Methods for high-throughput screening of high-permeability soft magnetic alloys, high-permeability amorphous soft magnetic alloys and their preparation methods

Abstract

This invention discloses a high-throughput screening method for high-permeability soft magnetic alloys, and a high-permeability Co alloy. 31.23 Fe 52.84 Ta 2.54 B 13.39 Amorphous soft magnetic alloys and their preparation methods. This invention utilizes high-throughput experimental methods to screen soft magnetic materials with excellent permeability. Magnetic thin films are templated into inductor coils for high-throughput characterization. The permeability of the soft magnetic material is indirectly reflected by measuring the inductance value of the magnetic thin film inductor. Co 31.23 Fe 52.84 Ta 2.54 B 13.39 The preparation method of amorphous soft magnetic alloy includes the following steps: S1, melting elemental raw materials of Co, Fe, Ta and B according to their chemical composition to obtain alloy ingots; S2, dividing the alloy ingots into blocks and then using vacuum single-roller spin quenching and spinning technology to prepare thin strips.

Description

Technical Field

[0001] This invention relates to the field of alloy permeability characterization, specifically to a method for high-throughput screening of high-permeability soft magnetic alloys, high-permeability amorphous soft magnetic alloys, and their preparation methods. Background Technology

[0002] Soft magnetic materials, with their low coercivity and high permeability, are key materials for achieving efficient electromagnetic energy conversion and signal processing. These materials can be easily magnetized under an applied magnetic field and rapidly demagnetized after the field is removed. High-permeability soft magnetic materials are particularly important for improving the efficiency of electrical equipment and reducing energy loss, especially in the design of high-performance transformers, motors, inductors, and other electromagnetic components. They can significantly reduce hysteresis and eddy current losses, thereby optimizing equipment performance and reducing energy consumption, which is of great significance for promoting energy efficiency improvements and the development of sustainable energy technologies.

[0003] Researchers have developed a variety of high-performance soft magnetic materials. At present, the development of new soft magnetic materials is based on the traditional trial-and-error method and sequential experimentation method, which involves a huge workload, a long development cycle, and a limited number of alloy systems, which consumes a lot of time and energy.

[0004] In contrast to the traditional trial-and-error approach, high-throughput experiments, as an important part of the Materials Genome New Materials R&D Program, change the traditional sequential iterative process to parallel experiments. Through rapid preparation of multi-component materials, high-throughput characterization of their properties and structures, phase diagrams can be drawn, material properties optimized, and new materials rapidly screened. This is a novel strategy for new material development.

[0005] High-throughput material preparation and performance screening enable the low-cost and rapid development of new material systems. Magnetic permeability is a crucial physical quantity for evaluating soft magnetic materials; high-permeability soft magnetic materials can respond quickly to changes in external magnetic fields. Currently, high-throughput experimental methods have demonstrated significant effectiveness in predicting the glass-forming ability of alloys, developing novel bulk amorphous alloys, novel catalytic materials, and alloys with excellent mechanical properties. However, research on high-throughput experimental and characterization methods for soft magnetic alloys is still limited. Patent specification CN114442012A discloses a device and method for high-throughput screening of the permeability of soft magnetic materials. The device includes: a test probe comprising a resonant circuit whose resonant frequency and reflection parameters are affected by the sample under test; a vector network analyzer electrically connected to the test probe and used to measure the resonant frequency and reflection parameters of the resonant circuit; a data processing mechanism for processing multiple sets of received resonant frequencies and reflection parameters to obtain the permeability of the sample under test; and a three-dimensional moving platform for placing the sample under test and moving it to a designated test position in a specified posture, while simultaneously measuring the distance between the sample under test and the test probe. This patented technology enables high-throughput real-time measurement of the sample under test, allowing for continuous, non-destructive, and rapid detection of multiple samples, with high resolution and sensitivity.

