Magnetic dielectric resin composition and application thereof

Abstract

The invention provides a magnetic dielectric resin composition and application thereof. The magnetic dielectric resin composition comprises a combination of resin and a composite hexagonal magnetic filler, the composite hexagonal magnetic filler comprises a combination of BaCoFe6O11, A (FexB1-x) O3 and (BayC8-y) Fe4O15, A comprises any one or a combination of at least two of Ba, Sr or La, B comprises any one or a combination of at least two of Ti, Ca, Bi, Co, Ni, Ir, Mn, Mg, Mo, Nb, Nd, Sr, V, Zn, Zr, La or Si, and C comprises any one or a combination of at least two of Ti, Ca, Bi, Co, Ni, Ir, Mn, Mg, Mo, Nb, Nd, Sr, V, Zn, Zr, La, Si or Li. The magnetic dielectric resin composition has high magnetic conductivity, high frequency and low magnetic loss.

Description

Technical Field

[0001] The invention belongs to the technical field of laminated boards and relates to a magnetic dielectric resin composition and application thereof. Background Art

[0002] With the development of emerging micro-processing technologies such as microelectronics and micro-mechanics, and in the context of high-density mounting technology, driver capacitors, integrated circuits, circuit modules, antenna RF modules, etc. are constantly moving towards miniaturization. As a key component in radar and modern wireless communication systems, as well as a bottleneck in miniaturization, antenna size reduction has attracted great attention.

[0003] One way to reduce the size of the antenna is to use high dielectric materials. CN103101252A and CN103351578A disclose high dielectric constant plates, which can reduce the size of the antenna. However, this method will reduce the gain of the antenna and reduce the overall performance of the antenna.

[0004] Another way to reduce the size of the antenna is to use magnetic dielectric materials as the substrate. Magnetic dielectric materials can be used as embedded inductors to reduce the size of the antenna, thereby reducing the size of electronic products and optimizing the performance of electronic products. The characteristic parameters of the antenna are shown in the following formula 1, where (ε r μ r ) 1 / 2 is the miniaturization factor, the dielectric constant ε r The higher the magnetic permeability μ r The larger the value, the higher the miniaturization factor, which is more conducive to miniaturization. If the dielectric constant cannot be changed, increasing the magnetic permeability can effectively reduce the size of the antenna while maintaining or improving the antenna gain and bandwidth.

[0005] λ=c / f(ε r μ r ) 1 / 2 (1)

[0006] Planar hexagonal ferrites have high cutoff frequencies, such as Ba3Co2Fe 24 O 41 (Co2Z) hexagonal ferrite, but its magnetic permeability is low, making it difficult to significantly reduce the size of the antenna. In addition, the high-frequency magnetic loss of hexagonal magnetic materials will also affect the size of the antenna.

[0007] Therefore, it is urgent to design a new hexagonal magnetic material so that the corresponding magnetic dielectric material has both high magnetic permeability and high frequency and low magnetic loss. Summary of the invention

[0008] In view of the shortcomings of the prior art, the present invention aims to provide a magnetic dielectric resin composition and its application. In the magnetic dielectric resin composition of the present invention, BaCoFe6O 11、A(Fe x B 1-x )O3 and (Ba y C 8-y )Fe4O 15 The synergistic cooperation of the three can improve the magnetic permeability of the composite hexagonal magnetic filler and reduce high-frequency magnetic loss, so that the magnetic dielectric resin composition has both high magnetic permeability and high-frequency low magnetic loss, meeting the performance requirements of the magnetic dielectric substrate and at a lower cost.

[0009] To achieve this object, the present invention adopts the following technical solutions:

[0010] In a first aspect, the present invention provides a magnetic dielectric resin composition, the magnetic dielectric resin composition comprising a combination of a resin and a composite hexagonal magnetic filler;

[0011] The composite hexagonal magnetic filler includes BaCoFe6O 11 、A(Fe x B 1-x )O3 and (Ba y C 8-y )Fe4O 15 , wherein 0.5≤x≤0.7, 4≤y≤7 and y is an integer, A includes any one or a combination of at least two of Ba, Sr or La, B includes any one or a combination of at least two of Ti, Ca, Bi, Co, Ni, Ir, Mn, Mg, Mo, Nb, Nd, Sr, V, Zn, Zr, La or Si, and C includes any one or a combination of at least two of Ti, Ca, Bi, Co, Ni, Ir, Mn, Mg, Mo, Nb, Nd, Sr, V, Zn, Zr, La, Si or Li;

