10_Nuclear Graphite Components
10_Nuclear Graphite Components
• Protection of fuel
§ Compacts within the prismatic fuel elements
§ Pebbles within the core center
Density 1.7 - 1.9 g/cm3 Neutron efficiency, Structural integrity, Thermal efficiency
From ASTM D7219 : Standard Specification for Isotropic and • CTE (Coefficient of Thermal Expansion)
Near-isotropic Nuclear Graphites § Indicates isotropy and needed for gas gap analysis
• Density
• Purity
§ Higher = Stronger
§ Requires additional heat treatment
§ Lower = Better irradiation performance
• Dimensional changes
• Conductivity
§ Affects structural integrity
§ Nearly a 70% drop almost immediately after reactor
startup § If internal stress exceeds inherent strength of 5
graphite = cracks
Graphite “Burning” and dust “Explosions”
• Graphite can not burn – just physically can not sustain self oxidation
§ Fire needs Heat, fuel, and oxygen
§ Fuel (carbon) is restricted to only the edges. Oxygen is restricted by the crystallography.
§ Self-sustained oxidation (better definition than simple burning) can not be sustained.
Graphite
Acheson
CornGraphite
(Maize) Dust
7
Graphite Oxidation and “Burning”
• Graphite can and does oxidize – high temperatures
• Needs continuous oxygen and temperatures above
200°C – 300°C
§ Temperatures > 400°C needed for more rapid acute
oxidation (accidents)
§ Temperatures < 400°C can still oxidize but at very slow
rates (chronic oxidation)
• Oxidation still restricted to edges of crystallites with
porosity dictating oxygen transport into component
8 700 C
∆L/L [%] 500 C
6
300 C
4
2
0
-2
-4
0 5 10 15 20 25
dose, dpa
140 Non-irradiated
120
Ti=950, 6 dpa
Conductivity, W/m-K
100
80
60
40
20
0
0 100 200 300 400 500 600 700 800 900 1000
Temperature, C
1.4
300 C
1.3 • Overall, graphite CTE is low
500 C
compared to other structural
1.2 700 C
materials, e.g., metals
1.1
900 C § Implies excellent shock
1100 C
resistance
1 • Along with dimensional
changes, must be accounted
CTE/CTEo
0.9
for in the design
0.8 • Initial increase with dose as
manufacturing-related
0.7
microcracks are closed
0.6
§ Limited dependence on
Turnaround
0.5 • Subsequent reduction of
CTE at increased dose rate
0.4
0 5 10 15 20 25
dose, dpa
13
Irradiation Creep – Life Limiting Mechanism
14
ASME Code for Graphite Core Components
16
ASME Code for Graphite Core Components
Dose
Most
Conservative
Dose Level
∆V/V
More Risk but
some Rx do
operate here
Highest Risk
18
Operational Lifetime Considerations
Pebble Bed Prismatic
• Highest component lifetime dose • Lower component lifetime dose
§ What is expected lifetime dose? § Still need expected lifetime dose
§ Turnaround dose? After Turnaround? • Periodic shutdown
• Continuous operation § Much easier to inspect components
§ Inspection of components is problematic § Components in high-fluence regions can be
replaced or shuffled
§ Component replacement is difficult
• Finer grain grades required
• Components in high-fluence regions
§ Webbing between fuel/coolant channels
should be designed for replacement requires smaller grain size
§ Will require shutdown and de-fueling of § Slightly lower Turnaround dose
pebbles from core § Higher oxidation rate
• Large grain grades are possible • Still requires irradiated test data to
§ Higher Turnaround dose than fine grain validate operational models
§ Lower oxidation rates than fine grain § Currently only limited irradiation data for
• Irradiated test data validating models newer nuclear grades
will be required § Design life to be appropriately adjusted
as data become available
§ Currently only limited irradiation data for
newer nuclear grades
§ Design life to be appropriately adjusted
as data become available.
• Dust?
