HIGH-THERMAL CONDUCTIVITY COMPOSITE MATERIAL, PREPARATION METHOD AND APPLICATION THEREOF

Abstract

A high-thermal conductivity composite material is AlN.sub.p/ZA27 composite material, including 2%, 4%, 6%, or 8% by volume of aluminum nitride (AlN) ceramic particles and zinc-aluminium-27 (ZA27) alloy. The ZA27 alloy includes 70.52-71.08% by weight of Zn, 25.58?27.65% by weight of Al, 1.27?3.45% by weight of Cu, and 0.50% or less by weight of Mg. In the preparation of the high-thermal conductivity composite material, an as-cast AlN.sub.p/ZA27 composite material is subjected to homogenizing annealing and reciprocating extrusion.

Claims

1. A method of preparing a thermally-conductive composite material, comprising: subjecting an as-cast AlN.sub.p/ZA27 composite material to reciprocating extrusion to produce the thermally-conductive composite material; wherein the thermally-conductive composite material is an AlN.sub.p/ZA27 composite material comprising a ZA27 alloy and 2%, 4%, 6%, or 8% by volume of AlN ceramic particles.

2. The method of claim 1, further comprising: performing homogenizing annealing on the as-cast AlN.sub.p/ZA27 composite material before the reciprocating extrusion.

3. The method of claim 1, wherein the reciprocating extrusion comprises: performing a first-pass extrusion at a temperature of 250?350? C. and an extrusion rate of 0.15?0.56 mm/s in a mold for 0.5?1 h.

4. The method of claim 3, wherein a heating coil is provided for heating; and a refractory cotton is wrapped around the heating coil.

5. The method of claim 3, wherein the reciprocating extrusion further comprises: after the first-pass extrusion is completed, turning the mold by 180?, and keeping the mold at 250?350? C. for 10?30 min; and performing a second-pass extrusion, and repeating such process until a multi-pass extrusion is completed, so as to obtain the thermally-conductive composite material.

6. The method of claim 5, wherein the number of passes in the multi-pass extrusion is 4-16.

7. The method of claim 1, wherein the ZA27 alloy comprises 70.52-71.08% by weight of Zn, 25.58?27.65% by weight of Al, 1.27?3.45% by weight of Cu, and 0.50% or less by weight of Mg.

8. The method of claim 1, wherein a size of each of the AlN ceramic particles is 0.5?1.2 ?m.

9. The method of claim 1, wherein the as-cast AlN.sub.p/ZA27 composite material is prepared through steps of: melting the ZA27 alloy at 560? C.-620? C. to obtain a melted ZA27 alloy; adding the AlN ceramic particles into the melted ZA27 alloy followed by stirring for 3-5 minutes to obtain a mixture; and pouring the mixture into a graphite mold at 540? C.-560? C. for molding to obtain the as-cast AlN.sub.p/ZA27 composite material.

10. The method of claim 2, wherein the homogenizing annealing is performed at 200? C. for 6 h.

Description

BRIEF DESCRIPTION OF THE DRAWINGS

[0034] FIG. 1 is a schematic diagram of a reciprocating extrusion mold according to one embodiment of the present disclosure;

[0035] FIGS. 2a-2d are scanning electron microscope (SEM) images of grain morphology of 1 ?m-8%-RE-250? C.-4PASSES; where (a) and (b) low and high magnifications of AlN.sub.p/ZA27 composite material with 1 ?m-8 vol % AlN-RE-250? C.-4PASSES showing more undistorted equiaxed q-Zn recrystallized grains (i.e. bright color grain in the image); (c) and (d) low and high magnifications of AlN.sub.p/ZA27 composite material with 1 ?m-8 vol % AlN-RE-250? C.-4PASSES showing more undistorted equiaxed ?-Al recrystallized grains (i.e., dark color grain in the image).

[0036] FIGS. 3a and 3b are SEM images of AlN morphology and distribution: 1 ?m-8%-RE-250? C.-4PASSES; where (a) and (b) low and high magnifications of AlN.sub.p/ZA27 composite material with 1 ?m-8 vol % AlN-RE-250? C.-4PASSES showing some AlN morphologies in the microstructures (i.e., rhombic and square AlN particles with grey color distributed over matrix grains).

[0037] In the figures: 1mold base; 2cushion block; 3buffer spring; 4screw rod; 5extrusion cylinder; 6extrusion rod; and 7mold unit.

DETAILED DESCRIPTION OF EMBODIMENTS

[0038] The technical solutions of the disclosure will be described clearly and completely below. Obviously, the described embodiments are merely some embodiments of the present disclosure, which are not intended to limit the disclosure. For those skilled in the art, other embodiments obtained based on these embodiments without paying creative efforts should fall within the scope of the disclosure.

