CN110105076A - A kind of low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity and implementation method - Google Patents
A kind of low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity and implementation method Download PDFInfo
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Abstract
The present invention relates to a kind of low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity and implementation methods, belong to cladding nuclear fuels pipe preparation field.Cladding tubes structure of the invention is double-layer structure；Internal layer is SiCf/ SiC ceramic matrix composite material layer, outer layer are SiC ceramic layer, and composite layer volume fraction is the 35~45% of total volume.The present invention obtains the structure design of low crash rate according to the practical service condition of cladding tubes.There are structural undulating regions in the appropriate one dimension SiC Nano fiber of tubulose SiC fiber preform internal layer introducing, change precast body, improve smoothness of inner wall, and SiC matrix is avoided to produce along fiber inner wall, become three layers of containment structure.To obtain the SiC cladding tubes that internal layer volume fraction is 35~45% composite layers, crash rate under cladding tubes stress loading is reduced.
Description
Technical field
The present invention relates to a kind of low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity and implementation methods, belong to core combustion
Expect cladding tubes preparation field.
Background technique
Silicon carbide (SiC) material is due to having good stability at elevated temperature, Flouride-resistani acid phesphatase and mechanical behavior under high temperature etc.
Advantage, it is considered to be the ideal crash-proof fuel canning material for replacing zircaloy.And SiC ceramic is due to its brittleness, Wu Fadan
Solely it is applied to reactor as cladding tubes.Compared with SiC ceramic, SiCf/ SiC ceramic matrix composite material has better fracture toughness.It is logical
Often, the good SiC of anti-radiation performancef/ SiC ceramic matrix composite material mostly uses chemical vapor infiltration technique (CVI) to prepare.Although CVI can
To provide the β-SiC of high-purity, but its higher porosity (10%~15%) makes SiCf/ SiC ceramic matrix composite material itself is insufficient
To prevent the leakage of fission gas.Therefore, existing SiC base cladding tubes are used SiC ceramic and SiCf/ SiC ceramic matrix composite material phase
In conjunction with multi-layer structure design, to give full play to SiC ceramic and SiCf/ SiC ceramic matrix composite material respective excellent properties meet core
The requirement of reactor involucrum.
A kind of SiC base cladding tubes of three-decker are disclosed in patent US20090032178A1, wherein outer layer and internal layer
It is single-phase SiC ceramic layer, middle layer is continuous SiC fiber toughening SiC ceramic matrix composite material.In document " Deck CP, Jacobsen
GM,Sheeder J,et al.Characterization of SiC-SiC composites for accident
tolerant fuel cladding[J].Journal of Nuclear Materials,2015；466:667-81. " in report
A kind of internal layer in road is SiC ceramic layer, middle layer SiCf/ SiC ceramic matrix composite material layer, the SiC base involucrum that outer layer is SiC ceramic layer
Manage multiple dimensioned characterizing method.In document " Kim D, Lee HG, Park JY, et al.Fabrication and
measurement of hoop strength of SiC triplex tube for nuclear fuel cladding
It is disclosed in applications [J] .Journal of Nuclear Materials, 2015,458:29-36. " three layers a kind of
The preparation method of SiC base cladding tubes deposits one layer of SiC ceramic layer in graphite pipe surface first, then weaves in surface ceramii layer
One layer of SiC fiber is simultaneously densified, and SiC is obtainedf/ SiC ceramic matrix composite material layer finally deposits one layer in composite material layer surface
SiC ceramic layer.
The three-decker SiC base cladding tubes of above-mentioned preparation mostly use greatly layer-by-layer preparation process, since SiC fiber itself has
Biggish rigidity, so in the weaving process, SiC fiber can not be bonded die surface or SiC ceramic layer surface completely, so that in advance
There are some structural undulating regions in body processed, these regions can not densify completely in CVI process, inevitably make
Occurs the problems such as hole between layers, to reduce the thermal conductivity of cladding tubes entirety.At the same time, above-mentioned multilayer SiC base
Cladding tubes contain single-phase SiC ceramic layer, but due to the service condition of the property of ceramic material and reactor core, as long as comprising
The design of single-phase SiC ceramic layer just has a possibility that certain stress induces failure.
