EP1963455A1 - Composite material, especially multilayer material, and adhesive or bonding material - Google Patents

Composite material, especially multilayer material, and adhesive or bonding material

Info

Publication number
EP1963455A1
EP1963455A1 EP06820829A EP06820829A EP1963455A1 EP 1963455 A1 EP1963455 A1 EP 1963455A1 EP 06820829 A EP06820829 A EP 06820829A EP 06820829 A EP06820829 A EP 06820829A EP 1963455 A1 EP1963455 A1 EP 1963455A1
Authority
EP
European Patent Office
Prior art keywords
material according
matrix
nanofiber
composite material
bonding
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.)
Withdrawn
Application number
EP06820829A
Other languages
German (de)
French (fr)
Inventor
Xinhe Tang
Ka Chun Tse
Ernst Hammel
Ben Zhong Tang
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.)
Rogers Germany GmbH
Original Assignee
Electrovac AG
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 Electrovac AG filed Critical Electrovac AG
Publication of EP1963455A1 publication Critical patent/EP1963455A1/en
Withdrawn legal-status Critical Current

Links

Classifications

    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J163/00—Adhesives based on epoxy resins; Adhesives based on derivatives of epoxy resins
    • 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
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/20—Layered products comprising a layer of metal comprising aluminium or copper
    • 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
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/18—Layered products comprising a layer of synthetic resin characterised by the use of special additives
    • B32B27/20—Layered products comprising a layer of synthetic resin characterised by the use of special additives using fillers, pigments, thixotroping agents
    • 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
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/36—Layered products comprising a layer of synthetic resin comprising polyesters
    • 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
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/38—Layered products comprising a layer of synthetic resin comprising epoxy resins
    • 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
    • B32B7/00—Layered products characterised by the relation between layers; Layered products characterised by the relative orientation of features between layers, or by the relative values of a measurable parameter between layers, i.e. products comprising layers having different physical, chemical or physicochemical properties; Layered products characterised by the interconnection of layers
    • B32B7/04—Interconnection of layers
    • B32B7/12—Interconnection of layers using interposed adhesives or interposed materials with bonding properties
    • 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
    • B32B9/00—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00
    • B32B9/005—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising one layer of ceramic material, e.g. porcelain, ceramic tile
    • 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
    • B32B9/00—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00
    • B32B9/04—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising such particular substance as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B9/041—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising such particular substance as the main or only constituent of a layer, which is next to another layer of the same or of a different material of metal
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y10/00—Nanotechnology for information processing, storage or transmission, e.g. quantum computing or single electron logic
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J11/00—Features of adhesives not provided for in group C09J9/00, e.g. additives
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L23/00—Details of semiconductor or other solid state devices
    • H01L23/34—Arrangements for cooling, heating, ventilating or temperature compensation ; Temperature sensing arrangements
    • H01L23/36—Selection of materials, or shaping, to facilitate cooling or heating, e.g. heatsinks
    • H01L23/373—Cooling facilitated by selection of materials for the device or materials for thermal expansion adaptation, e.g. carbon
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L23/00—Details of semiconductor or other solid state devices
    • H01L23/34—Arrangements for cooling, heating, ventilating or temperature compensation ; Temperature sensing arrangements
    • H01L23/36—Selection of materials, or shaping, to facilitate cooling or heating, e.g. heatsinks
    • H01L23/373—Cooling facilitated by selection of materials for the device or materials for thermal expansion adaptation, e.g. carbon
    • H01L23/3735—Laminates or multilayers, e.g. direct bond copper ceramic substrates
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K3/00—Apparatus or processes for manufacturing printed circuits
    • H05K3/38—Improvement of the adhesion between the insulating substrate and the metal
    • H05K3/386—Improvement of the adhesion between the insulating substrate and the metal by the use of an organic polymeric bonding layer, e.g. adhesive
    • 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
    • B32B2250/00—Layers arrangement
    • B32B2250/40—Symmetrical or sandwich layers, e.g. ABA, ABCBA, ABCCBA
    • 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
    • B32B2255/00—Coating on the layer surface
    • B32B2255/26—Polymeric coating
    • 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
    • B32B2262/02—Synthetic macromolecular 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
    • B32B2262/00—Composition or structural features of fibres which form a fibrous or filamentary layer or are present as additives
    • B32B2262/10—Inorganic fibres
    • B32B2262/106—Carbon fibres, e.g. graphite 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
    • B32B2264/00—Composition or properties of particles which form a particulate layer or are present as additives
    • B32B2264/10—Inorganic particles
    • B32B2264/102—Oxide or hydroxide
    • 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
    • B32B2307/00—Properties of the layers or laminate
    • B32B2307/20—Properties of the layers or laminate having particular electrical or magnetic properties, e.g. piezoelectric
    • B32B2307/208—Magnetic, paramagnetic
    • 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
    • B32B2307/00—Properties of the layers or laminate
    • B32B2307/30—Properties of the layers or laminate having particular thermal properties
    • B32B2307/302—Conductive
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K2201/00—Specific properties of additives
    • C08K2201/011—Nanostructured additives
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K7/00—Use of ingredients characterised by shape
    • C08K7/02—Fibres or whiskers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2924/00—Indexing scheme for arrangements or methods for connecting or disconnecting semiconductor or solid-state bodies as covered by H01L24/00
    • H01L2924/0001—Technical content checked by a classifier
    • H01L2924/0002—Not covered by any one of groups H01L24/00, H01L24/00 and H01L2224/00
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0306—Inorganic insulating substrates, e.g. ceramic, glass
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/02—Fillers; Particles; Fibers; Reinforcement materials
    • H05K2201/0203—Fillers and particles
    • H05K2201/0242—Shape of an individual particle
    • H05K2201/0251—Non-conductive microfibers
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/02—Fillers; Particles; Fibers; Reinforcement materials
    • H05K2201/0203—Fillers and particles
    • H05K2201/0242—Shape of an individual particle
    • H05K2201/026—Nanotubes or nanowires
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/03—Conductive materials
    • H05K2201/032—Materials
    • H05K2201/0323—Carbon
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/03—Conductive materials
    • H05K2201/0332—Structure of the conductor
    • H05K2201/0335—Layered conductors or foils
    • H05K2201/0355—Metal foils
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/08—Magnetic details
    • H05K2201/083—Magnetic materials
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K2203/00—Indexing scheme relating to apparatus or processes for manufacturing printed circuits covered by H05K3/00
    • H05K2203/10—Using electric, magnetic and electromagnetic fields; Using laser light
    • H05K2203/104—Using magnetic force, e.g. to align particles or for a temporary connection during processing
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/24—Structurally defined web or sheet [e.g., overall dimension, etc.]
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/24—Structurally defined web or sheet [e.g., overall dimension, etc.]
    • Y10T428/24058—Structurally defined web or sheet [e.g., overall dimension, etc.] including grain, strips, or filamentary elements in respective layers or components in angular relation
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/24—Structurally defined web or sheet [e.g., overall dimension, etc.]
    • Y10T428/24132—Structurally defined web or sheet [e.g., overall dimension, etc.] including grain, strips, or filamentary elements in different layers or components parallel
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/249921—Web or sheet containing structurally defined element or component
    • Y10T428/249924—Noninterengaged fiber-containing paper-free web or sheet which is not of specified porosity
    • Y10T428/24994—Fiber embedded in or on the surface of a polymeric matrix
    • Y10T428/249942—Fibers are aligned substantially parallel
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/31504—Composite [nonstructural laminate]
    • Y10T428/31511—Of epoxy ether
    • Y10T428/31515—As intermediate layer

