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WO1991003378A1 - Nid d'abeilles thermoplastique et procedes de preparation - Google Patents

Nid d'abeilles thermoplastique et procedes de preparation Download PDF

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Publication number
WO1991003378A1
WO1991003378A1 PCT/US1990/005037 US9005037W WO9103378A1 WO 1991003378 A1 WO1991003378 A1 WO 1991003378A1 US 9005037 W US9005037 W US 9005037W WO 9103378 A1 WO9103378 A1 WO 9103378A1
Authority
WO
WIPO (PCT)
Prior art keywords
thermoplastic
open
polymer
cell grid
laminated structure
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.)
Ceased
Application number
PCT/US1990/005037
Other languages
English (en)
Inventor
Warren D. Myers
Ernest M. Bishop
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.)
Hexcel Corp
Original Assignee
Hexcel Corp
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Hexcel Corp filed Critical Hexcel Corp
Publication of WO1991003378A1 publication Critical patent/WO1991003378A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29B—PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
    • B29B15/00—Pretreatment of the material to be shaped, not covered by groups B29B7/00 - B29B13/00
    • B29B15/08—Pretreatment of the material to be shaped, not covered by groups B29B7/00 - B29B13/00 of reinforcements or fillers
    • B29B15/10—Coating or impregnating independently of the moulding or shaping step
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B5/00—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts
    • B32B5/22—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed
    • B32B5/24—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed one layer being a fibrous or filamentary layer
    • B32B5/26—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed one layer being a fibrous or filamentary layer another layer next to it also being fibrous or filamentary
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29B—PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
    • B29B15/00—Pretreatment of the material to be shaped, not covered by groups B29B7/00 - B29B13/00
    • B29B15/08—Pretreatment of the material to be shaped, not covered by groups B29B7/00 - B29B13/00 of reinforcements or fillers
    • B29B15/10—Coating or impregnating independently of the moulding or shaping step
    • B29B15/105—Coating or impregnating independently of the moulding or shaping step of reinforcement of definite length with a matrix in solid form, e.g. powder, fibre or sheet form
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29D—PRODUCING PARTICULAR ARTICLES FROM PLASTICS OR FROM SUBSTANCES IN A PLASTIC STATE
    • B29D99/00—Subject matter not provided for in other groups of this subclass
    • B29D99/0089—Producing honeycomb structures
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B3/00—Layered products comprising a layer with external or internal discontinuities or unevennesses, or a layer of non-planar shape; Layered products comprising a layer having particular features of form
    • B32B3/10—Layered products comprising a layer with external or internal discontinuities or unevennesses, or a layer of non-planar shape; Layered products comprising a layer having particular features of form characterised by a discontinuous layer, i.e. formed of separate pieces of material
    • B32B3/12—Layered products comprising a layer with external or internal discontinuities or unevennesses, or a layer of non-planar shape; Layered products comprising a layer having particular features of form characterised by a discontinuous layer, i.e. formed of separate pieces of material characterised by a layer of regularly- arranged cells, e.g. a honeycomb structure
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B37/00—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding
    • B32B37/14—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the properties of the layers
    • B32B37/146—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the properties of the layers whereby one or more of the layers is a honeycomb structure
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B38/00—Ancillary operations in connection with laminating processes
    • B32B38/08—Impregnating
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2260/00—Layered product comprising an impregnated, embedded, or bonded layer wherein the layer comprises an impregnation, embedding, or binder material
    • B32B2260/02—Composition of the impregnated, bonded or embedded layer
    • B32B2260/021—Fibrous or filamentary layer
    • B32B2260/023—Two or more layers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2260/00—Layered product comprising an impregnated, embedded, or bonded layer wherein the layer comprises an impregnation, embedding, or binder material
    • B32B2260/04—Impregnation, embedding, or binder material
    • B32B2260/046—Synthetic resin
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2262/00—Composition or structural features of fibres which form a fibrous or filamentary layer or are present as additives
    • B32B2262/10—Inorganic fibres
    • B32B2262/101—Glass fibres
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2305/00—Condition, form or state of the layers or laminate
    • B32B2305/02—Cellular or porous
    • B32B2305/024—Honeycomb

