1. 04/03/2015 1 Stefano Corradetti ActiLab Closing Meeting ActiLab Activities at INFN Stefano Corradetti and Alberto Andrighetto SPES Target Group

2. Outline 04/03/2015 2 Stefano Corradetti - UC x synthesis (Task #1): 2013 activity - UC x thermal characterization (Task #2): 2014 activity

3. UC x synthesis 04/03/2015 3 Stefano Corradetti New equipment (purchased in Jan ‘13) - Reduce and homogenize the grain size of oxide and carbon source → selection and control of the precursors (as defined in ActiLab SC May 2012, strategy for UC X production at INFN) - Vibratory micromill and sieves purchased at UNIPD lab (grain size down to few  m) to treat small quantities of precursors

4. UC x synthesis 04/03/2015 4 Stefano Corradetti ‘Original’ UO 2 batch: ~ 20 g First milling → ~ 5 g of UO 2 Milling and sieving → UO 2 particle size control

5. UC x synthesis 04/03/2015 5 Stefano Corradetti Final particle size population Sieves below 10  m mesh also available (Nylon mesh) and tested Small amount of powder ground to < 10  m size in reasonable time < 20  m ("10-20  m") was selected as a precursor size to produce 10 pellets, sent to IPNO for off-line characterization and irradiation tests Subsequent millings to produce enough UO 2 for 10 UC x pellets

6. UC x synthesis 04/03/2015 6 Stefano Corradetti % wt. UO 2 % wt. C% wt. binderWeight (g) Diameter (mm) Thickness (mm) Density (g/cm³) 77.6020.302.100.5713.010.954.50 “Green” UO 2 + C pellets Weight (g)Diameter (mm) Thickness (mm) Density (g/cm³) Total porosity (%) Weight loss (%) Theoretical weight loss (%) 0.4712.660.864.33 Similar to SPES standard 58.9017.5716.90 UC 2 + 2C pellets after carburization (UO 2 +6C→UC 2 +2C+2CO) Thermal treatment: 2°C/min up to 1250°C (binder decomposition occurs) 8 hours at 1250 °C, then 2 °C/min up to 1350 °C (carburization) 8 hours at 1350 °C, then 1.5 °C/min up to 1730°C (carburization) 6 hours at 1730 °C Expected composition of the samples: UC 2, graphite and a minor amount of UC Pellets production → 10 UC x discs

7. UC x synthesis 04/03/2015 7 Stefano Corradetti Pellets production → 10 UC x discs H 2 O, binder decomposition CO, carburization

8. UC x synthesis 04/03/2015 8 Stefano Corradetti Pellets production → 10 UC x discs Sample before treatment Disc Weight (mg)  (g/cm 3 ) Thickness (mm) 14664.310.86 24764.360.87 34674.370.86 44664.310.86 54754.310.87 64734.380.86 74764.290.88 84734.420.85 94574.370.83 104744.220.89 Samples after treatment

9. UC x synthesis 04/03/2015 9 Stefano Corradetti Shipping of the pellets to IPNO 1)Authorization from IPNO to send the samples took 3 – 4 months 2) Shipping to Orsay (September 2013) took less than two weeks (Cost: ~ 1k€) INFN (UNIPD) →→→→ IPNO OK

10. UC x characterization 04/03/2015 10 Stefano Corradetti Original setup – INFN/LNLNewly developed setup (Padova) M. Manzolaro et al., Rev. Sci. Instr. 84 (2013) 054902. Allowing measurements for samples of smaller sizes (down to  ̴30 mm) Creation of a thermal gradient on the tested disc by means of irradiation from a heated graphite crucible Thermal conductivity

11. UC x characterization 04/03/2015 11 Stefano Corradetti Thermal conductivity Creation of thermal gradients in the disc caused by irradiation from the crucible A low temperature pyrometer (range 600 ÷ 1400 °C) is used to monitor temperature in the disc center and periphery (repeated cycles of heating) Inverse analysis → k (T) (tipically in 600 ÷ 1200 °C range) M. Manzolaro, S. Corradetti, A. Andrighetto, L. Ferrari, Rev. Sci. Instrum. 84, 054902 (2013)

