CN110357650A - It is a kind of for connecting the connecting material and its application of carbofrax material - Google Patents
It is a kind of for connecting the connecting material and its application of carbofrax material Download PDFInfo
- Publication number
- CN110357650A CN110357650A CN201910654769.8A CN201910654769A CN110357650A CN 110357650 A CN110357650 A CN 110357650A CN 201910654769 A CN201910654769 A CN 201910654769A CN 110357650 A CN110357650 A CN 110357650A
- Authority
- CN
- China
- Prior art keywords
- rare earth
- silicon carbide
- carbon silicide
- connection
- earth carbon
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
Classifications
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/90—Carbides
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B37/00—Joining burned ceramic articles with other burned ceramic articles or other articles by heating
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2002/00—Crystal-structural characteristics
- C01P2002/70—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data
- C01P2002/72—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data by d-values or two theta-values, e.g. as X-ray diagram
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2004/00—Particle morphology
- C01P2004/01—Particle morphology depicted by an image
- C01P2004/03—Particle morphology depicted by an image obtained by SEM
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2237/00—Aspects relating to ceramic laminates or to joining of ceramic articles with other articles by heating
- C04B2237/02—Aspects relating to interlayers, e.g. used to join ceramic articles with other articles by heating
- C04B2237/04—Ceramic interlayers
- C04B2237/08—Non-oxidic interlayers
- C04B2237/083—Carbide interlayers, e.g. silicon carbide interlayers
Abstract
The invention discloses a kind of for connecting the connecting material and its application of carbofrax material.The connecting material includes rare earth carbon silicide, and the chemical formula of the rare earth carbon silicide is Re3Si2C2, Re is rare earth element.The connection method of the purposes and carbofrax material that the invention also discloses rare earth carbon silicides in connection carbofrax material, comprising: which rare earth carbon silicide is arranged at the linkage interface of carbofrax material to be connected, and 1000~1800 DEG C are heated to, so that carbofrax material to be connected is combined into one.The present invention is changed into the characteristic of liquid phase using rare earth carbon silicide high-temp and silicon carbide by eutectic reaction, silicon carbide seamless connection temperature can be effectively reduced, and the generation of liquid phase is conducive to the densification sintering of linkage interface silicon carbide, under the effect of the pressure, Partial Liquid Phase rare earth can be extruded volatilization, another part can be spread along crystal boundary to silicon carbide substrate, to realize the seamless connection of silicon carbide.
Description
Technical field
The present invention relates to the interconnection technique fields of silicon carbide ceramics and its composite material, and in particular to a kind of to utilize rare earth carbon
Silicide (Re3Si2C2) connect the connecting material of carbofrax material, and its answering in silicon carbide and its composite material articulamentum
With can be used for silicon carbide and its composite material interconnection technique field.
Background technique
For silicon carbide (Silicon carbide, SiC) as one of modern project ceramics, hardness is only second to diamond, tool
Have thermal expansion coefficient is small, thermal conductivity is high, chemical stability is good, crocking resistance is high, at high temperature still have excellent mechanical performances
With the physicochemical properties outstanding such as antioxygenic property, become structural ceramics most with prospects.Meanwhile silicon carbide also has
Low neutron activity, good radiation resistance lesion capability, artificial radioactivity can be low, becomes accident error-tolerance type nuclear fuel packet of new generation
One of candidate of shell material.But due to the intrinsic brittleness and non-deformable of silicon carbide and its composite material, cause it that can add
Work is very poor, and complex-shaped, large-sized structural member is needed to realize by interconnection technique.
The optimal connection effect of silicon carbide is exactly to realize that silicon carbide is seamlessly connected, and makes jointing in heterogeneous microstructure
It is consistent on macro property with silicon carbide substrate.Core with severe use environment (neutron irradiation, high-temperature high-pressure steam,
Lead bismuth, fluoride salt corrosion etc.) to the performance of silicon carbide jointing, more stringent requirements are proposed.Currently, silicon carbide interconnection technique has
Active metal brazing, diffusion connection, moment eutectic be connected, glass ceramics connection, reaction forming, preceramic precursor connect,
Electric field-assisted connection etc..Since strong covalent bond is difficult to break between Si-C, transition zone is not added and is directly connected to be difficult to realize, is compared
Universal connection method is transition zone to be added to realize connection between silicon carbide connects matrix, and the introducing of middle layer must just be led
Cause the presence of heat, mechanical property difference between jointing and silicon carbide substrate.
Summary of the invention
The main purpose of the present invention is to provide a kind of for connecting the connecting material of carbofrax material, to overcome existing skill
The deficiency of art.
Another object of the present invention is to provide purposes of the connecting material in connection carbofrax material.
Further object of the present invention is to provide a kind of connection method of carbofrax material.
For realization aforementioned invention purpose, the technical solution adopted by the present invention includes:
The embodiment of the invention provides a kind of for connecting the connecting material of carbofrax material, and the connecting material includes dilute
Native carbon silicide, the chemical formula of the rare earth carbon silicide are Re3Si2C2, wherein Re is rare earth element.
Further, the Re includes any one in La, Ce, Pr, Nd, Sm, Gd, Tb, Dy, Ho, Er, Tm etc. or two
Kind or more combination, but not limited to this.