[0012] Taking the total mass of the magnetic dielectric resin composition as 100%, the mass fraction of the composite hexagonal magnetic filler is 20-90%, for example, it can be 20%, 25%, 30%, 35%, 40%, 45%, 50%, 55%, 60%, 65%, 70%, 75%, 80%, 85% or 90%, etc.

[0013] The present invention provides a magnetic dielectric resin composition, wherein the composite hexagonal magnetic filler is in BaCoFe6O 11 、A(Fe x B 1-x )O3 and (Ba y C 8-y )Fe4O 15 The synergistic cooperation of the three can improve the magnetic permeability of the composite hexagonal magnetic filler and reduce high-frequency magnetic loss, so that the magnetic dielectric resin composition has both high magnetic permeability and high-frequency low magnetic loss.

[0014] In the present invention, when the mass fraction of the composite hexagonal magnetic filler is too small, the magnetic permeability will be too small; when the mass fraction of the composite hexagonal magnetic filler is too large, the high-frequency magnetic loss will be too high.

[0015] Preferably, the molecules of the composite hexagonal magnetic filler include BaCoFe6O 11 Molecule, A(Fe x B 1-x )O3 molecules and (Ba y C 8-y )Fe4O 15 The composite hexagonal magnetic filler has a different 11 Molecule, A(Fe x B 1-x )O3 molecules and (Ba y C 8-y )Fe4O 15 A new molecular formula of the molecule, which includes the above three molecules at the same time, rather than a simple physical mixture of the three molecules.

[0016] Preferably, based on the total mass of the composite hexagonal magnetic filler as 100%, A(Fe x B 1-x )The mass fraction of O3 is 10-30%, for example, it can be 10%, 12%, 15%, 18%, 20%, 22%, 25%, 28% or 30%.

[0017] In the present invention, if A(Fe x B 1-x )O3 mass fraction is too low, resulting in high high-frequency magnetic loss; if A(Fe x B 1-x )If the mass fraction of O3 is too high, the magnetic permeability will be too low.

[0018] Preferably, based on the total mass of the composite hexagonal magnetic filler as 100%, (Ba y C 8-y )Fe4O 15 The mass fraction of is 5-20%, for example, it can be 5%, 6%, 7%, 8%, 10%, 12%, 14%, 16%, 18% or 20%.

[0019] In the present invention, if (Ba y C 8-y )Fe4O 15 If the mass fraction of is too low, it will lead to high high-frequency magnetic loss; y C 8-y )Fe4O 15 If the mass fraction is too high, the magnetic permeability will be too small.

[0020] Preferably, the composite hexagonal magnetic filler comprises BaCoFe6O 11 、Ba(Fe 0.6 Ca 0.4 )O3 and (Ba5Ti3)Fe4O 15 combination.

[0021] Preferably, the composite hexagonal magnetic filler further comprises a metal oxide; the single metal oxide comprises any one of manganese oxide, zinc oxide, nickel oxide or copper oxide, or a combination of at least two thereof.

[0022] Preferably, based on the total mass of the composite hexagonal magnetic filler being 100%, the mass fraction of the metal oxide is 5-10%, for example, 5%, 6%, 7%, 8%, 9% or 10%.

[0023] Preferably, the average particle size of the composite hexagonal magnetic filler is 0.1 to 30 μm, for example, 0.1 μm, 2 μm, 5 μm, 8 μm, 10 μm, 13 μm, 16 μm, 19 μm, 22 μm, 25 μm, 28 μm or 30 μm, etc. The filler particle size is tested by laser diffraction method, and the testing instrument is Malvern laser particle size analyzer, model MS3000.