Definitions

  • Composite material in particular multi-layer material and adhesive or
  • the invention relates to a composite material according to the preamble of claim 1 and in particular to a composite material consisting of a ceramic layer and at least one provided on this ceramic layer metallization or metal layer.
  • the invention further relates to an adhesive or bonding material according to the preamble of claim 18.
  • the production of composite materials is also known as printed circuit boards in the form of metal-ceramic substrates according to the so-called DCB process.
  • DCB direct copper-bond-technology
  • the metallization required for the formation of traces, terminals, etc., on a ceramic e.g. on an aluminum-oxide-ceramic by means of the so-called "direct copper-bond-technology" (DCB) applied, using the metallization forming metal or copper foils or metal or copper sheets having on their surface sides a Layer or a coating (reflow layer) of a chemical compound of the metal and a reactive gas, preferably oxygen.
  • DCB direct copper-bond-technology
  • this layer or coating forms a eutectic with a melting temperature below the melting temperature of the metal (eg copper), so that by laying the film on the ceramic and by heating all the layers they can be joined together, by melting the metal or copper substantially only in the region of the reflow layer or oxide layer.
  • the metal eg copper
  • This DCB method then has, for example, the following method steps: > Oxidizing a copper foil so that a uniform copper oxide layer results;
  • Ceramic material In this method, which is used especially for the production of metal-ceramic substrates, at a temperature between about 800 - 1000 0 C, a connection between a metal foil, such as copper foil, and a ceramic substrate, such as aluminum nitride ceramic, using a Brazing produced, which in addition to a main component such as copper, silver and / or gold also contains an active metal.
  • This active metal which is, for example, at least one element of the group Hf, Ti, Zr, Nb, Ce, establishes a chemical bond between the solder and the ceramic, while the bond between the solder and the metal is a metallic braze joint ,
  • Object of the present invention is to show a composite material which can be made particularly simple and inexpensive, while maintaining the best possible thermal properties.
  • a composite material according to claim 1 is formed.
  • An adhesive or bonding material is the subject of patent claim 18.
  • the composite material according to the invention is preferably a multilayer material and preferably a circuit board for electrical circuits, modules, etc. suitable multilayer material consisting of a plate-shaped on at least one surface side of an electrically insulating material consisting of support or substrate and at least one of a metal or copper plate or metal or copper foil formed metallization, which is connected via the composite material to the substrate.
  • the composite material according to the invention has the advantage of a simple and inexpensive production. Furthermore, a compensation of different coefficients of thermal expansion of the materials of the metallization and of the substrate is achieved via the layer formed by the adhesive or bonding agent. In particular, with appropriate orientation of at least part of the nanofiber material in the bonding layer parallel or approximately parallel to the joined surfaces, an effect compensating the thermal expansion of the metallization can be achieved.
  • Multi-layer material according to the invention 3 is a schematic representation of a measuring arrangement for determining the thermal behavior of a thermal paste formed as an adhesive or a thermal adhesive according to the invention; 4 schematically shows an arrangement for preparing different samples; Fig. 5 shows the thermal resistance measured on different samples; FIG. 6 shows a comparison of the thermal resistance measured with the device of FIG. 3 for different material connections or multilayer materials.
  • 1 is a multilayer material which is suitable, for example, as a printed circuit board for electrical circuits or modules.
  • the multi-layer material consists of a plate-shaped carrier or substrate 2, which in this embodiment is made entirely of an electrically insulating material, for. B. from a
  • Ceramics such as As alumina ceramic, aluminum nitride ceramic, silicon nitride ceramic, etc.
  • Other materials are conceivable for the substrate 2, for example, plastic, for. B. epoxy-based, etc.
  • This metallization 3 is connected in a planar manner to the substrate 2 via an adhesive or bonding layer 4 formed by an adhesive or a bonding material.
  • the substrate 2 is provided on both surface sides with the metallization 3.
  • multilayer material 1 is symmetrical, at least as regards the type and sequence of the individual layers, relative to a center plane of substrate 2.
  • metallization 3 it is possible to provide metallization 3 only on one surface side of substrate 2.
  • the metallization 3 is then structured correspondingly on one side of the substrate 2 using the customary known etching and masking techniques.
  • the substrate 2 itself multi-layered, consisting of a metallic support layer 2.1 z. B. of aluminum and an insulating layer 2.2 on the surface sides of the plate-shaped substrate 2, specifically where a metallization 3 is connected via a bonding layer 4.
  • a peculiarity of the multi-layer product 1 is that the bonding layer 4 contains in a matrix suitable as an adhesive, for example in an epoxy resin matrix, carbon nanofiber material or carbon nanofiber or nanotube, so that an extremely low thermal resistance Rth (.degree. W) or vice versa, a high thermal conductivity 1 / Rth result, so a
  • Multilayer material 1 with a substrate 2 of an alumina ceramic with respect to the thermal conductivity or the thermal resistance between the upper and lower metallization 3 is quite comparable to a multilayer material, in which the metallizations are applied to the ceramic substrate using the so-called DCB method , as will be explained in more detail below.
  • the matrix contains about 5 to 30% by weight of nanofiber material based on the total weight of the adhesive or bonding material.