The embodiment of the invention also provides purposes of the rare earth carbon silicide in connection carbofrax material, the rare earth carbon silicon
The chemical formula of compound is Re3Si2C2, wherein Re is rare earth element.
Further, the purposes includes: the setting rare earth carbon silication at the linkage interface of carbofrax material to be connected
Object, and 1000~1800 DEG C are heated to, so that the carbofrax material to be connected is combined into one.
The embodiment of the invention also provides a kind of connection methods of carbofrax material comprising: in silicon carbide to be connected
Rare earth carbon silicide is set at the linkage interface of material, and is heated to 1000~1800 DEG C, makes the silicon carbide material to be connected
Material is combined into one；The chemical formula of the rare earth carbon silicide is Re3Si2C2, wherein Re is rare earth element.
The embodiment of the invention also provides the silicon carbide connection structures as made from preceding method.
Compared with prior art, the beneficial effects of the present invention are:
1) rare earth carbon silicide (Re provided by the invention3Si2C2) coating can curved surface even complex geometric shapes silicon carbide
And its composite material surface preparation；
2) present invention utilizes rare earth carbon silicide (Re3Si2C2) coating high-temp and silicon carbide by eutectic reaction is changed into liquid
Phase can effectively reduce silicon carbide seamless connection temperature, and the generation of liquid phase can effectively improve atom active, and atom is promoted to expand
It dissipates, is conducive to the densification sintering of linkage interface silicon carbide, under the effect of the pressure, Partial Liquid Phase rare earth can be extruded volatilization,
Another part can be spread along crystal boundary to silicon carbide substrate, to realize the seamless connection of silicon carbide；
3) jointing of the present invention with connect matrix in microstructure and macro property and be consistent, form connecting elements
Integration, there is no jointings to crack the phenomenon that leading to fracture because of heat, power mismatch with matrix is connect.
Detailed description of the invention
In order to more clearly explain the embodiment of the invention or the technical proposal in the existing technology, to embodiment or will show below
There is attached drawing needed in technical description to be briefly described, it should be apparent that, the accompanying drawings in the following description is only this
The some embodiments recorded in invention, for those of ordinary skill in the art, without creative efforts,
It is also possible to obtain other drawings based on these drawings.
Fig. 1 is rare earth carbon silicide catenation principle schematic diagram in a typical embodiments of the invention.
Fig. 2 a and Fig. 2 b are rare earth carbon silicide (Re in the embodiment of the present invention 13Si2C2) coating cross sections topography scan Electronic Speculum
Photo.
Fig. 3 is connection sample object figure in the embodiment of the present invention 1.
Fig. 4 a, 4b, 4c are obtained rare earth carbon silicide (Re in the embodiment of the present invention 1,3,4 respectively3Si2C2) coating XRD
Phenogram.
Fig. 5 a and Fig. 5 b are that example interface pattern and back scattering stereoscan photograph are connected in the embodiment of the present invention 1.
Fig. 6 is connection example interface topography scan electromicroscopic photograph in the embodiment of the present invention 2.
Specific embodiment
For existing silicon carbide and its deficiency of composite material interconnection technique, inventor is studying for a long period of time and a large amount of realities
It during trampling, is found surprisingly that very much, rare earth carbon silicide (Re3Si2C2, Re=La-Nd, Sm, Gd-Tm) and it is used as a kind of Asia
Steady phase has in low-temperature stabilization, the characteristic of pyrolytic, and using the unstable phase of high temperature, the SiC that high temperature generates is on connection circle
Forming core is grown up at face, and silicon carbide substrate is sintered together, and can efficiently realize very much the seamless connection of carbofrax material, base
It is had been surprisingly found that in this, inventor is able to propose technical solution of the present invention, as follows will be to the technical solution, its implementation process
And principle etc. is further explained.
Technical principle of the invention is that the Si-C for breaking silicon carbide connection matrix surface first with rare earth element is covalent
Key forms Re-C, Re-Si (Re=La-Nd, Sm, Gd-Tm) key, with rare earth carbon silicide (Re3Si2C2, Re=La-Nd, Sm,
Gd-Tm form) is coated in silicon carbide and waits for joint face surface.Rare earth carbon silicide is in high temperature Re3Si2C2(Re=La-Nd, Sm,
Gd-Tm liquid phase) is changed by eutectic reaction with SiC, liquid phase is wrapped in silicon carbide, the effective activity for improving atom,
Promote the diffusion of atom.Under the effect of the pressure, liquid phase squeezes out volatilization, and middle layer is constantly consumed, until two silicon carbide
Face contact to be connected, high-activity carbon SiClx diffuse into one another, in interface densification sintering, to realize the seamless company of silicon carbide
It connects.
As the one aspect of technical solution of the present invention, involved in be a kind of for connecting the connection of carbofrax material
Material, the connecting material include rare earth carbon silicide, and the chemical formula of the rare earth carbon silicide is Re3Si2C2, wherein Re is
Rare earth element.
Further, the Re includes any one in La, Ce, Pr, Nd, Sm, Gd, Tb, Dy, Ho, Er, Tm etc. or two
Kind or more combination, but not limited to this.