[0024] Preferably, the composite hexagonal magnetic filler is prepared by method one or method two, preferably method one;

[0025] The method 1 comprises: 11 Magnetic materials, A(Fe x B 1-x )O3 magnetic materials and (Ba y C 8-y )Fe4O 15 Magnetic materials are co-fired, or BaCoFe6O 11 Raw materials of magnetic materials, A(Fe x B 1-x )O3 magnetic material raw materials and (Ba y C 8-y )Fe4O 15 Mixing and calcining raw materials of magnetic materials to obtain the composite hexagonal magnetic filler;

[0026] The second method comprises: 11 Magnetic materials, A(Fe x B 1-x )O3 magnetic materials and (Ba y C 8-y )Fe4O 15 The magnetic materials are blended to obtain the composite hexagonal magnetic filler.

[0027] In the present invention, when the composite hexagonal magnetic filler is prepared by method one, the crystal forms can be fully fused after co-firing or mixed firing, thereby improving the magnetic permeability of the material and reducing high-frequency magnetic loss. However, it is difficult for the crystal forms to be fully fused during blending in method two. However, the performance of the filler prepared by blending in method two is still better than that of a single magnetic component material.

[0028] Preferably, the co-firing and mixed-firing temperatures are each independently 700-1300°C, for example, 700°C, 800°C, 900°C, 910°C, 920°C, 930°C, 940°C, 950°C, 960°C, 970°C, 980°C, 990°C, 1000°C, 1100°C, 1200°C or 1300°C, etc.

[0029] Preferably, the co-firing and mixed-firing times are each independently 2 to 9 hours, for example, 2 hours, 3 hours, 4 hours, 5 hours, 6 hours, 7 hours, 8 hours or 9 hours, etc., preferably 3 to 7 hours.

[0030] Preferably, the blending method includes ball milling and / or sand milling.

[0031] Preferably, the blending speed is 2000-4000 r / min, for example, it can be 2000 r / min, 2200 r / min, 2500 r / min, 2800 r / min, 3000 r / min, 3200 r / min, 3500 r / min, 3800 r / min or 4000 r / min.

[0032] Preferably, the blending time is 4 to 8 hours, for example, 4 hours, 5 hours, 6 hours, 7 hours or 8 hours.

[0033] Preferably, the resin includes any one of epoxy resin, cyanate resin, polyphenylene ether resin, polybutadiene resin, butadiene-styrene resin, bismaleimide-triazine resin, bismaleimide resin, polytetrafluoroethylene resin, polyimide resin, phenolic resin, acrylic resin, liquid crystal resin, benzoxazine resin, nitrile rubber, carboxyl-terminated nitrile rubber or hydroxyl-terminated nitrile rubber, or a combination of at least two thereof.

[0034] Preferably, based on the total mass of the magnetic dielectric resin composition as 100%, the weight fraction of the resin is 10-80%, for example, it can be 10%, 15%, 20%, 30%, 40%, 50%, 60%, 70% or 80%.

[0035] Preferably, the magnetic dielectric resin composition further comprises a non-magnetic filler and a promoter.

[0036] Preferably, based on the total mass of the magnetic dielectric resin composition being 100%, the mass fraction of the non-magnetic filler is 5-20%, for example, 5%, 7%, 10%, 12%, 15% or 20%.

[0037] Preferably, based on the total mass of the magnetic dielectric resin composition as 100%, the mass fraction of the accelerator is 0.1-8%, for example, 0.1%, 0.2%, 0.5%, 1%, 2%, 3%, 5% or 8%.

[0038] Preferably, the non-magnetic filler includes any one of silicon dioxide, titanium dioxide, barium titanate, strontium titanate, magnesium titanate, calcium titanate, barium strontium titanate, calcium barium titanate, lead titanate, lead zirconate titanate, lead lanthanum zirconate titanate, barium lanthanum titanate, barium zirconate titanate, hafnium dioxide, lead magnesium niobate, barium magnesium niobate, lithium niobate, potassium niobate, strontium aluminum tantalate, potassium tantalum niobate, barium strontium niobate, lead barium niobate, barium titanium niobate, strontium bismuth tantalate, bismuth titanate, barium rubidium titanate, copper titanate or lead titanate-lead magnesium niobate, or a combination of at least two of them.