  • a nanofiber material is one under the
  • Polyrograf III commercially available carbon nanofiber used, which is also baked before being mixed into the matrix, if appropriate, also before a pretreatment at 3000 ° C.
  • the matrix used is an epoxy-based, for example polyester A solvent is used to obtain an optimum incorporation of the nanofiber material into the matrix material, triethylene glycol monobutyl ether being particularly suitable for this purpose.
  • FIG. 3 shows a schematic representation of an arrangement for measuring the thermal resistance caused by the bonding layer 4.
  • the arrangement consists of an upper heating plate 5, from a subsequent to this heating plate and with this for heat transfer optimally connected measuring plate 6 and from a lower measuring plate 7.
  • temperature sensors or sensors 6.1 and 7.1 are provided with the aid of which the temperature of these plates is accurately recorded and as measured values to a measuring or evaluation electronics can be forwarded.
  • the heating plate 5 is electrically operated, for example, with a heating voltage of 60 volts and with a constant heating current of, for example, 2.7 amps, so that during the measurement of the hot plate 5, a well-defined, constant amount of heat is generated.
  • the respective test piece 8 is arranged, which consists of two copper plates 9 and 10, which are connected to each other via the cured bonding layer 4.
  • the measuring plates 6 and 7 and the adjacent plates 9 and 10 each have a layer 1 1 or 12 of a conventional, in particular also known in terms of their properties Thermal compound provided.
  • FIG. 5 shows in a graph the thermal resistance Rth determined in the measurement in ° K / W for various samples, namely:
  • Position A when lying on one another, not connected by the bonding layer 4
  • Position B - E in each case with plates 9 and 10 connected to one another via the bonding layer 4, however: Position B: without further temperature treatment;
  • Position C when treating sample 8 for 2.8 days at one
  • Position D when treating the sample 8 for 6 days at a temperature of 120 0 C;
  • Position E when treating Sample 8 for 1 day at 160 ° C.
  • FIG. 5 shows that the thermal conductivity of the bonding layer 4 improves with a longer temperature influence, obviously by further hardening of this layer.
  • the measurements also showed that the thermal resistance Rth measured at each sample 8 was only initial, i. slightly decreases in an initial phase of each measurement, obviously due to inertia of the measuring system, but then remains constant at the end of this initial phase.
  • FIG. 6 shows in comparison the thermal resistance of a copper-ceramic multilayer material.
  • the thermal resistance Rth ( 0 KfW) of a sample in which the upper plate 9 made of copper rests without connection against the lower plate 10 made of ceramic (alumina ceramic).
  • the positions B and D relate to measurements in which the upper plate 9 made of copper through the bonding layer 4 with the lower plate 10 made of ceramic, namely position B - at a treatment of the sample 8 for 3 days at a temperature of 150 0 C and
  • the position C shows in comparison the thermal resistance of a DCB substrate.
  • the position E is the thermal resistance measured with the measuring device of FIG. 3, which results without the sample 8, ie. H. at immediately above the layers
  • the thermal conductivity of the bonding layer 4 can be substantially increased by the fact that the nanofibers of the nanofiber material used are optimally chosen with respect to their length, ie these fibers or at least a majority of these fibers have a length between 1 and 100 ⁇ , preferably 10 ⁇ and / or thereby in that the nanofiber material is pretreated and then optimally integrated into the matrix forming the bonding material by this pretreatment.
  • This length corresponds to the surface irregularities which are usually present in the case of ceramic substrates and / or copper foils, so that these irregularities can be bridged optimally with nanofibers of these lengths.
  • a further improvement in the thermal conductivity of the bonding layers 4 and thus an improvement in the thermal properties of the multilayer material 1 is achieved by orienting the nanofibers or nanotubes at least for the most part in the direction of the heat flow, for example by virtue of the nanofibers or nanotubes being introduced into the substrate before introduction the matrix is ferromagnetic, d. H.
  • the nanofibers or nanotubes being introduced into the substrate before introduction the matrix is ferromagnetic, d. H.
  • an optimal alignment of the nonofibers or nanotubes takes place by an external magnetic field (arrow H) in such a way that these nanofibers or nanotubes with their longitudinal extent are perpendicular or at least approximately perpendicular to the surface sides of the substrate 2 and the adjacent ones Metallization 3 are oriented in the bonding layer 4. After the bonding layer 4 has cured, the nanofibres or nanotubes are fixed in this orientation.
  • the application of the ferromagnetic material or the nanoparticles of this material to the nanofiber material or the nanofibers or nanotubes takes place by using a suitable surface-adhesion-layer-forming polymer, for example using polyanilines.
  • a further improvement of the thermal properties of the multilayer material 1 can be achieved by a compression of the bonding layer 4 after curing, for example by hooking (HI P method) or by a treatment in a vacuum, so possibly present in the respective bonding layer 4 bubbles or to close cavities.
  • the heat-conducting adhesive or the bonding material can be used not only for the production of multilayer materials or substrates, but also generally for all applications in which an adhesive bond between two components is required with simultaneous optimal heat transfer.
  • the bonding material is also electrically conductive, so it can be used optimally as an electrically conductive adhesive, ie everywhere where an electrical connection is required or required by gluing, for example, when assembling printed circuit boards with components, etc.