And cladding tube wall thickness is that key design parameter directly affects its global failure probability, considers that practical service condition passes through
Finite element simulation calculation can obtain, and internal layer is that volume fraction is 35~45%SiCf/ SiC ceramic matrix composite material layer, outer layer are volume fraction
The double-deck containment structure for 55~65%SiC ceramic layer is the lower SiC involucrum design of current presurized water reactor crash rate.And if will
SiCf/ SiC ceramic matrix composite material need to solve following problems as endothecium structure: one, can not be densified and be drawn by precursor structure region
The excessive problem of the cladding tubes inside surface roughness risen, it is whole that excessive inside surface roughness not can guarantee processed rear cladding tubes
The integrality of structure, to increase cladding tubes failure probability；Two, it needs to avoid SiC matrix along fiber inner wall over-deposit, become
For three layers of containment structure.In addition, the hole between its precast body fibre bundle is larger, CVI technique is difficult to densify it, sternly
Internal layer SiC is affected againfThe thermal conductivity of/SiC ceramic matrix composite material, and the higher inner layer composite material layer of thermal conductivity can greatly drop
The global failure rate of low cladding tubes.Therefore how to realize that internal layer is the high heat conductance SiC that volume fraction is 35~45%f/ SiC is multiple
Condensation material layer is the key that reduce cladding tubes crash rate.
Summary of the invention
The purpose of the present invention is to solve existing three layers of SiC base cladding tubes thermal conductivities it is low, global failure rate is high the problems such as,
The present invention proposes a kind of low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity and implementation method, is received by introducing appropriate SiC
Rice noodles change precursor structure, realize that internal layer be highly thermally conductive SiCf/ SiC ceramic matrix composite material layer (volume fraction is 35~45%)
The preparation of cladding tubes, to reduce its failure probability.
The purpose of the present invention is what is be achieved through the following technical solutions.
A kind of low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity is double-layer structure；Internal layer is SiCf/ SiC is compound
Material layer, outer layer are SiC ceramic layer, and composite layer volume fraction is the 35~45% of total volume.
A kind of implementation method of the low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity, the specific steps are as follows:
The preparation of step 1, SiC fiber preform: SiC nanowire is introduced in die surface, forms layer of nanomaterial；Then
One layer of continuous SiC fiber is woven outside the layer of nanomaterial forms SiC fiber preform；
The cleaning of step 2, SiC fiber preform: SiC fiber preform is cleaned by ultrasonic and is dried；
The preparation of step 3, interface: boundary layer is introduced in SiC fiber preform using chemical vapour deposition technique；The boundary
Surface layer is the mixed layer of pyrolytic carbon PyC layers or pyrolytic carbon and SiC；
Step 4, using chemical vapor infiltration technique, to step 3, treated that SiC fiber preform carries out at densification
Reason, obtains the SiC base cladding tubes of double-layer structure after demoulding.
The SiC nanowire is that length is 300~5000nm, and diameter is 30~50nm.
The SiC nanowire layer with a thickness of 30~100 μm.
The SiC fiber preform with a thickness of 100~350 μm.
The boundary layer with a thickness of 50~200nm.
Beneficial effect
1, a kind of low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity of the invention and implementation method, according to involucrum
The practical service condition of pipe obtains the structure design of low crash rate.Appropriate one dimension SiC is introduced in tubulose SiC fiber preform internal layer
Nano wire changes in precast body there are structural undulating region, improves smoothness of inner wall, and avoid SiC matrix along fiber
Wall production, becomes three layers of containment structure.To obtain the SiC cladding tubes that internal layer volume fraction is 35~45% composite layers,
Reduce crash rate under cladding tubes stress loading.
2, simultaneously, increase effective depositional area in chemical vapor infiltration technique using one dimension SiC Nano fiber, improve
SiCf/ SiC ceramic matrix composite material layer consistency, and increase SiC matrix crystallite dimension, to improve composite layer thermal conductivity.This
The heat transfer potential of SiC base cladding tubes will be substantially improved, while reducing cladding tubes crash rate.
Detailed description of the invention
Fig. 1 is the structural schematic diagram using SiC ceramic matrix composite material cladding tubes prepared by this method；
Fig. 2 is the pictorial diagram using SiC ceramic matrix composite material cladding tubes prepared by this method；
Fig. 3 is the cross-sectional scans electromicroscopic photograph using SiC ceramic matrix composite material cladding tubes prepared by this method；
Fig. 4 is using SiC ceramic matrix composite material involucrum pipe internal surface 3D scanned picture prepared by this method.
Wherein, the modified SiC of 1- one dimension SiC Nano fiberf/ SiC ceramic matrix composite material layer；2-CVI-SiC ceramic layer.