[0006] Conventional permeability testing has requirements regarding sample size and shape. The induction method involves a coil generating an electromotive force (EMF) within the coil under alternating current. When a magnetic material is placed near or inside the coil, its magnetic response affects the coil's self-induction properties. Therefore, the permeability can be indirectly measured by measuring the induced EMF or inductance change of the coil. This method is commonly used for long, strip-shaped samples. The ring sample method (also known as the ring core method) involves forming the material into a closed ring shape, winding a pair of coils around it, and measuring the magnetic flux under an applied magnetic field to calculate the permeability. This method is also suitable for long, strip-shaped samples or soft magnetic powder cores. Methods for testing the permeability of magnetic thin film materials generally fall into three categories: resonant cavity method, induction coil method, and transmission reflection method. However, all three methods involve inserting the sample into the measuring fixture, treating it as part of a transmission line, which severely limits the sample size and shape and is unsuitable for measuring gradient thin films.

[0007] Current methods for characterizing soft magnetic properties are not applicable to small-sized samples, especially methods for characterizing the permeability of small-sized samples. However, in magnetic thin-film inductors and planar inductors that directly use soft magnetic materials as conductors, researchers have provided a relationship between inductance and permeability, proving that the two are positively correlated.

[0008]

[0009] Where L is the inductance of the planar coil, l is the conductor length, w and d are the rectangular dimensions of the cross-section, and μ0 and μ' are the permeability of vacuum and relative permeability, respectively. Based on the relationship between the inductance of the planar coil and soft magnetic materials, a new approach is provided for the high-throughput fabrication and performance screening of soft magnetic alloys. Summary of the Invention

[0010] This invention provides a high-throughput screening method for high-permeability soft magnetic alloys. Utilizing high-throughput experimental technology, it can simultaneously test the permeability of hundreds or even thousands of material combinations, significantly accelerating the discovery and screening process of novel soft magnetic materials. Furthermore, leveraging the positive correlation between coil inductance and permeability, gradient coils with different compositions are designed. Directly measuring the coil inductance reflects the permeability of the corresponding component; this method is applicable to the testing of thin film samples.

[0011] This invention proposes for the first time a method to confine the formation of soft magnetic alloy coils by creating coil-shaped sub-regions, and further, to indirectly evaluate their permeability by measuring the inductance value of the coils. This provides an effective approach for rapidly screening and evaluating soft magnetic materials. Inductance, as a direct physical quantity reflecting the permeability of a coil, is relatively simple and quick to measure, providing immediate performance indicators for materials of each component proportion. This method utilizes electromagnetic principles, indirectly reflecting the magnetic properties of materials through changes in inductance, thereby avoiding the complex instruments and operations required for direct permeability measurement and accelerating the experimental process.

[0012] A method for high-throughput screening of soft magnetic alloys with high permeability includes:

[0013] A mask is set on the substrate to divide the substrate surface into multiple coil-shaped sub-regions;

[0014] A soft magnetic alloy coil with varying elemental content depending on its position on the substrate surface is obtained by physical vapor deposition co-sputtering based on multiple targets in a single deposition process on the substrate surface. The soft magnetic alloy coils deposited on different sub-regions have different compositions. The multiple targets can be any combination of metallic element targets, non-metallic element targets, or metallic-non-metallic composite targets.

[0015] The inductance of the soft magnetic alloy coils in each sub-region was measured. Based on the positive correlation between inductance and permeability, a soft magnetic alloy composition with high permeability was selected.

[0016] In some preferred embodiments, the number of sub-regions per square centimeter on the substrate is no more than two. If the sub-regions on the substrate are too dense, the gap between adjacent sub-regions will be too small, which may generate electromagnetic interference and affect the measurement results.

[0017] In some preferred embodiments, the gap between adjacent sub-regions is not less than 1 mm. Ensuring that the gap between adjacent sub-regions is not too small avoids electromagnetic interference and ensures accurate measurement results.

[0018] In this invention, the specific shape of the coil-shaped sub-region is not particularly limited; for example, it can be a square or other polygon, a circle, etc.

[0019] In one embodiment, the high-throughput screening method for high-permeability soft magnetic alloys is described in which the soft magnetic alloy coils deposited in each sub-region have the same size and number of turns.

[0020] In one embodiment, the substrate in the high-throughput screening method for high-permeability soft magnetic alloys may be a silicon wafer or quartz.

[0021] In one embodiment, the method for high-throughput screening of high-permeability soft magnetic alloys may use a Co-Fe-Ta-B amorphous soft magnetic alloy. Correspondingly, the multi-target material may be a Fe-palladium, Ta-palladium, and Co-B composite target.

