Layered quantum magnetic materials and their preparation methods

By inserting macromolecules into layered quantum magnetic materials and controlling their interlayer distance and coupling strength, the problem of controlling two-dimensional magnetic materials in existing technologies has been solved. This has enabled the control of magnetic phase transition temperature and the increase of lattice parameters, promoting the development of spintronic devices and the study of quantum critical phenomena.

CN115583637BActive Publication Date: 2025-10-31RENMIN UNIVERSITY OF CHINA
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Patent Information

Application Number
CN202110756014.6
Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
Filing Date
2021-07-05
Publication Date
2025-10-31
Estimated Expiration
2041-07-05

AI Technical Summary

Technical Problem

Existing technologies have difficulty effectively controlling the physical properties of two-dimensional magnetic materials, especially the interlayer coupling strength and magnetic phase transition temperature, which limits their application in spintronic devices.

Method used

By placing a quasi-two-dimensional layered quantum magnetic compound on a platinum sheet to form a negative electrode, winding a platinum wire to form a positive electrode, and then intercalating macromolecules, such as 1-ethyl-3-methylimidazolium tetrafluoroborate or diethylmethyl-(2-methoxyethyl)ammonium bis(trifluoromethanesulfonyl)imide, in a macromolecular solution, the voltage and temperature are controlled to insert the interlayer, thereby regulating the interlayer distance and coupling strength.

Benefits of technology

The magnetic phase transition temperature of layered quantum magnetic materials was successfully controlled, the lattice parameter in the c-direction was increased, the coupling effect was weakened, and the development of spintronic devices and the study of quantum critical phenomena were promoted.

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Abstract

This invention provides a layered quantum magnetic material and its preparation method. The method includes: (a) preparing a negative electrode; (b) preparing a positive electrode; (c) placing the positive and negative electrodes in a solution containing macromolecules; and (d) applying an electric current to the positive and negative electrodes at a predetermined temperature for a predetermined time to intercalate macromolecules into a quasi-two-dimensional layered quantum magnetic compound, thereby obtaining a layered quantum magnetic material intercalated with macromolecules. The quasi-two-dimensional layered quantum magnetic compound includes a transition metal phosphorus trichalcogenide, and the macromolecules include at least one of 1-ethyl-3-methylimidazolium tetrafluoroborate and diethylmethyl-(2-methoxyethyl)ammonium bis(trifluoromethanesulfonyl)imide. According to the method for preparing layered quantum magnetic materials of this invention, by applying a voltage to insert macromolecules into the interlayer of the layered quantum magnetic material, the lattice parameters in the c-direction of the layered quantum magnetic material are effectively increased, and the magnetic phase transition temperature is successfully reduced.
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Description

Technical Field

[0001] This invention relates to a layered quantum magnetic material and its preparation method, and more specifically, to a bulk layered quantum magnetic material and a method for preparing the bulk layered quantum magnetic material. Background Technology

[0002] The discovery of graphene in 2004 opened up research into various two-dimensional materials (such as transition metal sulfides and black phosphorus). These materials possess unique physical properties and potential applications, and their novel properties and application potential have made them an important research area in condensed matter and materials physics, with broad application prospects in many fields. However, currently, many two-dimensional materials are not magnetic, which poses a significant challenge to the research of spintronic devices.

[0003] In recent years, two-dimensional magnetic materials have become a research hotspot internationally. They can maintain spontaneous magnetization down to the thickness of a single unit cell, providing a new research platform for understanding and controlling low-dimensional magnetism. They also open up new directions for the development of two-dimensional magnetic and spintronic devices, and have significant application value in novel optoelectronic devices and spintronic devices. However, current research is still in its early stages, focusing mostly on ferromagnetic two-dimensional materials, and the methods for controlling them are relatively limited.

