Abstract

Self-healing of nuclear glass alteration gels under irradiation

Self-healing of nuclear glass alteration gels under irradiation

Pierre de LAHARPE 1, Xavier DESCHANELS 1, Sylvain PEUGET 2, Hélène ARENA 2, Mélanie TARON 2,3, Jun LIN 1, Bertrand SIBOULET 4, Jean-Marc DELAYE 5

1 Institut de Chimie Séparative de Marcoule (UMR 5257), Nanomaterials for Energy and Recycling *
2 CEA Marcoule, Active Materials and Processes *
3 Institut de Chimie Séparative de Marcoule (UMR 5257), Study of Matter in Environmental Conditions *
4 Institut de Chimie Séparative de Marcoule (UMR 5257), Mesoscopic Modelling and Theoretical Chemistry *
5 CEA Marcoule – Study of Materials in Complex Environment *
(*) site de Marcoule, 30207 Bagnols sur Cèze Cedex, FRANCE

Disposal in deep geological layers is the main course of action envisaged in France for the management of high-level nuclear waste, the chemical immobilization of radionuclides being ensured by the use of borosilicate glass. Over time and as groundwater permeates through the waste package’s protective barriers, the glass matrix is expected to undergo chemical alteration. Simplified borosilicate glass alteration in the presence of water and self-irradiation (α, β, γ) from radionuclides has been an object of research for several decades, and it was established that energy deposition via self-irradiation increases the alteration rate and formation of an altered layer [1], [2]. The observed morphology of the altered glass layer features a structure of pores up to a few nms in diameter [2], [3], the long-term role of which is still unclear [4]. The closure of such pores under certain conditions was observed as well [5], suggesting that competing processes may be at work. Concomitantly, electron and ion irradiation of mesoporous silica such as SBA-15 and MCM-41 was recently investigated, and the collapse of the pore structure was monitored using Small-Angle X-Ray Scattering (SAXS) [6], [7]. Here we propose a novel approach to the study of borosilicate glass alteration layers via the sol-gel synthesis of an appropriate mesoporous substitute, suitable for SAXS monitoring. Since the presence or absence of water is suspected to be a determining factor [5], an experimental setup is devised to provide a wet environment while irradiating the material.

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