EP3325681B1 - Procede de fabrication d'un piece en un materiau composite al/al3b48c2 - Google Patents

Procede de fabrication d'un piece en un materiau composite al/al3b48c2 Download PDF

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Publication number
EP3325681B1
EP3325681B1 EP16741604.9A EP16741604A EP3325681B1 EP 3325681 B1 EP3325681 B1 EP 3325681B1 EP 16741604 A EP16741604 A EP 16741604A EP 3325681 B1 EP3325681 B1 EP 3325681B1
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EP
European Patent Office
Prior art keywords
crucible
powder
graphite
temperature
composite material
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.)
Not-in-force
Application number
EP16741604.9A
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German (de)
English (en)
French (fr)
Other versions
EP3325681A1 (fr
Inventor
Olivier DEZELLUS
Laurent CHAFFRON
Jérôme ANDRIEUX
Nassim SAMER
Bruno GARDIOLA
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Centre National de la Recherche Scientifique CNRS
Commissariat a lEnergie Atomique et aux Energies Alternatives CEA
Claude Bernard University Lyon 1
Original Assignee
Centre National de la Recherche Scientifique CNRS
Commissariat a lEnergie Atomique CEA
Commissariat a lEnergie Atomique et aux Energies Alternatives CEA
Claude Bernard University Lyon 1
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Publication of EP3325681A1 publication Critical patent/EP3325681A1/fr
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    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C1/00—Making non-ferrous alloys
    • C22C1/10—Alloys containing non-metals
    • C22C1/1036—Alloys containing non-metals starting from a melt
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C1/00—Making non-ferrous alloys
    • C22C1/10—Alloys containing non-metals
    • C22C1/1036—Alloys containing non-metals starting from a melt
    • C22C1/1047—Alloys containing non-metals starting from a melt by mixing and casting liquid metal matrix composites
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C29/00—Alloys based on carbides, oxides, nitrides, borides, or silicides, e.g. cermets, or other metal compounds, e.g. oxynitrides, sulfides
    • C22C29/02—Alloys based on carbides, oxides, nitrides, borides, or silicides, e.g. cermets, or other metal compounds, e.g. oxynitrides, sulfides based on carbides or carbonitrides
    • C22C29/06—Alloys based on carbides, oxides, nitrides, borides, or silicides, e.g. cermets, or other metal compounds, e.g. oxynitrides, sulfides based on carbides or carbonitrides based on carbides, but not containing other metal compounds
    • C22C29/062—Alloys based on carbides, oxides, nitrides, borides, or silicides, e.g. cermets, or other metal compounds, e.g. oxynitrides, sulfides based on carbides or carbonitrides based on carbides, but not containing other metal compounds based on B4C
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C32/00—Non-ferrous alloys containing at least 5% by weight but less than 50% by weight of oxides, carbides, borides, nitrides, silicides or other metal compounds, e.g. oxynitrides, sulfides, whether added as such or formed in situ
    • C22C32/0047—Non-ferrous alloys containing at least 5% by weight but less than 50% by weight of oxides, carbides, borides, nitrides, silicides or other metal compounds, e.g. oxynitrides, sulfides, whether added as such or formed in situ with carbides, nitrides, borides or silicides as the main non-metallic constituents
    • C22C32/0052—Non-ferrous alloys containing at least 5% by weight but less than 50% by weight of oxides, carbides, borides, nitrides, silicides or other metal compounds, e.g. oxynitrides, sulfides, whether added as such or formed in situ with carbides, nitrides, borides or silicides as the main non-metallic constituents only carbides
    • C22C32/0057—Non-ferrous alloys containing at least 5% by weight but less than 50% by weight of oxides, carbides, borides, nitrides, silicides or other metal compounds, e.g. oxynitrides, sulfides, whether added as such or formed in situ with carbides, nitrides, borides or silicides as the main non-metallic constituents only carbides based on B4C

