A method for preparing an aluminum silicon carbide composite material and applications thereof

Abstract

The present disclosure relates to the technical field of inorganic material preparation, and particularly relates to a preparation method and application of aluminum silicon carbide composite material; the preparation method comprises the following steps: preparing an aluminum metal organic framework material; providing or preparing a silicon-containing organic compound; mixing the prepared aluminum metal organic framework material and the provided or prepared silicon-containing organic compound in an organic solution, adding a surfactant, performing in-situ reaction, and obtaining a silicon-containing aluminum metal organic framework material; and finally, performing heat treatment on the silicon-containing aluminum metal organic framework material to obtain the aluminum silicon carbide composite material.

Description

Technical Field

[0001] This disclosure relates to the field of inorganic material preparation technology, and in particular to a method for preparing aluminum silicon carbide composite materials and their applications. Background Technology

[0002] As a third-generation electronic packaging heat dissipation material, silicon carbide (SiC) material features a low coefficient of thermal expansion, high thermal conductivity, and excellent mechanical properties. It is used in the packaging of integrated circuits, electronic components, and precision instruments to address the thermal failure problems of highly integrated electronic circuits, high-power devices, and high-frequency devices. It is a very important ceramic-metal matrix composite material. Among these properties, mechanical properties are a key factor in the support of SiC substrates for integrated circuits, electronic components, and precision instruments, determining the thermal adaptation cycle life under operating conditions.

[0003] From a microscopic perspective, the interfaces of aluminum silicon carbide (ASC) materials are classified into ceramic-ceramic, ceramic-metal, and metal-metal interfaces. The bonding strength of the ceramic-metal and metal-metal interfaces is a key factor determining the mechanical properties of ASC materials. Currently, there are various methods for strengthening ASC materials, mainly including replacing high-strength alloys, increasing infiltration pressure, and reducing silicon carbide particle size. However, all of these methods suffer from the problem of uncontrollable cooling rates, leading to large fluctuations and poor stability in mechanical properties. Therefore, there is an urgent need to develop a novel method for preparing ASC composite materials to improve the bonding strength of ceramic-metal and metal-metal interfaces, thereby meeting the requirements for higher mechanical properties. Summary of the Invention

[0004] This disclosure provides a method for preparing aluminum silicon carbide composite materials and their applications, in order to address the shortcomings of related technologies.

[0005] According to a first aspect of the present disclosure, a method for preparing an aluminum silicon carbide composite material is provided, the method comprising the following steps: Step 1: preparing an aluminum-based metal-organic framework material.

[0006] Step 2: Provide or prepare a silicon-containing organic compound.

[0007] Step 3: Mix the aluminum-based metal-organic framework material prepared in Step 1 and the silicon-containing organic compound provided or prepared in Step 2 in an organic solution, and add a surfactant to carry out an in-situ reaction to obtain a silicon-containing aluminum-based metal-organic framework material.

[0008] Step 4: The silicon-containing aluminum-based metal-organic framework material is calcined successively in an inert gas environment, in air, and in a reducing gas environment to obtain the aluminum silicon carbide composite material.

[0009] In one aspect of this disclosure, the aluminum silicon carbide composite material is an aluminum silicon carbide powder material.

[0010] In an aspect of the embodiments of the present disclosure, a preparation method of an aluminum silicon carbide composite material is provided, and the preparation method comprises the following steps: step 1, preparing an aluminum metal organic framework material.

[0011] Step 2, providing or preparing a silicon-containing organic compound.

[0012] Step 3, mixing the aluminum metal organic framework material prepared in step 1 and the silicon-containing organic compound provided or prepared in step 2 in an organic solution, adding a surfactant, and performing an in-situ reaction to obtain a silicon-containing aluminum metal organic framework material.

[0013] Step 4, calcining the silicon-containing aluminum metal organic framework material in argon first, then in air, and finally in hydrogen / argon mixed gas to obtain the aluminum silicon carbide composite material.

[0014] In an aspect of the embodiments of the present disclosure, preferably, step 4 comprises: calcining the silicon-containing aluminum metal organic framework material in argon at 500-600°C for 3-8h first, then cooling to 420-450°C, introducing air, calcining for 2-3h, finally heating to 480-520°C, calcining in argon for 1-2h first, then in hydrogen / argon mixed gas for 2-3h, and cooling to room temperature to obtain the aluminum silicon carbide composite material.

