CN112899682A - Preparation method of zirconium cladding protective coating - Google Patents

Preparation method of zirconium cladding protective coating Download PDF

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CN112899682A
CN112899682A CN202110076670.1A CN202110076670A CN112899682A CN 112899682 A CN112899682 A CN 112899682A CN 202110076670 A CN202110076670 A CN 202110076670A CN 112899682 A CN112899682 A CN 112899682A
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zirconium
coating
deposition
zro
film layer
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卢松涛
郭宝
洪杨
吴晓宏
李杨
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Harbin Institute of Technology
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    • 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
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    • C23C28/00—Coating for obtaining at least two superposed coatings either by methods not provided for in a single one of groups C23C2/00 - C23C26/00 or by combinations of methods provided for in subclasses C23C and C25C or C25D
    • C23C28/30—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer
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    • 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
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    • C23C14/06—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the coating material
    • C23C14/14—Metallic material, boron or silicon
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    • C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
    • C23C14/22—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the process of coating
    • C23C14/34—Sputtering
    • C23C14/35—Sputtering by application of a magnetic field, e.g. magnetron sputtering
    • 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
    • C23C16/30—Deposition of compounds, mixtures or solid solutions, e.g. borides, carbides, nitrides
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    • C23C16/405—Oxides of refractory metals or yttrium
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    • 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
    • C23C16/44—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 method of coating
    • C23C16/455—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 method of coating characterised by the method used for introducing gases into reaction chamber or for modifying gas flows in reaction chamber
    • C23C16/45523—Pulsed gas flow or change of composition over time
    • C23C16/45525—Atomic layer deposition [ALD]
    • C23C16/45555—Atomic layer deposition [ALD] applied in non-semiconductor technology
    • 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
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    • C23C28/00—Coating for obtaining at least two superposed coatings either by methods not provided for in a single one of groups C23C2/00 - C23C26/00 or by combinations of methods provided for in subclasses C23C and C25C or C25D
    • C23C28/30—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer
    • C23C28/34—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates
    • C23C28/345—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates with at least one oxide layer
    • C23C28/3455—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates with at least one oxide layer with a refractory ceramic layer, e.g. refractory metal oxide, ZrO2, rare earth oxides or a thermal barrier system comprising at least one refractory oxide layer
    • 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
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    • 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

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Abstract

The invention discloses a preparation method of a zirconium cladding protective coating, and belongs to the technical field of zirconium cladding protective coatings. The invention solves the problems that the existing Cr coating is not firmly combined with the surface of the zirconium alloy substrate, the Cr coating is not wear-resistant and the like. The invention utilizes magnetron sputtering technology to plate a Cr layer on a zirconium alloy substrate by relying on an oxidation product Cr2O3Forming a compact protective film to greatly block oxygen from diffusing to the matrix, reducing the oxidation rate of the cladding tube, and utilizing the atomic layer deposition technology to deposit on the surface of the Cr layerDeposited ZrO2Film layer, ZrO controlled by process parameters2The micro-nano structure and the phase structure on the surface of the film layer are arranged, so that the binding force between the film layer and the Cr coating is effectively improved, and the film layer is based on ZrO2Has higher density and hardness, and ZrO under normal working conditions2The film layer has the functions of fretting wear resistance and corrosion resistance, so that the Cr coating is subjected to hole sealing and is not corroded and worn with the zirconium alloy substrate, and the overall comprehensive performance of the composite coating is improved.