Definitions

  • This invention lies in the fields of honeycomb structures and polymer processing techniques.
  • the particular area addressed by this invention is that relating to honeycomb structures formed of fabric-reinforced polymer.
  • Honeycomb has long been known for use in structural elements where a combination of lightness and strength are desirable.
  • nonmetallic materials such as ceramics and plastics offers additional advantages in terms of processing characteristics and the appearance and properties of the final product.
  • Thermoset plastics have been used in the manufacture of honeycomb, by fusing together corrugated ribbons of the plastic as well as by fusing together ribbons of fabric impregnated with thermosetting resin prior to the final cure. Difficulties with such materials include limitations on the manufacturing techniques, as well as minimal damage resistance with the result that the product is highly susceptible to damage during fabrication and lay-up, as well as fragmentation upon handling.
  • honeycomb structures can be prepared which have the strength, impact resistance and processing characteristics of thermoplastic materials and yet offer high temperature resistance and solvent resistance characteristics which permit such processing steps as the application of multiple coatings for purposes of density adjustment and the formation of composite layers.
  • a thermoplastic resin which has a soluble form and can be converted to an insoluble form.
  • a fiber web is initially impregnated with the resin in its soluble form, using any of a variety of techniques, thereby fusing the fibers together into a stable coherent structure.
  • the resulting impregnated web in the form of ribbons or sheets, is arranged in a stack, in which adjacent ribbons or sheets are fused together along transverse node lines to render the stack expandable into the open-cell structure which forms the honeycomb, the expansion facilitated by heating the stack up to the softening point of the resin.
  • the thermoplastic character of the insoluble resin permits this expansion to occur without damage to the resin, and the character of being insoluble permits further applications of the resin subsequent to the initial expansion.
  • the soluble form of the resin permits these applications to be made by dipping the expanded structure in a solution of the resin followed by removal of the solvent and conversion to the insoluble form. Expansion can be done in stages, with further applications of resin in between each stage.
  • the technique can also be used to apply layers of different resins or coating materials to form for example a composite structure with a specified combination of properties.
  • the initial impregnation is also done by dipping the fiber web in a solution of the resin in its soluble form.
  • the present invention has wide applicability in terms of the types of honeycomb which can be formed and the various procedural steps and different types and numbers of layers to be applied as well as the means by which they are applied.
  • the invention is of particular interest however as applied to thermoplastic-impregnated fabric in unexpanded stacks of ribbons or sheets which are then expanded into open-cell honeycomb panels to which further thermoplastic resin is applied by dipping the expanded honeycomb into a solution of the resin.
  • a wide variety of resins can be used, subject to the description in the preceding section. The choice of resin can thus depend on the choice of solvents.
  • the resin serving as the fabric impregnant may be the same as or different than the resin ' in the dip solution, and where more than one dip solution is used, the resins in the solutions themselves may be the same or different.
  • the resins must be compatible with each other. Compatibility in this context denotes the tendency of two resins to fuse together as one cures over a cured layer of the other, to the extent that the two are not easily separated by physical or mechanical means. The combining of two or more resins in this fashion permits the formation of hybrid structures and the achievement of useful as well as synergistic properties.
  • the resin serving as the fabric impregnant may be one which is applied in the same manner as the subsequent resin layers, i.e., by dipping followed by solvent removal and thermal conversion to a state permitting further processing.
  • the fabric impregnant may be applied by other techniques known to those skilled in the art. Examples of other techniques are electrostatic deposition of the resin directly onto the fiber web in dry powder form followed by thermal fusion, and hot calendering of the resin in solid form directly onto the fabric.
  • thermoplastic resins which are soluble in a given solvent but which are capable of thermal conversion to a form which is insoluble in the same solvent.
  • thermal conversion and related terms are used herein to denote a chemical reaction, such as curing or chain lengthening, which occurs at elevated temperature. Any thermoplastic resin which meets this description may be used.
  • thermoplastic polymers may be used as the resins.
  • examples include polyamides, poly(amide- imide) ⁇ , polyacetals, polycarbonates, poly(butylene terephthalate)s, poly(phenylene oxide)s and poly(phenylene sulphoxide)s.
  • Preferred polymers for both the initial fabric impregnant and the dipping solution(s) are poly(amide-imides) , particularly those of the following formula
  • R is alkyl, preferably C,-C 6 , straight-chain or branched-chain; aryl, preferably phenyl, naphthyl, diphenyl sulfide, diphenyl sulfoxide or diphenyl sulfone; or aryl-alkyl combinations such as benzyl and diphenylmethylene.
  • the formula shown above represents the polymer in reacted form, insoluble in any of a variety of polar organic solvents.
  • the prepolymer is any precursor form of the above which is soluble in the same solvents.
  • the precursor may be a partially polymerized analogue of the insoluble polymer, particularly one with a sufficient number of free acid groups remaining which render it solubEe.
  • One possibility for the precursor is a poly(amic acid) represented by the formula
  • a particularly preferred polymer within the scope of formula I above is one represented by the formula
  • This poly(amic acid) is formed by the reaction between diamino diphenyl sulfone and trimellitic anhydride.
  • Preferred poly(amic acids) within this formula as well as precursors in general to the polymer of formula II above are those having an acid number ranging from about 50 to about 100 when dissolved in a solvent as a 25% solution by weight.