[0015] In an aspect of the embodiments of the present disclosure, further preferably, step 4 comprises: calcining the silicon-containing aluminum metal organic framework material in argon at 550°C for 6h first, then cooling to 220°C, introducing air, calcining for 2.5h, finally heating to 450°C, calcining in argon for 1h first, then in hydrogen / argon mixed gas for 2.5h, and cooling to room temperature to obtain the aluminum silicon carbide composite material.

[0016] In an aspect of the embodiments of the present disclosure, the aluminum silicon carbide composite material further comprises a first metal element, wherein the first metal element is selected from V, Zr, Hf, Ta, Nb, Re, Mo or Y.

[0017] In an aspect of the embodiments of the present disclosure, the preparation method comprises the following steps: step 1, preparing an aluminum metal organic framework material.

[0018] Step 2, providing or preparing a silicon-containing organic compound, and providing or preparing a compound containing a first metal element.

[0019] Step 3: mixing the aluminum-based metal organic framework material prepared in step 1, the silicon-containing compound provided or prepared in step 2, and the compound containing the first metal element provided or prepared in step 2 in an organic solution, adding a surfactant, and performing in-situ reaction to obtain the aluminum-based metal organic framework material containing silicon and the first metal element.

[0020] Step 4: calcining the aluminum-based metal organic framework material containing silicon and the first metal element in argon first, then in air, and finally in hydrogen / argon mixed gas to obtain the aluminum silicon carbide composite material containing the first metal element.

[0021] In an aspect of the embodiments of the present disclosure, step 1 comprises: step 1-1: stirring aluminum nitrate, 1,3,5-tris(4-carboxylphenyl)benzene, nitric acid, and a first organic solvent uniformly and adding into a reaction kettle; and then reacting at 150-180°C for 24-48h to obtain the product of step 1-1.

[0022] Step 1-2: washing and drying the product of step 1-1 to obtain the aluminum-based metal organic framework material.

[0023] In an aspect of the embodiments of the present disclosure, the silicon-containing organic compound contains a carbodiimide group.

[0024] In an aspect of the embodiments of the present disclosure, the silicon-containing compound is selected from bis(trimethylsilyl)carbodiimide.

[0025] In an aspect of the embodiments of the present disclosure, the first metal element is selected from Zr.

[0026] In an aspect of the embodiments of the present disclosure, the organic compound containing the first metal element is selected from zirconium acetylacetonate.

[0027] In an aspect of the embodiments of the present disclosure, the first organic solvent is selected from DMF, DMA, or NMP.

[0028] In an aspect of the embodiments of the present disclosure, preferably, the first organic solvent is selected from DMF.

[0029] According to a second aspect of the embodiments of the present disclosure, an aluminum silicon carbide composite material is provided, which is prepared by the aforementioned preparation method.

[0030] According to a third aspect of the embodiments of the present disclosure, the use of the aluminum silicon carbide composite material prepared by the aforementioned preparation method or the aforementioned aluminum silicon carbide composite material in preparing high-mechanical-property and high-temperature-resistant materials is provided.

[0031] The technical scheme provided by the embodiments of the present disclosure can have the following beneficial effects: as can be known from the above embodiments, the present disclosure ingeniously utilizes the adsorption of MOF materials on small-molecule organic compounds, combines silicon-containing organic compounds with MOF materials based on aluminum, and obtains aluminum silicon carbide composite materials through heat treatment. Moreover, since the silicon-containing compounds are adsorbed in the interlayer space of the MOF materials, the aluminum silicon carbide composite materials obtained by the present disclosure have an interpenetrating phase composite structure, which greatly enhances the mechanical properties thereof.

[0032] It should be understood that the above general description and the following detailed description are only exemplary and explanatory, and cannot limit the present disclosure. BRIEF DESCRIPTION OF DRAWINGS

[0033] The accompanying drawings, which are incorporated into and form part of the specification, illustrate embodiments consistent with the present disclosure and, together with the description, serve to explain the principles of the disclosure.

[0034] Figure 1 is an SEM image of the sample obtained in Example 1.

[0035] Figure 2 is another SEM image of the sample obtained in Example 1.

[0036] Figure 3 is a TEM image of the sample obtained in Example 1.