Definitions

  • the present invention relates to the field of synthesis of metal matrix composite materials and ceramic particulate reinforcements.
  • the invention relates to a process for producing a composite material having an aluminum matrix in which Al 3 B 48 C 2 reinforcements are dispersed.
  • This process can notably be applied in the fields of aeronautics and the automobile.
  • CMM metal matrix materials
  • metal matrix materials which comprise a metal matrix (metal or metal alloy) in which are incorporated reinforcements (particles, fibers or other) metal or ceramic
  • CMM metal matrix materials
  • the advantage of CMM compared to light alloys is that they have ratios E / ⁇ (elastic modulus / density) and ⁇ / ⁇ (limit of elasticity / density) very high.
  • the chemical reactivity must also be controlled. Indeed, the equilibrium between the phases in the Al-BC system indicates that Al and B 4 C are not in equilibrium below a temperature which is not precisely known, but which is estimated in the literature to be superior at 1400 ° C.
  • any synthesis based on the mixture of Al and B 4 C precursor powders and carried out at a temperature below 1400 ° C. thus leads to the decomposition of the B 4 C reinforcement by Al and to the formation of Al 3 BC 3 carbide. .
  • the latter although less sensitive to hydrolysis in the presence of moisture than Al 4 C 3 carbide, still remains subject to this phenomenon which leads to the release of large amounts of CH 4 gas.
  • the gas produced in the core of the composite material then generates stresses that lead to the ruin of the composite material (return to the powder state).
  • other phases such as AlB 2 and AlB 12 borides can also be formed during the interaction between Al and B 4 C. The fragility of these phases then induces embrittlement of the composite material.
  • EP0322336 discloses a process wherein Al / Al 3 B 48 C 2 is formed from the high temperature reaction of molten aluminum with sintered B 4 C powder.
  • US5017217A discloses methods for obtaining Ti-Al-B-based composite via the peritectic decomposition reaction of AlB 2 with TiH 2 .
  • the first solution which will be called the cryogenic method, was developed by Julie Schoenung at the University of California, Davis. This method encounters the difficulty of implementing high energy grinding in liquid nitrogen for large quantities of material. The change of scale from laboratory to industrial production seems difficult. Moreover, this method can not ignore a consolidation step that must be carried out hot.
  • the second solution is to minimize the duration of the hot consolidation step to limit as far as possible the progress of the reaction between Al and B 4 C.
  • the main difficulty lies again in the amount of usable material. Indeed, the hot forming requires that the matrix Al is brought to a temperature sufficient to be subject to plastic deformation by creep. However, in the case of a large volume of material, the standardization of the temperature in the entire volume requires a significant temperature maintenance time as well.
  • the inventors have therefore set themselves the goal of designing a process for producing an alternative composite material to the Al / B 4 C composite, which has properties similar to those of the Al / B 4 C composite, while being able to be produced industrially. .
  • the graphite element for closing the cavity is a graphite piston.
  • the AlB 2 powder When placed in the graphite crucible in step a), the AlB 2 powder can be in various forms. According to a first variant, the powder is placed in the crucible in a compressed form, for example in the form of one or more pellets. According to a second variant, the powder is placed in the crucible in a powder form and step b) further comprises a compression of the powder. It is preferred to use the powder in powder form and compress it in the cavity of the crucible, since the AlB 2 diborure is weakly ductile, obtaining a compact is difficult.
  • step b) when the powder is placed in the crucible in pulverulent form, step b) further comprises the compression of the powder.
  • the compression of the powder and the closing of the cavity of the crucible are obtained by the use of a graphite piston.
  • the piston is dimensioned so as to slide in the opening of the crucible in order to compress the powder and to close this opening.
  • the crucible is heated at a temperature ranging from 1000 ° C. to 1400 ° C. for a period ranging from 5 minutes to 30 minutes.
  • the descent in temperature in step d) is fast. This makes it possible to limit the decomposition reactions of the phases formed at high temperature.
  • the cooling in step d) comprises a descent in temperature with a speed greater than or equal to 10 ° C / s until reaching 600 ° C.
  • step e) can be obtained separating the ingot of composite material obtained at the end of step d) (and which forms the composite material part to be obtained) of the crucible or else by proceeding to a turning operation that will destroy the crucible.
  • the Al / Al 3 B 48 C 2 composite material produced according to the process according to the invention is a good alternative to the Al / B 4 C composite material.
  • the ternary compound ⁇ 3 -Al 3 B 48 C 2 which forms the reinforcement, is in equilibrium with the matrix Al according to the literature.
  • it has properties similar to those of B 4 C, as can be seen from the table below, and is therefore a credible alternative to B 4 C for the production of a ceramic matrix composite and reinforcement of carbide type rich in boron.
  • the matrix and the reinforcement are formed at high temperature and in-situ, which has several advantages.
  • the reinforcements of the composite are obtained during the decomposition of the AlB 2 particles by germination / growth in the liquid phase.
  • the matrix / reinforcement interface is therefore chemically clean (no impurities, oxides or other) and thus leads to optimum resistance of the interface.
  • the reinforcements are formed in situ and have not had to undergo a grinding cycle, grinding which is often likely to induce defects which are then starting points for the cracking of the composite material.
  • the method of the invention also has the advantage of simplicity of its implementation.
  • it makes it possible to obtain a dense ingot directly from the internal geometry of the graphite crucible, since the ingot is shaped in the liquid state in the graphite crucible.
  • the single figure is an image obtained by scanning electron microscopy of an ingot obtained according to a first embodiment according to the method which is the subject of the invention.
  • the method which is the subject of the invention is based on a so-called reactive synthesis method.
  • the matrix and the reinforcement of the composite material are obtained in situ by a reaction between two precursors.
  • the precursors chosen are aluminum diboride (AlB 2 ) and graphite (C).
  • AlB 2 is in the form of a powder and is placed in a crucible which is made of graphite.
  • the same graphite element preferably a graphite piston, is used to compact the powder and to seal the cavity of the crucible.
  • the whole is then heated to high temperature.
  • the heating is carried out at a temperature above the decomposition temperature of AlB 2 , that is to say the temperature from which one begins to have a liquid phase.
  • the decomposition temperature of AlB 2 i.e. at 960 ° C, two phases are obtained, a liquid phase and a solid phase.
  • the heating is carried out at a temperature of between 1000 ° C. and 1400 ° C., preferably between 1200 ° C. and 1400 ° C., for a period of time. which can be variable, but will generally be between 5 and 30 minutes. In fact, the duration of heating at a given temperature is adjusted according to the desired microstructure: the longer the heating time, the larger the size of the reinforcing particles.
  • the climbs and descents in temperature are fast, in order to limit both the size of the reinforcing particles and their decomposition during cooling.
  • the graphite crucible can be removed by simple machining, releasing the ingot of CMM composite material contained therein. Since this was obtained at a temperature higher than the Al fusion, the presence of the matrix in the liquid state makes it possible to directly obtain a composite with a relative density greater than 99.5%.
  • a graphite crucible 8 mm in diameter, 5 mm high and whose walls have a thickness of 2 mm 750 mg of aluminum diboride powder (AlB 2 ) are placed. The whole is heated at 1400 ° C for 15 minutes. The heating ramp is about 340 ° C / min, while cooling is obtained by dipping the crucible directly in an oil bath cooled to 0 ° C.
  • AlB 2 aluminum diboride powder
  • the microstructure of the Al / Al 3 B 48 C 2 composite thus obtained is observed under SEM (single figure).
  • the white phase corresponds to the aluminum matrix and the black particles correspond to the reinforcement phase Al 3 B 48 C 2 . It is found that the reinforcements are homogeneously dispersed in the matrix and have a size of between 200 nm and 5 ⁇ m (average size of about 700 nm).
  • the method of the invention makes it possible to create an interface between a matrix and a reinforcement which is mechanically strong, but without leading to the decomposition of the reinforcement and the creation of deleterious secondary phases for the properties of the composite. Indeed, during the reactive synthesis between AlB 2 and graphite (C), there are very few minor phases that are created and the composite thus essentially comprises a phase of AI (forming the matrix) and a phase of Al 3 B 48 C 2 (reinforcement), the minor phases being present in minimal quantities.
  • the process according to the invention provides a new synthetic route for producing, in a simple manner and in quantity, Al-matrix composite materials reinforced with particles of a mixed boron (B) and aluminum (Al) carbide. whose properties are close to those of a B 4 C reinforcement.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Composite Materials (AREA)
  • Manufacture Of Alloys Or Alloy Compounds (AREA)
EP16741604.9A 2015-07-20 2016-07-19 Procede de fabrication d'un piece en un materiau composite al/al3b48c2 Not-in-force EP3325681B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
FR1556859A FR3039169B1 (fr) 2015-07-20 2015-07-20 Procede de fabrication d'une piece en un materiau composite al/al3b48c2
PCT/EP2016/067116 WO2017013087A1 (fr) 2015-07-20 2016-07-19 Procede de fabrication d'une piece en un materiau composite al/al3b48c2