  • a prepolymer which has been found to be particularly effective i a product defined as AI-10 Polymer, supplied by Amoco Chemical Corporation, Chicago, Illinois, which undergoes conversion at temperatures of 350°F and above.
  • the choice of solvent is not critical and may vary widely, provided that it dissolves the resin prior to its conversion to the insoluble state.
  • Polar organic solvents are preferred, and examples are dimethylformamide, dimethylacetamide, dimethyl sulfoxide, N-methylpyrrolidone and j ⁇ -cresol.
  • the properties of the solution may be modified by the use of a diluent, which may be any liquid which is miscibl with the solvent, does not cause premature precipitation of th unconverted resin, and yet does not dissolve the converted polymer.
  • diluents compatible with the solvents listed above are aromatic hydrocarbons, ethyl acetate, acetone, cyclohexanone, acetamide and acetanilide.
  • the diluent may serve as an aid in removing the solvent, as for example by evaporation, or as an additive for adjusting the viscosity of the solution, or both.
  • the concentration of resin in the solution may also vary, and will be chosen in accordance with the desired viscosity of the solution and other processing characteristics. In most applications, best results will be obtained using solutions having a dissolved solids content (i.e., the resin) of about 10% to about 30% by weight, preferably from about 15% to about 25% by weight.
  • a solution which has been found to be effective is a solution of the AI-10 polymer in a mixture of 40% acetone and 60% N-methylpyrrolidone, with a solids content of about 18% to 22% by weight.
  • the web or reinforcement may be any material capable of impregnation by a resin. Both woven and nonwoven fabrics may be used, including both natural and synthetic materials. Reinforcements made from glass fibers are particularly useful.
  • the porosity and weight of the fabric may also vary widely. In most cases, fabrics having a weight ranging from about 0.3 to about 3.0 ounces per square yard (10 to 100 grams per square meter) , preferably from about 0.5 to about 2.0 ounces per square yard (17 to 68 grams per square meter) will provide the best results.
  • honeycomb is used herein to denote any open-cell grid structure, and particularly such open-cell structures which are formed from fused sheet stacks which are expanded or drawn apart. Examples of such stacks and the honeycomb panels which they form upon expansion are found in Steele, R.C., et al., U.S. Patent No. 2,674,295 (April 6, 1954); Holland, K.M. , U.S. Patent No. 3,006,798 (October 31, 1961); Anderson, D.C., et al., U.S. Patent No. 3,466,957 (September 16, 1969); Noble, R.G., et al., U.S. Patent No. 3,598,676 (August 10, 1971); and Taylor, R.S., U.S. Patent No. 3,819,439 (June 25, 1974). The disclosures of these patents are incorporated herein by reference.
  • the fused stacks which are expanded into open-cell honeycomb structures may be of various dimensions of thickness, length and width. As addressed by the present invention, these stacks may be formed from components which range from long, narrow strips or ribbons, to relatively wide sheets. In practice, ribbon stacks are generally formed from sheet stacks by cutting with a band saw or similar equipment. Other methods of preparation are possible, however, and the present invention is not contemplated to be limited to any particular method or any particular configuration of the stack itself. For purposes of convenience, ribbons and sheets will be referred to herein generically as "layers.” As one example of a fabrication procedure, a roll of glass fiber fabric, typically 2 to 4 mils in thickness, is impregnated with a solution of the resin in its soluble state.
  • An example is the AI-10 polymer dissolved in a 40/60 mixture of acetone and N-methylpyrrolidone at a solids content of about 20% by weight.
  • the impregnated roll is then passed through an oven at a temperature of about 400°F (204°C) for 5 to 8 minutes, which results in the acetone and N-methyl ⁇ pyrrolidone being flashed off and the remaining resin being partially cured to a tack-free state.
  • the roll is then cut into sheets. In one embodiment the roll is cut into sheets about 36 inches (91 cm) in width, on a 45" bias, i.e., in a direction such that the fibers are aligned at an angle of approximately 45° with respect to the lateral edges of the sheets.
  • the longitudinal edges of the sheets are then overlapped, glued together and heat sealed. This is followed by rolling the sheets into rolls and heat soaking the rolls at about 350°F (177°C) for at least one hour for final curing of the glue.
  • the rolls are unrolled and node lines, typically of a nylon-modified epoxy, are printed on the at regular intervals using a standard gravure technique.
  • the rolls are then cut into rectangular sheets which are stacked t a thickness of about 4 to 5 inches (10 to 13 cm) .
  • the stacks are then placed in a press where they are heated to a temperature of about 350 ⁇ F (177°C) under a pressure of about
  • the unexpanded honeycomb block may be expanded to the desired dimensions, and restrained in the expanded state by a jig or frame.
  • expansion may occur at room temperature. In most applications, however, particularly those involving anything other than very low resin loadings, expansion is best done with the aid of heat, such as by the use of steam and/or hot water.
  • the honeycomb may be dipped in fresh AI-10 solution to form a film over the cured surface of the honeycomb. The solvent is then removed from the film and the resin converted to the final cured state in the same manner as the web impregnant. The dipping procedure may be repeated as often as desired to achieve a final honeycomb of the desired density and other characteristics.
  • the initial expansion is done to less than a full expansion, opening the cells only part way to their maximum opening. This prevents excessive strain on the node bonds.
  • the first dip followed by solvent removal and cure is then performed while the cells are still only partially opened.
  • the panel is then heated once again and expanded to its full expansion, opening the cells to their maximum opening, the node bonds being strengthened by the coating laid down by the dip.
  • the expansion ratio prior to the dip is not critical, and may range from about 20% to about 80% depending on the materials, conditions and dimensions of the system, although in most cases, an initial expansion ratio (i.e., the percent of total expansion) of about 50% will provide the best results.
  • the dipping process may be repeated several times, the number depending on the cell size and the desired final density.