Further, the connecting material includes rare earth carbon silicide coating, and the present invention is using rare earth element wait connect
Carbofrax material surface layer reaction in-situ generate rare earth carbon silicide (Re3Si2C2) coating.Using generated coating, pass through ceramics
Interconnection technique can realize the seamless connection of silicon carbide and its composite material.
Further, the rare earth carbon silicide coating is rare earth carbon silicide film.
Further, according to actual needs, the thickness of the rare earth carbon silicide coating can be in 50nm~2000nm range
Interior regulation.
Further, the rare earth carbon silicide selects molten-salt growth method original position plated film or PVD method deposition of rare-earth coating, Zhi Houre
Handle the rare earth carbon silicide film of synthesis.
As the one aspect of technical solution of the present invention, involved in be rare earth carbon silicide in connection carbofrax material
In purposes, the chemical formula of the rare earth carbon silicide is Re3Si2C2, wherein Re is rare earth element, preferably La, Ce, Pr,
Any one in Nd, Sm, Gd, Tb, Dy, Ho, Er, Tm etc. or two or more combinations.
In some embodiments, the purposes include: at the linkage interface of carbofrax material to be connected be arranged it is dilute
Native carbon silicide, and 1000~1800 DEG C are heated to, so that the carbofrax material to be connected is combined into one, that is, realizes seamless
Connection.
Further, the purposes includes: the setting rare earth carbon silicon at the linkage interface of carbofrax material to be connected
Compound coating.
Further, the purposes includes: the coating rare earth carbon at the linkage interface of carbofrax material to be connected
Silicide forms rare earth carbon silicide coating, preferably rare earth carbon silicide film.
Further, according to actual needs, the thickness of the rare earth carbon silicide coating can be in 50nm~2000nm range
Interior regulation.
Further, the rare earth carbon silicide selects molten-salt growth method original position plated film or PVD method deposition of rare-earth coating, Zhi Houre
Handle the rare earth carbon silicide film of synthesis.
The invention firstly uses the Si-C covalent bonds that rare earth element breaks silicon carbide connection matrix surface, form Re-C, Re-
Si (Re=La-Nd, Sm, Gd-Tm) key, with rare earth carbon silicide (Re3Si2C2, Re=La-Nd, Sm, Gd-Tm) form apply
It overlays on silicon carbide and waits for joint face surface.In high temperature Re3Si2C2(Re=La-Nd, Sm, Gd-Tm) and SiC are changed by eutectic reaction
For liquid phase, liquid phase is wrapped in silicon carbide, and the effective activity for improving atom promotes the diffusion of atom.In the effect of pressure
Under, liquid phase squeezes out volatilization, and middle layer is constantly consumed, until two silicon carbide face contacts to be connected, high-activity carbon SiClx are mutual
It mutually spreads, in interface densification sintering, to realize the seamless connection of silicon carbide.
In some embodiments, the carbofrax material includes pure thyrite, carbon/silicon carbide ceramic matrix composite wood
Material etc., but not limited to this.
Further, the carbon/silicon carbide ceramic matrix composite includes carbon fibre reinforced silicon carbide composite material, SiClx fibre
Dimension enhancing composite material of silicon carbide etc., but not limited to this.
Rare earth carbon silicide (Re of the invention3Si2C2, Re=La-Nd, Sm, Gd-Tm) and coating can be even complicated in curved surface
Geometry silicon carbide and its composite material surface preparation.
As the other side of technical solution of the present invention, a kind of connection method of carbofrax material, such as Fig. 1 are further related to
It is shown comprising: rare earth carbon silicide is set at the linkage interface of carbofrax material to be connected, and it is heated to 1000~
1800 DEG C, so that the carbofrax material to be connected is combined into one, that is, realize seamless connection；The change of the rare earth carbon silicide
Formula is Re3Si2C2, wherein Re is rare earth element, preferably in La, Ce, Pr, Nd, Sm, Gd, Tb, Dy, Ho, Er, Tm
Any one or two or more combinations.
Further, the connection method includes: the setting rare earth at the linkage interface of carbofrax material to be connected
Carbon silicide coating.
Further, the connection method include: at the linkage interface of carbofrax material to be connected coat it is dilute
Native carbon silicide forms rare earth carbon silicide coating, preferably rare earth carbon silicide film.
Further, according to actual needs, the thickness of the rare earth carbon silicide coating can be in 50nm~2000nm range
Interior regulation.
Further, the rare earth carbon silicide selects molten-salt growth method original position plated film or PVD method deposition of rare-earth coating, Zhi Houre
Handle the rare earth carbon silicide film of synthesis.
In some embodiments, the carbofrax material includes pure thyrite, carbon/silicon carbide ceramic matrix composite wood
Material etc., but not limited to this.
Further, the carbon/silicon carbide ceramic matrix composite includes carbon fibre reinforced silicon carbide composite material, SiClx fibre
Dimension enhancing composite material of silicon carbide etc., but not limited to this.
In some embodiments, the method using connecting material connection carbofrax material of the invention is unlimited, the side of heating
Formula includes hot pressed sintering connection, electric field-assisted heating connection or pressureless sintering connection etc., and preferably electric field-assisted heats connection, but
It is without being limited thereto.
The present invention utilizes rare earth carbon silicide (Re3Si2C2, Re=La-Nd, Sm, Gd-Tm) and coating high-temp and silicon carbide is total
Crystalline substance reaction is changed into the characteristic of liquid phase, can effectively reduce silicon carbide seamless connection temperature, and the generation of liquid phase is conducive to connect
The densification of layer.