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Abstract

Disclosed is a multilayer material in which at least two components are joined to each other via an adhesive bond. Said adhesive bond is formed by an adhesive or bonding layer containing nanofiber material in a matrix that is suitable as an adhesive.

Description

Verbundmaterial, insbesondere Mehrschichtmaterial sowie Kleber- oder Composite material, in particular multi-layer material and adhesive or
Bondmaterialbonding material
Die Erfindung bezieht sich auf ein Verbundmaterial gemäß Oberbegriff Patentanspruch 1 und dabei insbesondere auf ein Verbundmaterial bestehend aus einer Keramikschicht und aus wenigstens einer auf dieser Keramikschicht vorgesehenen Metallisierung oder Metallschicht. Die Erfindung bezieht sich weiterhin auf ein Kleber- oder Bondmaterial gemäß Oberbegriff Patentanspruch 18.The invention relates to a composite material according to the preamble of claim 1 and in particular to a composite material consisting of a ceramic layer and at least one provided on this ceramic layer metallization or metal layer. The invention further relates to an adhesive or bonding material according to the preamble of claim 18.
Bekannt ist die Herstellung von Verbundmaterialien auch als Leiterplatten in Form von Metall-Keramik-Substraten nach dem sogenannten DCB-Prozess. Hierbei wird die für die Erzeugung von Leiterbahnen, Anschlüssen usw. benötigte Metallisierung auf einer Keramik, z.B. auf einer Aluminium-Oxid-Keramik mit Hilfe des sogenannten „DCB- Verfahrens" (Direct-Copper-Bond-Technology) aufgebracht, und zwar unter Verwendung von die Metallisierung bildenden Metall- bzw. Kupferfolien oder Metallbzw. Kupferblechen, die an ihren Oberflächenseiten eine Schicht oder einen Überzug (Aufschmelzschicht) aus einer chemischen Verbindung aus dem Metall und einem reaktiven Gas , bevorzugt Sauerstoff aufweisen.The production of composite materials is also known as printed circuit boards in the form of metal-ceramic substrates according to the so-called DCB process. Here, the metallization required for the formation of traces, terminals, etc., on a ceramic, e.g. on an aluminum-oxide-ceramic by means of the so-called "direct copper-bond-technology" (DCB) applied, using the metallization forming metal or copper foils or metal or copper sheets having on their surface sides a Layer or a coating (reflow layer) of a chemical compound of the metal and a reactive gas, preferably oxygen.
Bei diesem beispielsweise in der US-PS 37 44 120 oder in der DE-PS 23 19 854 beschriebenen Verfahren bildet diese Schicht oder dieser Überzug (Aufschmelzschicht) ein Eutektikum mit einer Schmelztemperatur unter der Schmelztemperatur des Metalls (z.B. Kupfers), so dass durch Auflegen der Folie auf die Keramik und durch Erhitzen sämtlicher Schichten diese miteinander verbunden werden können, und zwar durch Aufschmelzen des Metalls bzw. Kupfers im wesentlichen nur im Bereich der Aufschmelzschicht bzw. Oxidschicht.In this method, for example, in US-PS 37 44 120 or in DE-PS 23 19 854 described method, this layer or coating (melting layer) forms a eutectic with a melting temperature below the melting temperature of the metal (eg copper), so that by laying the film on the ceramic and by heating all the layers they can be joined together, by melting the metal or copper substantially only in the region of the reflow layer or oxide layer.
Dieses DCB-Verfahren weist dann z.B. folgende Verfahrensschritte auf: > Oxidieren einer Kupferfolie derart, dass sich eine gleichmäßige Kupferoxidschicht ergibt;This DCB method then has, for example, the following method steps: > Oxidizing a copper foil so that a uniform copper oxide layer results;
> Auflegen des Kupferfolie auf die Keramikschicht;> Placing the copper foil on the ceramic layer;
> Erhitzen des Verbundes auf eine Prozesstemperatur zwischen etwa 1025 bis 10830C, z.B. auf ca. 1071 0C;> Heating the composite to a process temperature between about 1025 to 1083 0 C, for example to about 1071 0 C;
> Abkühlen auf Raumtemperatur.> Cool to room temperature.
Bekannt ist auch das sogenannte Aktivlot-Verfahren (DE 22 13 115; EP-A-153 618) zum Verbinden von Metallisierungen bildenden Metallschichten oder Metallfolien, insbesondere auch von Kupferschichten oder Kupferfolien mit dem jeweiligenAlso known is the so-called active soldering method (DE 22 13 115, EP-A-153 618) for joining metallization-forming metal layers or metal foils, in particular also copper layers or copper foils, to the respective one
Keramikmaterial. Bei diesem Verfahren, welches speziell zum Herstellen von Metall- Keramik-Substraten verwendet wird, wird bei einer Temperatur zwischen ca. 800 - 10000C eine Verbindung zwischen einer Metallfolie, beispielsweise Kupferfolie, und einem Keramiksubstrat, beispielsweise Aluminiumnitrid-Keramik, unter Verwendung eines Hartlots hergestellt, welches zusätzlich zu einer Hauptkomponente, wie Kupfer, Silber und/oder Gold auch ein Aktivmetall enthält. Dieses Aktivmetall, welches beispielsweise wenigstens ein Element der Gruppe Hf, Ti, Zr, Nb, Ce ist, stellt durch chemische Reaktion eine Verbindung zwischen dem Lot und der Keramik her, während die Verbindung zwischen dem Lot und dem Metall eine metallische Hartlöt- Verbindung ist.Ceramic material. In this method, which is used especially for the production of metal-ceramic substrates, at a temperature between about 800 - 1000 0 C, a connection between a metal foil, such as copper foil, and a ceramic substrate, such as aluminum nitride ceramic, using a Brazing produced, which in addition to a main component such as copper, silver and / or gold also contains an active metal. This active metal, which is, for example, at least one element of the group Hf, Ti, Zr, Nb, Ce, establishes a chemical bond between the solder and the ceramic, while the bond between the solder and the metal is a metallic braze joint ,
Aufgabe der vorliegenden Erfindung ist es, ein Verbundmaterial aufzuzeigen, welches besonders einfach und preiswert gefertigt werden kann, und zwar unter Beibehaltung möglichst optimaler thermischer Eigenschaften. Zur Lösung dieser Aufgabe ist ein Verbundmaterial entsprechend dem Patentanspruch 1 ausgebildet. Ein Kleber- oder Bondmaterial ist Gegenstand des Patentanspruchs 18.Object of the present invention is to show a composite material which can be made particularly simple and inexpensive, while maintaining the best possible thermal properties. To solve this problem, a composite material according to claim 1 is formed. An adhesive or bonding material is the subject of patent claim 18.
Das erfindungsgemäße Verbundmaterial ist bevorzugt ein Mehrschichtmaterial und dabei vorzugsweise ein als Leiterplatte für elektrische Schaltkreise, Module usw. geeignetes Mehrschichtmaterial bestehend aus einem plattenförmigen zumindest an einer Oberflächenseite aus einem elektrisch isolierenden Werkstoff bestehenden Träger oder Substrat sowie aus wenigstens einer von einer Metall- oder Kupferplatte bzw. Metall- oder Kupferfolie gebildeten Metallisierung, die über das Verbundmaterial mit dem Substrat verbunden ist.The composite material according to the invention is preferably a multilayer material and preferably a circuit board for electrical circuits, modules, etc. suitable multilayer material consisting of a plate-shaped on at least one surface side of an electrically insulating material consisting of support or substrate and at least one of a metal or copper plate or metal or copper foil formed metallization, which is connected via the composite material to the substrate.