[0039] Preferably, the accelerator includes any one of 2-methylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2-undecylimidazole, 1-benzyl-2-methylimidazole, 2-heptadecylimidazole, 2-isopropylimidazole, 2-phenyl-4-methylimidazole, 2-dodecylimidazole or 1-cyanoethyl-2-methylimidazole, or a combination of at least two thereof.

[0040] Preferably, the magnetic dielectric resin composition further comprises an initiator.

[0041] Preferably, based on the total mass of the magnetic dielectric resin composition as 100%, the mass fraction of the initiator is 0.1-8%, for example, 0.1%, 0.2%, 0.5%, 1%, 2%, 3%, 5% or 8%.

[0042] Preferably, the initiator includes any one of a,a'-di(tert-butylperoxy-m-isopropylbenzene)benzene, diisopropylbenzene peroxide, tert-butylperoxide, 1,1-bis(tert-hexylperoxide)-3,3,5-trimethylcyclohexane, 2,5-dimethyl-2,5-di(tert-butylperoxy)hex-3-yne, tert-butyl octanoate, tert-butyl perbenzoate, triethylamine, triethylamine salt compound, quaternary amine salt compound, 2,4,6-tris(dimethylaminomethylamine)phenol, benzyldimethylamine, imidazoles, tripentylphenol amine, monophenol compound, polyphenol compound, boron trifluoride, boron trifluoride organic complex, phosphoric acid or triphenyl phosphite, or a combination of at least two thereof.

[0043] Preferably, the magnetic dielectric resin composition further comprises a cross-linking agent.

[0044] Preferably, based on the total mass of the magnetic dielectric resin composition being 100%, the mass fraction of the crosslinking agent is 5-20%, for example, 5%, 7%, 10%, 12%, 15% or 20%.

[0045] Preferably, the crosslinking agent includes any one of triallyl isocyanurate, triallyl polyisocyanurate, triallyl cyanurate, trimethacrylic acid, diallyl phthalate, divinylbenzene or multifunctional acrylate, or a combination of at least two thereof.

[0046] In a second aspect, the present invention provides a resin adhesive, wherein the resin adhesive comprises the magnetic dielectric resin composition as described in the first aspect and a solvent.

[0047] Preferably, the solvent includes any one of ethers, ketones, aromatic hydrocarbons, esters or nitrogen-containing solvents, or a combination of at least two thereof.

[0048] Further preferably, the solvent includes ethers such as methanol, ethanol, butanol, ethyl cellosolve, butyl cellosolve, ethylene glycol methyl ether, diethylene glycol ethyl ether, diethylene glycol butyl ether, or acetone, butanone, methyl ethyl ketone, methyl isobutyl ketone, cyclohexanone, toluene, xylene, mesitylene, ethoxyethyl acetate, ethyl acetate, N,N-dimethylformamide, N,N-dimethylacetamide or N-methyl-2-pyrrolidine, or any one or a combination of at least two thereof.

[0049] In a third aspect, the present invention provides a prepreg, comprising a reinforcing material and the magnetic dielectric resin composition as described in the first aspect attached to the reinforcing material.

[0050] Preferably, the reinforcement material comprises glass fiber cloth.

[0051] In a fourth aspect, the present invention provides a magnetic film, comprising the magnetic dielectric resin composition described in the first aspect.

[0052] In a fifth aspect, the present invention provides a magnetic paste, wherein the magnetic paste comprises the magnetic dielectric resin composition described in the first aspect.

[0053] In a sixth aspect, the present invention provides a metal foil-clad laminate, the metal foil-clad laminate comprising at least one prepreg as described in the third aspect, at least one side surface (e.g., one side surface or both sides surface) of the prepreg after being stacked is coated with metal foil. The at least one prepreg may be, for example, 1, 2, 3, 4, 5, 7 or 10 prepregs.

[0054] In a seventh aspect, the present invention provides a printed circuit board, comprising at least one of the prepreg described in the third aspect and the metal foil-clad laminate described in the sixth aspect.

[0055] The numerical range described in the present invention not only includes the point values ​​listed above, but also includes any point values ​​between the above numerical ranges that are not listed. Due to space limitations and for the sake of simplicity, the present invention no longer exhaustively lists the specific point values ​​included in the range.

