SOFT MAGNETIC ANISOTROPIC COMPOSITE MATERIALS
The present invention concerns a new soft magnetic anisotropic composite material as well as a process for the preparation of this material.
The new composite material is characterized by high saturation flux density, high maximum permeability and low eddy current losses. These properties are the result of a considerably improved green density and indicate that the new composite material would be suitable for devices operating at power frequencies between 5.0 and 5000 Hz, e.g. relays, transformers, inductors and for magnetic shielding as well as for certain types of mo¬ tors. The material can also be used for devices opera¬ ting up to 50 kHz without significant eddy current losses. In brief, the new high density composite material consists of compacted, flaky shaped iron particles bonded together by a non-magnetic organic resin, whereby the particles are aligned in an essentially parallel re¬ lationship. The high density, which in this context means a density above 7.4 q/crY , is mainly the result of the flaky form of the particles in combination with cer¬ tain process steps such as the soft annealing step de¬ scribed below.
Materials of flaky shaped particles have previously been proposed for magnetic applications. Specifically, and contrary to the present invention, these materials are intended for static magnetic components such as mag¬ netic cores. Thus the US patents 2 937 964 and 3 255 052 both concern magnetic cores made of flaky shaped parti- cles of a nickel based alloy which also includes iron and molybdenum. According to the US patents the parti¬ cles are insulated by a plurality of layers including i . a. silicate. The article "Compressed Iron Motor Core for Electric Motors" by Kiyoshi Fukui et al. in IEEE Trans- actions on Magnetics, September 1972, describes the use
of flaky electrolytic iron and spherical atomised iron powders of different sizes in compressed iron powder cores for small electric motors. The article "A lami¬ nated flake-iron powder material for use at audio and ultrasonic frequencies", Soft magnetic materials in
Telecommunications, Pergamon Press, London 1953 pp 268 - 277 discloses an flaky shaped iron powder having a den¬ sity of about 7.0
which is taught not to be useful for power frequencies. According to the present invention the new material is a soft magnetic, amsotropic composite material, which essentially consists of compacted, essentially flaky shaped, electrically insulared particles, which have been prepared by cold rolling and disintegration of an essentially pure iron powder. The particles are aligned in an essentially parallel relationship and bonded together by an organic polymer resin in an amount of 0.15 to 0.75 % by weight. The diameter of the parti¬ cles is 3 to 35 times the thickness, preferably 5 to 20. A characterizing feature of the new material is the high density of at least 7.4 g/cm
3.
The present invention also concerns a process for the preparation of the composite material comprising the following steps:
a) cold rolling essentially pure iron powder into es¬ sentially flake shaped particles, b) disintegration of the rolled powder to a maximum particle size of 500 micron c) soft annealing the resulting powder at a temperature of 700 to 900 °C in a reducing atmosphere, such as H2 atmosphere,
d) disintegrating of the annealed powder in order to obtain essentially the same particle size distribution as in step b) e) mixing the powder with an organic binder resin, f) feeding the obtained mixture into a pressing tool such that the flakes are aligned in the tool in a substantially parallel relationship, g) compacting the material, h) removing the compacted material from the pressing tool and, optionally, i) stress relieving the material at an elevated temperature.
The starting material for the process is suitably an iron powder prepared by a conventional method, such as atomisation or direct reduction of iron ore partic¬ les. This powder is then annealed in order to reduce the content of impurities, such as carbon and oxygen, and to soften the iron. This operation is preferably carried out in a reducing atmosphere at a temperature of about 750-1000°C. The obtained powder contains less than C... % by weight of carbon. Powders of this type are avail¬ able from Hoganas AB, Sweden as ASC 100.29, which is ar. atomised powder containing less than 0.005 % by weight of carbon and NC 100.24 which is a sponge iron powder containing less than 0.01 % by weight of carbon. The oxygen contents are approximately 0.09 and 0.40% by weight, respectively. The annealed particles are ther. cold rolled into essentially flaky shape and disinte¬ grated such that the diameter of the particles are 3 tc 35 times the thickness and the maximum (diameter) par¬ ticle size is about 500 μm. The flaky shaped particles thus obtained are then soft annealed at a temperature lr. the range of 700-900°C in a reducing e.g. H2 atmosphere. In contrast to previously used soft annealing processes
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in this field, the annealing process according to the invention is carried out at lower temperature and no inert inorganic powder material, such as aluminia, has to be added before the heating in order to prevent sin- tering. As a consequence no step for removing the inert material is included in the process according to the present invention. After the soft annealing step the carbon and oxygen contents of the annealed products are essentially the same as before this step. In order to secure the correct particle size distribution the annea¬ led particles are subjected to an additional disintegra¬ tion step. According to a preferred embodiment of the invention the iron flakes are then subjected to a phos¬ phoric acid treatment in aqueous solution. The iron particles are subjected to the phosphoric acid at a temperature and for a time sufficient to form a thin electrically insulation layer around the individual iron flakes .