Das erfindungsgemäße Verbundmaterial weist den Vorteil einer einfachen und preiswerten Fertigung auf. Weiterhin wird über die von dem Kleber oder Bondmittel gebildete Schicht auch ein Ausgleich unterschiedlicher Temperaturausdehnungskoeffizienten der Materialien der Metallisierung und des Substrates erreicht. Insbesondere bei entsprechender Orientierung zumindest eines Teils des Nanofasermaterials in der Bond-Schicht parallel oder annähernd parallel zu den verbundenen Flächen lässt sich ein die thermische Ausdehnung der Metallisierung kompensierender Effekt erreichen.The composite material according to the invention has the advantage of a simple and inexpensive production. Furthermore, a compensation of different coefficients of thermal expansion of the materials of the metallization and of the substrate is achieved via the layer formed by the adhesive or bonding agent. In particular, with appropriate orientation of at least part of the nanofiber material in the bonding layer parallel or approximately parallel to the joined surfaces, an effect compensating the thermal expansion of the metallization can be achieved.
Weiterbildungen der Erfindung sind Gegenstand der Unteransprüche. Die Erfindung wird im Folgenden anhand der Figuren an einem Ausführungsbeispiel näher erläutert. Es zeigen:Further developments of the invention are the subject of the dependent claims. The invention will be explained in more detail below with reference to the figures of an embodiment. Show it:
Fig. 1 und 2 in vereinfachter Darstellung jeweils einen Schnitt durch ein1 and 2 in a simplified representation in each case a section through a
Mehrschichtmaterial gemäß der Erfindung; Fig. 3 in schematischer Darstellung eine Messanordnung zur Bestimmung des thermischen Verhaltens einer als Kleber ausgebildeten Wärmeleitpaste bzw. eines Wärmeleitklebers gemäß der Erfindung; Fig. 4 schematisch eine Anordnung zur Vorbereitung unterschiedlicher Proben; Fig. 5 den Wärmewiderstand, gemessen an verschiedenen Proben; Fig. 6 einen Vergleich des mit der Vorrichtung der Figur 3 gemessenen thermischen Widerstandes bei verschiedenen Materialverbindungen bzw. Mehrschichtmaterialien. In der Figur 1 ist 1 ein Mehrschicht-Material, welches beispielsweise als Leiterplatte für elektrische Schaltkreise oder Module geeignet ist. Das Mehrschichtmaterial besteht einem plattenförmigen Träger oder Substrat 2, welches bei dieser Ausführungsform insgesamt aus einem elektrisch isolierenden Werkstoff gefertigt ist, z. B. aus einerMulti-layer material according to the invention; 3 is a schematic representation of a measuring arrangement for determining the thermal behavior of a thermal paste formed as an adhesive or a thermal adhesive according to the invention; 4 schematically shows an arrangement for preparing different samples; Fig. 5 shows the thermal resistance measured on different samples; FIG. 6 shows a comparison of the thermal resistance measured with the device of FIG. 3 for different material connections or multilayer materials. In FIG. 1, 1 is a multilayer material which is suitable, for example, as a printed circuit board for electrical circuits or modules. The multi-layer material consists of a plate-shaped carrier or substrate 2, which in this embodiment is made entirely of an electrically insulating material, for. B. from a
Keramik, wie z. B. Aluminiumoxid-Keramik, Aluminiumnitrid-Keramik, Siliziumnitrid- Keramik usw. Auch andere Werkstoffe sind für das Substrat 2 denkbar, beispielsweise Kunststoff, z. B. auf Epoxy-Basis usw.Ceramics, such as As alumina ceramic, aluminum nitride ceramic, silicon nitride ceramic, etc. Other materials are conceivable for the substrate 2, for example, plastic, for. B. epoxy-based, etc.
Auf einer Oberflächenseite des Substrates 2 ist flächig eine von einer dünnen Metallplatte oder Folie, beispielsweise von einer Kupferplatte oder Kupferfolie gebildete Metallisierung 3 vorgesehen. Diese Metallisierung 3 ist über eine von einem Kleber oder einem Bondmaterial gebildete Kleber- oder Bondschicht 4 flächig mit dem Substrat 2 verbunden. Bei der dargestellten Ausführungsform ist das Substrat 2 an beiden Oberflächenseiten mit der Metallisierung 3 versehen. Das Verbund- oderOn one surface side of the substrate 2, a metallization 3 formed by a thin metal plate or foil, for example by a copper plate or copper foil, is provided flatly. This metallization 3 is connected in a planar manner to the substrate 2 via an adhesive or bonding layer 4 formed by an adhesive or a bonding material. In the illustrated embodiment, the substrate 2 is provided on both surface sides with the metallization 3. The compound or
Mehrschicht-Material 1 ist dadurch zumindest hinsichtlich Art und Folge der einzelnen Schichten symmetrisch bezogen auf eine Mittelebene des Substrates 2. Grundsätzlich ist es aber möglich die Metallisierung 3 nur an einer Oberflächenseite des Substrats 2 vorzusehen. Zur Herstellung der Leiterbahnen, Kontaktflächen usw. ist dann zumindest die Metallisierung 3 an einer Seite des Substrates 2 unter Verwendung der üblichen bekannten Ätz- und Maskierungstechniken entsprechend strukturiert.As a result, multilayer material 1 is symmetrical, at least as regards the type and sequence of the individual layers, relative to a center plane of substrate 2. In principle, however, it is possible to provide metallization 3 only on one surface side of substrate 2. For the production of the conductor tracks, contact surfaces, etc., at least the metallization 3 is then structured correspondingly on one side of the substrate 2 using the customary known etching and masking techniques.
Wie in der Figur 2 dargestellt, ist es weiterhin auch möglich das Substrat 2 selbst mehrschichtig auszubilden, und zwar bestehend aus einer metallischen Tragschicht 2.1 z. B. aus Aluminium und einer isolierenden Schicht 2.2 an den Oberflächenseiten des plattenförmigen Substrates 2, und zwar dort wo über eine Bondschicht 4 eine Metallisierung 3 anschließt. Eine Besonderheit des Mehrschichtproduktes 1 besteht darin, dass die Bondschicht 4 ■ in einer als Kleber geeigneten Matrix, beispielsweise in einer Epoxydharz-Matrix, Kohlenstoffnanofasermaterial bzw. Kohlenstoffnanofasem oder -nanotubes enthält, sodass sich für die Bondschicht ein extrem niedriger Wärmewiderstand Rth (°K/W) bzw. umgekehrt eine hohe Wärmeleitfähigkeit 1/Rth ergeben, also einAs shown in Figure 2, it is also possible to form the substrate 2 itself multi-layered, consisting of a metallic support layer 2.1 z. B. of aluminum and an insulating layer 2.2 on the surface sides of the plate-shaped substrate 2, specifically where a metallization 3 is connected via a bonding layer 4. A peculiarity of the multi-layer product 1 is that the bonding layer 4 contains in a matrix suitable as an adhesive, for example in an epoxy resin matrix, carbon nanofiber material or carbon nanofiber or nanotube, so that an extremely low thermal resistance Rth (.degree. W) or vice versa, a high thermal conductivity 1 / Rth result, so a
Mehrschichtmaterial 1 mit einem Substrat 2 aus einer Aluminiumoxyd-Keramik bezüglich der thermischen Leitfähigkeit bzw. des thermischen Widerstandes zwischen der oberen und unteren Metallisierung 3 durchaus vergleichbar mit einem Mehrschichtmaterial ist, bei dem die Metallisierungen unter Verwendung des sogenannten DCB-Verfahrens auf das Keramiksubstrat aufgebracht sind, wie dies nachstehend noch näher erläutert wird. Die Matrix enthält bezogen auf das Gesamtgewicht des Klebers oder Bondmaterials etwa 5 bis 30 Gewichts% an Nanofasermaterial.Multilayer material 1 with a substrate 2 of an alumina ceramic with respect to the thermal conductivity or the thermal resistance between the upper and lower metallization 3 is quite comparable to a multilayer material, in which the metallizations are applied to the ceramic substrate using the so-called DCB method , as will be explained in more detail below. The matrix contains about 5 to 30% by weight of nanofiber material based on the total weight of the adhesive or bonding material.