[0056] Compared with the prior art, the present invention has the following beneficial effects:

[0057] The present invention provides a magnetic dielectric resin composition, wherein the composite hexagonal magnetic filler is in BaCoFe6O 11 、A(Fe x B 1-x )O3 and (Ba y C 8-y )Fe4O 15 The synergistic cooperation of the three can improve the magnetic permeability of the composite hexagonal magnetic filler and reduce high-frequency magnetic loss, so that the magnetic dielectric resin composition has both high magnetic permeability and high-frequency low magnetic loss. DETAILED DESCRIPTION

[0058] The technical solution of the present invention is further illustrated below through specific implementation methods.

[0059] Preparation Example

[0060] The molecular composition and properties of the composite hexagonal magnetic filler used in the following examples and comparative examples of the present invention are shown in Table 1. In Table 1, the content of each molecule in the composite hexagonal magnetic filler is in mass percentage.

[0061] Table 1

[0062]

[0063] The preparation method of composite hexagonal magnetic filler is as follows:

[0064] Weigh each raw material component according to the proportion in Table 1, perform physical dry mixing for 1 hour, prepare a ring-shaped embryo, and then sinter at 1300°C for 4 hours; the sintered product obtained is a ring-shaped sample (inner diameter 3.04mm, outer diameter 6.96mm and thickness 3mm); the sintered product is wet-milled in a ball mill at a speed of 3000 rpm for 6 hours, and the particle size of the zirconium beads is 1 to 10mm; dry after ball milling to obtain a composite hexagonal magnetic filler.

[0065] In Table 1, the average particle size of the composite hexagonal magnetic filler is tested by laser diffraction method, and the testing instrument is Malvern laser particle size analyzer, model MS3000.

[0066] In Table 1, the test method for 2GHz relative permeability and magnetic loss tangent is:

[0067] (1) The annular sample obtained by the sintering was tested using a Keysight Technologies E5071C network analyzer + N1500 test system as the test instrument to test the relative magnetic permeability and magnetic loss tangent of the material at 2 GHz.

[0068] The materials used in the following examples and comparative examples are as follows:

[0069] Hydrocarbon resin: Japan Soda B3000

[0070] Polyphenylene ether resin: Sabic SA9000;

[0071] Brominated epoxy resin B: BEB531A80P, Changchun, Taiwan, China;

[0072] Phenoloxy resin C: Nippon Steel YP-50EK35;

[0073] Epoxy resin A: Nippon Steel ZX1059;

[0074] 1,4-bis-tert-butylperoxyisopropylbenzene (BIPB) initiator: Hunan Fangruida Chemical Co., Ltd.;

[0075] 2-Methylimidazole (2-MI): BASF (Germany).

[0076] Example 1

[0077] This embodiment provides a magnetic dielectric resin composition, including 74g of polyphenylene ether resin SA9000, 6g of BIPB initiator and 20g of composite hexagonal magnetic filler A.

[0078] The magnetic dielectric resin composition is used for preparing a copper-clad laminate, and the specific method is as follows:

[0079] (1) mixing the magnetic dielectric resin composition with ethylene glycol methyl ether and uniformly dispersing them at room temperature to obtain a resin glue solution;

[0080] (2) using a reinforcing material (glass fiber cloth) to impregnate the resin glue obtained in step (1), and baking in an oven at 155° C. for 5 min to achieve curing, thereby obtaining a prepreg; placing 6 sheets of the 5 mil thick prepreg between two copper foils, laminating and curing in a hot press at 210° C. and 5 MPa pressure for 2 h, thereby obtaining the copper clad laminate.

[0081] Example 2

[0082] This embodiment provides a magnetic dielectric resin composition, including 4g of epoxy resin A, 5g of brominated epoxy resin B, 0.9g of phenolic resin C, 0.1g of 2-MI and 90g of composite hexagonal magnetic filler B.

[0083] The magnetic dielectric resin composition is used for preparing a copper-clad laminate, and the specific method is the same as that in Example 1 to obtain the copper-clad laminate.

[0084] Example 3

[0085] This embodiment provides a magnetic dielectric resin composition, including 45g of hydrocarbon resin B3000, 5g of BIPB initiator and 50g of composite hexagonal magnetic filler C.

