Joint ICTP-IAEA International School on Nuclear Waste Vitrification 23 - 27 September 2019, Trieste, Italy Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 1 25-Sept-19
Laboratory Introduction Subatomic Physics and Associated Technologies (SUBATECH) Laboratory – High energy universe – Nuclear and environment (Radiochemistry Group) – Nuclear and Health (Radiochemistry Group) Under the Guidance of Prof. Abdesselam ABDELOUAS Dr. Tomo SUZUKI-MURESAN Ms. Haohan ZHANG Head of Radiochemistry Group Associate Professor, IMT Atlantique Ph.D. fellow (SUBATECH Laboratory) (SUBATECH Laboratory) (SUBATECH Laboratory) Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 2 25-Sept-19
Subatech laboratory & IMT Atlantique (Nantes) Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 3 25-Sept-19
Outlines • Background • Objectives • Literature review • Materials and Methods • Characterization Techniques • Results and Discussion • Conclusion Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 4 25-Sept-19
Background • French policy for Spent Nuclear Fuel – recycling/reprocessing • Immobilization of fission products and minor actinides in named R7T7 • High level nuclear waste glass in – Current project at Meuse/Haute-Marne centre (Cigéo project- ANDRA) Picture- ANDRA.fr Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 5 25-Sept-19
Background (cont.) to of waste package waste package prevent the production, entrance of creates internal groundwater fluid pressure to waste Glass alteration package (glass+container) Picture- Retrieval Test of HLW package in the Cigeo Project, Andra (IGD-TP Technical Forum, Berlin- 2018) Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 6 25-Sept-19
Literature review: evolution of glass under vapor condition • Number of water layers adsorbed on the glass surface W.L.Ebert et al., The Sorption of Water on Obsidian and a Nuclear Waste Glass (1991) Figure- Chemical durability of Glasses (Abdelouas et al.- 2019) Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 7 25-Sept-19
Literature review: evolution of glass under vapor condition (cont.) • The hydrated layer thickness depends on , , and also . • Hydration rate increases with the RH and Temperature increases Figures- Vapor hydration of SON68 glass from 90 ° C to 200 ° C: A kinetic study and corrosion products investigation (J. Neeway et al.- 2012) Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 8 25-Sept-19
Objectives I. Investigation of hydration kinetics in Vapor phase of French surrogate SON68 glass and ISG (International Simple Glass). • at two temperatures (90 ° C and 125 ° C) • at two RH- Relative Humidities (95% and 99%) II. In Autoclave and Climate Test Chamber (which is not widely used). Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 9 25-Sept-19
Materials & Methods Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 10 25-Sept-19
Materials Oxides ISG (wt %) SON68 (wt %) SiO 2 56.2 45.85 B 2 O 3 17.3 14.02 Na 2 O 12.2 9.86 SON68 glass Al 2 O 3 6.1 4.91 CaO 5.0 4.04 ZrO 2 3.3 2.65 Fe 2 O 3 - 2.91 Li 2 O - 1.98 MoO 3 - 1.70 Others - 12.08 ISG glass Glass composition- ISG (Chaoua et al.- 2014), SON68 (K M Davis et al.- 1996) Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 11 25-Sept-19
Autoclave (AC) Climate Test Chamber (CC) Autoclave figure- Chemical durability of Glasses (Abdelouas et al.- 2019) Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 12 25-Sept-19
Experimental conditions Time of Temperature ( ° C) Glass RH (%) hydration (days) 125 112 99 90 112 SON68 47 95 90 37 Autoclave (AC) 125 112 99 90 112 ISG 47 95 90 37 44 SON68 37 Climate Test 95 90 Chamber (CC) 44 ISG 37 Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 13 25-Sept-19
Characterization Techniques Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 14 25-Sept-19
Characterization Techniques SEM • Determination of hydrated thickness FTIR • To follow the glass hydration • To determine the physical hydration thickness ICP-MS • Determination of chemical hydration thickness Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 15 25-Sept-19
Sample preparation for SEM analysis SEM- Scanning Electron Microscopy Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 16 25-Sept-19