Bei einer bevorzugten Ausführungsform wird als Nanofasermaterial eine unter derIn a preferred embodiment, a nanofiber material is one under the
Bezeichnung „Pyrograf III" im Handel erhältliche Carbon-Nanofaser verwendet. Diese wird vor dem Einmischen in die Matrix, gfs. auch vor einer Vorbehandlung bei 30000C ausgeheizt. Als Matrix wird eine solche auf Epoxy-Basis, beispielsweise Polyester verwendet. Um u.a. ein optimales Einbinden des Nanofasermaterials in das Matrixmaterial zu erhalten, wird ein Lösungsmittel verwendet. Hierfür eignet sich insbesondere triethyleneglykol monobutylether."Pyrograf III" commercially available carbon nanofiber used, which is also baked before being mixed into the matrix, if appropriate, also before a pretreatment at 3000 ° C. The matrix used is an epoxy-based, for example polyester A solvent is used to obtain an optimum incorporation of the nanofiber material into the matrix material, triethylene glycol monobutyl ether being particularly suitable for this purpose.
Die Figur 3 zeigt in schematischer Darstellung eine Anordnung zur Messung des durch die Bondschicht 4 bedingten thermischen Widerstandes. Die Anordnung besteht aus einer oberen Heizplatte 5, aus einer an diese Heizplatte anschließenden und mit dieser für eine Wärmeübertragung optimal verbundenen Messplatte 6 sowie aus einer unteren Messplatte 7. An den Messplatten 6 und 7 sind Temperaturfühler bzw. -Sensoren 6.1 bzw. 7.1 vorgesehen, mit deren Hilfe die Temperatur dieser Platten exakt erfasst und als Messwerte an eine Mess- oder Auswertelektronik weitergeleitet werden können. Die Heizplatte 5 wird elektrisch betrieben, und zwar beispielsweise mit einer Heizspannung von 60 Volt und mit einem konstanten Heizstrom von beispielsweise 2,7 Ampere, sodass während des Messvorgangs von der Heizplatte 5 eine genau definierte, konstante Wärmemenge erzeugt wird.FIG. 3 shows a schematic representation of an arrangement for measuring the thermal resistance caused by the bonding layer 4. The arrangement consists of an upper heating plate 5, from a subsequent to this heating plate and with this for heat transfer optimally connected measuring plate 6 and from a lower measuring plate 7. At the measuring plates 6 and 7 temperature sensors or sensors 6.1 and 7.1 are provided with the aid of which the temperature of these plates is accurately recorded and as measured values to a measuring or evaluation electronics can be forwarded. The heating plate 5 is electrically operated, for example, with a heating voltage of 60 volts and with a constant heating current of, for example, 2.7 amps, so that during the measurement of the hot plate 5, a well-defined, constant amount of heat is generated.
Zwischen den beiden Messplatten 6 und 7 ist der jeweilige Prüfling 8 angeordnet, der aus zwei Kupferplatten 9 und 10 besteht, die über die ausgehärtete Bondschicht 4 miteinander verbunden sind. Um einen möglichst verlustfreien Wärmeübergang zwischen dem Prüfling 8 und den Messplatten 6 und 7 zu erreichen, ist zwischen den Messplatten 6 und 7 und den benachbarten Platten 9 und 10 jeweils eine Schicht 1 1 bzw. 12 aus einer herkömmlichen, insbesondere auch hinsichtlich ihrer Eigenschaften bekannten Wärmeleitpaste vorgesehen.Between the two measuring plates 6 and 7, the respective test piece 8 is arranged, which consists of two copper plates 9 and 10, which are connected to each other via the cured bonding layer 4. In order to achieve a loss-free heat transfer between the specimen 8 and the measuring plates 6 and 7, between the measuring plates 6 and 7 and the adjacent plates 9 and 10 each have a layer 1 1 or 12 of a conventional, in particular also known in terms of their properties Thermal compound provided.
Der thermische Widerstand Rth ist dabei, wie folgt, definiert: Rth (°K/W) = (T1 - T2) / Leistung des Heizers 5 in W. Die thermische Leitfähigkeit ist dann 1/Rth.The thermal resistance Rth is defined as follows: Rth (° K / W) = (T1-T2) / power of the heater 5 in W. The thermal conductivity is then 1 / Rth.
Die Figur 5 zeigt in einer Graphik den bei der Messung ermittelten Wärmewiderstand Rth in °K/W für verschiedene Proben, und zwar:FIG. 5 shows in a graph the thermal resistance Rth determined in the measurement in ° K / W for various samples, namely:
Position A: bei aufeinander liegenden, nicht durch die Bondschicht 4 verbundenenPosition A: when lying on one another, not connected by the bonding layer 4
Platten 9 und 10; Position B - E: jeweils bei über die Bondschicht 4 miteinander verbundenen Platten 9 und 10, jedoch: Position B: ohne weitere Temperaturbehandlung;Plates 9 and 10; Position B - E: in each case with plates 9 and 10 connected to one another via the bonding layer 4, however: Position B: without further temperature treatment;
Position C: bei einer Behandlung der Probe 8 über 2,8 Tage bei einerPosition C: when treating sample 8 for 2.8 days at one
Temperatur von 120 0C;Temperature of 120 0 C;
Position D: bei einer Behandlung der Probe 8 über 6 Tage bei einer Temperatur von 120 0C; Position E: bei einer Behandlung der Probe 8 über 1 Tag bei 160 0C.Position D: when treating the sample 8 for 6 days at a temperature of 120 0 C; Position E: when treating Sample 8 for 1 day at 160 ° C.
Die Figur 5 zeigt, dass sich die thermische Leitfähigkeit der Bondschicht 4 bei einer längeren Temperatureinwirkung verbessert, offensichtlich durch weiteres Aushärten dieser Schicht. Die Messungen haben weiterhin ergeben, dass der an der jeweiligen Probe 8 gemessene thermische Widerstand Rth nur anfänglich, d.h. in einer Anfangsphase jeder Messung leicht abnimmt, und zwar offensichtlich bedingt durch Trägheit des Messsystems, dann nach Ablauf dieser Anfangsphase aber konstant bleibt.FIG. 5 shows that the thermal conductivity of the bonding layer 4 improves with a longer temperature influence, obviously by further hardening of this layer. The measurements also showed that the thermal resistance Rth measured at each sample 8 was only initial, i. slightly decreases in an initial phase of each measurement, obviously due to inertia of the measuring system, but then remains constant at the end of this initial phase.
Die Figur 6 zeigt im Vergleich den thermischen Widerstand eines Kupfer-Keramik- Mehrschichtmaterials. Für diese Messung wurden anstelle der Proben 8 mit den beiden Kupferplatten 9 und 10 Proben verwendet, bei denen die untere KupferplatteFIG. 6 shows in comparison the thermal resistance of a copper-ceramic multilayer material. For this measurement, instead of the samples 8 with the two copper plates 9 and 10 samples were used, in which the lower copper plate
10 durch eine Keramikplatte oder durch ein Keramiksubstrat gleicher Größe ersetzt ist. Dargestellt ist in der Figur 6 in der Position A der thermische Widerstand Rth (0KfW) einer Probe, bei der die obere Platte 9 aus Kupfer ohne Verbindung gegen die untere Platte 10 aus Keramik (Aluminiumoxid-Keramik) anliegt. Die Positionen B und D betreffen Messungen, bei denen die obere Platte 9 aus Kupfer über die Bondschicht 4 mit der unteren Platte 10 aus Keramik verbunden ist, und zwar Position B - bei einer Behandlung der Probe 8 über 3 Tage bei einer Temperatur von 150 0C und10 is replaced by a ceramic plate or by a ceramic substrate of the same size. Shown in Figure 6 in the position A, the thermal resistance Rth ( 0 KfW) of a sample in which the upper plate 9 made of copper rests without connection against the lower plate 10 made of ceramic (alumina ceramic). The positions B and D relate to measurements in which the upper plate 9 made of copper through the bonding layer 4 with the lower plate 10 made of ceramic, namely position B - at a treatment of the sample 8 for 3 days at a temperature of 150 0 C and