[0086] The magnetic dielectric resin composition is used for preparing a copper-clad laminate, and the specific method is the same as that in Example 1 to obtain the copper-clad laminate.

[0087] Example 4

[0088] This embodiment provides a magnetic dielectric resin composition, which is different from Embodiment 2 only in that the composite hexagonal magnetic filler B is replaced by composite hexagonal magnetic filler D in terms of mass.

[0089] The magnetic dielectric resin composition is used for preparing a copper-clad laminate, and the specific method is the same as that in Example 1 to obtain the copper-clad laminate.

[0090] Example 5

[0091] This embodiment provides a magnetic dielectric resin composition, which is different from Embodiment 2 only in that the composite hexagonal magnetic filler B is replaced by the composite hexagonal magnetic filler E.

[0092] The magnetic dielectric resin composition is used for preparing a copper-clad laminate, and the specific method is the same as that in Example 1 to obtain the copper-clad laminate.

[0093] Example 6

[0094] This embodiment provides a magnetic dielectric resin composition, which is different from Embodiment 2 only in that the composite hexagonal magnetic filler B is replaced by composite hexagonal magnetic filler F in terms of mass.

[0095] The magnetic dielectric resin composition is used for preparing a copper-clad laminate, and the specific method is the same as that in Example 1 to obtain the copper-clad laminate.

[0096] Example 7

[0097] This embodiment provides a magnetic dielectric resin composition, which differs from Embodiment 2 only in that the composite hexagonal magnetic filler B is replaced by a composite hexagonal magnetic filler G in terms of mass.

[0098] The magnetic dielectric resin composition is used for preparing a copper-clad laminate, and the specific method is the same as that in Example 1 to obtain the copper-clad laminate.

[0099] Comparative Example 1

[0100] This comparative example provides a magnetodielectric resin composition, which is only different from that of Example 1 in that the mass of the modified Y-type hexagonal magnetic filler A is adjusted to 8 g.

[0101] The magnetodielectric resin composition is used for the preparation of a copper clad laminate, and the specific method is the same as that of Example 1 to obtain the copper clad laminate.

[0102] Comparative Example 2

[0103] This comparative example provides a magnetodielectric resin composition, which is only different from that of Example 2 in that the mass of the composite hexagonal magnetic filler B is adjusted to 95 g.

[0104] The magnetodielectric resin composition is used for the preparation of a copper clad laminate, and the specific method is the same as that of Example 1 to obtain the copper clad laminate.

[0105] Comparative Example 3

[0106] This comparative example provides a magnetodielectric resin composition, which is only different from that of Example 2 in that the composite hexagonal magnetic filler B is replaced with the composite hexagonal magnetic filler H in equal mass.

[0107] The magnetodielectric resin composition is used for the preparation of a copper clad laminate, and the specific method is the same as that of Example 1 to obtain the copper clad laminate.

[0108] Comparative Example 4

[0109] This comparative example provides a magnetodielectric resin composition, which is only different from that of Example 2 in that the composite hexagonal magnetic filler B is replaced with the composite hexagonal magnetic filler I in equal mass.

[0110] The magnetodielectric resin composition is used for the preparation of a copper clad laminate, and the specific method is the same as that of Example 1 to obtain the copper clad laminate.

[0111] Comparative Example 5

[0112] This comparative example provides a magnetodielectric resin composition, which is only different from that of Example 2 in that the composite hexagonal magnetic filler B is replaced with pure BaCoFe6O 11 。

[0113] The magnetodielectric resin composition is used for the preparation of a copper clad laminate, and the specific method is the same as that of Example 1 to obtain the copper clad laminate.

[0114] Performance Test

[0115] (1) Sample preparation: The copper clad laminate is processed into a ring-shaped sample (inner diameter 3.04 mm, outer diameter 6.96 mm, thickness 3 mm) with a CNC milling machine for magnetic plates;

[0116] (2) The Keysight E5071C network analyzer + N1500 test system was used as the test instrument to measure the relative permeability and magnetic loss tangent of the material at 2 GHz.

[0117] According to the above performance test method, the performance of the copper clad laminates obtained in Examples 1-7 and Comparative Examples 1-2 was tested. The components of the magnetodielectric resin composition and the test results of the performance of the copper clad laminates containing it were summarized, as shown in Table 2.

