A (Sm,T)(Fe,M) based on diffusion multi-node 12 High-throughput preparation method for phase alloys

Abstract

The present invention discloses a high-throughput preparation method of (Sm,T)(Fe,M) 12 phase alloy based on diffusion multi-joints. In (Sm,T)(Fe,M) 12 phase, Sm is samarium element, Fe is iron element, T is one or more of Y, Gd, Zr, Nd or Ce elements, and M is one or more of Ti, Cr, Mn, Mo, Si, Al, Co or V elements. The high-throughput preparation method based on diffusion multi-joints of the present invention includes: preparing a sheath, a lid and metal strips with appropriate sizes, assembling the metal strips in the sheath, then performing vacuum electron beam welding and hot isostatic pressing on the sheath, and then 12 sealing the obtained diffusion multi-joint slices in tubes and performing heat treatment to obtain (Sm,T)(Fe,M) 12 phase alloy. The high-throughput experimental method based on diffusion multi-joints of the present invention overcomes the traditional trial-and-error method for new material R & D, can obtain a large number of parallel samples in a short time, and combines with high-throughput characterization methods to reveal the formation rule of (Sm,T)(Fe,M) 12 phase, providing guidance for the R & D of SmFe -based rare earth permanent magnets.

Description

Technical Field

[0001] The present invention relates to the field of rare earth permanent magnets, and in particular to a (Sm, T) (Fe, M) 12 High-throughput preparation method for phase alloys. Background Art

[0002] Rare earth permanent magnet materials have been developed so far, and the mature rare earth permanent magnet materials are mainly samarium cobalt and neodymium iron boron. Among them, neodymium iron boron permanent magnet is called the "king of magnets" due to its high magnetic energy product. The reported maximum magnetic energy product of sintered neodymium iron boron permanent magnet is close to the theoretical value, and it is difficult to achieve a substantial improvement. In order to further promote the development of permanent magnet materials, researchers have focused on two aspects of research. On the one hand, based on the idea of ​​artificially constructing metamaterials, the hard magnetic phase with high coercivity and the soft magnetic phase with high magnetization intensity are composited at the nanoscale to prepare nano-duplex permanent magnets in order to obtain ultra-high magnetic energy product; however, the magnetic energy product of the experimentally prepared bulk nanocomposite permanent magnet material still cannot reach a high level. The main reason is that it is difficult to control the grain size of the soft and hard magnetic phases and to achieve uniform dispersion distribution, and to obtain oriented hard magnetic phase grains at the same time, which is also called an "engineering nightmare". On the other hand, the search for magnetic compounds with better intrinsic properties continues. Among them, ThMn, which was first reported in 1981, 12 This type of rare earth iron permanent magnet compound, due to its 3d iron element and large unit cell c / a value, is expected to have both high saturation magnetization intensity and high magnetocrystalline anisotropy constant, attracting widespread attention from permanent magnet researchers.

[0003] In addition, in the process of research and development of rare earth permanent magnet materials, the composition design tends to be diversified, and the phase law, microstructure, and preparation method tend to be complicated. If the traditional model of "experiment-guided experiment" is continued, the research and development of new materials will face long cycles, large investments, and slow results. For example, the phase stability of 1:12 permanent magnet materials is improved by element substitution, and their intrinsic properties are improved. However, the above methods all require continuous adjustment of experimental parameters in order to maximize the optimization of phase behavior and comprehensive magnetic properties. This traditional method of trial and error of "experiment-theory-experiment" has a long experimental cycle and little effective data, which has become a key common problem faced by the high research and development of rare earth permanent magnet materials. The use of high-throughput experimental methods, through the preparation of multi-nodes to obtain a large number of parallel samples in a short time, combined with centralized parallel characterization, can effectively improve the experimental efficiency. Summary of the invention

[0004] The purpose of the present invention is to overcome the shortcomings of the prior art and provide a (Sm, T) (Fe, M) 12 The high-throughput preparation method of phase alloy comprises the following steps:

[0005] (1) preparing a package and a cover matching the package, and processing a rectangular parallelepiped groove of 3a*2b*c in the package; in millimeters, 10≥a≥3, 10≥b≥3, c≥10;

[0006] (2) preparing six metal strips each having a size of a*b*c, and performing surface grinding and polishing on each of the metal strips, wherein the components of the six metal strips are Fe, Sm, T1, T2, M1, and M2, respectively, wherein T1 and T2 are respectively one element selected from Y, Gd, Zr, Nd, or Ce, or an alloy consisting of several elements; M1 and M2 are respectively one element selected from Ti, Cr, Mn, Mo, Si, Al, Co, or V, or an alloy consisting of several elements, wherein a, b, and c are respectively the length, width, and height of the metal strip;