[0004] Transition metal phosphorus trichalcogenides (MPX3, where M = Mn, Fe, Ni, etc., and X = S, Se) are quasi-two-dimensional layered quantum magnetic compounds with weak van der Waals interactions between their layers and intrinsic magnetism. These compounds exhibit different antiferromagnetic states in their ground state, which has great potential for future applications in information storage. Furthermore, the manipulation of these materials can provide a deeper understanding of their magnetic coupling and magnetic phase transition mechanisms, promoting their application in the fabrication of spintronic devices. It also allows for the manipulation and suppression of magnetic order to study quantum critical phenomena.

[0005] Therefore, a means that can be widely applied to control the properties of two-dimensional magnetic materials is needed. Summary of the Invention

[0006] The purpose of this invention is to provide a method for preparing layered quantum magnetic materials, which can control the interlayer distance of the layered quantum magnetic materials, change their interlayer coupling strength, and thus control the magnetic phase transition temperature of the layered quantum magnetic materials.

[0007] Another object of the present invention is to provide a layered quantum magnetic material having a large c-direction lattice parameter and a controllable magnetic phase transition temperature.

[0008] According to one aspect of the present invention, a method for preparing a layered quantum magnetic material is provided, the method comprising: (a) placing a quasi-two-dimensional layered quantum magnetic compound on a platinum sheet to obtain a negative electrode; (b) winding a platinum wire around a coil to obtain a positive electrode; (c) placing the positive and negative electrodes in a solution comprising macromolecules; and (d) energizing the positive and negative electrodes at a predetermined temperature for a predetermined time to intercalate macromolecules in the quasi-two-dimensional layered quantum magnetic compound, thereby obtaining a layered quantum magnetic material intercalated with macromolecules, wherein the quasi-two-dimensional layered quantum magnetic compound comprises a transition metal phosphorus trichalidinium compound, wherein the macromolecules comprise at least one of 1-ethyl-3-methylimidazolium tetrafluoroborate and diethylmethyl-(2-methoxyethyl)ammonium bis(trifluoromethanesulfonyl)imide.

[0009] According to embodiments of the present invention, a transition metal phosphorus trichalcogenide can be represented by MPX3, wherein M = Mn, Fe or Ni, and X = S or Se.

[0010] According to embodiments of the present invention, the quasi-two-dimensional layered quantum magnetic compound can be one of FePS3 and FePSe3.

[0011] According to an embodiment of the present invention, a quasi-two-dimensional layered quantum magnetic compound can be placed on a platinum sheet using conductive adhesive.

[0012] According to an embodiment of the present invention, after the quasi-two-dimensional layered quantum magnetic compound is placed on a platinum sheet using conductive adhesive, it can be left for 30 minutes to 1 hour to ensure good conductivity at the conductive adhesive joint.

[0013] According to an embodiment of the present invention, step (d) can be performed at a voltage of 2V to 4V.

[0014] According to an embodiment of the present invention, the predetermined time can be from 24 hours to 48 hours.

[0015] According to an embodiment of the present invention, the predetermined temperature can be from 30°C to 80°C.

[0016] According to another aspect of the present invention, a layered quantum magnetic material is provided, wherein the c-direction lattice parameter of the layered quantum magnetic material is... to Furthermore, the antiferromagnetic phase transition temperature of this layered quantum magnetic material is 72K to 82K.

[0017] According to the method for preparing layered quantum magnetic materials of the present invention, macromolecular substances are inserted into the interlayer of the layered quantum magnetic material by applying voltage, which effectively increases the c-direction lattice parameter of the layered quantum magnetic material, weakens its coupling effect, and successfully reduces the magnetic phase transition temperature of the layered quantum magnetic material. Thus, the material system can be controlled by this method, which can also promote the development of spintronic devices and help study quantum critical phenomena. Attached Figure Description

[0018] The above and / or other features and aspects of the invention will become clear and readily understood through the description of examples in conjunction with the accompanying drawings.

[0019] Figure 1 This is a flowchart illustrating a method for preparing layered quantum magnetic materials according to an embodiment of the present invention.

[0020] Figure 2 The XRD diffraction patterns shown are those of Comparative Example 1 and Example 1 according to the present invention.