FTIR Spectroscopy SON68_125 ° C-99%RH_AC 2.0000 OH stretching silica matrix 1.8000 mode in the OH stretching bound water 1.6000 mode in the free silanol groups water molecule 0 day 1.4000 Absorbance (a.u.) 7 days 1.2000 14 days OH stretching 1.0000 mode in bound 29 days silanol groups 0.8000 42 days OH stretching mode in SiOH 56 days 0.6000 77 days 0.4000 91 days 0.2000 112 days 0.0000 2500 2700 2900 3100 3300 3500 3700 3900 4100 Wavenumber (cm -1 ) Deconvolution - five Gaussian using Origin 8.0 software (OriginLab) H.Tomozawa, M.Tomozawa. Diffusion of water into a borosilicate glass Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 17 25-Sept-19
NL calculation Boron Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 18 25-Sept-19
Results & Discussion Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 19 25-Sept-19
Effect of relative humidity at 90 ° C 0.12 ISG_90 ° C 0.1 Absorbance (a.u.) 90 ° C ISG glass 0.08 2.6 × 10 -4 per day 95% RH 0.06 9.8 × 10 -4 per day 99% RH 0.04 Factor 3.8 0.02 0 0 20 40 60 80 100 120 Hydration time (days) 95% RH 99% RH • Hydration rate increases with the RH increases • The results consistent with the literature @ @ literature (Abdelouas et al.- 2013) (Neeway et al.- 2012) (Chaou et al.- 2017) Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 20 25-Sept-19
Effect of temperature at 99% RH 0.18 SON68_99%RH 0.16 0.14 Absorbance (a.u.) 99% RH SON68 glass 0.12 0.1 4.3 × 10 -4 per day 90 ° C 0.08 45.0 × 10 -4 per day 125 ° C 0.06 0.04 Factor 10.5 0.02 0 0 20 40 60 80 100 120 Hydration time (days) 90 ° C 125 ° C • Hydration rate increases with the Temperature increases • The results consistent with the literature @ @ literature (Abdelouas et al.- 2013) (Neeway et al.- 2012) (Chaou et al.- 2017) Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 21 25-Sept-19
Effect of Glass Composition SON68 glass ISG glass 45.0 × 10 -4 per day 12.0 × 10 -4 per day At 125 ° C-99%RH 4.3 × 10 -4 per day 9.8 × 10 -4 per day At 90 ° C-99%RH • The glass composition also affect the hydration rate Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 22 25-Sept-19
Physical & Chemical Thicknesses 1.6 SON68_99%RH 1.4 • The physical thicknesses (FTIR) 1.2 shows the maximum hydration. Thickness (µm) 1 • The difference between physical 0.8 (FTIR) and chemical (NL) thicknesses 0.6 is maybe boron were not released 0.4 from hydrated layer to the solution. 0.2 0 0 10 20 30 40 50 60 Hydration time (days) SON68_125 ° C_NL SON68_90 ° C_NL SON68_125 ° C_FTIR SON68_90 ° C_FTIR Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 23 25-Sept-19
Comparison of Autoclave (AC) and Climate Test Chamber (CC) 0.03 0.016 SON68_90 ° C-95%RH ISG_90 ° C-95%RH 0.014 0.025 Absorbance (a.u.) 0.012 Absorbance (a.u.) 0.02 0.01 0.008 0.015 0.006 0.01 0.004 0.005 0.002 0 0 0 5 10 15 20 25 30 35 40 0 5 10 15 20 25 30 35 40 AC CC AC CC Hydration time (days) Hydration time (days) SON68 glass ISG glass 2.1 × 10 -4 per day 2.6 × 10 -4 per day Autoclave (AC) 3.3 × 10 -4 per day 7.6 × 10 -4 per day Climate test chamber (CC) Factor 1.6 3.0 • The hydration rate in the climate test chamber is higher than the autoclave Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 24 25-Sept-19
Surface analysis 90 ° C-95%RH_CC SON68 glass ISG glass 0.24 μ m 0.37 μ m SEM analysis • Hydrated layer is not clearly visible in SEM images, not sure about the hydrated layer thickness CC- Climate Test Chamber Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 25 25-Sept-19
Surface analysis (cont.) gap 99% RH_AC SON68 glass ISG glass 1.44 μ m 0.69 μ m SEM analysis 1.10 μ m 0.63 μ m FTIR • Found a gap between Resin and Glass sample AC- Autoclave Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 26 25-Sept-19
Conclusion • Correlation factor, 0.1 SiOH absorbance unit per 0.99 μ m of hydrated layer (125 ° C-99%RH) 0.1 SiOH absorbance unit per 1.5 μ m of hydrated layer (90 ° C-99%RH) Jeet PATEL Abdelouas et al. @ Jeet PATEL J. Neeway # (for ISG_125 ° C-99%RH) (for ISG_175 ° C-98%RH) (for SON68_90 ° C-99%RH) (for SON68 glass) 0.07 0.09 0.1 0.11 • Verifying, – The hydration rate increasing with the RH and temperature increases @ Primary Investigation of the ISG Glass Vapor Hydration (Abdelouas et al.- 2013), # Ph.D. thesis, University of Nantes (J. Neeway- 2010) Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 27 25-Sept-19
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