Publications (2)

Publication Number Publication Date
EP3325681A1 EP3325681A1 (fr) 2018-05-30
EP3325681B1 true EP3325681B1 (fr) 2019-05-01

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EP16741604.9A Not-in-force EP3325681B1 (fr) 2015-07-20 2016-07-19 Procede de fabrication d'un piece en un materiau composite al/al3b48c2

Country Status (5)

Country Link
US (1) US20180209016A1 (ru)
EP (1) EP3325681B1 (ru)
FR (1) FR3039169B1 (ru)
RU (1) RU2018106104A (ru)
WO (1) WO2017013087A1 (ru)

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN110002447B (zh) * 2019-05-13 2020-11-06 中南大学 一种Al8B4C7粉体的制备方法

Family Cites Families (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4514268A (en) * 1982-12-30 1985-04-30 Corning Glass Works Electrolytic Al production with reaction sintered cermet component
US5017217A (en) * 1986-02-03 1991-05-21 Eltech Systems Corporation Ceramic/metal or ceramic/ceramic composite article
US4940679A (en) * 1987-07-15 1990-07-10 Lanxide Technology Company, Lp Process for preparing self-supporting bodies and products made thereby

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* Cited by examiner, † Cited by third party
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Also Published As

Publication number Publication date
EP3325681A1 (fr) 2018-05-30
FR3039169B1 (fr) 2017-07-21
FR3039169A1 (fr) 2017-01-27
US20180209016A1 (en) 2018-07-26
WO2017013087A1 (fr) 2017-01-26
RU2018106104A (ru) 2019-08-20

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