[0039] In the disclosure, unless expressly specified otherwise, all the embodiments involved herein as well as the preferred implementation methods can be combined with each other to form new technical solutions.

[0040] In the disclosure, unless expressly specified otherwise, all technical features involved herein as well as preferred features can be combined with each other to form new technical solutions.

[0041] In the disclosure, unless expressly specified otherwise, the percentage (%) or part refers to the weight percentage or weight part relative to the composition.

[0042] In the disclosure, unless expressly specified otherwise, the components involved herein, or preferred components may be combined with each other to form new technical solutions.

[0043] In the disclosure, unless expressly specified otherwise, the value range ?-b denotes an abbreviated form of any combination of real numbers between a and b, where both a and b are real numbers. For example, the value range 6?22 means that all real numbers between 6?22 have been listed herein, and 6?22 is only an abbreviated representation of the combination of these values.

[0044] The range disclosed herein may be one or more lower limits and one or more upper limits in the form of lower and upper limits, respectively.

[0045] In the disclosure, the term and/or as used herein refers to any combination and all possible combinations of one or more of the listed items.

[0046] In the disclosure, unless expressly specified otherwise, the individual reactions or steps may be performed sequentially. Preferably, the reaction methods herein are performed sequentially.

[0047] Unless expressly specified otherwise, technical terms used herein have the same meaning as those familiar to those skilled in the art. In addition, any method or material similar or equivalent to what is documented in this disclosure may also be applied in the disclosure.

[0048] Provided herein is a high-thermal conductivity composite material and preparation method and application thereof. The as-cast AlN.sub.p/ZA27 composite materials are used as the raw materials, and the final product is processed by multi-pass reciprocating extrusion large plastic deformation process. By introducing ceramic reinforced phases with strengthening effect and high-thermal conductivity, and by refining the matrix grains and improving the distribution of the reinforced phases through large plastic deformation, the as-cast AlN.sub.p/ZA27 composite materials are deformed by reciprocating extrusion to improve the morphology, thermal conductivity, and mechanical properties of the AlN.sub.p/ZA27 composite materials. According to ZnAl phase diagram, ?-Al phase, ?-Zn phase, and AlN ceramic particle reinforced phase with high-thermal conductivity exist in the reciprocating extrusion AlN.sub.p/ZA27 composite materials. After reciprocating extrusion, the ?-Al phase and ?-Zn phase undergoes dynamic recrystallization, the grains are obviously refined as undistorted and equiaxed recrystallized grains, and the AlN ceramic particles are broken and uniformly distributed along the extrusion direction. The mechanical properties and thermal conductivity of the composite materials are significantly improved under the effect of the fine grain reinforcement and second phase reinforcement.

[0049] The high-thermal conductivity composite materials are expressed as AlN.sub.p/ZA27. The volume fraction (?) of AlN ceramic particles in the composite is equal to 2%, 4%, 6%, 8%, respectively.

[0050] By mass percentage, the ZA27 matrix alloy includes 70.52?71.08% by weight of Zn, 25.58?27.65% by weight of Al, 1.27?3.45% by weight of Cu, and 0.50 or less by weight of Mg. The particle size of the reinforcement AlN ceramic particles is 0.5-1.2 ?m.

[0051] A method of preparing the high-thermal conductivity composite materials includes the following steps. [0052] (S1) The as-cast AlN.sub.p/ZA27 composite materials are subjected to homogenizing annealing at 200? C. for 6 hours, and turning machining to fit the inner cavity of the extrusion mold. [0053] (S2) The AlN.sub.p/ZA27 composite materials obtained in step (S1) as the raw materials are placed into the reciprocating extrusion mold. The clamp, the extrusion rod, the heating coil of the mold are mounted and connected with a reciprocating extrusion support. The reciprocating extrusion mold is pre-pressed by the hydraulic machine to eliminate the gap between the billet and the reciprocating extrusion mold. [0054] (S3) The heating coil and thermocouples as well as the temperature-controlled meter are connected to the temperature control device. The refractory cotton is wrapped outside the heating coil. The heating temperature is set as 250?350? C. to start heating. [0055] (S4) The billet is heated to 250?350? C. and held for 0.5?1 h, and then the hydraulic machine is started to complete the first-pass extrusion at an extrusion rate of 0.15?0.56 mm/s. [0056] (S5) The reciprocating extrusion mold is flipped, heated to the preset temperature and held for 10?30 min. After that, the hydraulic machine is started to complete a second-pass extrusion at an extrusion rate of 0.15?0.56 mm/s. The extrusion is repeated for 4, 8, 12 or 16 passes until the reciprocating extrusion process is completed. [0057] (S6) The reciprocating extrusion mold is disassembled, and placed on the sleeve with a set of die separation tools, and the hydraulic machine is started to extrude the as-extruded billets to obtain the AlN.sub.p/ZA27 composite materials.