Description

Preparation method of zirconium cladding protective coating
Technical Field
The invention relates to a preparation method of a zirconium cladding protective coating, and belongs to the technical field of zirconium cladding protective coatings.
Background
After the fukushima nuclear leakage accident, accident-resistant fuel is highly valued by scientific researchers. The zirconium alloy cladding is a key material applied to a nuclear reactor core, is called as a '1 st safety barrier' of a nuclear reactor, and has the key points of ensuring the safety and the reliability of the nuclear reactor core in terms of stable performance and prolonged service life.
At present, the preparation of an oxidation resistant coating with high bonding strength on the surface of a zirconium alloy is one of important research directions. The technical challenges faced by zirconium cladding coatings, however, are primarily that the coating does not change the size of the fuel cladding, while meeting various performance requirements for the fuel cladding and components, such as accident tolerance of the coating with high temperature oxidation resistance, and that the coating should have some stability under corrosive, creep, and abrasive conditions during long term operation. Therefore, the preparation of the coating on the surface of the zirconium alloy cladding needs to continuously explore and optimize the preparation technology of the zirconium alloy surface coating, which has important significance for improving the safety performance of nuclear reaction.
The chromium metal is a zirconium alloy coating candidate material with great development prospect, but the chromium coating prepared by the conventional process has the defects of poor bonding force with a substrate, uneven thickness, poor film density and the like, and related structural design, coating performance, behaviors under various working conditions and change mechanisms are not deeply understood. Attention needs to be paid to research on the reaction mechanism of the coating and various medium environments, the interface stability, the optimization of the preparation process and the like, and guidance is provided for later-stage practical application. Therefore, it is necessary to provide a method for preparing the protective coating of the zirconium cladding.
Disclosure of Invention
The invention provides a preparation method of a zirconium cladding protective coating, aiming at solving the problems that a Cr coating is not firmly combined with the surface of a zirconium alloy substrate, the Cr coating is not wear-resistant and the like in the prior art.
A method for preparing a protective coating for a zirconium cladding includes the following steps:
step 1, plating a Cr coating on a zirconium alloy tube shell by utilizing a magnetron sputtering technology;
step 2, depositing ZrO on the Cr coating by utilizing an atomic layer deposition technology2And (5) film layer.
Further, the operation process of step 1 is as follows: chromium target is used as target material, argon gas is used as working gas, and the vacuum degree of the back bottom is 5X 10-4And Pa, the sputtering power is 50-200W, the sputtering pressure is 0.5-1.5Pa, and the sputtering time is 1-3 h.
Further, the size of the chromium target is
Figure BDA0002907788410000011
Furthermore, the target distance is 100-200 mm.
Further, the gas flow rate of argon gas was 20 sccm.
Further, the operation process of step 2 is: placing the Cr-coated zirconium alloy tube shell in a deposition cavity of an atomic layer deposition instrument, and pumping the deposition cavity to 4 x 10-3Torr～6×10-3Torr, then introducing carrier gas to make the pressure of the deposition cavity be 0.1 Torr-0.2 Torr, setting the temperature in the deposition cavity to be 100 ℃ to 200 ℃, and then carrying out ZrO2Periodically depositing and growing the film atomic layer, and repeatedly executing 170-300 growth and deposition periods to finish ZrO2And (5) depositing a film layer.
Furthermore, the operation process of each atomic layer deposition growth cycle is as follows: 1) injecting oxygen source into the deposition cavity of the atomic layer deposition instrument in a pulse mode, wherein the pulse time t is1Is 0.02s to 0.04 s; 2) opening the air inlet valve and the air outlet valve, purging by using nitrogen, and purging for time t2Is 30s to 60 s; 3) into a deposition chamber of an atomic layer deposition apparatusPulse-wise injecting a zirconium source for a pulse time t3Is 0.2s to 0.4 s; 4) opening the air inlet valve and the air outlet valve, purging by using nitrogen, and purging for time t430-60 s, completing a deposition growth period.
Further, the zirconium source is tetrakis (dimethylamino) zirconium, and the oxygen source is deionized water or ozone.
Further, the carrier gas is nitrogen having a purity of 99.99%.
Further, ZrO2The thickness of the film layer is 30-60 nm.