19
Conclusions
• All graphite nuclear grades are proprietary
§ Graphite is porous – by design
§ Compressive applications only (σc >> σt)
• Irradiation behavior is required for design
§ Dimensional change and creep is life limiting mechanism
§ Strength/internal stress is dose dependent
• Degradation/Oxidation of graphite
§ Graphite does not burn (but it does oxidize at high temperatures)
§ Oxidation limited to 10% mass loss. Then replace the component
• In-service Inspection
§ Easy for Prismatic designs. More difficult for Pebble designs
• Visual and physical inspection of accessible areas during refueling or maintenance
• In-situ Measurements (primarily interest to pebble reactors)
• ASME Code
§ Probabilistic design calculations
• Some amount of failure (i.e., a crack) is nearly certain over time
• Operational considerations – Pebble and prismatic
§ What is the lifetime dose of component?
• Is this after Turnaround dose?
§ Can core be inspected? How are components to be replaced if required?
§ Oxidation rates of graphite (small versus larger grain grade) 20
Suggested Reading
• Manufacturing
§ ASTM D7219, Standard Specification for Isotropic and Near-isotropic Nuclear Graphites.
§ Kelly, B. T., 1981, Physics of Graphite, Applied Sciences Publishers LTD, London U.K. and New Jersey USA, 1981.
§ R.E. Nightingale, 1962, Nuclear Graphite, Academic Press, ISBN: 978-1-4832-2854-9.
• Oxidation
§ International Atomic Energy Agency, 1992, INSAG 7, “The Chernobyl Accident: Updating of INSAG 1, International
Nuclear Safety Advisory Group, IAEA, Safety Series No. 75 INSAG 7, (ISBN: 9201046928), 1992.
§ Cristian I. Contescu, Robert W Mee, Yoonjo (Jo Jo) Lee, Jose D Arregui-Mena, Nidia C Gallego, Timothy D Burchell,
Joshua J Kane, William E Windes, “Beyond the Classical Kinetic Model for Chronic Graphite Oxidation by Moisture in
High Temperature Gas-Cooled Reactors”, Carbon, 127 (2018) 158-169.
§ Joshua J. Kane, Cristian I. Contescu, Rebecca E. Smith, Gerhard Strydom, and William E. Windes, “Understanding
the Reaction of Nuclear Graphite with Molecular Oxygen: Kinetics, Transport, and Structural Evolution", Journal of
Nuclear Materials, Volume 493, September 2017, Pages 343–367.
§ Windes, W., G. Strydom, R. Smith, and J. Kane, 2014, “Role of Nuclear Grade Graphite in Controlling Oxidation in
Modular HTGRs,” INL/EXT-14-31720, Rev. 0, November 2014.
§ Laine, N. R., Vastola, F. J., and Walker Jr., P.L., 1963, “The importance of active surface area in the carbon oxygen
reaction,” J Phys Chem, Vol. 67, pp. 2030–2034.
§ Walker Jr., P. L., Rusinko, F., and Austin, L. G., 1958, “Gas Reactions of Carbon,” Advances in Catalysis, Vol. 11, pp.
133–221.
§ Bradbury, D., Wickham, A., Graphite Decommissioning: Options for graphite treatment, recycling, or disposal,
including a discussion of safety related issues, EPRI Technical Report 1013091, March 2006.
§ Walker Jr., P. L., 1990, “Carbon: An old but new material revisited,” Carbon, Vol. 28, pp. 261–279.
§ Walker Jr., P. L., Taylor, T. L., and Ranish, J. M., 1991, “An update on the graphite-oxygen reaction,” Carbon, Vol. 29,
pp. 411–421.
21
Suggested Reading (cont.)
• Dust
§ Bradbury, D., Wickham, A., Graphite Decommissioning: Options for graphite treatment, recycling, or disposal, including a
discussion of safety related issues, EPRI Technical Report 1013091, March 2006.
§ P. W. Humrickhouse, HTGR Dust Safety Issues and Needs for Research and Development, INL/EXT-11-21097, June 2011.
§ A. Bentaib & J. Vendel, ITER Project: Dust Mobilization and Explosion, Introductory Meeting on the Planned PSI Research
Project on HTR Graphite Dust Issues, PSI, Villigen, 26-27 November 2009.