[0022] In one embodiment, the high-throughput screening method for high-permeability soft magnetic alloys can utilize an impedance analyzer to test the inductance value of the soft magnetic alloy coils in each sub-region at a set frequency using a probe. Further, the set frequency can be 1 MHz.

[0023] The method for high-throughput screening of high-permeability soft magnetic alloys of the present invention has the following characteristics:

[0024] 1. This invention utilizes a high-throughput experimental method to screen soft magnetic materials with excellent permeability;

[0025] 2. The magnetic thin film was templated into an inductor coil for high-throughput characterization;

[0026] 3. The permeability of soft magnetic materials can be indirectly reflected by testing the inductance value of magnetic thin film inductors.

[0027] As a general inventive concept, this invention also provides a high-permeability Co-Fe-Ta-B amorphous soft magnetic alloy, with a chemical composition of Co (based on atomic ratio). 31.23 Fe 52.84 Ta 2.54 B 13.39 .

[0028] This invention also provides a method for preparing the aforementioned high-permeability Co-Fe-Ta-B amorphous soft magnetic alloy, comprising the following steps:

[0029] S1, smelt elemental raw materials of Co, Fe, Ta and B according to the chemical composition to obtain alloy ingots;

[0030] S2, after the alloy ingot is divided into blocks, a thin strip is prepared using vacuum single-roller spin quenching and spinning technology.

[0031] In one embodiment, in the preparation method of the high-permeability Co-Fe-Ta-B amorphous soft magnetic alloy, step S1 can be performed by vacuum arc melting, and the melting atmosphere can be an inert atmosphere such as a rare gas. In this invention, the inert atmosphere refers to a gaseous atmosphere that does not participate in the reaction.

[0032] In one embodiment, in the preparation method of the high permeability Co-Fe-Ta-B amorphous soft magnetic alloy, in step S2, the molten alloy ingot can be sprayed onto the surface of a copper roller under a vacuum of less than 10 Pa, and the linear velocity of the copper roller surface can be greater than 20 m / s.

[0033] Compared with the prior art, the beneficial effects of this invention are as follows:

[0034] This invention can accelerate the discovery and screening of novel soft magnetic materials by utilizing high-throughput experimental techniques. Simultaneously, by leveraging the positive correlation between coil inductance and permeability, the inductance of the coil can be directly measured to reflect the permeability of the corresponding component, thus solving the problem of testing the permeability of small-sized thin-film samples.

[0035] This invention successfully screened and verified Co 31.23 Fe 52.84 Ta 2.54 B 13.39 High permeability of amorphous soft magnetic alloys. Attached Figure Description

[0036] To more clearly illustrate the technical solutions in the embodiments of the present invention or the prior art, the drawings used in the description of the embodiments or the prior art will be briefly introduced below. Obviously, the drawings described below are only some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort.

[0037] Figure 1 This is a schematic diagram of multi-target magnetron sputtering deposition and gradient coil in Example 1.

[0038] Figure 2 This is a spatial distribution map of different elements in the high-throughput sample library prepared in Example 1.

[0039] Figure 3 The diagram shows the distribution of coil inductance values ​​as a function of elemental composition for the high-throughput sample library prepared in Example 1.

[0040] Figure 4 For Co 31.23 Fe 52.84 Ta 2.54 B 13.39Co 37.45 Fe 44.10 Ta 2.4 B 16.05 The permeability results of actual samples of amorphous soft magnetic alloys are shown in the figure. Detailed Implementation

[0041] The present invention will be further described below with reference to the accompanying drawings and specific embodiments. It should be understood that these embodiments are for illustrative purposes only and are not intended to limit the scope of the invention.

[0042] Unless otherwise specified, the operating methods in the following examples are generally performed under conventional conditions or as recommended by the manufacturer.