[0037] Figure 4 is an XRD image of the samples obtained in Example 1 and Example 2. DETAILED DESCRIPTION

[0038] The exemplary embodiments will be described in detail herein with reference to the attached drawings. When the description below refers to the drawings, the same numbers in different drawings refer to the same or similar elements unless otherwise noted. The implementations described in the following exemplary embodiments do not represent all implementations consistent with the present disclosure. Instead, they are merely examples of apparatuses and methods consistent with some aspects of the present disclosure as detailed in the appended claims.

[0039] For the purposes of the present application, the technical solutions and advantages will be more apparent, the technical solutions of the present application will be described in detail below in conjunction with the embodiments. Obviously, the described embodiments are part of the embodiments of the present application, rather than all the embodiments. The embodiments described herein are illustrative in nature and serve to provide a basic understanding of the present application. The embodiments of the present application should not be interpreted as a limitation of the present application.

[0040] For the sake of brevity, only some numerical ranges are specifically disclosed herein. However, any lower limit can be combined with any upper limit to create a range not expressly recited; and, any lower limit can be combined with any other lower limit, and any upper limit can be combined with any other upper limit, to create a range not expressly recited. Further, each individual disclosed point or singular value can be combined with any other point or singular value, either as a lower or upper limit, or with other lower or upper limits, to create a range not expressly recited.

[0041] In this document, the terms "comprise", "comprising", or any other variation thereof, are intended to cover a non-exclusive inclusion, such that a process, method, article, or apparatus that comprises a list of elements does not include only those elements but can include other elements not expressly listed or inherent to such process, method, article, or apparatus. An element proceeded by "comprises... a" does not, without more constraints, exclude the presence of additional identical elements in the process, method, article, or apparatus that comprises the element.

[0042] In the description herein, "above", "below" include the number itself, unless otherwise indicated.

[0043] Unless otherwise defined, all terms used in the disclosure, including technical or scientific terms, have the meaning commonly understood by one of ordinary skill in the art to which the disclosure pertains. Unless otherwise stated, the numerical values of various parameters set forth in the disclosure can be measured using any of the various measuring methods commonly used in the art (for example, can be tested according to the methods given in the examples of the disclosure).

[0044] The term "about" is used to describe and account for small variations. When used in connection with an event or circumstance, the term can refer to instances in which the event or circumstance occurs exactly, as well as instances in which the event or circumstance occurs with a close approximation. For example, when used in connection with a numerical value, the term can refer to a range of variation less than or equal to ±10% of the numerical value, such as less than or equal to ±5%, less than or equal to ±4%, less than or equal to ±3%, less than or equal to ±2%, less than or equal to ±1%, less than or equal to ±0.5%, less than or equal to ±0.1%, or less than or equal to ±0.05%. Additionally, quantities, ratios, and other numerical values are sometimes presented herein in a range format. It is to be understood that such range format is used for convenience and brevity and should be understood as having been preceeded by the word "about". Also, a number of different aspects are presented with respect to the various embodiments. However, these aspects are not mutually exclusive; a single aspect can implement one or more features from a number of aspects.

[0045] The list of items connected by “at least one of,” “at least one,” “at least one of the items in,” or other similar phrases is meant not to be limited to just the items listed. For example, if a list is provided that includes items A, B, and C, then “at least one of A, B, and C” means A alone; B alone; C alone; both A and B together; both A and C together; both B and C together; or all three of A, B, and C together. Item A can include a single component or multiple components. Item B can include a single component or multiple components. Item C can include a single component or multiple components.

[0046] In the present disclosure, the present disclosure provides a preparation method of an aluminum silicon carbide composite material: Step 1-1: aluminum nitrate, 1,3,5-tris(4-carboxylphenyl)benzene, nitric acid and DMF are stirred uniformly and added into a reaction kettle; then reacted at 150-180°C for 24-48h to obtain the product of step 1-1.

[0047] Step 1-2: The product of step 1-1 is washed and dried to obtain an aluminum metal organic framework material (MOF-519).

[0048] Step 2: Provide bis(trimethylsilyl)carbodiimide.

[0049] Step 3: Bis(trimethylsilyl)carbodiimide and the prepared aluminum metal organic framework material (MOF-519) are added into acetone, and cetyltrimethylammonium bromide is added as a surfactant, ultrasonic at room temperature for 1h, then heated to 42°C and kept ultrasonic for 5h to obtain a silicon-containing aluminum metal organic framework material.