• Irradiation Effects
§ J. H. W. Simmons, Radiation Damage in Graphite: International Series of Monographs in Nuclear Energy, Elsevier publications,
2013, ISBN: 1483186490
§ Kelly, B. T., 1981, Physics of Graphite, Applied Sciences Publishers LTD, London U.K. and New Jersey, USA, 1981.
§ R.E. Nightingale, 1962, Nuclear Graphite, Academic Press, ISBN: 978-1-4832-2854-9.
§ Idaho National Laboratory, NGNP High Temperature Materials White Paper, INL/EXT-09-17187 R1, August 2012.
§ N. C. Gallego and T. D. Burchell, A Review of Stored Energy Release of Irradiated Graphite, ORNL/TM-2011/378, September
2011.
23
Source-dependence on graphite properties
• There is no generic “nuclear grade” graphite that can be made by all vendors
§ All nuclear graphite grades are proprietary. How they are made is secret to the
individual vendor
• Completely different than metals. There is no fabrication information available for any grade.
§ Graphite users must select the grades that match their specific requirements
§ And no, vendors wont give up their recipes. There is no customer base asking for it
• As discussed in fabrication slide the unique graphite manufacturing processes
dictate the graphite behavior – both unirradiated and irradiated
§ Main fabrication parameters are:
• coke source: petroleum or coal-based coke source
• grain size: coke particles (grains) range in size from 1800 μm to 15 μm
• fabrication method: iso-static molded, vibration molded, or extruded fabrication
• Grain-binder ratio: the amount of carbonaceous binder added to the grain particles
§ Modifying these parameters can dramatically alter the unirradiated material
properties and irradiation performance
Parameter Unirradiated Behavior Irradiated Behavior
Increased Density Increased strength and modulus A general decrease in Turnaround dose
Higher fracture strength • Shorter component lifetime
Isostatic fabrication Higher isotropy (than extruded) Better, more predictable, irradiation
Higher cost material performance.
Smaller grain size More uniform, finer microstructure Super-fine grades may have lower Turnaround
• Especially when isostatic molded dose
Higher oxidation rate than larger grained 24
Minimal effects to graphite from irradiation
• No significant changes occur in:
§ Neutron moderation – Carbon atoms not removed
§ Specific heat capacity – Crystal structure remains intact
§ Oxidation rate - Minimal changes if any due to densification during irradiation.
§ Molten salt interaction – Graphite behavior (unirr. and irr.) similar to gas-cooled
• Physical damage possible from salt intrusion into pores in graphite components
§ Emissivity:
• Unaffected by irradiation but oxidation
may leave impurity oxides on outer
surface.
Rate of stored energy release, ds/dT, J/g·°C
Ti = 150°C
• Minimal Wigner energy release if
components irradiated above 300°C.
§ Annealing of point defects in graphite is
Ti = 200°C
rapid above 250°C
§ Minimal accumulation of stored energy
Ti = 250°C • Need high dose & low Ti
§ Low dose/low Ti components have
reduced risk 25
Graphite Component Failure
• What do we mean by structural integrity
§ U.K.’s AGR bricks – Now past Turnaround dose
• Example of graphite component failure.
§ Both axial as well as radial cracking in components
• Lifetime is completely dependent upon graphite
core now
§ Not fuel design/performance, metallic internals, or
secondary systems
360
26
Graphite Component Failure
• CAUTION!
§ U.K. AGR uses CO2 for coolant
§ Radiolytic oxidation exacerbates all strength changes
• Inert gas cooled designs will be more robust
§ Component strength, internal stresses, and POF will
be much different than CO2 cooled AGRs
360
27
Component inspection (NDE techniques)
• Visual inspection, Eddy current, Ultrasonic, and X-ray inspection is possible
§ Thick graphite components are difficult to inspect
• Flaw size resolution (i.e., cracks) are difficult to resolve in thick components
§ Visual, Eddy current, and small sample trepanning are current methods used
• U.K.’s AGR inspection program
• No good technique exists. Destructive analysis (trepanning) yields most information
Eddy Currents Induction Coil
AC Magnetic Field
Sg(P) , Rtf
POFcomponent