CN117305805A - Nuclear fuel cladding modification method based on nano diamond coating - Google Patents
Nuclear fuel cladding modification method based on nano diamond coating Download PDFInfo
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- CN117305805A CN117305805A CN202311253006.5A CN202311253006A CN117305805A CN 117305805 A CN117305805 A CN 117305805A CN 202311253006 A CN202311253006 A CN 202311253006A CN 117305805 A CN117305805 A CN 117305805A
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- nuclear fuel
- zirconium
- diamond coating
- coating
- nano diamond
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- 239000011248 coating agent Substances 0.000 title claims abstract description 42
- 238000000576 coating method Methods 0.000 title claims abstract description 42
- 238000005253 cladding Methods 0.000 title claims abstract description 40
- 239000002113 nanodiamond Substances 0.000 title claims abstract description 33
- 239000003758 nuclear fuel Substances 0.000 title claims abstract description 24
- 238000002715 modification method Methods 0.000 title claims abstract description 8
- 229910001093 Zr alloy Inorganic materials 0.000 claims abstract description 22
- 238000000034 method Methods 0.000 claims abstract description 15
- 238000006243 chemical reaction Methods 0.000 claims abstract description 9
- 229910003460 diamond Inorganic materials 0.000 claims abstract description 8
- 239000010432 diamond Substances 0.000 claims abstract description 8
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 8
- 239000000498 cooling water Substances 0.000 claims abstract description 6
- 238000010438 heat treatment Methods 0.000 claims abstract description 6
- 238000000151 deposition Methods 0.000 claims abstract description 4
- 230000006911 nucleation Effects 0.000 claims abstract description 4
- 238000010899 nucleation Methods 0.000 claims abstract description 4
- 238000005229 chemical vapour deposition Methods 0.000 claims abstract description 3
- 230000008021 deposition Effects 0.000 claims abstract description 3
- 238000002474 experimental method Methods 0.000 claims description 11
- 230000000694 effects Effects 0.000 claims description 7
- 238000009835 boiling Methods 0.000 claims description 4
- 238000002360 preparation method Methods 0.000 claims description 4
- 239000000758 substrate Substances 0.000 claims description 4
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 abstract description 11
- 229910052726 zirconium Inorganic materials 0.000 abstract description 11
- 238000012546 transfer Methods 0.000 abstract description 8
- 229910045601 alloy Inorganic materials 0.000 abstract description 4
- 239000000956 alloy Substances 0.000 abstract description 4
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 abstract description 3
- 238000004880 explosion Methods 0.000 abstract description 3
- 229910052739 hydrogen Inorganic materials 0.000 abstract description 3
- 239000001257 hydrogen Substances 0.000 abstract description 3
- ATYZRBBOXUWECY-UHFFFAOYSA-N zirconium;hydrate Chemical compound O.[Zr] ATYZRBBOXUWECY-UHFFFAOYSA-N 0.000 abstract description 3
- 230000004927 fusion Effects 0.000 abstract description 2
- 239000011159 matrix material Substances 0.000 description 12
- 238000010791 quenching Methods 0.000 description 10
- 230000000171 quenching effect Effects 0.000 description 7
- 239000000446 fuel Substances 0.000 description 6
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- 239000002245 particle Substances 0.000 description 4
- 238000001878 scanning electron micrograph Methods 0.000 description 4
- 238000005728 strengthening Methods 0.000 description 4
- 238000012512 characterization method Methods 0.000 description 3
- 230000006866 deterioration Effects 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000000724 energy-dispersive X-ray spectrum Methods 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 150000002430 hydrocarbons Chemical class 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- 238000001069 Raman spectroscopy Methods 0.000 description 1
- 238000001237 Raman spectrum Methods 0.000 description 1
- 229910003481 amorphous carbon Inorganic materials 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000003574 free electron Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 1
- 238000007654 immersion Methods 0.000 description 1
- 238000012994 industrial processing Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 230000001681 protective effect Effects 0.000 description 1
- 239000012495 reaction gas Substances 0.000 description 1
- 229920006395 saturated elastomer Polymers 0.000 description 1
- 238000004381 surface treatment Methods 0.000 description 1
Classifications
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C3/00—Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