[0118] Table 2

[0119]

[0120]

[0121] Analysis:

[0122] As can be seen from Table 2, the copper clad laminates prepared in Examples 1-5 have a relatively high permeability, low high-frequency (2 GHz) loss, and good comprehensive performance, which can meet the performance requirements of the magnetodielectric substrate.

[0123] From the data results of Comparative Example 1 and Example 1, it can be seen that if the addition ratio of the composite filler is low, the permeability is small.

[0124] From the data results of Comparative Example 2 and Example 2, it can be seen that if the addition ratio of the composite filler is high, it will lead to poor processability and unable to prepare qualified products.

[0125] From the data results of Examples 6-7 and Example 2, for the F and G fillers whose component contents of A(Fe x B 1-x )O3 and (Ba y C 8-y )Fe4O 15 are not within the preferred range, it is impossible to obtain both a relatively high permeability and a low high-frequency (2 GHz) loss at the same time.

[0126] From the data results of Comparative Example 3 and Example 2, it can be seen that if the composite hexagonal magnetic filler does not contain A(Fe x B 1-x )O3, the permeability is low.

[0127] From the data results of Comparative Example 4 and Example 2, it can be seen that if the composite hexagonal magnetic filler does not contain (Ba y C 8-y )Fe4O 15 , the permeability is low.

[0128] From the data results of Comparative Example 5 and Example 2, it can be seen that if the composite hexagonal magnetic filler only contains BaCoFe6O 11 , the permeability is low.

[0129] The above are only specific embodiments of the present invention, but the protection scope of the present invention is not limited thereto. Those skilled in the art should understand that any changes or substitutions that can be easily thought of by those skilled in the art within the technical scope disclosed by the present invention fall within the protection scope and the disclosure scope of the present invention.

Claims

1. A magnetodielectric resin composition, characterized in that, The magnetic dielectric resin composition comprises a combination of a resin and composite hexagonal magnetic fillers; The composite hexagonal magnetic filler includes BaCoFe6O 11 , A(Fe x B 1-x )O3 and (Ba y C 8-y )Fe4O 15 in combination, where 0.5 ≤ x ≤ 0.7, 4 ≤ y ≤ 7 and y is an integer, A includes any one or a combination of at least two of Ba, Sr or La, B includes any one or a combination of at least two of Ti, Ca, Bi, Co, Ni, Ir, Mn, Mg, Mo, Nb, Nd, Sr, V, Zn, Zr, La or Si, and C includes any one or a combination of at least two of Ti, Ca, Bi, Co, Ni, Ir, Mn, Mg, Mo, Nb, Nd, Sr, V, Zn, Zr, La, Si or Li; Based on the total mass of the magnetic dielectric resin composition being 100%, the mass fraction of the composite hexagonal magnetic fillers is 20-90%.

2. The magnetodielectric resin composition according to claim 1, wherein Based on the total mass of the composite hexagonal magnetic filler being 100%, the mass fraction of A(Fe x B 1-x )O3 is 10 - 30%; Preferably, based on the total mass of the composite hexagonal magnetic filler being 100%, the mass fraction of (Ba y C 8-y )Fe4O 15 is 5 to 20%; Preferably, the average particle size of the composite hexagonal magnetic fillers is 0.1-30 μm.

3. The magnetodielectric resin composition according to claim 1 or 2, characterized in that, The composite hexagonal magnetic fillers are prepared by Method 1 or Method 2; The first method includes: co-firing the BaCoFe6O 11 magnetic material, the A(Fe x B 1-x )O3 magnetic material, and the (Ba y C 8-y )Fe4O 15 magnetic material, or co-firing the raw materials of the BaCoFe6O 11 magnetic material, the raw materials of the A(Fe x B 1-x )O3 magnetic material, and the raw materials of the (Ba y C 8-y )Fe4O 15 magnetic material to obtain the composite hexagonal magnetic filler; The second method includes: mixing BaCoFe6O 11 magnetic material, A(Fe x B 1-x )O3 magnetic material and (Ba y C 8-y )Fe4O 15 magnetic materials to obtain the composite hexagonal magnetic filler; Preferably, the co-firing and co-mixing temperatures are each independently 700-1300 °C; Preferably, the co-firing and co-mixing times are each independently 2-9 h; Preferably, the co-blending method includes ball milling and / or sand milling; Preferably, the co-blending rotation speed is 2000-4000 r / min; Preferably, the co-blending time is 4-8 h.

