Hydrogen Isotope Transport in the Graphitic Fuel Elements of Fluoride-Salt Cooled High-Temperature Reactors (FHR)
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1 Hydrogen Isotope Transport in the Graphitic Fuel Elements of Fluoride-Salt Cooled High-Temperature Reactors (FHR) Raluca O. Scarlat Nuclear Engineering, UW Madison Nuclear Engineering Colloquium University of California Berkeley 26 October 2015 HEATandMASS.ep.wisc.edu
2 Outline 1. Reflections on Year 1 as an Assistant Professor 2. Overview of FHR technology and related research at UW Madison 3. Tritium management in the FHR 4. Tritium transport in the salt-graphite system Raluca Scarlat HEATandMASS.ep.wisc.edu 2
3 Reflections on Year 1 as an Assistant Professor Raluca Scarlat HEATandMASS.ep.wisc.edu Recruiting a research group Learning a (or at least one) new field Developing courses Establishing a laboratory Writing grants Training students Envisioning the future 3
4 Raluca Scarlat HEATandMASS.ep.wisc.edu 4
5 Outline 1. Reflections on Year 1 as an Assistant Professor 2. Overview of FHR technology and related research at UW Madison 3. Tritium management in the FHR 4. Tritium transport in the salt-graphite system Raluca Scarlat HEATandMASS.ep.wisc.edu 5
6 Pebble Bed FHR Mark 1 Core Design Technical Description of the "Mark 1" Pebble-Bed Fluoride-Salt-Cooled High-Temperature Reactor (PB-FHR) Power Plant. UCBTH Raluca Scarlat HEATandMASS.ep.wisc.edu 6
7 FHRs: Fluoride-Salt Cooled High-Temperature Reactors Liquid fluoride salt coolants 2LiF - BeF2 (flibe) Coated particle fuel ( TRISO Fuel ) Embedded in a Graphite Matrix Ceramographic Examinations of Irradiated AGR-1 Fuel Compacts. Sept INL/EXT Revision 1 Raluca Scarlat HEATandMASS.ep.wisc.edu 7
8 Freezing phenomenology: phase diagram
9 Freezing phenomenology: uncertainty in salt composition F. Carotti, M. Abou Dbai, K. Ahmed, J. P. Kallas, E. Alkindi, Raluca O. Scarlat. Experimental and Modeling Studies of Over-Cooling Transients in Fluoride-Salt Cooled High- Temperature Reactors (FHR). NURETH-16: 16th International Topical Meeting on Nuclear Reactor Thermal-hydraulics. 30 Aug. 4 Sept Chicago, IL.
10 Nuclear Air-Brayton Combined Cycle (NACC) Modified GE 7FA Turbine for Co-fired NACC Base-load power: 42% efficiency (100 MWe) Gas co-firing: 66% efficiency (242 MWe) Technical Description of the "Mark 1" Pebble-Bed Fluoride-Salt-Cooled High-Temperature Reactor (PB-FHR) Power Plant. UCBTH Raluca Scarlat HEATandMASS.ep.wisc.edu 10
11 Outline 1. Overview of FHR technology 2. Tritium management in the FHR 3. Tritium transport in the salt-graphite system 4. Ongoing work Raluca Scarlat HEATandMASS.ep.wisc.edu 11
12 Tritium Source Term in FHR! The main sources of tritium production are Li-6 and Li n+ Li H He Li+ n He+ n H ! Natural Li isotopic composition: 7.5% 6 Li 92.5% 7 Li! Target 6 Li start-up concentration: 60 ppm 6 Li! Steady state 6 Li concentration: 8 ppm 6 Li! Lithium-6 is continuously created: n+ Be He He He Li+ e ! Natural Be isotopic composition: 100% 9 Be 10000$ Cross Sections for (n,α) Reactions 1000$ 100$ Cross%Sec)on%(b)% 10$ 1$ 0.1$ 0.01$ 0.001$ $ $ $ 0.001$ 0.01$ 0.1$ 1$ 10$ 100$ 1000$ 10000$ $ $ $ Energy%(eV)%