- G21C3/02—Fuel elements
- G21C3/04—Constructional details
- G21C3/06—Casings; Jackets
- G21C3/07—Casings; Jackets characterised by their material, e.g. alloys
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y40/00—Manufacture or treatment of nanostructures
-
- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/22—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the deposition of inorganic material, other than metallic material
- C23C16/26—Deposition of carbon only
- C23C16/27—Diamond only
- C23C16/271—Diamond only using hot filaments
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Physics & Mathematics (AREA)
- Metallurgy (AREA)
- Nanotechnology (AREA)
- General Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- General Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Materials Engineering (AREA)
- Mechanical Engineering (AREA)
- High Energy & Nuclear Physics (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- General Physics & Mathematics (AREA)
- Manufacturing & Machinery (AREA)
- Crystallography & Structural Chemistry (AREA)
- Plasma & Fusion (AREA)
- Chemical Vapour Deposition (AREA)
Abstract
The nuclear fuel cladding modification method based on the nano diamond coating is characterized in that the nano diamond coating is deposited outside a zirconium alloy cladding tube by chemical vapor deposition, and specifically comprises the following steps: the hot wires are connected to the electrodes at the two ends, and the surfaces of the zirconium alloy cladding tubes are subjected to chemical reaction deposition by heating the hot wires at high temperature, so that a nucleation process and a growth process are realized to form the nanoscale diamond film. The invention adopts the zirconium-based nano diamond coating to strengthen the heat transfer performance of the zirconium alloy cladding and relieve the serious accidents that the high Wen Gao alloy directly contacts cooling water to generate zirconium water reaction in the water loss accident (LOCA) and re-flooding process so as to generate hydrogen explosion or reactor core fusion.
Description
Technical Field
The invention relates to a technology in the field of reactor control, in particular to a nuclear fuel cladding modification method based on a nano diamond coating.
Background
Accident Tolerant Fuels (ATF) are new generation fuel systems developed to improve the ability of fuel elements to withstand severe accidents, comprising 1) conventional zirconium alloy fuel cladding surface treatments; 2) Developing a novel material; 3) A novel composite fuel system was developed.
Disclosure of Invention
Aiming at the problem that the existing ATF material is easy to cause the peeling of a coating film or the reduction of the protective performance after oxidation, the invention provides a nuclear fuel cladding modification method based on a nano diamond coating, which adopts the zirconium-based nano diamond coating to strengthen the heat transfer performance of a zirconium alloy cladding and relieve the serious accident that the high Wen Gao alloy directly contacts with cooling water to react in the water loss accident (LOCA) and re-flooding process so as to cause hydrogen explosion or core fusion.
The invention is realized by the following technical scheme:
the invention relates to a nuclear fuel cladding modification method based on a nano diamond coating, which comprises the following steps of: the hot wires are connected to the electrodes at the two ends, and the surfaces of the zirconium alloy cladding tubes are subjected to chemical reaction deposition by heating the hot wires at high temperature, so that a nucleation process and a growth process are realized to form the nanoscale diamond film.
The high-temperature heating means: the ambient temperature of the preparation process is maintained by a high Wen Resi, wherein the hot wire temperature is maintained at 1950-2100 degrees celsius to promote the preparation of CH in the feedstock 4 /H 2 The mixed gas is capable of undergoing a chemical reaction.
The invention relates to an application of a nuclear fuel cladding with a nano-diamond coating, which is prepared based on the method, and is used for water loss accident (LOCA) and re-flooding experiments, and the nano-diamond coating is used for isolating the direct contact of a matrix and cooling water so as to improve the boiling heat exchange effect.
The processing thickness of the nano diamond coating is about 1 mu m, and the specific thickness can be deposited with different thicknesses according to the requirements in an actual reactor so as to achieve the corresponding required effects, so that the existing industrial processing system is not influenced, and the assembly with other accessories is not influenced.