[0043] This invention first selects a soft magnetic material exhibiting excellent permeability, whose components can include both metallic and non-metallic materials. The metallic materials can be magnetic metals such as Fe, Co, and Ni, with small amounts of non-magnetic metals such as Cu, Al, Mo, and Nb also added. The non-metallic materials can be B, Si, C, P, etc. The components of the soft magnetic material are sputtered using high-throughput multi-target magnetron sputtering. The target material can be a single-element target or a composite target. Using a mask, 27 coils with different formulations, each 0.8mm × 0.8mm in diameter and having two turns, are fabricated on a 50mm × 50mm silicon wafer or quartz surface. Then, using an impedance analyzer and a probe, the inductance value of each coil at different frequencies can be measured (1MHz is used as an example here). This allows obtaining the inductance values ​​of different test areas in the sample library, and plotting the inductance performance. Since permeability and inductance are positively correlated, the inductance value reflects the permeability of different test areas. Compositional analysis of different test areas in the sample library yields the compositional map of the high-throughput sample library. By comparing the inductance performance diagram with the composition diagram, components corresponding to high permeability are identified. To verify the accuracy of this method, corresponding component points can be selected and verified using conventional permeability testing methods.

[0044] Example 1

[0045] This embodiment takes a Co-Fe-Ta-B amorphous soft magnetic alloy with high magnetic permeability as an example. It selects magnetic metals Fe and Co, does not dope with a small amount of non-magnetic metal Ta, and introduces a metalloid element B to improve its amorphous forming ability. For example... Figure 1 As shown, Fe, Ta, and Co-B (7:3 atomic ratio) composite targets were used to prepare coils with different compositions via multi-target co-sputtering. The alloy element content of the deposited coils was analyzed by energy-dispersive spectroscopy (EDS). The inductance value at 1 MHz was measured using an impedance analyzer. Based on the positive correlation between inductance and permeability, the relationship between permeability and composition can be indirectly reflected. The sample with the highest inductance value (Co) was selected from the sample library. 31.23 Fe 52.84 Ta2.54 B 13.39 ) and minimum inductance value (Co) 37.45 Fe 44.10 Ta 2.4 B 16.05 The two components of the sample were experimentally verified. Two samples were prepared by induction melting and single-roller spinning, and then the magnetic permeability of the two strip samples was measured by impedance analyzer. The results showed that the relationship between the magnetic permeability and the inductance of the two strip samples was in good agreement.

[0046] Preparation of a Co-Fe-Ta-B quaternary alloy high-throughput sample library: A high-throughput sample library was synthesized by physical vapor deposition (PVD) co-sputtering. Three targets were used for the four elements: a Fe target (C target), a Ta target (A target), and a Co-B (7:3 atomic ratio) composite target (B target). The centerlines of targets A, B, and C were 10 cm above the substrate plane and formed a 60-degree angle with the substrate. The sputtering powers of each target were 21 W for target A, 120 W for target B, and 80 W for target C. With constant sputtering power, the gradient distribution of each element was achieved by varying the distances from the sputtering targets to different regions of the substrate. Furthermore, the sputtering parameters included a basic gas pressure within the chamber below 10 °C. -5 The working pressure was 0.5 Pa, the argon flow rate was 50 standard cubic centimeters per minute (SCCM), and the deposition time was 90 minutes. The alloy element content of the deposited coil was analyzed by energy-dispersive spectroscopy (EDS). The spatial distribution of different elements in the prepared high-throughput sample library is shown in the figure. Figure 2 As shown. The inductance value at 1MHz was measured using an impedance analyzer. The inductance value of the prepared high-throughput sample library coil varies with the elemental composition distribution as shown. Figure 3 As shown.

[0047] The conventional method for testing magnetic permeability is the induction coil method, and the sample is usually in the form of a strip. Therefore, strip-shaped samples were prepared by induction melting and single-roller spinning for experimental verification. The specific procedure for sample preparation is as follows: the oxide scale and impurities on the surface of the elemental or alloy components were removed by ultrasonic cleaning and grinding; the raw materials were weighed using a high-precision electronic balance to prepare a mixture that conforms to the chemical formula ratio, ensuring a weighing accuracy of ±0.05 mg for each raw material; the prepared raw materials were then placed in a high-vacuum electric arc melting furnace until the vacuum degree reached 4 × 10⁻⁶. -3After Pa, the gas is repeatedly purged with argon gas more than three times, then argon gas is introduced, and an arc is ignited on the Ti ingot with a current of 30A. Then, a current of 30-360A is continued to melt the raw materials. Each alloy ingot is repeatedly turned over 4 times and melted 5 times to ensure the uniformity of the composition of the master alloy ingot. The master alloy ingot melted in the previous step is divided into small pieces, and the oxide scale and grease and other impurities on the surface of the master alloy ingot are removed by grinding. The metal strip is prepared by vacuum single-roller spin quenching and spinning technology, keeping the vacuum degree below 10Pa. High-purity argon gas is introduced to keep the gas pressure in the spinning machine cavity at -0.09MPa, and the pressure difference between the gas pressure in the quartz tube and the cavity is kept at 0.05MPa. The molten master alloy ingot is sprayed onto the surface of the copper roller, and the linear velocity on the surface of the copper roller is greater than 20m / s.

