A general mechanism for gel layer formation on borosilicate glass under aqueous corrosion
| Autor: | Anamul H. Mir, Alkiviadis Gourgiotis, Amreen Jan, Sebastien N. Kerisit, E. Chauvet, Stéphane Gin, J.M. Delaye, Y. De Puydt |
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| Přispěvatelé: | Département de recherche sur les technologies pour l'enrichissement, le démantèlement et les déchets (DE2D), 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), School of Computing and Engineering, University of Huddersfield, TESCAN Analytics, Institut de Radioprotection et de Sûreté Nucléaire (IRSN), Pacific Northwest National Laboratory (PNNL), Département de recherche sur les Procédés et Matériaux pour les Environnements complexes (DPME) |
| Jazyk: | angličtina |
| Rok vydání: | 2020 |
| Předmět: |
Mineral
Materials science Silicon Borosilicate glass Aqueous corrosion chemistry.chemical_element 02 engineering and technology [CHIM.MATE]Chemical Sciences/Material chemistry 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences 0104 chemical sciences Surfaces Coatings and Films Electronic Optical and Magnetic Materials Corrosion Secondary ion mass spectrometry General Energy chemistry Chemical engineering Physical and Theoretical Chemistry 0210 nano-technology Dissolution Layer (electronics) |
| Zdroj: | Journal of Physical Chemistry C Journal of Physical Chemistry C, American Chemical Society, 2020, 124 (9), pp.5132-5144. ⟨10.1021/acs.jpcc.9b10491⟩ Journal of Physical Chemistry C, 2020, 124 (9), pp.5132-5144. ⟨10.1021/acs.jpcc.9b10491⟩ |
| ISSN: | 1932-7447 1932-7455 |
| DOI: | 10.1021/acs.jpcc.9b10491⟩ |
| Popis: | International audience; Mineral and glass dissolution is a scientific topic deeply investigated but incompletely understood and of a great interest for the geochemical and materials science communities. If the interfacial dissolution/reprecipitation mechanism seems to be applicable to most of silicate minerals, the debate remains open concerning glass. Here we studied two model glasses, a ternary borosilicate (CJ1) and the same glass doped with 4.1 mol % of Al2O3 (CJ2). The two glasses were altered at 90°C, pH 9, and in conditions far and close to saturation with respect to amorphous silica, to determine the initial and residual rates. Moreover, a specific experiment was conducted for a short duration with a solution highly enriched with 18O and 29Si isotopes to understand how passivating gels form. SEM, TEM and ToF-SIMS characterization, along with Monte Carlo simulations were used to understand the rate limiting reactions at play and infer the role of Al. We show that Al yields a slower matrix dissolution in dilute conditions. However, it slows down the formation and the maturation of the passivating gel and favors alteration by partial hydrolysis of Si and Al entities followed by in-situ reorganization/relaxation into a porous network. Unexpectedly, CJ1 experienced both interfacial dissolution/reprecipitation and partial hydrolysis followed by in situ reorganization of the silicate network during the course of a single experiment. This study offers a unified concept that can pave the way for the future development of a predictive kinetic model based on a detailed description of bond breaking and bond forming as a function of glass composition and alteration conditions. |
| Databáze: | OpenAIRE |
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