[0050] Step 4: The silicon-containing aluminum metal organic framework material is first calcined at 500-600°C for 3-8h in argon, then cooled to 420-450°C, air is introduced and calcined for 2-3h, and finally heated to 480-520°C, first calcined in argon for 1-2h, then calcined in hydrogen / argon mixed gas for 2-3h, and cooled to room temperature to obtain an aluminum silicon carbide composite material.

[0051] The present disclosure will be further described below in conjunction with examples. It should be understood that these examples are only used to illustrate the present disclosure and not to limit the scope of the present disclosure.

[0052] Example and Comparative Example: Example 1: Example 1 includes the following steps: stirring aluminum nitrate nonahydrate (25.6 g, 68 mmol), 1,3,5-tris(4-carboxyphenyl)benzene (20 g, 46 mmol), 2 mol / L nitric acid (27.8 mL), and DMF (250 mL) uniformly, adding into a reaction kettle; then reacting at 165 °C for 32 h, washing the product obtained after the reaction with DMF 3 times, with acetone 3 times, and with deionized water 3 times, and then drying at 60 °C to obtain an aluminum-based metal organic framework material (MOF-519) of Example 1.

[0053] Weighing 15 g of the aluminum-based metal organic framework material prepared, 8 g of bis(trimethylsilyl)carbodiimide, adding into 80 mL of acetone, then adding 1.5 g of cetyltrimethylammonium bromide, and then ultrasonicating at room temperature for 1 h, and then heating to 42 °C and ultrasonicating for 5 h to obtain a silicon-containing aluminum-based metal organic framework material of Example 1.

[0054] The silicon-containing aluminum-based metal organic framework material of Example 1 is first calcined at 550 °C for 6 h under argon, then cooled to 435 °C, and then calcined under air for 2.5 h, and finally heated to 510 °C, calcined under argon for 1 h, and then calcined under hydrogen / argon mixed gas for 2.5 h, and then cooled to room temperature to obtain an aluminum silicon carbide composite material of Example 1. According to EDS and XRD tests, the purity of the aluminum silicon carbide obtained in Example 1 is above 99.6%, indicating that a high-purity aluminum silicon carbide material has been obtained.

[0055] The SEM image of Example 1 is shown in Figure 1 and Figure 2 The TEM image of Example 1 is shown in Figure 3 .

[0056] Example 2: Example 2 includes the following steps: stirring aluminum nitrate nonahydrate (25.6 g, 68 mmol), 1,3,5-tris(4-carboxyphenyl)benzene (20 g, 46 mmol), 2 mol / L nitric acid (27.8 mL), and DMF (250 mL) uniformly, adding into a reaction kettle; then reacting at 165 °C for 32 h, washing the product obtained after the reaction with DMF 3 times, with acetone 3 times, and with deionized water 3 times, and then drying at 60 °C to obtain an aluminum-based metal organic framework material (MOF-519) of Example 1.

[0057] Take 15 g of the prepared aluminum metal organic framework material, 10.5 g of γ-glycidoxypropyltrimethoxysilane (KH560), add to 80 mL of acetone, then add 1.5 g of cetyltrimethylammonium bromide, ultrasonic at room temperature for 1 h, then heat to 42℃ and keep ultrasonic for 5 h to obtain the aluminum metal organic framework material of Example 2.

[0058] The aluminum metal organic framework material of Example 2 is first calcined at 550℃ for 6 h under argon, then cooled to 435℃, and air is introduced for calcination for 2.5 h, and finally heated to 510℃, first calcined under argon for 1 h, then calcined under hydrogen / argon mixed gas for 2.5 h, and cooled to room temperature to obtain the composite material of Example 2.

[0059] The main difference between Example 2 and Example 1 is that Example 2 uses KH560 silane coupling agent instead of bis(trimethylsilyl)carbonyldiimide used in Example 1.

[0060] The XRD images of Example 1 and Example 2 are shown in Figure 4 As can be seen from the XRD images, there is no SiC peak in Example 2, indicating that the aluminum silicon carbide composite material is not successfully obtained in Example 2; while there is a SiC peak in Example 1; this is because the MOF-519 used in the example has a good adsorption effect on small molecule organic compounds containing carbonyl groups and imine groups, so in Example 1, the silicon-containing compound is well combined with the MOF material, while the silane coupling agent used in Example 2 is difficult to combine with the MOF material.