4. The magnetodielectric resin composition according to any one of claims 1 to 3, characterized in that, The resin includes any one or a combination of at least two of epoxy resin, cyanate resin, polyphenylene ether resin, polybutadiene resin, styrene-butadiene resin, bismaleimide-triazine resin, bismaleimide resin, polytetrafluoroethylene resin, polyimide resin, phenolic resin, acrylic resin, liquid crystal resin, benzoxazine resin, nitrile rubber, carboxyl-terminated nitrile rubber or hydroxyl-terminated nitrile rubber; Preferably, based on the total mass of the magnetic dielectric resin composition being 100%, the weight fraction of the resin is 10-80%; Preferably, the magnetic dielectric resin composition further includes non-magnetic fillers and a promoter; Preferably, the non-magnetic fillers include any one or a combination of at least two of silica, titanium dioxide, barium titanate, strontium titanate, magnesium titanate, calcium titanate, strontium barium titanate, barium calcium titanate, lead titanate, lead zirconate titanate, lead lanthanum zirconate titanate, barium lanthanum titanate, barium zirconate titanate, hafnium dioxide, lead magnesium niobate, barium magnesium niobate, lithium niobate, potassium niobate, strontium aluminum tantalate, potassium tantalum niobate, strontium barium niobate, barium lead niobate, barium titanium niobate, strontium bismuth tantalate, bismuth titanate, rubidium barium titanate, copper titanate or lead titanate-lead magnesium niobate; Preferably, the promoter includes any one or a combination of at least two of 2-methylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2-undecylimidazole, 1-benzyl-2-methylimidazole, 2-heptadecylimidazole, 2-isopropylimidazole, 2-phenyl-4-methylimidazole, 2-dodecylimidazole or 1-cyanoethyl-2-methylimidazole; Preferably, the magnetic dielectric resin composition further includes an initiator; Preferably, the initiator includes any one or a combination of at least two of a,a'-bis(tert-butylperoxy-m-isopropylbenzene)benzene, dicumyl peroxide, tert-butylcumyl peroxide, 1,1-bis(tert-hexylperoxy)-3,3,5-trimethylcyclohexane, 2,5-dimethyl-2,5-bis(tert-butylperoxy)hex-3-yne, tert-butyl octanoate, tert-butyl peroxybenzoate, triethylamine, triethylamine salt compounds, quaternary ammonium salt compounds, 2,4,6-tris(dimethylaminomethyl)phenol, benzyldimethylamine, imidazoles, tripentylphenol amide, monophenol compounds, polyphenol compounds, boron trifluoride, complexes of boron trifluoride with organic substances, phosphoric acid or triphenyl phosphite; Preferably, the magnetic dielectric resin composition further includes a crosslinking agent; Preferably, the crosslinking agent includes any one or a combination of at least two of triallyl isocyanurate, poly(triallyl isocyanurate), triallyl cyanurate, trimethacrylic acid, diallyl phthalate, divinylbenzene, or polyfunctional acrylate.

5. A resin glue solution, characterized in that, The resin solution includes the magnetodielectric resin composition according to any one of claims 1-4 and a solvent.

6. A prepreg, characterized in that, The prepreg includes a reinforcing material and the magnetodielectric resin composition according to any one of claims 1-4 attached to the reinforcing material; Preferably, the reinforcing material includes a glass fiber cloth.

7. A magnetic film, characterized in that, The magnetic film includes the magnetodielectric resin composition according to any one of claims 1-4.

8. A magnetic paste, characterized in that, The magnetic paste includes the magnetodielectric resin composition according to any one of claims 1-4.

9. A metal-clad laminate, characterized in that, The metal-clad laminate includes at least one prepreg according to claim 6, and at least one surface of the stacked prepregs is covered with a metal foil.

10. A printed circuit board, characterized in that, The printed circuit board includes at least one of the prepreg according to claim 6 and the metal-clad laminate according to claim 9.

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