The invention has the following beneficial effects: the invention adopts the means of combining the atomic layer deposition technology and the magnetron sputtering technology to construct a novel composite coating on the surface of the zirconium alloy. Firstly, a Cr layer is plated on a zirconium alloy substrate by utilizing a magnetron sputtering technology, and the Cr layer is formed by depending on an oxidation product Cr2O3The compact protective film is formed, oxygen can be greatly prevented from being diffused to the matrix, the oxidation rate of the cladding tube is reduced, and the high-temperature steam oxidation resistance is excellent. Then depositing ZrO on the surface of the Cr layer by utilizing the atomic layer deposition technology2Film layer, ZrO controlled by process parameters2The micro-nano structure and the phase structure on the surface of the film layer are arranged, so that the binding force between the film layer and the Cr coating is effectively improved, and ZrO is realized2Has higher density and hardness, and ZrO under normal working conditions2The film layer plays roles of fretting wear resistance and corrosion resistance, the Cr coating is subjected to hole sealing, and the Cr coating and the zirconium alloy substrate are not corroded and worn, so that the purpose of playing a synergistic effect with each structure of the composite coating is achieved, and meanwhile, the film layer is compatible with the use conditions of conventional working conditions and accident working conditions, so that the overall comprehensive performance of the composite coating is improved.
Drawings
FIG. 1 is an XRD spectrum of the composite film obtained in example 1;
FIG. 2a is a photograph of a zirconium alloy vessel sample that has not been subjected to an oxidation treatment;
fig. 2b is a photograph of the zirconium alloy bulb coated with the composite film layer in example 1 after the oxidation treatment.
Detailed Description
The experimental procedures used in the following examples are conventional unless otherwise specified. The materials, reagents, methods and apparatus used, unless otherwise specified, are conventional in the art and are commercially available to those skilled in the art.
Embodiment mode 1:
(1) preparing functional metal layer Cr coating
Adopting magnetron sputtering technology, using chromium target as target material, and making backing vacuum degree be 5X 10-4And Pa, Ar gas is working gas, the sputtering power is 150W, the sputtering time is 45min, and the sputtering pressure is 0.5Pa, and a functional metal layer Cr coating is plated on the zirconium alloy tube shell, wherein the diameter of the chromium target material is 50mm, the target distance is 150mm, and the gas flow of argon is 20 sccm.
(2) Preparation of the protective layer
Placing the Cr-coated zirconium alloy tube shell in a deposition cavity of an atomic layer deposition instrument, and pumping the deposition cavity to 5 x 10-3Torr, introducing nitrogen with the purity of 99.99 percent until the pressure of a cavity is 0.15Torr and the temperature in the deposition cavity is 150 ℃, and repeatedly executing 230 atomic layer deposition growth cycles to obtain ZrO2Film layer of ZrO2The thickness of the film layer is 60nm, ZrO2The microstructure of the film surface is a discrete island distribution structure
Wherein, the operation process of each atomic layer deposition growth cycle is as follows: 1) injecting oxygen source into the deposition cavity of the atomic layer deposition instrument in a pulse mode, wherein the pulse time t is1Is 0.03 s; 2) opening the air inlet valve and the air outlet valve, purging by using nitrogen, and purging for time t2Is 40 s; 3) injecting tetra (dimethylamino) zirconium into a deposition cavity of an atomic layer deposition instrument in a pulse mode to serve as a zirconium source, wherein the pulse time t3Is 0.3 s; 4) opening the air inlet valve and the air outlet valve, purging by using nitrogen, and purging for time t4For 40s, one deposition growth cycle was completed.
In this example, an XRD spectrum of the composite film layer obtained on the surface of the zirconium alloy tube shell is shown in fig. 1, and it can be seen from fig. 1 that the positions of characteristic peaks obtained by grazing incidence XRD and normal XRD scanning are substantially the same.
In order to simulate the coolant loss accident which can occur when the emergency (earthquake and tsunami) occurs during the nuclear power operation, the zirconium alloy tube shell coated with the composite film layer on the surface and the zirconium alloy tube shell which is not processed, which are obtained in the embodiment, are oxidized by using a high-temperature high-pressure tube furnace, wherein the oxidation treatment conditions are as follows: heating to 1000 deg.C for 60min, maintaining at 1000 deg.C for 40min, and naturally cooling. Before and after oxidation, the coating is weighed by a high-precision balance respectively, and the oxidation resistance of the coating is judged qualitatively by weight increment. The photographs of the untreated zirconium alloy case sample and the zirconium alloy case coated with the composite film layer after the oxidation treatment are shown in fig. 2a and fig. 2b, respectively. As can be seen from fig. 2a and 2b, the untreated zirconium alloy tube shell has severe surface corrosion after oxidation; after the composite film layer is coated on the surface of the zirconium alloy tube shell by adopting the method, and after oxidation treatment, the surface of the composite film has no corrosion phenomenon, the composite film layer still shows good compactness, and the weight gain data of the coated zirconium alloy tube shell can be seen through oxidation, so that the coated zirconium alloy tube shell has very little weight gain, and the composite film layer has a better protection effect on the substrate zirconium alloy tube shell material.
Oxidation weight gain data:
Figure BDA0002907788410000031
Figure BDA0002907788410000041