[0007] (3) Arranging the six metal strips after surface grinding and polishing in order into a rectangular structure of 3a*2b*c, assembling them into the rectangular groove, covering them with a lid, and performing vacuum electron beam welding on the package; the arrangement is that the metal strip with a composition of Sm and the metal strip with a composition of Fe are respectively located in the middle of the upper and lower rows of the rectangular structure, the metal strip with a composition of M1 and the metal strip with a composition of M2 are respectively located on the left and right sides of the metal strip with a composition of Fe, and the metal strip with a composition of T1 and the metal strip with a composition of T2 are respectively located on the left and right sides of the metal strip with a composition of Sm;

[0008] (4) subjecting the welded package to hot isostatic pressing to obtain a diffusion multi-element node;

[0009] (5) Cut the diffusion multi-node into multiple slices in the height direction, seal the slices of the diffusion multi-node, and perform diffusion heat treatment after sealing to obtain (Sm, T)(Fe, M) based on the diffusion multi-node 12 Phase alloy.

[0010] Furthermore, in step (1), the sheath material is one of 304 stainless steel, pure iron or Cr metal, and the cover is made of the same material as the sheath.

[0011] Furthermore, the surface grinding and polishing treatment in step (2) includes sandpaper grinding and polishing by a polishing machine.

[0012] Furthermore, the vacuum degree of the vacuum electron beam welding in step (3) should be 5*10 -5 ~5*10 -4 Pa, weld width is 0.5~1.5mm.

[0013] Furthermore, the temperature of the hot isostatic pressing treatment in step (4) is 650-950° C., the time is 2-5 hours, and the pressure is 50-200 MPa.

[0014] Furthermore, the atmosphere of the tube sealing in step (5) is an argon atmosphere of 0.03-0.06 MPa.

[0015] Furthermore, the diffusion heat treatment in step (5) is carried out for 2 to 30 days, at a temperature of 800 to 1300° C., and the cooling method of the diffusion heat treatment is quenching.

[0016] Furthermore, in step (5), (Sm, T)(Fe, M) 12 In the phase alloy, Sm is samarium, Fe is iron, T is one or more of Y, Gd, Zr, Nd or Ce; and M is one or more of Ti, Cr, Mn, Mo, Si, Al, Co or V.

[0017] The present invention also provides a (Sm, T) (Fe, M) prepared according to the high-throughput method based on diffusion multi-nodes 12 Phase alloy.

[0018] The beneficial effects of the present invention compared with the prior art are as follows:

[0019] 1) The present invention prepares diffusion multi-nodes with different compositions to study the effect of different element substitution on SmFe 12 Phase formation behavior and phase stability, and (Sm,T)(Fe,M) 12 The changes in the intrinsic magnetic properties of phase alloys provide guidance for the research and development of 1:12 permanent magnet materials.

[0020] 2) The present invention explores different (Sm, T)(Fe, M) by different heat treatment temperatures and times. 12 The critical formation temperature of phase alloys, as well as some intermediate phases produced in this process and their relationship with (Sm,T)(Fe,M) 12 phase relationship of the phase alloy, thereby improving the subsequent preparation of (Sm, T)(Fe, M) 12 The purity of the phase alloy.

[0021] 3) The present invention adopts a high-throughput experimental method to overcome the traditional trial-and-error method of new material research and development. A large amount of data can be obtained through a single experiment, and a large number of parallel samples can be obtained in a short period of time. Through centralized parallel characterization, the diffusion multi-node samples are demonstrated for preparation and analytical verification, thereby establishing a relevant database to provide reference for subsequent research. BRIEF DESCRIPTION OF THE DRAWINGS

[0022] Figure 1 Schematic diagram of a diffusion multi-node. DETAILED DESCRIPTION

[0023] The present invention is further described and illustrated below in conjunction with specific embodiments. The embodiments are merely exemplary of the present disclosure and do not define the scope of limitation. The technical features of each embodiment of the present invention may be combined accordingly without conflicting with each other.

[0024] Embodiment 1:

[0025] (1) Preparation size is 30*18*45mm 3 The runway-shaped package and the size is 30*18*1mm 3 The lid is processed into 21*14*40mm 3 The rectangular tank; the cover and lid are made of 304 stainless steel;

[0026] (2) Preparation size is 7*7*40mm 3 Sm, Y, Zr, Fe, V and Ti metal strips, the surface is sanded and polished by a polishing machine;

[0027] (3) Assemble the metal strip into the rectangular groove, cover it with a lid, and perform vacuum electron beam welding; the vacuum degree of vacuum electron beam welding is 5*10 -4 Pa, the weld width is 0.5 mm, and the assembly method is that the metal strip with the composition of Sm and the metal strip with the composition of Fe are respectively located in the middle of the upper and lower rows of the rectangular grooves, the metal strip with the composition of V and the metal strip with the composition of Ti are respectively located on the left and right sides of the metal strip with the composition of Fe, and the metal strip with the composition of Y and the metal strip with the composition of Zr are respectively located on the left and right sides of the metal strip with the composition of Sm;