After the phosphoric acid treatment the powder is dried and mixed with an organic binder resin in an amount of less than 1 % by weight, preferably between 0.15 and 0.75% by weight and most preferably between 0.30 and 0.70 % by weight of the iron powder. If the binder content is less than 0.3 % the edge brittleness increases rapidly and makes the material hard to ma¬ chine. The organic binder could be selected from ther- mosetting or thermoplastic resins and is preferably se¬ lected from the group consisting of epoxy resins such as Araldite, PPS (polyphenylene sulphide) or PEEK (polyetherether ketone) .
The mixture of iron flakes and organic binder is then fed into a pressing tool such that the flakes are aligned in the tool in a substantially parallel rela¬ tionship. This can be accomplished by allowing the flakes to fall freely into the die from a funnel which is positioned over the die, by vibrations, by magnetic
alignment or combinations thereof. The pressing tool could optionally be evacuated before the compaction of the flaky material, and, if the organic binder used is a thermoplastic resin, the material should be heated to a temperature above the melting point of the thermoplastic resin before the compacting step. The evacuation step is especially preferred if very high densities are re¬ quired, and it has been found that va-cuum pressing in¬ creases the density by about 0.1 g/cm3 which under cer- tain circumstances is of great importance. Generally, the compacting step is carried out as a high-pressure isostatic or uniaxial pressing at pressures in the range of 400-1000 MPa. The compacting temperatures vary depending on the type of binder and the intended use of the final product. For epoxy resins the compacting step could e.g. be carried out at 70°C and a curing step might be carried out at 70-100°C. For PPS and PEEK type of resins the compacting could be carried out at 300°C and the crosslinking at 400-450°C. The compacting times are not critical but should be relatively short, such as 5-20 s, for economical reasons.
When removed from the pressing tool, the compacted material is either stress relieved at an elevated tem¬ perature or subjected to an elevated temperature and subsequently to a controlled cooling.
Due to the high densities, up to 7.58 g/cm3, the properties of the new material are unique and similar to those of stacked 35-50 μm thick sheets of pure iron separated by very thin electric isolators. Thus, the bandwidth of the soft magnetic composite material can be as high as 100 kHz, the saturation flux density more than 1.9 Tesla and the maximum permeability, μmax. •= 400. The mechanical properties of new material seem to have an optimum of about 150 MPa at a binder content of 0.35-0.50% by weight.
The invention is further illustrated by the follow¬ ing non-limiting example:
An atomised iron powder, ASC 100.29 (commercially available from Hoganas AB, Sweden) was used as base ma- terial for the new material according to the invention. The base powder consisted of irregularly, uniaxially shaped particles, which were rolled between two steel rolls in such a way that virtually each particle without contact with other particles was subjected to a press force corresponding to 3 ton/cm. After rolling the pow¬ der was disintegrated in order to separate particles which have stuck to each other during rolling, in order to obtain a powder having a maximum particle size of 42C μm. The obtained powder was in the form of flaky shapeα particles having an average diameter of 250 μm and a thickness of 35 μm.
The powder was very hard as it has been subjected to strong deformation and, as a consequence, it was dif¬ ficult to compact. The density when compacting at 800 MPa was 6.8 g/cm3. The powder was soft annealed m a re¬ ducing H2 atmosphere at 750°C during 45 minutes. At th_r temperature the iron powder could be soft annealed es¬ sentially without risking that the powder particles s_* - tered together. After the annealing step another disintegrating c: the powder was carried out in order to restore its par¬ ticle size distribution without deforming the particle which would once more result in hardening due to defor¬ mation. Bodies compacted with this powder had a density of 7.45 g/cm3 (800 MPa) , which can be compared with thr_ density of the base material of 7.3 g/cm3.
A thin insulating layer on the ron flakes was prc- vided by subjecting the powder to a treatment with aque¬ ous phosphoric acid. The oxygen and phosphorus contents of the obtained flakes were 0.41 and 0.02 % by weight, respectively.
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The obtained powder was subsequently mixed with different amounts (from 0.2 to 1.0% by weight) of Araldite LY 5052, an epoxy resin available from Ciba- Geigy, and was compacted to ring cores for measuring of magnetic properties. After the compacting operation the ring cores were heated (80°C, 2 h) , for curing of the epoxy binder. By compacting (800 MPa) the powder mixture in vacuum in an uniaxial tool a density of 7.58 g/cm3 was obtained when the content of epoxy binder was 0.6% by weight. On average the vacuum compacting gave 0.1 g/cm3 higher densities than conventional compacting in uniaxial tools. Densities of at least 7.4 g/cm3 were ob¬ served for all components based on powders having an epoxy content between 0.2 and 0.7 also with conventional compacting.
A comparison between the results obtained with the material according to the present invention and a con¬ ventional material is given below.