Claims (10)

1. a preparation method of a zirconium cladding protective coating is characterized by comprising the following steps:
step 1, plating a Cr coating on a zirconium alloy tube shell by utilizing a magnetron sputtering technology;
step 2, depositing ZrO on the Cr coating by utilizing an atomic layer deposition technology2And (5) film layer.
2. The method of claim 1, wherein the protective coating is applied to the zirconium claddingCharacterized in that the operation process of the step 1 is as follows: chromium target is used as target material, argon gas is used as working gas, and the vacuum degree of the back bottom is 5X 10-4And Pa, the sputtering power is 50-200W, the sputtering pressure is 0.5-1.5Pa, and the sputtering time is 1-3 h.
3. The method of claim 1, wherein the chromium target is sized to provide a protective coating for the zirconium cladding
Figure FDA0002907788400000011
4. The method of claim 1, wherein the target distance is 100-200 mm.
5. The method of claim 1, wherein the argon gas is flowed at a rate of 20 seem.
6. The method of claim 1, wherein the step 2 comprises the steps of: placing the Cr-coated zirconium alloy tube shell in a deposition cavity of an atomic layer deposition instrument, and pumping the deposition cavity to 4 x 10-3Torr～6×10-3Torr, then introducing carrier gas to make the pressure of the deposition cavity be 0.1 Torr-0.2 Torr, setting the temperature in the deposition cavity to be 100 ℃ to 200 ℃, and then carrying out ZrO2Periodically depositing and growing the film atomic layer, and repeatedly executing 170-300 growth and deposition periods to finish ZrO2And (5) depositing a film layer.
7. The method of claim 6, wherein each atomic layer deposition growth cycle is performed by: 1) injecting oxygen source into the deposition cavity of the atomic layer deposition instrument in a pulse mode, wherein the pulse time t is1Is 0.02s to 0.04 s; 2) the air inlet valve and the air outlet valve are opened,purging with nitrogen for a time t2Is 30s to 60 s; 3) injecting a zirconium source into a deposition cavity of an atomic layer deposition instrument in a pulse mode with a pulse time t3Is 0.2s to 0.4 s; 4) opening the air inlet valve and the air outlet valve, purging by using nitrogen, and purging for time t430-60 s, completing a deposition growth period.
8. The method of claim 6, wherein the source of zirconium is tetrakis (dimethylamino) zirconium and the source of oxygen is deionized water or ozone.
9. The method of claim 6, wherein the carrier gas is nitrogen having a purity of 99.99%.
10. The method of claim 6, wherein the ZrO 2 cladding protective coating is formed by a thermal spray method2The thickness of the film layer is 30-60 nm.
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KR20130125985A (en) * 2012-05-10 2013-11-20 한국원자력연구원 Plasma spray surface coating on zirconium alloy for increasing the corrosion resistance at very high temperature
US20150063523A1 (en) * 2013-09-03 2015-03-05 Uchicago Argonne, Llc Coating of nuclear fuel cladding materials, method for coating nuclear fuel cladding materials
CN108796454A (en) * 2018-07-06 2018-11-13 中国核动力研究设计院 A kind of used by nuclear reactor zirconium cladding surface metal coating PVD preparation processes
CN110055496A (en) * 2019-04-04 2019-07-26 中国核动力研究设计院 A kind of preparation process preparing Cr coating in nuclear-used zirconium alloy substrate surface
CN110791730A (en) * 2019-12-07 2020-02-14 西北有色金属研究院 Preparation method of zirconium alloy cladding surface composite coating for nuclear fuel
CN111636082A (en) * 2020-06-16 2020-09-08 西安稀有金属材料研究院有限公司 Method for electrochemically preparing accident fault-tolerant Cr coating of nuclear fuel cladding element
CN112164479A (en) * 2020-08-21 2021-01-01 上海核工程研究设计院有限公司 High-temperature steam corrosion resistant coating for zirconium alloy cladding tube

Patent Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20040077162A (en) * 2003-02-28 2004-09-04 학교법인 한양학원 Zirconium―alloy cladding tube having excellent corrosion resistance for a nuclear fuel rod and process for the manufacture of the cladding tube
KR20130125985A (en) * 2012-05-10 2013-11-20 한국원자력연구원 Plasma spray surface coating on zirconium alloy for increasing the corrosion resistance at very high temperature
US20150063523A1 (en) * 2013-09-03 2015-03-05 Uchicago Argonne, Llc Coating of nuclear fuel cladding materials, method for coating nuclear fuel cladding materials
CN108796454A (en) * 2018-07-06 2018-11-13 中国核动力研究设计院 A kind of used by nuclear reactor zirconium cladding surface metal coating PVD preparation processes
CN110055496A (en) * 2019-04-04 2019-07-26 中国核动力研究设计院 A kind of preparation process preparing Cr coating in nuclear-used zirconium alloy substrate surface
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