistry, 2019, 162, pp.136-145. ⟨10.1016/j.radphyschem.2018.09.022⟩ Radiation Physics and Chemistry, Elsevier, 2019, 162, pp.136-145. ⟨10.1016/j.radphyschem.2018.09.022⟩ |
| ISSN: | 0969-806X |
| DOI: | 10.1016/j.radphyschem.2018.09.022⟩ |
| Popis: | International audience; Radiolysis of water adsorbed on PuO$_2$ surface has been the subject of several studies but still remains poorly understood. The present study brings new experimental results helping to further understand the phenomena occurring at PuO$_2$ surface. Radiolysis of adsorbed water on PuO2 surface leads to the reach of a steady state in hydrogen content when relative humidity is kept constant implying an equilibrium between generation and consumption of hydrogen. The influences of specific surface area, relative humidity, PuO$_2$ dose rate and composition of the atmosphere (Ar vs air) on hydrogen generation were investigated. A significant evolution of the hydrogen generation kinetics was observed upon PuO$_2$ surface aging. This result might be related to an evolution of the surface physicochemical state induced by a long-term storage in H$_2$O/H$_2$/O$_2$ atmosphere. The surface evolution modifies the equilibrium between generation and consumption of hydrogen. Several annealing thermal treatment were necessary to retrieve H$_2$ accumulations kinetics similar to the ones obtained with the same sample as freshly prepared. This indicates an important evolution of PuO$_2$ surface and subsurface. A mechanism is described to explain the surface evolution and its effect on H$_2$ accumulation through radiolysis of adsorbed water. |
| Databáze: | OpenAIRE |
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