Correspondingly, the other side of the embodiment of the present invention additionally provides the connection knot of the silicon carbide as made from preceding method
Structure.
Further, articulamentum can disappear and be not present or connecting portion is mainly by carbon in the silicon carbide connection structure
SiClx phase composition.
Further, the jointing of the silicon carbide connection structure on heterogeneous microstructure and macro property with matrix
It is consistent, forms connecting elements integration, there is no jointings to cause with connecting matrix and crack due to hot, power mismatch
The phenomenon that fracture, improves the use scope of silicon carbide and its composite material.Make it can be in high temperature, Strong oxdiative, large dosage of neutron
The environment such as irradiation are on active service.
Further, the four point bending strength of the silicon carbide connection structure is up to 190MPa, the silicon carbide connection knot
Structure can be applied to the fields such as electronics, aerospace, nuclear industry.
In order to make the objectives, technical solutions, and advantages of the present invention clearer, below in conjunction with attached drawing and it is several preferably
Embodiment carries out further details of explanation to technical solution of the present invention.It should be appreciated that specific reality described herein
Example is applied only to explain the present invention, is not intended to limit the present invention.In addition, in the various embodiments of the present invention described below
Involved technical characteristic can be combined with each other as long as they do not conflict with each other.
Embodiment 1
It is silicon carbide ceramics to connecting material in the present embodiment, connection layer material is Dy3Si2C2Coating, Dy3Si2C2's
XRD is characterized as shown in fig. 4 a.Connection method is electric field-assisted connection.Specific implementation step is as follows:
It (1) is 20mm by diameter, the silicon carbide ceramics surface of high 20mm is polished roughly with 5 μm of diamond polishing liquids, is removed
The biggish defect in surface and impurity；
(2) molten-salt growth method is used, 900 DEG C of heat preservation 60min in tube furnace, rare earth dysprosium (Dy) is in silicon carbide reaction in-situ
Generate the Dy that thickness is about 1 μm3Si2C2Coating, as shown in Figure 2 a and 2 b；
(3) then by the silicon carbide of two pieces of coatings in the graphite jig that diameter is 20mm；
(4) graphite jig for installing sample is placed in discharge plasma sintering furnace, galvanization, with 100 DEG C/min's
Heating rate rises to 1300 DEG C, 1400 DEG C, 1500 DEG C of heat preservations 10min, pressure 47MPa, is then dropped with the rate of 100 DEG C/min
It warms to room temperature, sample object is as shown in Figure 3 after connection.
(5) sample connected in step (4), by cutting, polishing is processed into the batten of 3*4*40mm, using 4 points
Curved method, the four point bending strength of test sample.In 1500 DEG C of achievable silicon carbide seamless connections, intensity is
140MPa.The interface microscopic appearance of articulamentum is observed with scanning electron microscope, and articulamentum pattern and back scattering scanned photograph are such as
Shown in Fig. 5 a and Fig. 5 b.
Embodiment 2
It is silicon carbide ceramics to connecting material in the present embodiment, connection layer material is Dy3Si2C2Coating, connection method are
Electric field-assisted connection.Specific implementation step is as follows:
It (1) is 20mm by diameter, the silicon carbide ceramics surface of high 20mm is polished roughly with 5 μm of diamond polishing liquids, is removed
The biggish defect in surface and impurity；
(2) the Dy rare earth films with a thickness of 2000nm are plated in silicon carbide with the method for PVD, then at 900 DEG C
It is heat-treated to obtain Dy3Si2C2Coating；
(3) then by the silicon carbide of two pieces of coatings in the graphite jig that diameter is 20mm；
(4) graphite jig for installing sample is placed in discharge plasma sintering furnace, galvanization, with 100 DEG C/min's
Heating rate rises to 1300 DEG C, 1400 DEG C, 1500 DEG C, 1600 DEG C, 10min, pressure 47MPa is kept the temperature, then with 100 DEG C/min
Rate be cooled to room temperature；
(5) sample connected in step (4), by cutting, polishing is processed into the batten of 3*4*40mm, using 4 points
Curved method, 4 points of anti-intensity of test sample.In 1600 DEG C of achievable silicon carbide seamless connections, intensity 180MPa.
Jointing topography scan photo is as shown in Figure 6.
Embodiment 3
It is silicon carbide ceramics to connecting material in the present embodiment, connection layer material is Sm3Si2C2Coating, Sm3Si2C2's
As shown in Figure 4 b, connection method is electric field-assisted connection to XRD characterization.Specific implementation step is as follows:
It (1) is 20mm by diameter, the silicon carbide ceramics surface of high 20mm is polished roughly with 5 μm of diamond polishing liquids, is removed
The biggish defect in surface and impurity；
(2) Sm is prepared in situ in silicon carbide with molten-salt growth method3Si2C2Coating；
(3) then by the silicon carbide of two pieces of coatings in the graphite jig that diameter is 20mm.
(4) graphite jig for installing sample is placed in discharge plasma sintering furnace, galvanization, with 100 DEG C/min's
Heating rate rises to 1300 DEG C, 1400 DEG C, 1500 DEG C, 1600 DEG C, 1700 DEG C respectively, keeps the temperature 10min, pressure 47MPa, then
Room temperature is cooled to the rate of 100 DEG C/min.