[0021] Figure 3 The XRD diffraction patterns of Comparative Example 2 and Example 2 according to the present invention are shown.

[0022] Figure 4 and Figure 5 The figures shown are comparative example 1 and example 1 according to the present invention, respectively, showing magnetic susceptibility measurement graphs.

[0023] Figure 6 and Figure 7 The graphs shown are comparative example 2 and example 2 according to the present invention, respectively, showing the magnetic susceptibility measurement. Detailed Implementation

[0024] The present invention will now be explained by referring to the accompanying drawings, which illustrate embodiments. However, the invention may be embodied in many different forms and should not be construed as limited to the exemplary embodiments set forth herein. These embodiments are provided so that the disclosure of the invention will be thorough and complete, and will fully convey the scope of the invention to those skilled in the art.

[0025] Figure 1 This is a flowchart illustrating a method for preparing layered quantum magnetic materials according to an embodiment of the present invention.

[0026] Reference Figure 1 According to an embodiment of the present invention, a method for preparing layered quantum magnetic materials includes the following steps: preparing a negative electrode (S100), preparing a positive electrode (S200), placing the positive electrode and the negative electrode in a solution containing macromolecules (S300), and energizing the positive electrode and the negative electrode at a predetermined temperature for a predetermined time (S400).

[0027] In the step of preparing the negative electrode (S100), a quasi-two-dimensional layered quantum magnetic compound is placed on a platinum sheet to obtain the negative electrode. Specifically, the quasi-two-dimensional layered quantum magnetic compound can be placed (e.g., adhered) on the platinum sheet using conductive adhesive to obtain the negative electrode. More specifically, after placing (e.g., adhering) the quasi-two-dimensional layered quantum magnetic compound on the platinum sheet using conductive adhesive, the negative electrode can be left for 30 minutes to 1 hour to ensure good conductivity at the conductive adhesive joints.

[0028] In embodiments of the present invention, the quasi-two-dimensional layered quantum magnetic compound includes (for example, a transition metal phosphorus trichalcogenide). The transition metal phosphorus trichalcogenide can be represented by MPX3, where M = Mn, Fe, or Ni, and X = S or Se. In a preferred embodiment of the present invention, the quasi-two-dimensional layered quantum magnetic compound can be one of FePS3 and FePSe3.

[0029] In the step of preparing the positive electrode (S200), a platinum wire is wound around a coil to obtain the positive electrode. However, the present invention is not limited to this, and the positive electrode can be obtained by any suitable method.

[0030] Furthermore, in embodiments of the present invention, the steps of preparing the negative electrode and preparing the positive electrode are not sequential. For example, the steps of preparing the positive electrode can be performed first and then the steps of preparing the negative electrode can be performed, or the steps of preparing the negative electrode and preparing the positive electrode can be performed simultaneously.

[0031] In the step (S300) of placing the positive and negative electrodes in a solution containing macromolecules, the positive and negative electrodes are placed in a solution containing macromolecules, and it is ensured that the solution containing macromolecules can completely impregnate the positive and negative electrodes.

[0032] In embodiments of the present invention, the macromolecule includes 1-ethyl-3-methylimidazolium tetrafluoroborate (C6H 11 BF4N2) and diethylmethyl-(2-methoxyethyl)ammonium bis(trifluoromethanesulfonyl)imide (C 10 H 20 At least one of F6N2O5S2).

[0033] In the step (S400) of energizing the positive and negative electrodes at a predetermined temperature for a predetermined time, by applying voltage and through the action of electric field and diffusion, macromolecules can be intercalated into the quasi-two-dimensional layered quantum magnetic compound to obtain a layered quantum magnetic material with intercalated macromolecules.

[0034] Specifically, step (S400) can be performed at a voltage of 2V to 4V. In embodiments of the present invention, if the voltage is too low, the intercalation of macromolecules cannot be completed; if the voltage is too high, the formed layered quantum magnetic material will be damaged. By controlling the voltage within this range, macromolecules can be intercalated into the quasi-two-dimensional layered quantum magnetic compound through the action of electric field and diffusion, increasing the interlayer distance in the c-direction of the layered quantum magnetic material. In embodiments of the present invention, preferably, step (S400) can be performed at a voltage of 3V.