Specific embodiment
Now in conjunction with embodiment, the invention will be further described with attached drawing.
Embodiment 1:
A kind of low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity is double-layer structure；Internal layer is SiCf/ SiC is compound
Material layer, outer layer are SiC ceramic layer, and composite layer volume fraction is the 40% of total volume.It is introduced using precursor pyrolysis and hot pressing
SiC nanowire selects the interface pyrolytic carbon (PyC), prepares SiC ceramic matrix composite material cladding tubes.
A kind of implementation method of the low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity, the specific steps are as follows:
1, liquid Polycarbosilane, ferrocene and dimethylbenzene are mixed, water-bath magnetic agitation stirs evenly；Wherein: liquid is poly-
The mass ratio of carbon silane and ferrocene is 97:3, and the mass fraction of dimethylbenzene is 8%, and bath temperature is 60 DEG C, magnetic agitation
30min；
2, die surface is cleaned up, dries, is then uniformly brushed on one layer of liquid Polycarbosilane solution；
3, the mold for having brushed liquid Polycarbosilane solution is directly placed into tube furnace, under argon atmosphere protection, 1300 DEG C
4h is cracked, growth in situ SiC nanowire, the thickness of obtained SiC nanowire layer is about 70 μm；
4, in die surface braiding one layer of continuous SiC fiber of winding with SiC nanowire, fiber layer thickness is about 150 μ
m；
5, woven SiC fiber preform is cleaned by ultrasonic and is dried；
6, using vapour deposition process is learned, one layer of pyrolytic carbon (PyC) interface is introduced in SiC fiber preform, thickness is about
150nm；
7, using vapour deposition process is learned, SiC fiber preform is densified；
8, it demoulds, obtains the SiC ceramic matrix composite material cladding tubes of double-layer structure, inner layer composite material layer is with a thickness of 40%, involucrum
Pipe density reaches 2.71g/cm3, for thermal conductivity up to 23.8W/mK, it is about 10 that maximum stress, which loads lower cladding tubes crash rate,-7。
Embodiment 2
A kind of low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity is double-layer structure；Internal layer is SiCf/ SiC is compound
Material layer, outer layer are SiC ceramic layer, and composite layer volume fraction is the 35% of total volume.SiC nanometers are introduced using coating process
Line selects the interface pyrolytic carbon (PyC), prepares SiC ceramic matrix composite material cladding tubes.
A kind of implementation method of the low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity, specific implementation method: 1. will
SiC nanowire, PVB (binder) and water are uniformly mixed by weight 1:10:100 ratio, are configured to slurry；
2. die surface is cleaned up, dries, one layer of SiC nanowire slurry is then uniformly coated；
It is dried 3. the mold for being coated SiC nanowire is put into baking oven, the thickness of obtained SiC nanowire layer is about 70
μm；
4. fiber layer thickness is about 150 μ in die surface braiding one layer of continuous SiC fiber of winding containing SiC nanowire
m；
5. woven SiC fiber preform to be cleaned by ultrasonic and be dried；
6. using conventional chemical vapor method, one layer of pyrolytic carbon (PyC) interface is introduced in SiC fiber preform, it is thick
Degree is about 150nm；
7. using conventional chemical vapor method, SiC fiber preform is densified；
8. demoulding, obtains the SiC ceramic matrix composite material cladding tubes of double-layer structure.Inner layer composite material layer is with a thickness of 40%, involucrum
Pipe density reaches 2.75g/cm3, for thermal conductivity up to 22.6W/mK, it is about 10 that maximum stress, which loads lower cladding tubes crash rate,-7。
Embodiment 3
A kind of low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity is double-layer structure；Internal layer is SiCf/ SiC is compound
Material layer, outer layer are SiC ceramic layer, and composite layer volume fraction is the 45% of total volume.SiC is introduced using electrophoretic deposition
Nano wire selects pyrolytic carbon and SiC mixed interface, prepares SiC ceramic matrix composite material cladding tubes.