(5) sample connected in step (4), by cutting, polishing is processed into the batten of 3*4*40mm, using 4 points
Curved method, the four point bending strength of test sample.
Embodiment 4
It is silicon carbide ceramics to connecting material in the present embodiment, connection layer material is Er3Si2C2Coating, Er3Si2C2's
XRD is characterized as illustrated in fig. 4 c, and connection method is electric field-assisted connection.Specific implementation step is as follows:
It (1) is 20mm by diameter, the silicon carbide ceramics surface of high 20mm is polished roughly with 5 μm of diamond polishing liquids, is removed
The biggish defect in surface and impurity；
(2) Er is prepared in situ in silicon carbide with molten-salt growth method3Si2C2Coating；
(3) then by the silicon carbide of two pieces of coatings in the graphite jig that diameter is 20mm.
(4) graphite jig for installing sample is placed in discharge plasma sintering furnace, galvanization, with 100 DEG C/min's
Heating rate rises to 1300 DEG C, 1400 DEG C, 1500 DEG C, 1600 DEG C, 1700 DEG C, 1800 DEG C respectively, keeps the temperature 10min, and pressure is
Then 47MPa is cooled to room temperature with the rate of 100 DEG C/min.
(5) sample connected in step (4), by cutting, polishing is processed into the batten of 3*4*40mm, using 4 points
Curved method, the four point bending strength of test sample.
Embodiment 5
It is silicon carbide ceramics to connecting material in the present embodiment, connection layer material is La3Si2C2Coating, connection method are
Electric field-assisted connection.Specific implementation step is as follows:
It (1) is 20mm by diameter, the silicon carbide ceramics surface of high 20mm is polished roughly with 5 μm of diamond polishing liquids, is removed
The biggish defect in surface and impurity；
(2) the La rare earth films with a thickness of 2000nm are plated in silicon carbide with the method for PVD, then at 900 DEG C
It is heat-treated to obtain La3Si2C2Coating；
(3) then by the silicon carbide of two pieces of coatings in the graphite jig that diameter is 20mm；
(4) graphite jig for installing sample is placed in discharge plasma sintering furnace, galvanization, with 100 DEG C/min's
Heating rate rises to 1000 DEG C, 1100 DEG C, 1200 DEG C, 1300 DEG C, 1400 DEG C, 1500 DEG C, 1600 DEG C, keeps the temperature 10min, and pressure is
Then 47MPa is cooled to room temperature with the rate of 100 DEG C/min；
(5) sample connected in step (4), by cutting, polishing is processed into the batten of 3*4*40mm, using 4 points
Curved method, 4 points of anti-intensity of test sample.
Embodiment 6
It is silicon carbide ceramics to connecting material in the present embodiment, connection layer material is Nd3Si2C2Coating, connection method are
Electric field-assisted connection.Specific implementation step is as follows:
It (1) is 20mm by diameter, the silicon carbide ceramics surface of high 20mm is polished roughly with 5 μm of diamond polishing liquids, is removed
The biggish defect in surface and impurity；
(2) the Nd rare earth films with a thickness of 2000nm are plated in silicon carbide with the method for PVD, then at 900 DEG C
It is heat-treated to obtain Nd3Si2C2Coating；
(3) then by the silicon carbide of two pieces of coatings in the graphite jig that diameter is 20mm；
(4) graphite jig for installing sample is placed in discharge plasma sintering furnace, galvanization, with 100 DEG C/min's
Heating rate rises to 1000 DEG C, 1100 DEG C, 1200 DEG C, 1300 DEG C, 1400 DEG C, 1500 DEG C, 1600 DEG C, keeps the temperature 10min, and pressure is
Then 47MPa is cooled to room temperature with the rate of 100 DEG C/min；
(5) sample connected in step (4), by cutting, polishing is processed into the batten of 3*4*40mm, using 4 points
Curved method, 4 points of anti-intensity of test sample.
Embodiment 7
It is silicon carbide ceramics to connecting material in the present embodiment, connection layer material is Ce3Si2C2Coating, connection method are
Electric field-assisted connection.Specific implementation step is as follows:
It (1) is 20mm by diameter, the silicon carbide ceramics surface of high 20mm is polished roughly with 5 μm of diamond polishing liquids, is removed
The biggish defect in surface and impurity；
(2) the Ce rare earth films with a thickness of 2000nm are plated in silicon carbide with the method for PVD, then at 900 DEG C
It is heat-treated to obtain Ce3Si2C2Coating；
(3) then by the silicon carbide of two pieces of coatings in the graphite jig that diameter is 20mm；
(4) graphite jig for installing sample is placed in discharge plasma sintering furnace, galvanization, with 100 DEG C/min's
Heating rate rises to 1000 DEG C, 1100 DEG C, 1200 DEG C, 1300 DEG C, 1400 DEG C, 1500 DEG C, 1600 DEG C, keeps the temperature 10min, and pressure is
Then 47MPa is cooled to room temperature with the rate of 100 DEG C/min；
(5) sample connected in step (4), by cutting, polishing is processed into the batten of 3*4*40mm, using 4 points
Curved method, 4 points of anti-intensity of test sample.