[0035] Furthermore, the predetermined time in step (S400) can be determined based on the hardness of the layered quantum magnetic material to be formed. Preferably, the predetermined time can be 24 hours to 48 hours. If the predetermined time is too short, it will be insufficient to complete the intercalation of macromolecules; if the predetermined time is too long, it will damage the formed layered quantum magnetic material.

[0036] For example, step (S400) can be performed at a temperature of 30°C to 80°C (e.g., preferably 60°C) and a voltage of 2V to 4V for 24h to 48h.

[0037] According to the method for preparing layered quantum magnetic materials of the present invention, macromolecular substances are inserted into the interlayer of the layered quantum magnetic material by applying voltage, which effectively increases the c-direction lattice parameter of the layered quantum magnetic material, weakens its coupling effect, and successfully reduces the magnetic phase transition temperature of the layered quantum magnetic material. Thus, the material system can be controlled by this method, which can also promote the development of spintronic devices and help study quantum critical phenomena.

[0038] The c-direction lattice parameters of the layered quantum magnetic material according to the present invention are as follows: to Furthermore, the antiferromagnetic phase transition temperature of this layered quantum magnetic material is 72K to 82K.

[0039] The process of testing XRD patterns and magnetic susceptibility will be described below.

[0040] XRD patterns were measured using a stepwise scanning method. X-ray (Cu): voltage 40 kV, current 30 mA; angle: resolution 1.00000 deg, scan angle 1.00000 deg, acceptance 0.30000 mm; scanning: drive shafts 1 Theta-2 Theta linked, scanning range 10.000-30.000, continuous scanning mode, scanning speed 2.0000 deg / min.

[0041] The magnetic susceptibility was measured by applying a 100 Gauss magnetic field in the c direction using an MPMSy instrument and cooling at a rate of 2 K / min.

[0042] The layered quantum magnetic material and its preparation method according to the present invention will be described in detail below with reference to examples.

[0043] Example 1

[0044] The FePS3 material is adhered to a platinum sheet using conductive adhesive and left for about half an hour to ensure good conductivity at the adhesive joint, thus obtaining the negative electrode. The platinum wire is wound around a coil to obtain the positive electrode. The negative and positive electrodes are completely immersed in 1-ethyl-3-methylimidazolium tetrafluoroborate. The material is then energized at 3V for 24 hours at 50°C to obtain a layered quantum magnetic material.

[0045] FePS3 that was not treated by the method of the present invention was used as Comparative Example 1, and XRD diffraction measurements were performed on Comparative Example 1 and Example 1, with reference to... Figure 2 The lattice parameters in the c-direction of Example 1 are as follows: The c-direction lattice parameter of Example 1 after macromolecular intercalation is: This indicates that the lattice of Example 1, after the macromolecules are inserted into the interlayer, expands to approximately 1.54 times its original size in the c-direction. (Refer to...) Figure 4 and Figure 5 Magnetic susceptibility measurements revealed that the antiferromagnetic phase transition temperature (T1) of the unintercalated comparative example 1 was significantly lower. N The temperature of the antiferromagnetic phase transition (T) in Example 1 after intercalation is approximately 123 K, while the temperature of the antiferromagnetic phase transition (T) in Example 1 after intercalation is approximately 123 K. N The value was approximately 72 K, indicating that the method successfully inserted macromolecules into layered quantum magnetic materials and controlled their magnetic phase transition temperature.

[0046] Example 2

[0047] The FePSe3 material was adhered to a platinum sheet using conductive adhesive and left for about half an hour to ensure good conductivity at the adhesive joint, thus obtaining the negative electrode. The platinum wire was wound around the coil to obtain the positive electrode. The negative and positive electrodes were completely immersed in diethylmethyl-(2-methoxyethyl)ammonium bis(trifluoromethanesulfonyl)imide. The material was then energized at 3.3V at 60°C for 24 hours to obtain a layered quantum magnetic material.

