"DESIGN ISSUES CONCERNING COMPOSITE MATERIAL FUEL-ELEMENT JACKETS BASED ON SILICIUM CARBIDE WITHIH A MATTER OF SAFETY CONCEPT OF WATER- COOLED

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1 "DESIGN ISSUES CONCERNING COMPOSITE MATERIAL FUEL-ELEMENT JACKETS BASED ON SILICIUM CARBIDE WITHIH A MATTER OF SAFETY CONCEPT OF WATER- COOLED REACTOR UNDER ACCIDENTS" *V. N. Bezumov, *V. V. Novikov, *A. A. Kabanov, *R. G. Zakharov, **Y. V. Pimenov *OJSC "Vysokotechnologitchesky Nauchno-issledovatelsky Institut Neorganitcheskikh materialov named after academician A.A. Botchvar" (OJSC "VNIINM"), Moscow,**OJSC "TVEL", Moscow.

2 General Information Properties of zirconium alloys fuel-element jackets are one of the most important factors, influencing on the safety of the WWER type reactor. When the temperature increases in the range between 600 and 900 С zirconium alloy looses its strength quickly due to ά-β transformation. When the temperature of about 1200 С is reached the zirconium-steam reaction starts and that reaction produces hydrogen which subsequently will explode. Therefore, the upcoming trend is substitution of zirconium alloy fuel-element jackets for silicium carbide (SiC) fuel-element jackets Physical, thermal and mechanical characteristics of silicium carbide in comparison with characteristics of zirconium alloy with 1% of niobium. Characteristics SiC Zr-1%Nb Density, g/cm Melting point, С Thermal conductivity coefficient, cal/(cm sec С) (50 С) Specific heat capacitance, cal/(g С) ( С) Temperature coefficient of linear expansion (TCLE), K -1 ( С) 5, , Microhardness (H),kgf/mm Tensile strength (σв), MPa Thermal-neutron capture cross-section, barn/atom Elasticity modulus (20 С), GPa

3 General Information SiC jackets have thermal-neutron capture cross-section 25% less than zirconium alloys' cross-section. SiC does not react with water at high temperatures. In practice, silicium carbide's degree of corrosion is next lower than zirconium. Thus using of silicium carbide fuel-element jackets in WWER type reactors will provide significant improvement of modern NPPs' radiological safety.. 3

4 Methods used in work for producing silicium carbide fuel-element jackets It is conducted comparative study of physical/chemical properties of pipe jackets's engineering prototype, produced using various methods: isostatic pressing and subsequent hard firing; isostatic pressing with application of silicium carbide additional layer from gas phase (CVD-process Chemical vapor deposition); silicium carbide deposition (SiC M ) on a frame (SiC fiber ) from gas phase or frame impregnation (SiC fiber ) (SiC M ) from liquid phase); silicium carbide deposition on graphite rod from gas phase. 4

5 Source raw materials, additives, activating silicium carbide agglomerating, temporary and molding binders Powder with predominant content of cubic modification particles β- SiC, in which the total amount of impurities (Hf, Ti, Sc, N, Cd, In, Sm, B), having high level of thermalneutron capture cross-section, does not exceed values of < < 0.003%, with fineness from nanoscale up to 3-5 µm Select criteria of additives, activating silicium carbide powders' agglomerating: high radiation resistance, small neutron-capture cross-section; lack of interaction (chemical or physical-chemical) of additives with silicium carbide, which leads to ceramic formulation complication due to new phase formation, and to new silicium carbide polytypes formation; hydrophobic nature; ensuring the composite material oxidation resistance and mechanical characteristics under temperatures up to 1200 C; ensuring silicium carbide composite materials with operation temperatures not less than 1300 C; ensuring obtaining of maximum close packing when a semi-finished product forming and as consequence higher density of a semi-finished product by using silicium carbide powder of various fractions. Activating additives: Al 2 O 3 Y 2 O 3 MgO Binder material: Silicium carbide-forming organic olygomers 5

6 Initial data Crystalline lattice β-sic Crystallographic properties Properties Value Crystalline lattice Cubic, a= nm Ratio of Si : C

7 Source raw materials, additives, activating silicium carbide agglomerating, temporary and molding binders Ceramic sample SiC heat treated at 1500 С 7