[0058] The high-thermal conductivity composite materials of the disclosure can be applied in microelectronics and 5G device packaging materials.

[0059] The high-thermal conductivity composite materials of the disclosure are mainly applied to the metal encapsulation housing of chips with high airtightness requirements, which has better heat dissipation performance and electromagnetic shielding performance and is suitable for the encapsulation of high-power and high-frequency devices.

[0060] Further, the high-thermal conductivity composite materials of the disclosure are also applied to radiators of automobiles, electronic components, and high-power LED lampshade, effectively controlling and dispersing heat to ensure that the devices do not fail due to overheating. The high-thermal conductivity composite materials are the new materials for high-end thermal management.

[0061] The present disclosure will be further described in detail below in conjunction with the accompanying drawings and embodiments to understand the objects, technical solutions, and advantages of the present disclosure more clearly. Obviously, described below are merely some embodiments of the disclosure, which are not intended to limit the disclosure. It should be noted that the components in the embodiments and the drawings herein may be arranged and designed in different forms. Accordingly, the following detailed description is merely illustrative, and is not intended to limit the scope of the disclosure. For those skilled in the art, other embodiments obtained based on these embodiments without paying creative efforts should fall within the scope of the disclosure defined by the appended claims.

Embodiment 1

[0062] The ZA27 alloy was melted at 560? C.-620? C., added with AlN ceramic particles and stirred for 3-5 minutes to obtain a mixture, where the AlN ceramic particles were added such that the composite included 4% by volume of AlN. The mixture was poured into a graphite mold at 540? C.-560? C. for molding to obtain the as-cast AlN.sub.p/ZA27 composite material.

[0063] The AlN.sub.p/ZA27 composite material with 4% by volume of AlN was subjected to homogenization annealing at 200? C. for 6 hours, and turning machining to fit the inner cavity of the extrusion mold. After that, the AlN.sub.p/ZA27 composite material was loaded into the extrusion mold, and the extrusion mold was assembled, heated to 250? C. and kept for 30 min. The hydraulic machine was started to perform a single-pass extrusion at an extrusion rate of 0.15 mm/s. Then, the extrusion mold was turned, and kept at 250? C. for 10 min, and the hydraulic machine was started to perform the second-pass extrusion at an extrusion rate of 0.15 mm/s, and then the above-mentioned process was repeated. After the fourth-pass extrusion was completed, the extrusion mold was dissembled, and a 4%-250? C.-4PASSES-AlN/ZA27 composite material was obtained by demolding.

Embodiment 2

[0064] An AlN.sub.p/ZA27 composite material with 4% by volume of AlN was subjected to homogenization annealing at 200? C. for 6 hours, and turning machining to fit the inner cavity of the extrusion mold. After that, the AlN.sub.p/ZA27 composite material was loaded into the extrusion mold, and the extrusion mold was assembled, heated to 300? C. and kept for 1 h. The hydraulic machine was started to perform a single-pass extrusion at an extrusion rate of 0.15 mm/s. Then, the extrusion mold was turned, and kept at 300? C. for 15 min, and the hydraulic machine was started to perform the second-pass extrusion at an extrusion rate of 0.15 mm/s, and then the above-mentioned process was repeated. After the fourth-pass extrusion was completed, the extrusion mold was dissembled, and a 4%-300? C.-4PASSES-AlN/ZA27 composite material was obtained by demolding.

Embodiment 3

[0065] An AlN.sub.p/ZA27 composite material with 8% by volume of AlN was subjected to homogenization annealing at 200? C. for 6 hours, and turning machining to fit the inner cavity of the extrusion mold. After that, the AlN.sub.p/ZA27 composite material was loaded into the extrusion mold, and the extrusion mold was assembled, heated to 250? C. and kept for 1 h. The hydraulic machine was started to perform a single-pass extrusion at an extrusion rate of 0.50 mm/s. Then, the extrusion mold was turned, and kept at 250? C. for 20 min, and the hydraulic machine was started to perform the second-pass extrusion at an extrusion rate of 0.50 mm/s, and then the above-mentioned process was repeated. After the fourth-pass extrusion was completed, the extrusion mold was dissembled, and an 8%-250? C.-4PASSES-AlN/ZA27 composite material was obtained by demolding.

Embodiment 4

[0066] An AlN.sub.p/ZA27 composite material with 8% by volume of AlN was subjected to homogenization annealing at 200? C. for 6 hours, and turning machining to fit the inner cavity of the extrusion mold. After that, the AlN.sub.p/ZA27 composite material was loaded into the extrusion mold, and the extrusion mold was assembled, heated to 300? C. and kept for 30 min. The hydraulic machine was started to perform a single-pass extrusion at an extrusion rate of 0.36 mm/s. Then, the extrusion mold was turned, and kept at 300? C. for 10 min, and the hydraulic machine was started to perform the second-pass extrusion at an extrusion rate of 0.36 mm/s, and then the above-mentioned process was repeated. After the eighth-pass extrusion was completed, the extrusion mold was dissembled, and an 8%-300? C.-8PASSES-AlN/ZA27 composite material was obtained by demolding.