Embodiment 8
It is silicon carbide ceramics to connecting material in the present embodiment, connection layer material is Pr3Si2C2Coating, connection method are
Electric field-assisted connection.Specific implementation step is as follows:
It (1) is 20mm by diameter, the silicon carbide ceramics surface of high 20mm is polished roughly with 5 μm of diamond polishing liquids, is removed
The biggish defect in surface and impurity；
(2) the Pr rare earth films with a thickness of 2000nm are plated in silicon carbide with the method for PVD, then at 900 DEG C
It is heat-treated to obtain Pr3Si2C2Coating；
(3) then by the silicon carbide of two pieces of coatings in the graphite jig that diameter is 20mm；
(4) graphite jig for installing sample is placed in discharge plasma sintering furnace, galvanization, with 100 DEG C/min's
Heating rate rises to 1000 DEG C, 1100 DEG C, 1200 DEG C, 1300 DEG C, 1400 DEG C, 1500 DEG C, 1600 DEG C, keeps the temperature 10min, and pressure is
Then 47MPa is cooled to room temperature with the rate of 100 DEG C/min；
(5) sample connected in step (4), by cutting, polishing is processed into the batten of 3*4*40mm, using 4 points
Curved method, 4 points of anti-intensity of test sample.
Reference examples 1
It is silicon carbide ceramics to connecting material in reference examples, connection layer material is Ti metal coating, and connection method is electric field
Auxiliary connection.Specific implementation steps are as follows:
It (1) is 20mm by diameter, the silicon carbide ceramics surface of high 20mm is polished with 0.1 μm of diamond polishing liquid；
(2) wait for that joint face plates with a thickness of 100nm, 500nm, 1000nm, 6000nm in silicon carbide using the method for PVD
Ti coating.
(3) then by the silicon carbide of two pieces of coatings in the graphite jig that diameter is 20mm；
(4) graphite jig for installing sample is placed in discharge plasma sintering furnace, galvanization, with 100 DEG C/min's
Heating rate rises to 600-1600 DEG C, keeps the temperature 5min, then pressure 30MPa is cooled to room temperature i.e. with the rate of 100 DEG C/min
It can；
The reference examples are although the Ti coating using 100nm fails to reach seamless still with the presence of middle layer in jointing
Connection effect.It can be because of intermediate layer material TiC (7.4 × 10 in applied at elevated temperature-6K-1)、Ti3SiC2(9.1×10-6K-1) and carbonization
Silicon (4.4 × 10-6K-1) coefficient of thermal expansion mismatch and cause to be broken.
By the result of 1-8 of the embodiment of the present invention, it may be said that the bright present invention utilizes rare earth carbon silicide high-temp and silicon carbide
It is changed into the characteristic of liquid phase by eutectic reaction, silicon carbide seamless connection temperature can be effectively reduced, and the generation of liquid phase is advantageous
In the densification sintering of linkage interface silicon carbide, under the effect of the pressure, Partial Liquid Phase rare earth can be extruded volatilization, another part
It can be spread along crystal boundary to silicon carbide substrate, to realize the seamless connection of silicon carbide.
Each aspect of the present invention, embodiment, feature and example should be regarded as to be illustrative and is not intended to limit in all respects
The system present invention, the scope of the present invention are only defined by tbe claims.Without departing substantially from the spirit and scope of the present invention advocated
In the case of, it will be apparent to those skilled in the art that other embodiments, modification and use.
The use of title and chapters and sections is not intended to limit the present invention in case of the present invention；Each chapters and sections can be applied to the present invention
Any aspect, embodiment or feature.
Case of the present invention in the whole text in, composition is being described as have, containing or comprising in place of specific component or will
Process description is in place of having, containing or comprising particular procedure step, it is contemplated that the composition of teachings of this disclosure is also substantially by institute
Narration component composition is made of described component, and the process of teachings of this disclosure is also substantially made of described process steps
Or it is made of described process steps group.
Unless otherwise specific statement, otherwise term " include (include, includes, including) ", " have
The use of (have, has or having) " is it is generally understood that be open and without limitation.
It should be understood that the order of each step or the order of execution specific action are not particularly significant, as long as teachings of this disclosure is protected
Holding can operate.In addition, two or more steps or movement can be carried out simultaneously.
In addition, inventor also refers to previous embodiment, other raw materials for being addressed with this specification, technological operation, work
Skill condition is tested, and obtains ideal result.
Although describing the present invention with reference to an illustrative embodiment, those skilled in the art will appreciate that, it is not carrying on the back
Various other changes can be made in the case where from spirit and scope of the present invention, are omitted and/or are added and can use substantial equivalents
Substitute the element of the embodiment.In addition, many modifications can be made without departing substantially from the scope of the present invention so that specific
Situation or material adapt to teachings of the present invention.Therefore, it is not to restrict the invention to herein for executing institute of the invention
Specific embodiment is disclosed, and being intended to makes the present invention by all implementations comprising falling within the scope of the appended claims
Example.In addition, removing non-specific statement, otherwise any use of term first, second etc. does not indicate any order or importance, but
An element and another element are distinguished using term first, second etc..
Claims (10)
1. a kind of for connecting the connecting material of carbofrax material, it is characterised in that: the connecting material includes rare earth carbon silication
Object, the chemical formula of the rare earth carbon silicide are Re3Si2C2, wherein Re is rare earth element.