A kind of implementation method of the low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity, specific implementation method: 1. will
SiC nanowire, PVB, n-butanol and water are uniformly mixed by weight 1:10:20:500 ratio, prepare electrophoretic deposition liquid；
2. die surface is cleaned up, dry, be then placed in electrophoretic deposition set, deposits 15min；
It is dried 3. the mold for having deposited SiC nanowire is put into baking oven, the thickness of obtained SiC nanowire layer is about 70
μm；
4. fiber layer thickness is about 150 μ in the heavy die surface braiding one layer of continuous SiC fiber of winding for having SiC nanowire
m；
5. woven SiC fiber preform to be cleaned by ultrasonic and be dried；
6. using conventional chemical vapor method, pyrolytic carbon is introduced in SiC fiber preform and replaces interface with SiC, it is thick
Degree is about 100nm；
7. using conventional chemical vapor method, SiC fiber preform is densified；
8. demoulding, obtains the SiC ceramic matrix composite material cladding tubes of double-layer structure, obtains the SiC ceramic matrix composite material involucrum of double-layer structure
Pipe, for inner layer composite material layer with a thickness of 40%, cladding tubes density reaches 2.73g/cm3, thermal conductivity reaches 23.3W/mK, and maximum stress adds
Carrying lower cladding tubes crash rate is about 10-7。
Above-described specific descriptions have carried out further specifically the purpose of invention, technical scheme and beneficial effects
It is bright, it should be understood that the above is only a specific embodiment of the present invention, the protection model being not intended to limit the present invention
It encloses, all within the spirits and principles of the present invention, any modification, equivalent substitution, improvement and etc. done should be included in the present invention
Protection scope within.
Claims (6)
1. a kind of low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity, it is characterised in that: be double-layer structure；Internal layer is
SiCf/ SiC ceramic matrix composite material layer, outer layer are SiC ceramic layer, and composite layer volume fraction is the 35~45% of total volume.
2. a kind of preparation method of the low crash rate SiC ceramic matrix composite material cladding tubes structure of high thermal conductivity, it is characterised in that: specific steps are such as
Under:
The preparation of step 1, SiC fiber preform: SiC nanowire is introduced in die surface, forms layer of nanomaterial；Then in institute
It states and weaves one layer of continuous SiC fiber formation SiC fiber preform outside layer of nanomaterial；
The cleaning of step 2, SiC fiber preform: SiC fiber preform is cleaned by ultrasonic and is dried；
The preparation of step 3, interface: boundary layer is introduced in SiC fiber preform using chemical vapour deposition technique；The boundary layer
For the mixed layer of PyC layers of pyrolytic carbon or PyC layers of pyrolytic carbon and SiC；
Step 4, using chemical vapor infiltration technique, to step 3, treated that SiC fiber preform carries out densification, takes off
The SiC base cladding tubes of double-layer structure are obtained after mould.
3. method as claimed in claim 2, it is characterised in that: the SiC nanowire is that length is 300~5000nm, and diameter is
30~50nm.
4. method as claimed in claim 2, it is characterised in that: the SiC nanowire layer with a thickness of 30~100 μm.
5. method as claimed in claim 2, it is characterised in that: the SiC fiber preform with a thickness of 100~350 μm.
6. method as claimed in claim 2, it is characterised in that: the boundary layer with a thickness of 50~200nm.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115611660A (en) * | 2022-10-12 | 2023-01-17 | 南京工程学院 | C/C composite material surface 1600-DEG C wind tunnel gas scouring resistant coating and preparation method and application thereof |
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| CN101019193A (en) * | 2004-06-07 | 2007-08-15 | 西屋电气有限责任公司 | Multi-layered ceramic tube for fuel containment barrier and other applications in nuclear and fossil power plants |
| CN106083116A (en) * | 2016-06-16 | 2016-11-09 | 西北工业大学 | One-step method prepares the method for SiC ceramic matrix composite material cladding tubes |
| CN106747453A (en) * | 2016-12-07 | 2017-05-31 | 中核北方核燃料元件有限公司 | A kind of SiC composite fibres wind the Pintsch process processing method of involucrum |
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101019193A (en) * | 2004-06-07 | 2007-08-15 | 西屋电气有限责任公司 | Multi-layered ceramic tube for fuel containment barrier and other applications in nuclear and fossil power plants |
| CN106083116A (en) * | 2016-06-16 | 2016-11-09 | 西北工业大学 | One-step method prepares the method for SiC ceramic matrix composite material cladding tubes |
| CN106747453A (en) * | 2016-12-07 | 2017-05-31 | 中核北方核燃料元件有限公司 | A kind of SiC composite fibres wind the Pintsch process processing method of involucrum |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115611660A (en) * | 2022-10-12 | 2023-01-17 | 南京工程学院 | C/C composite material surface 1600-DEG C wind tunnel gas scouring resistant coating and preparation method and application thereof |
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Application publication date: 20190809 |