[0048] Figure 4 Showcasing Co 31.23 Fe 52.84 Ta 2.54 B 13.39 Co 37.45 Fe 44.10 Ta 2.4 B 16.05 The results of the permeability of the actual samples of amorphous soft magnetic alloys are consistent with the results of the relationship between the inductance value and the permeability.

[0049] Furthermore, it should be understood that after reading the above description of the present invention, those skilled in the art can make various alterations or modifications to the present invention, and these equivalent forms also fall within the scope defined by the appended claims.

Claims

1. A method for high-throughput screening of soft magnetic alloys with high permeability, characterized in that, include: A mask is set on the substrate to divide the substrate surface into multiple coil-shaped sub-regions; A soft magnetic alloy coil with varying elemental content depending on its position on the substrate surface is obtained by physical vapor deposition co-sputtering based on multiple targets in a single deposition process on the substrate surface. The soft magnetic alloy coils deposited on different sub-regions have different compositions. The multiple targets can be any combination of metallic element targets, non-metallic element targets, or metallic-non-metallic composite targets. The inductance of the soft magnetic alloy coils in each sub-region was measured. Based on the positive correlation between inductance and permeability, a soft magnetic alloy composition with high permeability was selected.

2. The method for high-throughput screening of high-permeability soft magnetic alloys according to claim 1, characterized in that, The number of sub-regions per square centimeter on the substrate is no more than two, and the gap between adjacent sub-regions is no less than 1 mm.

3. The method for high-throughput screening of high-permeability soft magnetic alloys according to claim 1, characterized in that, Using an impedance analyzer and probes, the inductance of the soft magnetic alloy coils in each sub-region is tested at a set frequency. The set frequency is 1 MHz.

4. The method for high-throughput screening of high-permeability soft magnetic alloys according to claim 1, characterized in that, The soft magnetic alloy coils deposited in each sub-region have the same size and number of turns.

5. The method for high-throughput screening of high-permeability soft magnetic alloys according to claim 1, characterized in that, The substrate is a silicon wafer or quartz.

6. The method for high-throughput screening of high-permeability soft magnetic alloys according to claim 1, characterized in that, The soft magnetic alloy is a Co-Fe-Ta-B amorphous soft magnetic alloy; The multi-target material is a composite target of Fe palladium, Ta palladium and Co-B.

7. A method for high-throughput screening of high-permeability soft magnetic alloys according to any one of claims 1 to 6, wherein the high-permeability Co-Fe-Ta-B amorphous soft magnetic alloy obtained by screening is characterized in that, The chemical composition, based on atomic ratio, is Co. 31.23 Fe 52.84 Ta 2.54 B 13.39 .

8. The method for preparing a high-permeability Co-Fe-Ta-B amorphous soft magnetic alloy according to claim 7, characterized in that, Including the following steps: S1, smelt elemental raw materials of Co, Fe, Ta and B according to the chemical composition to obtain alloy ingots; S2, after the alloy ingot is divided into blocks, a thin strip is prepared using vacuum single-roller spin quenching and spinning technology.

9. The method for preparing a high-permeability Co-Fe-Ta-B amorphous soft magnetic alloy according to claim 8, characterized in that, In step S1, vacuum arc melting is used, and the melting atmosphere is an inert atmosphere.

10. The method for preparing a high-permeability Co-Fe-Ta-B amorphous soft magnetic alloy according to claim 8, characterized in that, In step S2, the molten alloy ingot is sprayed onto the surface of a copper roller under a vacuum of less than 10 Pa, and the linear velocity of the copper roller surface is greater than 20 m / s.

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