2. according to claim 1 for connecting the connecting material of carbofrax material, it is characterised in that: the Re includes
Any one in La, Ce, Pr, Nd, Sm, Gd, Tb, Dy, Ho, Er, Tm or two or more combinations；
And/or the connecting material includes rare earth carbon silicide coating, preferably rare earth carbon silicide film, with a thickness of 50nm
~2000nm；Preferably, the rare earth carbon silicide selects molten-salt growth method original position plated film or PVD method deposition of rare-earth coating, Zhi Houre
Handle the rare earth carbon silicide film of synthesis.
3. purposes of the rare earth carbon silicide in connection carbofrax material, the chemical formula of the rare earth carbon silicide are Re3Si2C2,
Wherein, Re is rare earth element, preferably any one in La, Ce, Pr, Nd, Sm, Gd, Tb, Dy, Ho, Er, Tm or two kinds with
On combination.
4. purposes according to claim 3, which is characterized in that the purposes includes: in carbofrax material to be connected
Linkage interface at rare earth carbon silicide is set, and be heated to 1000~1800 DEG C, make the carbofrax material knot to be connected
Integrator.
5. purposes according to claim 3 or 4, which is characterized in that the purposes includes: in silicon carbide material to be connected
Rare earth carbon silicide coating is set at the linkage interface of material；Preferably, the purposes includes: in carbofrax material to be connected
Linkage interface at coat rare earth carbon silicide, formed rare earth carbon silicide coating；Preferably, the rare earth carbon silicide coating
With a thickness of 50nm~2000nm；Preferably, the rare earth carbon silicide selects molten-salt growth method original position plated film or PVD method deposition of rare-earth
Coating is heat-treated the rare earth carbon silicide film of synthesis later.
6. purposes according to claim 3, it is characterised in that: the carbofrax material includes pure thyrite
And/or carbon/silicon carbide ceramic matrix composite；Preferably, the carbon/silicon carbide ceramic matrix composite includes carbon fibre reinforced silicon carbide
Composite material and/or silicon carbide fiber reinforced silicon carbide composite material.
7. a kind of connection method of carbofrax material, characterized by comprising: in the linkage interface of carbofrax material to be connected
Place's setting rare earth carbon silicide, and 1000~1800 DEG C are heated to, so that the carbofrax material to be connected is combined into one；Institute
The chemical formula for stating rare earth carbon silicide is Re3Si2C2, wherein Re is rare earth element, preferably La, Ce, Pr, Nd, Sm, Gd, Tb,
Any one in Dy, Ho, Er, Tm or two or more combinations.
8. connection method according to claim 7, characterized by comprising: in connection circle of carbofrax material to be connected
Rare earth rare earth carbon silicide coating is set at face；Preferably, the connection method includes: in carbofrax material to be connected
Rare earth carbon silicide is coated at linkage interface, forms rare earth carbon silicide coating；Preferably, the rare earth carbon silicide coating
With a thickness of 50nm~2000nm；Preferably, the rare earth carbon silicide selects molten-salt growth method original position plated film or PVD method deposition of rare-earth to apply
Layer, is heat-treated the rare earth carbon silicide film of synthesis later.
9. connection method according to claim 7, it is characterised in that: the carbofrax material includes pure silicon carbide ceramics material
Material and/or carbon/silicon carbide ceramic matrix composite；Preferably, the carbon/silicon carbide ceramic matrix composite includes fibre reinforced carbonization
Silicon composite and/or silicon carbide fiber reinforced silicon carbide composite material；
And/or the mode of the heating includes that hot pressed sintering connection, electric field-assisted heating connection or pressureless sintering connect, preferably
It heats and connects for electric field-assisted.
10. the silicon carbide connection structure as made from any one of claim 7-9 the method.