Technical effects
According to the invention, by depositing the nano diamond coating on the surface of the nuclear fuel cladding, various performances of the nuclear fuel cladding in the water loss accident re-flooding process are enhanced. Compared with the prior art, the method obviously strengthens the quenching heat exchange performance and the high-temperature steam oxidation resistance of the zirconium alloy cladding in the nuclear reactor nuclear fuel cladding, relieves the zirconium alloy cladding from directly contacting with water to generate zirconium water reaction under the condition of water loss accident re-flooding, and further avoids serious accidents such as reactor core melting and hydrogen explosion.
Drawings
FIG. 1 is a schematic illustration of a zirconium-based nano-diamond coated nuclear fuel cladding;
FIG. 2 is a SEM image of the surface and cross-section of a zirconium-based nano-diamond nuclear fuel cladding;
in the figure: a) 500 μm, b) 10 μm, c) 5 μm, d) schematic cross-sectional views;
FIG. 3 is a Raman diagram of a zirconium-based nano-diamond nuclear fuel cladding;
FIG. 4 is a comparative graph of a high temperature quenching heat exchange experiment of a zirconium-4 alloy and a zirconium-based nano-diamond nuclear fuel cladding;
FIG. 5 is a cross-sectional SEM image and EDS image of a sample after a high temperature quench heat exchange experiment;
in the figure: a) a Zr cladding cross-sectional view with NCD coating, b) a Zr cladding cross-sectional view without NCD coating, c) a Zr matrix EDS view with NCD coating, d) a Zr matrix EDS view without NCD coating;
FIG. 6 is a surface SEM image after a high temperature quench heat exchange experiment;
the left side is NCD coating, the right side is Zr alloy cladding;
FIG. 7 is a surface EDS plot after a high temperature quench heat exchange experiment;
in the figure: a) NCD surface EDS plot; b) EDS diagram of the surface of the zirconium matrix.
Detailed Description
As shown in fig. 1, this embodiment relates to a modification method of nuclear fuel cladding based on nano diamond coating by chemical vapor deposition of nano on the outside of zirconium alloy cladding tubeThe diamond coating comprises the following specific components: the hot wire is connected to the electrodes at the two ends, and the CH is promoted by heating the hot wire at high temperature 4 /H 2 The hydrocarbon reaction gas is cracked and excited to form reactive particles such as active hydrocarbon groups, free hydrogen atoms, free electrons, ion groups and the like, then the reactive particles are deposited on the surface of a matrix through a series of chemical reactions, a diamond film is formed on the surface of the matrix through nucleation and growth processes, when the concentration of the used auxiliary gas Ar is gradually increased, the growth rate of the diamond film is gradually increased, and the grain size of the diamond film is gradually changed from a micron level to a nanometer level.
The zirconium alloy cladding tube is made of zirconium-4 alloy, and comprises the following specific components: 1.3% of Sn, 0.21% of Fe, 0.11% of Cr, 0.32% of Fe+Cr, 0.1279% of O, 0.0089% of Si and the balance of Zr.
As shown in fig. 2, for the prepared nuclear fuel cladding SEM, the surface and cross-sectional morphology of the nuclear fuel cladding containing the nanodiamond coating were observed at different scales, including 500 μm (fig. 2. A), 10 μm (fig. 2. B), 5 μm (fig. 2. C) and a schematic cross-sectional view (fig. 2. D), respectively. From the surface SEM image, the extremely compact nano diamond particles are adhered to the surface of the zirconium alloy matrix, so that the zirconium alloy matrix can be ensured not to be in direct contact with cooling water to a great extent.
To verify that the coating of the present invention was truly nanodiamond in structure, raman spectra characterization was performed on the as-deposited samples, as shown in fig. 3. 1332cm in the figure -1 The vicinity is typical diamond, 1400-1550cm -1 Amorphous carbon in the vicinity of 1580cm -1 Graphite in the vicinity of 1620cm -1 The graphite-like disordered carbon is nearby, so that the fact that the surface of the coating designed by the invention is of a nano diamond structure can be verified.