[0061] Mechanical property test: the product of Example 1 is tested according to GBT12444-2006 "Metal material wear test method" test ring-test block sliding wear test, and equal quality of Example 1 and commercially available aluminum-based silicon carbide powder material is coated on a polycarbonate substrate, then the wear rate of the sample to be tested is tested under the conditions of loading force of 204 g, friction time of 10 min, rotation speed of 180 revolutions / minute, and rotation number of 1800 times; the wear rate of commercially available aluminum-based silicon carbide material is also tested; the wear rate of commercially available aluminum-based silicon carbide material is measured to be 8.71*10 -15 m 3 / m·N, and the wear rate of the product of Example 1 is 1.58*10 -15 m 3 / m·N. This is due to the adsorption of silicon-containing compounds in the interlayer space of the MOF material, so that the aluminum silicon carbide composite material obtained by the present disclosure has an interpenetrating phase composite structure, which greatly enhances its mechanical properties. The interpenetrating phase composite structure prepared by the present disclosure is a composite material composed of two or more topological co-continuous phases, having a three-dimensional penetrating interconnected structure; compared with traditional particle reinforced composites, the co-continuous interconnected structure of the interpenetrating phase composite structure has excellent performance at room temperature and high temperature.

[0062] Other embodiments of the present disclosure will be apparent to those skilled in the art from consideration of the specification and practice of the present disclosure. It is intended that the present disclosure cover any variations, uses, or adaptations of the present disclosure following, in general, the principles of the present disclosure and including such departures from the present disclosure that come within known or customary practice within the art to which the present disclosure pertains or that are otherwise obvious.

Claims

1. A method for preparing an aluminum-silicon carbide composite material, characterized in that, The preparation method includes the following steps: Step 1: preparing an aluminum-based metal-organic framework material; Step 2: providing or preparing a silicon-containing organic compound; Step 3: mixing the aluminum-based metal-organic framework material prepared in Step 1 and the silicon-containing organic compound provided or prepared in Step 2 in an organic solution, and adding a surfactant to carry out an in-situ reaction to obtain a silicon-containing aluminum-based metal-organic framework material; Step 4: calcining the silicon-containing aluminum-based metal-organic framework material successively in an inert gas environment, in air, and in a reducing gas to obtain the aluminum silicon carbide composite material.

2. The preparation method according to claim 1, characterized in that, The aluminum silicon carbide composite material further includes a first metallic element, wherein the first metallic element is selected from V, Zr, Hf, Ta, Nb, Re, Mo or Y.

3. The preparation method according to claim 2, characterized in that, The preparation method The process includes the following steps: Step 1: preparing an aluminum-based metal-organic framework material; Step 2: providing or preparing a silicon-containing organic compound, and providing or preparing a compound containing a first metal element; Step 3: mixing the aluminum-based metal-organic framework material prepared in Step 1, the silicon-containing compound provided or prepared in Step 2, and the compound containing the first metal element provided or prepared in Step 2 in an organic solution, and adding a surfactant to carry out an in-situ reaction to obtain an aluminum-based metal-organic framework material containing silicon and a first metal element; Step 4: calcining the aluminum-based metal-organic framework material containing silicon and a first metal element first in argon, then in air, and finally in a hydrogen / argon mixture to obtain the aluminum silicon carbide composite material containing the first metal element.

4. The preparation method according to any one of claims 1-3, characterized in that, Step 1 includes: Step 1-1: Aluminum nitrate, 1,3,5-tris(4-carboxyphenyl)benzene, nitric acid and the first organic solvent are stirred evenly and added to a reaction vessel; then the reaction is carried out at 150℃-180℃ for 24-48h to obtain the product of Step 1-1; Step 1-2: The product of Step 1-1 is washed and dried to obtain the aluminum-based metal-organic framework material.

5. The preparation method according to claim 3, characterized in that, The silicon-containing organic compound contains a carbodiimide group.

6. The preparation method according to claim 5, characterized in that, The silicon-containing compound is selected from di(trimethylsilyl)carbodiimide.

7. The preparation method according to claim 3, characterized in that, The first metallic element is selected from Zr.

8. The preparation method according to claim 7, characterized in that, The organic compound containing the first metallic element is selected from zirconium acetylacetone.

9. An aluminum-silicon carbide composite material, characterized in that, The aluminum silicon carbide composite material is prepared by the preparation method according to any one of claims 1-8.

10. The aluminum silicon carbide composite material prepared by the preparation method according to any one of claims 1-8, or the aluminum silicon carbide composite material according to claim 9, in the preparation of materials with high mechanical properties and high temperature resistance.

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