23 - 27 September 2019, Trieste, Italy Hydration of Nuclear Waste - - PowerPoint PPT Presentation

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23 - 27 September 2019, Trieste, Italy Hydration of Nuclear Waste - - PowerPoint PPT Presentation

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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

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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

Joint ICTP-IAEA International School on Nuclear Waste Vitrification 23 - 27 September 2019, Trieste, Italy

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Subatomic Physics and Associated Technologies (SUBATECH) Laboratory – High energy universe – Nuclear and environment (Radiochemistry Group) – Nuclear and Health (Radiochemistry Group)

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Laboratory Introduction Under the Guidance of

  • Prof. Abdesselam ABDELOUAS

Head of Radiochemistry Group (SUBATECH Laboratory)

  • Dr. Tomo SUZUKI-MURESAN

Associate Professor, IMT Atlantique (SUBATECH Laboratory)

  • Ms. Haohan ZHANG

Ph.D. fellow (SUBATECH Laboratory)

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Subatech laboratory & IMT Atlantique (Nantes)

Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

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  • Background
  • Objectives
  • Literature review
  • Materials and Methods
  • Characterization Techniques
  • Results and Discussion
  • Conclusion

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Outlines

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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

  • 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)

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Background

Picture- ANDRA.fr

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Background (cont.)

Picture- Retrieval Test of HLW package in the Cigeo Project, Andra (IGD-TP Technical Forum, Berlin- 2018)

to waste package

  • f

waste package production, creates internal pressure prevent the entrance of groundwater fluid to waste package (glass+container) Glass alteration

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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

  • Number of water layers adsorbed on the glass surface

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Literature review: evolution of glass under vapor condition

Figure- Chemical durability of Glasses (Abdelouas et al.- 2019)

W.L.Ebert et al., The Sorption of Water on Obsidian and a Nuclear Waste Glass (1991)

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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

  • The hydrated layer thickness depends on

, , and also .

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Figures- Vapor hydration of SON68 glass from 90°C to 200°C: A kinetic study and corrosion products investigation (J. Neeway et al.- 2012)

Literature review: evolution of glass under vapor condition (cont.)

  • Hydration rate increases with the RH and Temperature increases
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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

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).

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Objectives

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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

Materials & Methods

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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

Materials

Oxides ISG (wt %) SON68 (wt %) SiO2 56.2 45.85 B2O3 17.3 14.02 Na2O 12.2 9.86 Al2O3 6.1 4.91 CaO 5.0 4.04 ZrO2 3.3 2.65 Fe2O3

  • 2.91

Li2O

  • 1.98

MoO3

  • 1.70

Others

  • 12.08

SON68 glass ISG glass

Glass composition- ISG (Chaoua et al.- 2014), SON68 (K M Davis et al.- 1996)

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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

Autoclave (AC)

Autoclave figure- Chemical durability of Glasses (Abdelouas et al.- 2019)

Climate Test Chamber (CC)

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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

Experimental conditions

Glass RH (%) Temperature (°C) Time of hydration (days)

Autoclave (AC) SON68 99 125 112 90 112 95 90 47 37 ISG 99 125 112 90 112 95 90 47 37 Climate Test Chamber (CC) SON68 95 90 44 37 ISG 44 37

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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

Characterization Techniques

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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
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Sample preparation for SEM analysis

SEM- Scanning Electron Microscopy

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FTIR Spectroscopy

0.0000 0.2000 0.4000 0.6000 0.8000 1.0000 1.2000 1.4000 1.6000 1.8000 2.0000 2500 2700 2900 3100 3300 3500 3700 3900 4100 Absorbance (a.u.) Wavenumber (cm-1)

SON68_125°C-99%RH_AC

0 day 7 days 14 days 29 days 42 days 56 days 77 days 91 days 112 days

Deconvolution - five Gaussian using Origin 8.0 software (OriginLab) H.Tomozawa, M.Tomozawa. Diffusion of water into a borosilicate glass

OH stretching mode in SiOH OH stretching mode in the bound water silanol groups OH stretching mode in the free water molecule OH stretching mode in bound silanol groups silica matrix

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NL calculation

Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

Boron

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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

Results & Discussion

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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 90°C ISG glass 95% RH 2.6×10-4 per day 99% RH 9.8×10-4 per day Factor 3.8