[0028] (4) The welded package is subjected to hot isostatic pressing to obtain a diffusion multi-element joint; the hot isostatic pressing temperature is 750°C, the time is 4 hours, and the pressure is 100 MPa;

[0029] (5) The multi-node is cut into 8 pieces parallel to the racetrack shape, and the tube is sealed and then subjected to diffusion heat treatment at 900°C, 1000°C, 1100°C, and 1200°C. The tube is sealed in an argon atmosphere of 0.04 MPa. The diffusion heat treatment time is 15 days and 30 days. The cooling method is quenching, and (Sm, T)(Fe, M) is obtained. 12 Phase alloy.

[0030] Embodiment 2:

[0031] (1) Preparation size is 32*20*51mm 3 The runway-shaped package and the size is 32*20*1mm 3 The lid is processed into 24*16*45mm 3 The rectangular tank; the cover and lid are made of 304 stainless steel;

[0032] (2) Preparation size is 8*8*45mm 3 Fe, Sm, Nd, Gd, Co and Ti metal strips, the surface of which is sanded and polished by a polishing machine;

[0033] (3) Assemble the metal strip into the rectangular groove, cover it with a lid, and perform vacuum electron beam welding; the vacuum degree of vacuum electron beam welding is 5*10 -5 Pa, the weld width is 1.5 mm, and the assembly method is that the metal strip with the composition of Sm and the metal strip with the composition of Fe are respectively located in the middle of the upper and lower rows of the rectangular grooves, the metal strip with the composition of Co and the metal strip with the composition of Ti are respectively located on the left and right sides of the metal strip with the composition of Fe, and the metal strip with the composition of Nd and the metal strip with the composition of Gd are respectively located on the left and right sides of the metal strip with the composition of Sm;

[0034] (4) The welded package is subjected to hot isostatic pressing to obtain a diffusion multi-node; the hot isostatic pressing temperature is 650°C, the time is 2h, and the pressure is 50MPa;

[0035] (5) The multi-node was cut into 10 slices parallel to the runway surface, and the tube was sealed and then subjected to diffusion heat treatment at 900°C, 950°C, 1000°C, 1050°C, and 1100°C. The tube was sealed in an argon atmosphere of 0.06 MPa. The diffusion heat treatment time was 20 days and 30 days. The cooling method was quenching, and (Sm, T)(Fe, M) was obtained. 12 Phase alloy.

[0036] Embodiment 3:

[0037] (1) Preparation size is 28*20*51mm 3 The runway-shaped package and the size is 28*20*1mm 3 The lid is processed into 21*16*40mm 3 The rectangular tank; the cover and lid are made of 304 stainless steel;

[0038] (2) Preparation size is 7*8*40mm 3 Fe, Sm, V, Gd, Mn and Ce metal strips, the surface of which is sanded and polished by a polishing machine;

[0039] (3) Assemble the metal strip into the rectangular groove, cover it with a lid, and perform vacuum electron beam welding; the vacuum degree of vacuum electron beam welding is 5*10 -5Pa, the weld width is 1.5 mm, and the assembly method is that the metal strip with the composition of Sm and the metal strip with the composition of Fe are respectively located in the middle of the upper and lower rows of the rectangular grooves, the metal strip with the composition of V and the metal strip with the composition of Mn are respectively located on the left and right sides of the metal strip with the composition of Fe, and the metal strip with the composition of Gd and the metal strip with the composition of Ce are respectively located on the left and right sides of the metal strip with the composition of Sm;

[0040] (4) The welded package is subjected to hot isostatic pressing to obtain a diffusion multi-node; the hot isostatic pressing temperature is 650°C, the time is 2h, and the pressure is 50MPa;

[0041] (5) The multi-node was cut into 10 slices parallel to the runway surface, and the tube was sealed and then subjected to diffusion heat treatment at 900°C, 950°C, 1000°C, 1050°C, and 1100°C. The tube was sealed in an argon atmosphere of 0.06 MPa. The diffusion heat treatment time was 20 days and 30 days. The cooling method was quenching, and (Sm, T)(Fe, M) was obtained. 12 Phase alloy.