Priority Applications (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201910654769.8A CN110357650A (en) | 2019-07-19 | 2019-07-19 | It is a kind of for connecting the connecting material and its application of carbofrax material |
| PCT/CN2019/108906 WO2020082995A1 (en) | 2018-10-24 | 2019-09-29 | Connecting material for connecting a silicon carbide material, and application thereof |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201910654769.8A CN110357650A (en) | 2019-07-19 | 2019-07-19 | It is a kind of for connecting the connecting material and its application of carbofrax material |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN110357650A true CN110357650A (en) | 2019-10-22 |
Family
ID=68220402
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN201910654769.8A Pending CN110357650A (en) | 2018-10-24 | 2019-07-19 | It is a kind of for connecting the connecting material and its application of carbofrax material |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN110357650A (en) |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113233909A (en) * | 2021-05-18 | 2021-08-10 | 中国科学院宁波材料技术与工程研究所 | Novel fiber-toughened ceramic-based composite material, and preparation method and application thereof |
| CN115490530A (en) * | 2022-08-12 | 2022-12-20 | 广东工业大学 | Method for preparing ceramic connecting piece by liquid phase extrusion strategy and application thereof |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107488046A (en) * | 2016-06-12 | 2017-12-19 | 中国科学院宁波材料技术与工程研究所 | Method for connecting the connecting material of silicon carbide ceramics and connecting silicon carbide ceramics |
| CN107488045A (en) * | 2016-06-12 | 2017-12-19 | 中国科学院宁波材料技术与工程研究所 | The method of silicon carbide ceramics connecting material and connection silicon carbide ceramics with low connection temperature high bending strength |
| CN109437957A (en) * | 2018-11-15 | 2019-03-08 | 广东工业大学 | A kind of ceramic connecting piece of connection method and the preparation of nm immersion transient state eutectic phase combination chemical vapor infiltration realization SiC ceramic |
-
2019
- 2019-07-19 CN CN201910654769.8A patent/CN110357650A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107488046A (en) * | 2016-06-12 | 2017-12-19 | 中国科学院宁波材料技术与工程研究所 | Method for connecting the connecting material of silicon carbide ceramics and connecting silicon carbide ceramics |
| CN107488045A (en) * | 2016-06-12 | 2017-12-19 | 中国科学院宁波材料技术与工程研究所 | The method of silicon carbide ceramics connecting material and connection silicon carbide ceramics with low connection temperature high bending strength |
| CN109437957A (en) * | 2018-11-15 | 2019-03-08 | 广东工业大学 | A kind of ceramic connecting piece of connection method and the preparation of nm immersion transient state eutectic phase combination chemical vapor infiltration realization SiC ceramic |
Non-Patent Citations (1)
| Title |
|---|
| JUNQI SHAO ET AL.: ""Fabrication and characterization of SPS sintered SiC-based ceramic from Y3Si2C2-coated SiC powders"", 《 JOURNAL OF THE EUROPEAN CERAMIC SOCIETY》 * |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113233909A (en) * | 2021-05-18 | 2021-08-10 | 中国科学院宁波材料技术与工程研究所 | Novel fiber-toughened ceramic-based composite material, and preparation method and application thereof |
| CN115490530A (en) * | 2022-08-12 | 2022-12-20 | 广东工业大学 | Method for preparing ceramic connecting piece by liquid phase extrusion strategy and application thereof |
| CN115490530B (en) * | 2022-08-12 | 2023-08-22 | 广东工业大学 | Method for preparing ceramic connecting piece by liquid phase extrusion strategy and application thereof |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| CN106588060B (en) | A kind of high-densit carbon/silicon carbide ceramic matrix composite and preparation method thereof | |
| JP5095923B2 (en) | Method for manufacturing parts from impervious heat-resistant structural composites | |
| KR101960264B1 (en) | Residual stress free joined SiC ceramics and the processing method of the same | |
| JP4974209B2 (en) | Silicon infiltration treatment method for ceramic matrix composites | |
| CN110330357A (en) | It is a kind of for connecting the connecting material and its application of carbofrax material | |
| Zhao et al. | Fast interdiffusion and Kirkendall effects of SiC-coated C/SiC composites joined by a Ti-Nb-Ti interlayer via spark plasma sintering | |
| He et al. | Pre-infiltration and brazing behaviors of Cf/C composites with high temperature TiSi eutectic alloy | |
| CN108838504B (en) | Composite intermediate layer for diffusion bonding of silicon carbide ceramic and bonding process thereof | |
| JP2002356381A (en) | METHOD OF MANUFACTURING SiC COMPOSITE MATERIAL OF SiC REINFORCED TYPE | |
| CN110357650A (en) | It is a kind of for connecting the connecting material and its application of carbofrax material | |
| CN110002890A (en) | A kind of Cf/ HfC-SiC ultra-temperature ceramic-based composite material and preparation method thereof | |
| CN108863425A (en) | The connection method of silicon carbide ceramics and its composite material | |
| Yan et al. | An unusual carbon–ceramic composite with gradients in composition and porosity delivering outstanding thermal protection performance up to 1900 C | |
| Zhao et al. | Improved shear strength of SiC-coated 3D C/SiC composite joints with a tailored Ti-Si-C interlayer | |
| CN212451221U (en) | System for connecting silicon carbide materials, multilayer composite film structure and connecting structure | |
| CN111087251B (en) | Connecting material for connecting silicon carbide materials and application thereof | |
| Li et al. | Microstructure and properties of C/SiC‐diamond composites prepared by the combination of CVI and RMI | |
| JP5773331B2 (en) | Manufacturing method of ceramic joined body | |
| Cao et al. | The microstructure and properties of SiC/SiC-based composites fabricated by low-temperature melt infiltration of Al–Si alloy | |
| TW440893B (en) | Semiconductor supporting device and its manufacture, composite body and its manufacture | |
| KR20120078270A (en) | Susceptor using low thermal expansion composite materials and method for manufacturing esc component | |
| CN116693311A (en) | Preparation and application of high-heat-conductivity matrix and coating integrated design and ablation-resistant composite material | |
| CN109942297A (en) | A kind of silicon carbide nanometer line enhances highly oriented graphite composite material and preparation method | |
| JP4707854B2 (en) | Method for producing high-strength SiC fiber / SiC composite material | |
| Lan et al. | High-temperature property of carbon/carbon composite joints bonded with ternary Ti–Si–C compound |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| PB01 | Publication | ||
| PB01 | Publication | ||
| SE01 | Entry into force of request for substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| RJ01 | Rejection of invention patent application after publication | ||
| RJ01 | Rejection of invention patent application after publication |
Application publication date: 20191022 |