Effect of relative humidity at 90°C

  • 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) 0.02 0.04 0.06 0.08 0.1 0.12 20 40 60 80 100 120 Absorbance (a.u.) Hydration time (days)

ISG_90°C

95% RH 99% RH

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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL 99% RH SON68 glass 90°C 4.3×10-4 per day 125°C 45.0×10-4 per day Factor 10.5

Effect of temperature at 99% RH

@ literature (Abdelouas et al.- 2013) (Neeway et al.- 2012) (Chaou et al.- 2017) 0.02 0.04 0.06 0.08 0.1 0.12 0.14 0.16 0.18 20 40 60 80 100 120 Absorbance (a.u.) Hydration time (days)

SON68_99%RH

90°C 125°C

  • Hydration rate increases with the Temperature increases
  • The results consistent with the literature@
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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

SON68 glass ISG glass At 125°C-99%RH 45.0×10-4 per day 12.0×10-4 per day At 90°C-99%RH 4.3×10-4 per day 9.8×10-4 per day

Effect of Glass Composition

  • The glass composition also affect the hydration rate
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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

Physical & Chemical Thicknesses

0.2 0.4 0.6 0.8 1 1.2 1.4 1.6 10 20 30 40 50 60

Thickness (µm) Hydration time (days)

SON68_99%RH

SON68_125°C_NL SON68_90°C_NL SON68_125°C_FTIR SON68_90°C_FTIR

  • The physical thicknesses (FTIR)

shows the maximum hydration.

  • The difference between physical

(FTIR) and chemical (NL) thicknesses is maybe boron were not released from hydrated layer to the solution.

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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL SON68 glass ISG glass Autoclave (AC) 2.1×10-4 per day 2.6×10-4 per day Climate test chamber (CC) 3.3×10-4 per day 7.6×10-4 per day Factor 1.6 3.0

Comparison of Autoclave (AC) and Climate Test Chamber (CC)

0.002 0.004 0.006 0.008 0.01 0.012 0.014 0.016 5 10 15 20 25 30 35 40 Absorbance (a.u.) Hydration time (days)

SON68_90°C-95%RH

AC CC

0.005 0.01 0.015 0.02 0.025 0.03 5 10 15 20 25 30 35 40 Absorbance (a.u.) Hydration time (days)

ISG_90°C-95%RH

AC CC

  • The hydration rate in the climate test chamber is higher than the autoclave
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  • Hydrated layer is not clearly visible in SEM images, not sure about the hydrated layer thickness

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90°C-95%RH_CC SON68 glass ISG glass SEM analysis 0.24 μm 0.37 μm

Surface analysis

CC- Climate Test Chamber

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99% RH_AC SON68 glass ISG glass SEM analysis 1.44 μm 0.69 μm FTIR 1.10 μm 0.63 μm

Surface analysis (cont.)

AC- Autoclave

  • Found a gap between Resin and Glass sample

gap

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  • Correlation factor,

0.1 SiOH absorbance unit per 0.99 μm of hydrated layer (125°C-99%RH) 0.1 SiOH absorbance unit per 1.5 μm of hydrated layer (90°C-99%RH)

  • Verifying,

– The hydration rate increasing with the RH and temperature increases

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@ Primary Investigation of the ISG Glass Vapor Hydration (Abdelouas et al.- 2013), # Ph.D. thesis, University of Nantes (J. Neeway- 2010)

Conclusion

Jeet PATEL (for ISG_125°C-99%RH) Abdelouas et al. @ (for ISG_175°C-98%RH)

0.1 0.11

Jeet PATEL (for SON68_90°C-99%RH)

  • J. Neeway #

(for SON68 glass)

0.07 0.09

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Acknowledgment

Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

  • Guillaume Blain (Subatech) for FTIR

formation.

  • Nicolas Stéphant from Centre of

Micro-characterization, University of Nantes (France) for SEM analysis.

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Hydration of Nuclear Waste Glass in Vapor Phase by Jeet PATEL

  • Prof. Abdesselam ABDELOUAS
  • Dr. Tomo SUZUKI-MURESAN
  • Ms. Haohan ZHANG

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Special Thanks to

Thank you very much !

Jeet PATEL

Email: jeetpatel9409@gmail.com LinkedIn: www.linkedin.com/in/jeet-patel-b70bbbb7 Mob.: +91-9408247952 (India)