[0042] There is only a very small amount of SmFe at the binary interface of Sm and Fe. 12 phase formation, namely, undoped SmFe 12 Phase formation is difficult. A large number of 1:12 phases were obtained at the interface of Sm, Fe, and T, indicating that T can reduce the formation energy of the phase and play a role in stabilizing the structure, among which the effect of Ti element is the most significant. However, the addition of Ti will also significantly reduce its magnetic properties. Only a small amount of 1:12 phases are formed at the interface of Sm, Fe, and M, among which the saturation magnetization and Curie temperature of the 1:12 phase are significantly improved when M is Co. At the quaternary interface of Sm, Fe, M, and T, a large number of 1:12 phases with different substitution ratios appeared, which ensured the stability of the phase structure while minimizing the loss of magnetic properties.

[0043] The above-mentioned embodiments only express several implementation methods of the present invention, and the description is relatively specific and detailed, but it cannot be understood as limiting the scope of the present invention. For ordinary technicians in this field, several modifications and improvements can be made without departing from the concept of the present invention, which all belong to the protection scope of the present invention.

Claims

1. A (Sm,T)(Fe,M) based on diffusion multi-node 12 High-throughput preparation method of phase alloys, It is characterized in that The following steps are involved: (1) preparing a package and a cover matching the package, and processing a rectangular parallelepiped groove of 3a*2b*c in the package; in millimeters, 10≥a≥3, 10≥b≥3, c≥10; (2) preparing six metal strips each having a size of a*b*c, and performing surface grinding and polishing on each of the metal strips, wherein the components of the six metal strips are Fe, Sm, T1, T2, M1, and M2, respectively, wherein T1 and T2 are respectively one element selected from Y, Gd, Zr, Nd, or Ce, or an alloy consisting of several elements; M1 and M2 are respectively one element selected from Ti, Cr, Mn, Mo, Si, Al, Co, or V, or an alloy consisting of several elements, wherein a, b, and c are respectively the length, width, and height of the metal strip; (3) Arranging the six metal strips after surface grinding and polishing in order into a rectangular structure of 3a*2b*c, assembling them into the rectangular groove, covering them with a lid, and performing vacuum electron beam welding on the package; the arrangement is that the metal strip with a composition of Sm and the metal strip with a composition of Fe are respectively located in the middle of the upper and lower rows of the rectangular structure, the metal strip with a composition of M1 and the metal strip with a composition of M2 are respectively located on the left and right sides of the metal strip with a composition of Fe, and the metal strip with a composition of T1 and the metal strip with a composition of T2 are respectively located on the left and right sides of the metal strip with a composition of Sm; (4) subjecting the welded package to hot isostatic pressing to obtain a diffusion multi-element node; (5) Cut the diffusion multi-node into multiple slices in the height direction, seal the diffusion multi-node slices, and perform diffusion heat treatment at different heat treatment temperatures and times after sealing. The diffusion heat treatment time is 2 to 30 days, the diffusion heat treatment temperature is 800 to 1300°C, and the cooling method of the diffusion heat treatment is quenching to obtain (Sm, T)(Fe, M) based on the diffusion multi-node. 12 Phase alloy.

2. The (Sm, T) (Fe, M) based diffusion multi-node according to claim 1 12 High-throughput preparation method of phase alloys, It is characterized in that In step (1), the sheath material is one of 304 stainless steel, pure iron or Cr metal, and the cover is made of the same material as the sheath.

3. The (Sm, T) (Fe, M) based diffusion multi-node according to claim 1 12 High-throughput preparation method of phase alloys, It is characterized in that The surface grinding and polishing treatment in step (2) includes sandpaper grinding and polishing by a polishing machine.

4. The (Sm, T) (Fe, M) based diffusion multi-node according to claim 1 12 High-throughput preparation method of phase alloys, It is characterized in that The vacuum degree of the vacuum electron beam welding in step (3) should be 5*10 -5 ~5*10 -4 Pa, weld width is 0.5~1.5mm.

5. The (Sm, T) (Fe, M) based diffusion multi-node according to claim 1 12 High-throughput preparation method of phase alloys, It is characterized in that The temperature of the hot isostatic pressing treatment in step (4) is 650-950° C., the time is 2-5 hours, and the pressure is 50-200 MPa.

6. The high-throughput preparation method of the (Sm,T)(Fe,M) 12 phase alloy based on diffusion multiple joints according to claim 1 It is characterized in that The atmosphere of the tube sealing in step (5) is 0.03-0.06 MPa argon atmosphere.

7. The (Sm, T) (Fe, M) based diffusion multi-node according to claim 1. 12 High-throughput preparation method of phase alloys, It is characterized in that In the step (5), (Sm, T) (Fe, M) 12 In the phase alloy, Sm is samarium, Fe is iron, T is one or more of Y, Gd, Zr, Nd or Ce; and M is one or more of Ti, Cr, Mn, Mo, Si, Al, Co or V.

8. A (Sm, T) (Fe, M) prepared by a high-throughput method based on diffusion multi-nodes according to any one of claims 1 to 7 12 Phase alloy.

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