13 Tritium Source Term in FHR Tritium Production Rate (Ci/ EFPY) Estimated Tritum Production Rate in the Mk1 PB- FHR Core Effective Full Power Years g/year per GWe Ci/year per GWe PB-FHR x 10 6 PWR (average) CANDU (Darlington) x 10 6 (mol T/EFPD) FHR Tritium Emission Design Goal (Based on tritium production at steady state flibe isotopic composition, per GWe)! FHR production: (1.7)10 6 Ci/yr (176 g/yr)! If 100% released to air: 10-5 Ci/kg air (0.5x10-7 NRC limit)! Reduce by a factor of 200! PWR emissions: (0.7)10 3 Ci/yr (0.075 g/yr)! Reduce by a factor of Ohashi, Hirofumi and Sherman, Steven R. Tritium Movement and Accumulation in the NGNP System Interface and Hydrogen Plant. s.l. : Idaho National Laboratory, INL/EXT
14 Tritium Sinks and Sources in FHR Raluca Scarlat HEATandMASS.ep.wisc.edu 14
15 Gas Sparging Studies at SINAP Raluca Scarlat HEATandMASS.ep.wisc.edu 15
16 Outline 1. Overview of FHR technology 2. Tritium management in the FHR 3. Tritium transport in the salt-graphite system 4. Ongoing work Raluca Scarlat HEATandMASS.ep.wisc.edu 16
17 Perfect Sink Calculations Perfect Sink Calculations Literature Data for Tritium Saturation in Graphite Michael C. Young, Huali Wu, Raluca O. Scarlat. Characterization of Tritium Transport in the FLiBe-Graphite System, for In-Situ Tritium Absorption by the Fuel Elements of the Fluoride-Salt Cooled High-Temperature Reactor (FHR). NURETH-16: 16th International Topical Meeting on Nuclear Reactor Thermalhydraulics. 30 Aug. 4 Sept Chicago, IL. Raluca Scarlat HEATandMASS.ep.wisc.edu 17
18 The Scientific Questions! Goals:! How much tritium will be retained in an FHR fuel pebble?! How long will it take for the pebble to reach equilibrium tritium concentration?! Studies:! What is the rate-limiting step for tritium absorption into the fuel elements?! What is the mechanism of tritium transport and trapping in matrix graphite?! What are the interface mechanisms that contribute to tritium transport?! What are the effects of graphite irradiation damage?! What data from nuclear graphite is relevant?! What is the effect of salt intrusion?! What are the desorption characteristics?! What effects do salt chemistry and graphite pre-treatment have? Raluca Scarlat HEATandMASS.ep.wisc.edu 18
19 Ongoing Research Activities 1. Salt intrusion experiment 2. Contact angle measurements 3. Hydrogen absorption experiment 4. Matrix graphite characterization 5. Modeling tool for tritium transport in graphite 6. Electrochemical impedance spectroscopy Raluca Scarlat HEATandMASS.ep.wisc.edu 19
20 Background Information: MSRE! ORNL-4865: Graphite stringers (CGB) from MSRE were analyzed for tritium with depth profiling. Contains information on FP distributions and transport.! ORNL-5011: Small graphite samples were exposed to T 2 gas and analyzed.! Briggs (1972): Measured and calculated distributions of tritium in the MSRE.! Does this data lend itself to useful benchmark exercises?! If so, what assumptions about the MSRE and its operations limit application to FHR?