12. UC x characterization 04/03/2015 12 Stefano Corradetti Thermal conductivity FEM model of the chamber – crucible – disc system  T between center and peryphery: comparison between numerical and experimental k (T) is obtained minimizing the differences between the  Ts k (T) = C 0 +C 1 *T (average T)

13. UC x characterization 04/03/2015 13 Stefano Corradetti Thermal conductivity 1)UO 2 + C + binder, UO 2 < 20  m → same material sent to IPNO (only this was tested) 2)UO 2 + C + binder, 20  m < UO 2 < 40  m 3)UO 2 + C + binder, 40  m < UO 2 < 71  m Treatment Mat. Weight (g)  (g/cm 3 ) Thickness (mm) 13.513.871.38 23.573.851.40 33.583.481.54  30 mm samples produced

14. UC x characterization 04/03/2015 14 Stefano Corradetti Thermal conductivity Temperature [°C] measurements vs. numerical data Inverse analysis gives Thermal conductivity [W/m°C] Calibration of the system with a graphite disc LNL Manzolaro 2013 UNIPD Corradetti 2014

15. UC x characterization 04/03/2015 15 Stefano Corradetti Thermal conductivity Measurements on UC x discs Temperature [°C] measurements vs. numerical data Inverse analysis gives Thermal conductivity [W/m°C]

16. UC x characterization 04/03/2015 16 Stefano Corradetti Emissivity Measurement of the thermal emissivity of a sample placed on a heated graphite crucible by means of a dual-frequency pyrometer Pyrometer (Kodial viewport in the vacuum chamber)

17. UC x characterization 04/03/2015 17 Stefano Corradetti Emissivity Pellets shipment from IPNO pelletn°mass (g)main phasemass of U (g)diameter (mm)thickness (mm) GATCHINA2991.80UC1.7113.171.03 PARRNe89430.82UC 2 0.7412.951.92 OXA1 of the 70.61UC0.707.401.87 PARRNeBP70.87UC 2 0.7912.631.53 COMP3040.68UC 2 0.628.282.51 TOTAL 4.78 4.57 Selected samples from the batch tested in March 2013 at IPNO (unirradiated) Authorization to send requested in summer 2013 Samples received at UNIPD in July 2014 IPNO →→→→ INFN (UNIPD) ~OK

18. UC x characterization 04/03/2015 18 Stefano Corradetti Emissivity SPES UC X (  30 mm) with <20  m UO 2 IPNO UC X by U 3 O 8 + C Designed to obtain UC, but result is UC 2 + minor am. C HD UC

19. UC x characterization 04/03/2015 19 Stefano Corradetti Emissivity Instability in emissivity can be related to reaction with the graphite crucible (both UC-based samples, Gatchina and OXA, were found sticked on the crucible)?

20. UC x characterization 04/03/2015 20 Stefano Corradetti Emissivity UC-based samples De Coninck, 1975

21. UC x characterization 04/03/2015 21 Stefano Corradetti Emissivity pure UC 2 -based sample De Coninck, 1976

22. UC x characterization 04/03/2015 22 Stefano Corradetti Emissivity UC x -based samples Biasetto 2010 - UC x Biasetto 2008 - graphite

23. UC x characterization 04/03/2015 23 Stefano Corradetti Conclusions Consistency of the thermal conductivity setup with the previous one verified (graphite test samples) Among the first results of ISOL-like UC x materials thermal conductivity obtained Numerical model still to be improved (non-linear behavior for high temperatures, reduction of differences between experimental and numerical leading to narrower confidence bands) Temperature spectrum to be widened to explore more realistic operating conditions Emissivity correlation to structure and phases → useful in defining parameters for thermo-electrical simulations

24. 04/03/2015 24 Stefano Corradetti Thank you for your attention