As shown in fig. 4, a high-temperature quenching heat exchange experiment was performed on the heat transfer performance of the zirconium alloy nuclear fuel cladding of the nano diamond coating, and it is noted that at 0s (the dotted line in the figure), the sample starts to enter into saturated water, after complete immersion, the Zr-4 sample shows heat transfer deterioration caused by film boiling (the part of the temperature curve on the left side in the figure), while the sample containing the nano diamond coating shows no heat transfer deterioration phenomenon, indicating the heat transfer strengthening performance of the present invention.
As shown in fig. 5, SEM and EDS characterization were performed on the cross section of the sample after the high-temperature quenching heat exchange experiment of the zirconium alloy nuclear fuel cladding of the nano diamond coating, and it is notable that the NCD coating is not significantly changed, is only thinned in thickness, and no granular oxide is generated on the surface after the high-temperature quenching heat exchange experiment, as shown in fig. 5 a) and b). By comparing EDS spectra of the zirconium matrix, as shown in fig. 5 c) and d), the content of O in the zirconium matrix without the NCD coating is obviously increased, and the oxidation resistance strengthening effect of the NCD coating on the zirconium alloy matrix is proved.
As shown in fig. 6, SEM and EDS characterization were performed on the surface of the sample after the high-temperature quenching heat exchange experiment of the nano-diamond coated zirconium alloy nuclear fuel cladding, and it is notable that the surface morphology of the NCD coating is not significantly changed after the high-temperature quenching heat exchange experiment, whereas cracks appear on the surface of the zirconium alloy cladding, which proves that the NCD coating also has a certain strengthening effect on the mechanical properties of the surface of the zirconium substrate. By comparing EDS spectra of the surfaces, as shown in fig. 7 a) and b), the content of O in the surface of the zirconium substrate without the NCD coating is obviously increased, and the oxidation resistance strengthening effect of the NCD coating on the surface of the zirconium alloy substrate is proved.
Compared with the prior art, the method can effectively enhance the heat transfer characteristic of the nuclear fuel cladding, avoid the heat transfer deterioration phenomenon caused by film boiling, and effectively isolate the direct contact of the zirconium alloy matrix and cooling water by taking the nano diamond coating as a compact particle crystal coating, thereby avoiding the occurrence of zirconium water reaction. In summary, the excellent physical characteristics of the nanodiamond coating can improve the heat exchange efficiency and the safety characteristics of the fuel core.
The foregoing embodiments may be partially modified in numerous ways by those skilled in the art without departing from the principles and spirit of the invention, the scope of which is defined in the claims and not by the foregoing embodiments, and all such implementations are within the scope of the invention.
Claims (3)
1. A nuclear fuel cladding modification method based on a nano diamond coating, which is characterized in that the nano diamond coating is deposited outside a zirconium alloy cladding tube by chemical vapor deposition, specifically comprising the following steps: the hot wires are connected to the electrodes at the two ends, and the surfaces of the zirconium alloy cladding tubes are subjected to chemical reaction deposition by heating the hot wires at high temperature, so that a nucleation process and a growth process are realized to form the nanoscale diamond film.
2. The method for modifying a nuclear fuel cladding based on a nano-diamond coating according to claim 1, wherein the high-temperature heating means: the ambient temperature of the preparation process is maintained by a high Wen Resi, wherein the hot wire temperature is maintained at 1950-2100 degrees celsius to promote the preparation of CH in the feedstock 4 /H 2 The mixed gas is capable of undergoing a chemical reaction.
3. Use of the nuclear fuel cladding with nanodiamond coating prepared by the method of claim 1 or 2, for loss of water accident (LOCA) and re-flooding experiments, to isolate the substrate from direct contact with cooling water by nanodiamond coating, to improve boiling heat exchange effect.
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CN202311253006.5A CN117305805A (en) | 2023-09-27 | 2023-09-27 | Nuclear fuel cladding modification method based on nano diamond coating |
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CN202311253006.5A CN117305805A (en) | 2023-09-27 | 2023-09-27 | Nuclear fuel cladding modification method based on nano diamond coating |
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