21 Comparison with MSRE Data Diffusion only 21
22 Comparison with MSRE Data Diffusion and Trapping Trapping Model Raluca Scarlat HEATandMASS.ep.wisc.edu 22
23 Matrix Graphite Characterization Raluca Scarlat HEATandMASS.ep.wisc.edu 23
24 Matrix Graphite Characterization Graphitization Process ( 24
25 Matrix Graphite Characterization Some Preliminary Results Goal: 1) To study mainly matrix graphite physical properties density, porosity, pore distribution, surface area, graphitization; 2) To understand the difference between Matrix graphite and nuclear graphite Graphite Characterization Property Technique IG-110 A3 Apparent Density Density (g/cc) Intruded Density 2.11 Gas Pycnometer Porosity Numerical Calculation BET(Krypton) Matlab Image Analysis Pore Distribution Mercury Porosimetry See Slide- See Slide- Surface Area BET(Krypton) Graphitization (d 002 ) X-ray Diffraction 88.40% 75.60% In-plane Crystalline Size(nm) Raman Other Techniques SEM See Slide- See Slide- Optical Microscopy See Slide- See Slide- Huali Wu huali@wisc.edu HEATandMASS.ep.wisc.edu Slide 1
26 Matrix Graphite Characterization Irradiation Effects Raluca Scarlat HEATandMASS.ep.wisc.edu 26
27 Hydrogen Absorption Experiment Huali Wu Goal: to study hydrogen behavior in flibe-graphite system (saturation-limited or diffusion-rate-limited) Constant Volume Method Diaphragm Valve Gas Reservoir Diaphragm Valve T Fittings T Fittings Absolute Pressure Gauge Differentia Pressure Gauge T Fittings Diaphragm Valve Leak Valve Diaphragm Vavlve Sample Container Heating Tape T Fittings Vacuum Gauge Insulation Gas Cylinder Vacuum Pump Graphite Sample Huali Wu huali@wisc.edu HEATandMASS.ep.wisc.edu Slide 1
28 FHR Capsule Irradiations at the MIT Reactor! Two in-core irradiations completed: 300 and 1000 hours at 700 C! Double-encapsulation with nickel inner vessel, graphite liner, titanium cold-wall! g of MSRE secondary flibe! Nuclear heating with ±3 C temperature control (He/Ne)! Separate gas flows in each containment, tritium collected Raluca Scarlat HEATandMASS.ep.wisc.edu 28
29 Electrochmical Techniques in Flibe Francesco Carotti Jenkins et al Used by: Dr.Straka et al. at UJV (Czech Republic) Problems: Never used for more than 80hrs Reaction of Ni2+ ions with boron nitrite (important at low concentrations) LaF3 difficult to machine? Expensive? Fragile? Raluca Scarlat HEATandMASS.ep.wisc.edu 29
30 Research Topic 2: Salt Infiltration into Graphite Goal: to investigate salt infiltration in graphite: penetration depth, amount, and mechanism Vertical Furnace Graphite Crucible Sample Holder Pressure Release Hole Sample (1200 grit polished & DI water ultrasonic cleaned) NG: g MG: g Huali Wu HEATandMASS.ep.wisc.edu Slide 1
31 Flibe Intrusion in Graphite Preliminary Results Electron Microprobe Results F ppmwt F vs depth Depth in microns F ppmwt detection limit mg/kg [ppm wt] Mass Spectroscopy Li (With Salt) Micrometers Matrix Graphite Characterization Raluca Scarlat HEATandMASS.ep.wisc.edu 31
32 Summary of Ongoing Tritium Transport Work in the Scarlat Group! Goals: 1. How much tritium will be retained in an FHR fuel pebble? 2. What are the dominant transport mechanisms relevant to FHR?! Ongoing work: 1. Salt intrusion experiment 2. Contact angle measurements 3. Hydrogen absorption experiment 4. Matrix graphite characterization 5. Modeling tool for tritium transport in graphite 6. Electrochemical impedance spectroscopy Raluca Scarlat HEATandMASS.ep.wisc.edu 32
33 Thank you Heat & Mass Transport Group HEATandMASS.ep.wisc.edu 33
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