Landscapes

  • Engineering & Computer Science (AREA)
  • Mechanical Engineering (AREA)
  • Laminated Bodies (AREA)

Abstract

On prépare un nid d'abeilles thermoplastique pouvant être formé par dilatation d'une pile de rubans compactée et d'immersions répétées dans une solution de résine afin de former des panneaux en nids d'abeilles densifiés, par imprégnation d'une bande en fibres d'une matière thermoplastique ayant une forme soluble et une forme insoluble, et on la fait passer facilement de la première à la seconde. Les poly(amide-imide)s sont un exemple de résine adaptée. L'invention est particulièrement utile pour former des piles de rubans compactées en fibre de verre imprégnée de résine, pour dilater les piles à une température élevée jusqu'à une dilatation partielle suffisante pour exposer l'intérieur des cellules, puis pour immerger les piles partiellement dilatées dans une solution de résine, pour éliminer le solvant du film obtenu et durcir ce dernier, puis pour dilater à nouveau les piles à une température élevée jusqu'à obtention de leur dilatation totale, suivie par de nouvelles immersions jusqu'à obtention de la densité finale voulue.
PCT/US1990/005037 1989-09-07 1990-09-06 Nid d'abeilles thermoplastique et procedes de preparation Ceased WO1991003378A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US40424089A 1989-09-07 1989-09-07
US404,240 1989-09-07

Publications (1)

Publication Number Publication Date
WO1991003378A1 true WO1991003378A1 (fr) 1991-03-21

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PCT/US1990/005037 Ceased WO1991003378A1 (fr) 1989-09-07 1990-09-06 Nid d'abeilles thermoplastique et procedes de preparation

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1008566A1 (fr) * 1998-12-10 2000-06-14 Showa Aircraft Industry Co., Ltd. Structure en nid d'abeilles et méthode de sa production
WO2001030718A1 (fr) * 1999-10-22 2001-05-03 Air & Refrigeration Corp Support pour refroidisseur evaporatif
US8440290B2 (en) 1999-10-22 2013-05-14 Anne Yaeger Contact media for evaporative coolers

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3899626A (en) * 1972-09-11 1975-08-12 Rhone Poulenc Sa Composite articles based on heat-resistant resins
US4710432A (en) * 1985-08-08 1987-12-01 Teijin Limited Base material for honeycomb core structure and process for producing the same

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3899626A (en) * 1972-09-11 1975-08-12 Rhone Poulenc Sa Composite articles based on heat-resistant resins
US4710432A (en) * 1985-08-08 1987-12-01 Teijin Limited Base material for honeycomb core structure and process for producing the same

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1008566A1 (fr) * 1998-12-10 2000-06-14 Showa Aircraft Industry Co., Ltd. Structure en nid d'abeilles et méthode de sa production
US6331340B1 (en) 1998-12-10 2001-12-18 Showa Aircraft Industry Co., Ltd. Honeycomb structure and method for preparing the same
EP1544179A3 (fr) * 1998-12-10 2006-06-07 Showa Aircraft Industry Co., Ltd. Structure en nid d'abeille et sa méthode de production
WO2001030718A1 (fr) * 1999-10-22 2001-05-03 Air & Refrigeration Corp Support pour refroidisseur evaporatif
US8440290B2 (en) 1999-10-22 2013-05-14 Anne Yaeger Contact media for evaporative coolers

Also Published As

Publication number Publication date
AU6624390A (en) 1991-04-08

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