8 Isostatic pressing and subsequent hard firing method С Si Tubes' samples, produced using Isostatic pressing and subsequent hard firing method Microstructure of tube's surface coating, produced using Isostatic pressing and subsequent hard firing method Method σ(bending), MPa E, GPa Porosity, % Density, g/cm 3 Microhardness, HV Corrosion studies, weight loss, % Pressing Extrusion

9 Isostatic pressing method with application of silicium carbide additional layer from gas phase 1 2 Appearance of the primary ceramic semi-finished product (1) and the semi-finished product with SiC packing layer (2) Ceramic semi-finished product surface's photo with coating thickness of 100 µm Internal hardening coating's structure longitudinal chipped pot Magnification 405. External hardening coating's structure Cross section. Magnification 405. σ(bending), MPa E, GPa Porosity, % Density, g/cm 3 Microhardness, HV Corrosion studies, weight loss, %

10 Method based on silicium carbide deposition on graphite rod from gas phase. Si Surface coating photo, х 7400 Photomicrogram of the 3C-SiC layer, produced under gas phase stoichiometric composition, х 300 σ(bending), MPa E, GPa Porosity, % Density, g/cm 3 Microhardness, HV Corrosion studies, weight loss, %

11 Method using a composite material based on carbon fiber frame with silicium carbide applied on its surface Produced tube's appearance С-SiC composite microstructure after gas phase saturation (silicium carbide phase is highlighted in white color) C-SiC composite cross-sectional view (dark phase carbon fibers, white phase stoichiometric β-sic) 11

12 Comparative analysis ,2-0,4-0,8-1 -1,2-1,6-1,8 0 0,2 0, Cross-breaking strength, MPa 0-0,5-0,6-1 -1,5-1, Corrosion testing (Weight loss, %) 40 3, , , , Porosity, % 1 Isostatic pressing and subsequent hard firing method 2 Isostatic pressing method with application of silicium carbide additional layer from gas phase 3 Method based on silicium carbide deposition on graphite rod from gas phase 12

13 Fuel Fuel-element jacket sample's diagram Ø 9.1 mm Ø 7.72 mm Polycrystalline SiC, produced using the pyrolytic method (x 300) SiC fiber /SiC matrix composite (x 300) Picture 15 - SiC/SiC tripple jacket diagram 13

14 Composite material fuel-element jackets based on silicium carbide should ensure: - leaktightness of fuel elements (gas impermeability); - operation of fuel elements in active zone with a glance: - radiation form change (growth, radiation creep); - corrosion from coolant; - influence of processes inside fuel element; - mechanical interaction fuel jacket; - behavior in LOCA and RIA; - effective retention of fission products in any accidents; - possibility of installation of fuel assembly (mechanical load); - possibility of manufacture (raw materials, circulating materials, waste processing). 14

15 SiC f /SiC m ceramic composite's required values Composite composition Parameter Density > 3.0 g/cm 3 Porosity < 3 % Required value 1) β-sic external indistinguishable layer 2) Internal layer β-sic fiber, interface layer, β-sic matrix 3) β-sic external indistinguishable layer Heat conductivity > 40 W/(m K) Tensile strength at ⁰С Easticity modulus at ⁰С Irradiation stability at 1000 С Content of elements with a large thermal-neutron capture cross-section > 300 MPa GPa > 10 dpa < 0.003% High chemical and thermal resistance < 1200 С 15

16 Conclusion Conclusion 1.Physical-chemical studies of tubes' samples produced according to various methods are conducted/ It is found that: tube jackets' samples with SiC coating applied from gas phase on the external and internal tube's surface, have the best corrosion resistance properties. 2 The analysis of the provided research results and the published sources confirms that the ceramic composite fuel-element jacket's future-proof design should include: β-sic external indistinguishable layer; internal layer β-sic fiber, interface layer, β-sic matrix; β-sic external indistinguishable layer. 3 It is defined the requirements applied to a finished article. Focus area in : Radiation-resistant ceramic materials' manufacturing process improvement; Manufacturing of composite long length pipes based on silicium carbide; 16

17 THANK YOU FOR YOUR ATTENTION Bezumov V.N. 17

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