Position D - ohne eine weitere Behandlung der Probe 8.Position D - without further treatment of sample 8.
Die Position C zeigt im Vergleich den thermischen Widerstand eines DCB-Substrates. Die Position E ist der mit der Messvorrichtung der Figur 3 gemessene thermische Widerstand, der sich ohne die Probe 8 ergibt, d. h. bei unmittelbar über die SchichtenThe position C shows in comparison the thermal resistance of a DCB substrate. The position E is the thermal resistance measured with the measuring device of FIG. 3, which results without the sample 8, ie. H. at immediately above the layers
11 und 12 gegeneinander anliegenden Messplatten 6 und 7.11 and 12 abutting measuring plates 6 and 7.
Es versteht sich, dass bei allen Messungen jeweils Platten 9 und 10 gleicher Größe verwendet wurden. Die thermische Leitfähigkeit der Bondschicht 4 kann wesentlich dadurch gesteigert werden, dass die Nanofasern des verwendeten Nanofasermaterials hinsichtlich ihrer Länge optimal gewählt werden, d. h. diese Fasern oder zumindest ein Großteil dieser Fasern eine Länge zwischen 1 und 100 μ, vorzugsweise 10μ aufweist und/oder aber dadurch, dass das Nanofasermaterial vorbehandelt und durch diese Vorbehandlung dann in die das Bondmaterial bildende Matrix optimal eingebunden wird. Diese Länge entspricht den üblicherweise bei Keramiksubstraten und/oder Kupferfolien vorhandenen Oberflächenunebenheiten, so dass diese Unebenheiten mit Nanofasern dieser Längen möglichst optimal überbrückt werden können.It is understood that in all measurements plates 9 and 10 of the same size were used. The thermal conductivity of the bonding layer 4 can be substantially increased by the fact that the nanofibers of the nanofiber material used are optimally chosen with respect to their length, ie these fibers or at least a majority of these fibers have a length between 1 and 100 μ, preferably 10μ and / or thereby in that the nanofiber material is pretreated and then optimally integrated into the matrix forming the bonding material by this pretreatment. This length corresponds to the surface irregularities which are usually present in the case of ceramic substrates and / or copper foils, so that these irregularities can be bridged optimally with nanofibers of these lengths.
Eine weitere Verbesserung der thermischen Leitfähigkeit der Bondschichten 4 und damit eine Verbesserung der thermischen Eigenschaften des Mehrschichtmaterials 1 wird dadurch erreicht, dass die Nanofasern oder Nanotubes zumindest zum Großteil in Richtung des Wärmeflusses orientiert werden, beispielsweise dadurch, dass die Nanofasern oder Nanotubes vor dem Einbringen in die Matrix ferromagnetisch ausgebildet, d. h. beispielsweise mit Nanopartikeln aus einem ferromagnetischen Material überzogen werden. Beim Herstellen des Mehrschichtmaterials 1 erfolgt dann durch ein äußeres Magnetfeld (Pfeil H) ein optimales Ausrichten der Nonofasern bzw. Nanotubes in der Weise, dass diese Nanofasern bzw. Nanotubes mit ihrer Längserstreckung senkrecht oder zumindest annähernd senkrecht zu den Oberflächenseiten des Substrates 2 und der benachbarten Metallisierung 3 in der Bondschicht 4 orientiert sind. Nach dem Aushärten der Bondschicht 4 sind die Nanofasern bzw. Nanotubes in dieser Orientierung fixiert.A further improvement in the thermal conductivity of the bonding layers 4 and thus an improvement in the thermal properties of the multilayer material 1 is achieved by orienting the nanofibers or nanotubes at least for the most part in the direction of the heat flow, for example by virtue of the nanofibers or nanotubes being introduced into the substrate before introduction the matrix is ferromagnetic, d. H. For example, be coated with nanoparticles of a ferromagnetic material. When producing the multilayer material 1, an optimal alignment of the nonofibers or nanotubes takes place by an external magnetic field (arrow H) in such a way that these nanofibers or nanotubes with their longitudinal extent are perpendicular or at least approximately perpendicular to the surface sides of the substrate 2 and the adjacent ones Metallization 3 are oriented in the bonding layer 4. After the bonding layer 4 has cured, the nanofibres or nanotubes are fixed in this orientation.
Das Aufbringen des ferromagnetischen Materials bzw. der Nanopartikel aus diesem Material auf das Nanofasermaterial bzw. die Nanofasern oder Nanotubes erfolgt unter Verwendung eines geeigneten, eine Oberflächenhaftschicht bildenden Polymers, beispielsweise unter Verwendung von Polyaniline. Eine weitere Verbesserung der thermischen Eigenschaften des Mehrschichtmaterials 1 lässt sich durch eine Kompression der Bondschicht 4 nach dem Aushärten erreichen, und zwar beispielsweise durch Hippen (H I P- Verfahren) oder durch eine Behandlung im Vakuum, um so eventuell in der jeweiligen Bondschicht 4 vorhandene Blasen oder Hohlräume zu schließen.The application of the ferromagnetic material or the nanoparticles of this material to the nanofiber material or the nanofibers or nanotubes takes place by using a suitable surface-adhesion-layer-forming polymer, for example using polyanilines. A further improvement of the thermal properties of the multilayer material 1 can be achieved by a compression of the bonding layer 4 after curing, for example by hooking (HI P method) or by a treatment in a vacuum, so possibly present in the respective bonding layer 4 bubbles or to close cavities.
Die Erfindung wurde voranstehend an einem Ausführungsbeispiel beschrieben. Es versteht sich, dass zahlreiche Änderungen sowie Abwandlungen möglich sind, ohne das dadurch der der Erfindung zugrunde liegende Erfindungsgedanke verlassen wird.The invention has been described above by means of an embodiment. It is understood that numerous changes and modifications are possible without thereby departing from the inventive idea underlying the invention.
Insbesondere kann der Wärmeleitkleber bzw. das Bondmaterial nicht nur für die Herstellung von Mehrschichtmaterialien bzw. -Substraten, sondern auch generell für alle Anwendungen eingesetzt werden, bei denen eine klebende Verbindung zwischen zwei Komponenten bei gleichzeitiger optimaler Wärmeübertragung erforderlich ist.In particular, the heat-conducting adhesive or the bonding material can be used not only for the production of multilayer materials or substrates, but also generally for all applications in which an adhesive bond between two components is required with simultaneous optimal heat transfer.
Durch das Nanofasermaterial auf Kohlenstoffbasis ist das Bondmaterial auch elektrisch leitend, es kann somit in optimaler Weise auch als elektrisch leitender Kleber, d. h. überall dort eingesetzt werde, wo eine elektrische Verbindung durch Kleben gewünscht oder erforderlich ist, beispielsweise beim Bestücken von Leiterplatten mit Bauteilen usw. Due to the carbon-based nanofiber material, the bonding material is also electrically conductive, so it can be used optimally as an electrically conductive adhesive, ie everywhere where an electrical connection is required or required by gluing, for example, when assembling printed circuit boards with components, etc.
BezugszeichenlisteLIST OF REFERENCE NUMBERS
1 Mehrschichtmaterial 2 Substrat1 multilayer material 2 substrate
2.1 Trägermaterial2.1 carrier material
2.2 Isolierschicht2.2 Insulating layer
3 Metallisierung3 metallization
4 Kleber- oder Bondschicht 5 Heizplatte4 adhesive or bonding layer 5 heating plate
6, 7 Messplatte6, 7 measuring plate
8 Probe8 sample
9, 10 Platte9, 10 plate
1 1 , 12 Schicht aus Wärmeleitpaste 1 1, 12 layer of thermal compound