Embodiment 5

[0067] An AlN.sub.p/ZA27 composite material with 2% by volume of AlN was subjected to homogenization annealing at 200? C. for 6 hours, and turning machining to fit the inner cavity of the extrusion mold. After that, the AlN.sub.p/ZA27 composite material was loaded into the extrusion mold, and the extrusion mold was assembled, heated to 250? C. and kept for 30 min. The hydraulic machine was started to perform a single-pass extrusion at an extrusion rate of 0.40 mm/s. Then, the extrusion mold was turned, and kept at 250? C. for 30 min, and the hydraulic machine was started to perform the second-pass extrusion at an extrusion rate of 0.40 mm/s, and then the above-mentioned process was repeated. After the fourth-pass extrusion was completed, the extrusion mold was dissembled, and a 2%-250? C.-4PASSES-AlN/ZA27 composite material was obtained by demolding.

[0068] FIG. 1 is a schematic diagram of the reciprocating extrusion mold. The reciprocating extrusion mold mainly includes a mold base 1, a cushion block 2, a buffer spring 3, a screw rod 4 to fasten a mold support, an extrusion cylinder as U-type extrusion rod (i.e., driving a mold unit to move down to accomplish the counter motion of billet) 5, an extrusion support rod 6, and a mold unit (i.e., containers of extrusion billet) 7. The reciprocating extrusion is carried out by first placing the extrusion billets into the mold unit 7 and fixing the two mold units (i.e., containers of extrusion billet) 7 through the clamps, followed by placing the extrusion support rod 6 from both ends of the extrusion mold and connecting the extrusion support rod 6 with the mold support through the screws. After completing the connection between the extrusion support rod 6 and the mold support frame, the screw 4 is tightened, and the cushion block 2 and the extrusion cylinder 5 are placed in sequence to complete the subsequent extrusion process.

[0069] FIGS. 2a-2d show grain morphology of 1 ?m-8%-RE-250? C.-4PASSES, where RE represents reciprocal extrusion; and PASS represents the number of extrusion passes; and 1 ?m represents the size of added AlN in the composites; and 8% represents the volume fraction of AlN in the composites; and 250? C. represents the extrusion temperature. After four passes of reciprocating extrusion at 250? C., 1 ?m-8% AlN/ZA27 sample showed obvious thermal processing flow lines. The original dendrites in the as-cast composite materials were broken, and the ?-Al phase and ?-Zn phase underwent dynamic recrystallization to form undistorted and equiaxed recrystallized grains, wherein ?-Al (i.e., dark color grain) is the phase with darker lining in the FIGS. 2a-2d, and ?-Zn (i.e., light color grain) is the phase with lighter lining in the FIGS. 2a-2d, and it can be observed that ?-Al was distributed in a mesh-like manner on the f-Zn matrix. Moreover, the grains are obviously refined and equiaxed after subjecting to reciprocating extrusion, and most of grains are recrystallized grains. The grain size is only about 1 ?m. The mechanical properties of the composite materials are effectively improved.

[0070] FIGS. 3a and 3b show morphology and distribution of AlN ceramic particles in 1 ?m-8%-RE-250? C.-4PASSES, where RE represents reciprocal extrusion; and PASS represents the number of extrusion processes, as mentioned above. The grain size of the AlN ceramic particles is about 1 ?m, and some of the AlN particles are broken during the reciprocating extrusion process and tend to be distributed along the extrusion direction, which effectively improves the thermal conductivity of the composite materials.

[0071] In summary, in the high-thermal conductivity composite materials and preparation method and application thereof in this disclosure, the reciprocating extrusion large plastic deformation technology can effectively eliminate the compositional segregation of the ca-cast AlN.sub.p/ZA27 composite materials, so that the composite materials undergo dynamic recrystallization to form undistorted and equiaxed recrystallized grains and significantly refine the grains, which effectively enhances the mechanical properties of the composite materials. At the same time, the morphology and distribution of the AlN ceramic particles are improved, so that the AlN ceramic particles are distributed along the extrusion direction, which effectively enhances the thermal conductivity of AlN.sub.p/ZA27 composite material and has a good application prospect in the microelectronic packaging materials.

[0072] It should be noted that the above embodiments are only used to illustrate the technical solutions of the disclosure, and are not intended to limit the disclosure. It should be understood that any modifications and replacements made by those skilled in the art without departing from the spirit of the disclosure should fall within the scope of the disclosure defined by the appended claims.