[0048] FePSe3 that was not treated by the method of the present invention was used as Comparative Example 2, and XRD diffraction measurements were performed on Comparative Example 2 and Example 2, with reference to... Figure 3 The lattice parameters in the c-direction of Example 2 are as follows: The c-direction lattice parameter of Example 2 after macromolecular intercalation is: This indicates that the lattice of Example 2, after the macromolecules are inserted into the interlayer, expands to approximately 1.54 times its original size in the c-direction. (Refer to...) Figure 6 and Figure 7Magnetic susceptibility measurements revealed that the antiferromagnetic phase transition temperature (T) of the unintercalated comparative example 2 was significantly lower. N The temperature of the antiferromagnetic phase transition (T) in Example 2 after intercalation is approximately 120 K, while the temperature of the antiferromagnetic phase transition (T) in Example 2 is approximately 120 K. N The value was approximately 82 K, indicating that the method successfully inserted macromolecules into layered quantum magnetic materials and controlled their magnetic phase transition temperature.

[0049] In summary, the method for preparing layered quantum magnetic materials according to embodiments of the present invention effectively increases the c-direction lattice parameters of the layered quantum magnetic materials by inserting macromolecular substances into the interlayer space of the layered quantum magnetic materials through the application of voltage, thereby weakening the coupling effect and successfully reducing the magnetic phase transition temperature of the layered quantum magnetic materials. This method enables the control of the material system, promotes the development of spintronic devices, and helps in the study of quantum critical phenomena.

[0050] While the invention has been specifically shown and described with reference to exemplary embodiments thereof, those skilled in the art will understand that various changes in form and detail may be made herein without departing from the spirit and scope of the invention as defined by the claims and their equivalents. The embodiments should be considered merely in a descriptive sense and not for limiting purposes. Therefore, the scope of the invention is not defined by the specific embodiments thereof, but by the claims, and all differences within that scope will be construed as included in the invention.

Claims

1. A method for preparing layered quantum magnetic materials, the method comprising: (a) A quasi-two-dimensional layered quantum magnetic compound is placed on a platinum sheet to obtain a negative electrode; (b) Wrap a platinum wire around a coil to obtain the positive electrode; (c) Place the positive and negative electrodes in a solution containing macromolecules; as well as (d) Applying current to the positive and negative electrodes at a predetermined temperature for a predetermined time to intercalate macromolecules into a quasi-two-dimensional layered quantum magnetic compound, thereby obtaining a layered quantum magnetic material intercalated with macromolecules. Among them, the quasi-two-dimensional layered quantum magnetic compound is one of FePS3 and FePSe3. The macromolecules include at least one of 1-ethyl-3-methylimidazolium tetrafluoroborate and diethylmethyl-(2-methoxyethyl)ammonium bis(trifluoromethanesulfonyl)imide.

2. The method according to claim 1, wherein, Quasi-two-dimensional layered quantum magnetic compounds are placed on a platinum sheet using conductive adhesive.

3. The method according to claim 2, wherein, After placing the quasi-two-dimensional layered quantum magnetic compound onto a platinum sheet using conductive adhesive, leave it for 30 minutes to 1 hour to ensure good conductivity at the adhesive joints.

4. The method according to claim 1, wherein, Perform step (d) at a voltage of 2V to 4V.

5. The method according to claim 1 or 4, wherein, The reservation time is from 24 hours to 48 hours.

6. The method according to claim 1 or 4, wherein, The target temperature is 30℃ to 80℃.

7. A layered quantum magnetic material, wherein the layered quantum magnetic material is prepared by the method according to any one of claims 1 to 6. in, The c-direction lattice parameter of the layered quantum magnetic material is 10.4 Å to 30.6 Å, and the antiferromagnetic phase transition temperature of the layered quantum magnetic material is 72 K to 82 K.