Claims

Patentansprüche claims
1. Verbundmaterial, insbesondere Mehrschichtmaterial, bestehend aus wenigstens zwei Komponenten (2, 3), die an einander benachbarten und für eine Wärmeübertragung vorgesehenen Flächen durch eine Klebeverbindung (4) miteinander verbunden sind, dadurch gekennzeichnet, dass die Klebeverbindung von einer Nanofasermaterial enthaltenden Kleber- oder Bondschicht (4) gebildet ist, die das Nanofasermaterial in einer als Kleber geeigneten Kunststoff-Matrix enthält.1. Composite material, in particular multi-layer material, consisting of at least two components (2, 3), which are connected to one another by an adhesive connection (4) on adjacent surfaces intended for heat transfer, characterized in that the adhesive bond is formed by an adhesive material containing nanofiber material. or bonding layer (4) is formed, which contains the nanofiber material in a plastic matrix suitable as an adhesive.
2. Verbundmaterial nach Anspruch 1, dadurch gekennzeichnet, dass die Bondschicht (4) aus einer Matrix auf Epoxy-Basis besteht.2. Composite material according to claim 1, characterized in that the bonding layer (4) consists of an epoxy-based matrix.
3. Verbundmaterial nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass das Nanofasermaterial bzw. die dieses Material bildenden Nanofasern oder3. Composite material according to claim 1 or 2, characterized in that the nanofiber material or the material forming nanofibers or
Nanotubes zumindest zum Großteil in einer Achsrichtung senkrecht zu den einander benachbarten Flächen orientiert sind.Nanotubes are oriented at least for the most part in an axial direction perpendicular to the adjacent surfaces.
4. Verbundmaterial nach Anspruch 3, dadurch gekennzeichnet, dass das Nanofasermaterial bzw. die dieses Material bildenden Nanofasern oder4. Composite material according to claim 3, characterized in that the nanofiber material or the material forming nanofibers or
Nanotubes für das Ausrichten bzw. Orientieren durch ein äußeres Magnetfeld ferromagnetisch ausgebildet sind.Nanotubes are designed ferromagnetic for aligning or orienting by an external magnetic field.
5. Verbundmaterial nach Anspruch 4, dadurch gekennzeichnet, dass das Nanofasermaterial bzw. die dieses Material bildenden Nanofasern und/oder5. Composite material according to claim 4, characterized in that the nanofiber material or the material forming nanofibers and / or
Nanotubes mit Nanopartikeln ferromagnetisch sind, beispielsweise mit einem ferromagnetischen Material, z.B. mit Fe2θ3 versehen bzw. beschichtet sind. Nanotubes with nanoparticles are ferromagnetic, for example, provided with a ferromagnetic material, eg with Fe2θ3 or coated.
6. Verbundmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass die Matrix eine Matrix auf Epoxy-Basis ist.6. Composite material according to one of the preceding claims, characterized in that the matrix is an epoxy-based matrix.
7. Verbundmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass die Matrixkomponente Polyester ist.7. Composite material according to one of the preceding claims, characterized in that the matrix component is polyester.
8. Verbundmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass die Matrix bezogen auf das Gesamtgewicht 5 - 30 Gewichts% Nanofasermaterial enthält.8. Composite material according to one of the preceding claims, characterized in that the matrix based on the total weight 5 to 30% by weight of nanofiber material.
9. Verbundmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass als Nanofasern der Bezeichnung „Pyrograf IM" verwendet werden.9. Composite material according to one of the preceding claims, characterized in that are used as nanofibers the name "Pyrograf IM".
10. Verbundmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass das Nanofasermaterial vor dem Einbringen in die Matrix in einer Vorbehandlung bei 30000C ausgeheizt wurde.10. Composite material according to one of the preceding claims, characterized in that the nanofiber material was baked before being introduced into the matrix in a pretreatment at 3000 0 C.
11. Verbundmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass das Einbringen des Nanofasermaterials in die Matrix unter11. Composite material according to one of the preceding claims, characterized in that the introduction of the nanofiber material into the matrix below
Verwendung eines Lösungsmittel, beispielsweise unter Verwendung von Triethyleneglykol Monobutylether erfolgt.Use of a solvent, for example, using triethylene glycol monobutyl ether.
12. Verbundmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass eine Komponente des Verbundmaterials zumindest an der mit der weiteren Komponente verbundenen Oberfläche aus einem elektrisch isolierenden Material und die weitere Komponente aus Metall, beispielsweise aus Kupfer besteht. 12. Composite material according to one of the preceding claims, characterized in that a component of the composite material at least at the surface connected to the further component of an electrically insulating material and the further component consists of metal, for example copper.
13. Verbundmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass die eine Komponente ein plattenförmiger Träger oder ein plattenförmiges Substrat (2) ist, und dass auf das Substrat (2) beidseitig jeweils über eine Bondschicht (4) eine Metallschicht (3) aufgebracht ist.13. The composite material according to any one of the preceding claims, characterized in that the one component is a plate-shaped carrier or a plate-shaped substrate (2), and that applied to the substrate (2) on both sides in each case via a bonding layer (4) has a metal layer (3) is.
14. Verbundmaterial nach Anspruch 9 oder 10, dadurch gekennzeichnet, dass die eine Komponente ein Keramik-Substrat, beispielsweise ein Substrat aus einer Aluminiumoxid, Aluminiumnitrid und/oder Siliziumnitrid-Keramik ist.14. Composite material according to claim 9 or 10, characterized in that the one component is a ceramic substrate, for example a substrate made of an aluminum oxide, aluminum nitride and / or silicon nitride ceramic.
15. Verbundmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass das Nanofasermaterial zumindest an seiner Oberfläche chemisch vorbehandelt ist.15. Composite material according to one of the preceding claims, characterized in that the nanofiber material is chemically pretreated at least on its surface.
16. Verbundmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass die wenigstens eine Klebeschicht (4) nach dem Aushärten durch Kompression, beispielsweise durch Hippen oder durch Behandlung im Vakuum verdichtet ist.16. Composite material according to one of the preceding claims, characterized in that the at least one adhesive layer (4) is compacted after curing by compression, for example by dipping or by treatment in a vacuum.
17. Verbundmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass das Nanofasermaterial solches auf Carbon- odr17. Composite material according to one of the preceding claims, characterized in that the nanofiber material such on carbon odr
Kunststoffbasis ist.Plastic base is.
18. Kleber oder Bondmaterial zum klebenden Verbinden von wenigstens zwei einander benachbarten und für eine Wärmeübertragung bestimmten Flächen, bestehend aus einer als Kleber geeigneten Matrix, dadurch gekennzeichnet, dass die Matrix Nanofasermaterial enthält. 18. adhesive or bonding material for adhesively bonding at least two adjacent surfaces intended for heat transfer, consisting of a matrix suitable as an adhesive, characterized in that the matrix contains nanofiber material.
19. Bondmaterial nach Anspruch 18, dadurch gekennzeichnet, dass die Matrix eine Matrix auf Epoxy-Basis ist.19. Bonding material according to claim 18, characterized in that the matrix is an epoxy-based matrix.
20. Bondmaterial nach Anspruch 18 oder 19, dadurch gekennzeichnet, dass die Matrixkomponente Polyester ist.20. Bonding material according to claim 18 or 19, characterized in that the matrix component is polyester.
21. Bondmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass die Matrix bezogen auf das Gesamtgewicht 5 - 30 Gewichts% Nanofasermaterial enthält.21. Bonding material according to one of the preceding claims, characterized in that the matrix based on the total weight 5 - contains 30% by weight of nanofiber material.
22. Bondmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass als Nanofasern der Bezeichnung „Pyrograf IM" verwendet werden.22. Bonding material according to one of the preceding claims, characterized in that are used as nanofibers the name "Pyrograf IM".
23. Bondmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass das Nanofasermaterial vor dem Einbringen in die Matrix in einer Vorbehandlung bei 30000C ausgeheizt wurde.23. Bonding material according to one of the preceding claims, characterized in that the nanofiber material was baked before being introduced into the matrix in a pretreatment at 3000 0 C.
24. Bondmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass das Einbringen des Nanofasermaterials in die Matrix unter24. Bonding material according to one of the preceding claims, characterized in that the introduction of the nanofiber material in the matrix below
Verwendung eines Lösungsmittel, beispielsweise unter Verwendung von Triethyleneglykol Monobutylether erfolgt.Use of a solvent, for example, using triethylene glycol monobutyl ether.
25. Bondmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass das Nanofasermaterial mit einem ferromagnetischen25. Bonding material according to one of the preceding claims, characterized in that the nanofiber material with a ferromagnetic
Material versehen, beispielsweise beschichtet ist.Material provided, for example, is coated.
26. Bondmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass das Nanofasermaterial zumindest an seiner Oberfläche chemisch vorbehandelt ist.26. Bond material according to one of the preceding claims, characterized in that the nanofiber material at least on its surface chemically pretreated.
27. Bondmaterial nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass das Nanofasermaterial solches auf Carbon- odr Kunststoffbasis ist. 27. Bonding material according to one of the preceding claims, characterized in that the nanofiber material is such on carbon odr plastic base.
EP06820829A 2005-12-23 2006-08-10 Composite material, especially multilayer material, and adhesive or bonding material Withdrawn EP1963455A1 (en)

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PCT/IB2006/003030 WO2007072126A1 (en) 2005-12-23 2006-08-10 Composite material, especially multilayer material, and adhesive or bonding material

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