A nylon-based thermally conductive composite material and a preparation method thereof

By introducing cage-like rigid nodes, dynamic reversible cross-linking structures, and intermolecular hydrogen bond networks into the nylon matrix, combined with interface-regulating components and organic small molecule functional regulators, a continuous and stable thermal conductivity pathway is constructed, solving the problems of low thermal conductivity and decreased mechanical properties of nylon materials, and achieving a synergistic improvement in thermal conductivity, mechanical properties, and processing performance.

CN122234597APending Publication Date: 2026-06-19JIANGSU JIAYUAN GONGJU NEW MATERIALS CO LTD

Patent Information

Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
JIANGSU JIAYUAN GONGJU NEW MATERIALS CO LTD
Filing Date
2026-04-26
Publication Date
2026-06-19

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Abstract

This invention relates to the field of polymer composite materials technology, specifically to a nylon-based thermally conductive composite material and its preparation method. The composite material comprises a synergistically modified nylon resin, a thermally conductive filler, an interface structure regulating component, an organic small molecule functional regulator, and additives. Specifically, by introducing octa(3-aminopropyl)silsesquioxane into the nylon resin to construct cage-like rigid nodes, and utilizing 3-deoxy-D-fructophenone to form a dynamically rearrangeable crosslinked structure, while simultaneously constructing a hydrogen-bonded synergistic network, multi-scale synergistic modification of the nylon matrix is ​​achieved. Furthermore, the interface structure regulating component and the organic small molecule functional regulator enhance the interfacial bonding between the thermally conductive filler and the matrix, constructing a continuous thermally conductive pathway. The preparation method of this invention is simple and feasible, and the resulting material exhibits high thermal conductivity, low interfacial thermal resistance, and excellent overall performance, making it suitable for heat dissipation in electronic devices.
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Description

Technical Field

[0001] This invention relates to the field of polymer composite materials technology, specifically to a nylon-based thermally conductive composite material and its preparation method. Background Technology

[0002] Nylon resin, as an important class of engineering plastics, possesses excellent mechanical properties, wear resistance, heat resistance, and processing performance, and is widely used in electronics, automotive parts, and structural functional materials. However, nylon materials have a low intrinsic thermal conductivity, typically in the range of 0.2–0.4 W / m·K, which makes it difficult to meet the requirements of high thermal conductivity applications such as heat dissipation in electronic devices and thermal management structural components.

[0003] To improve the thermal conductivity of nylon materials, existing technologies typically involve introducing thermally conductive fillers, such as hexagonal boron nitride and alumina, into the nylon matrix to create thermally conductive pathways and enhance the overall thermal conductivity of the material. However, this approach generally suffers from the following problems: Firstly, achieving higher thermal conductivity usually requires a higher filler content, leading to decreased material processing fluidity and deterioration of mechanical properties. Secondly, the interfacial compatibility between the thermally conductive filler and the nylon matrix is ​​poor, resulting in high interfacial thermal resistance, which limits further improvements in thermal conductivity.

[0004] Furthermore, current technologies for modifying nylon matrices primarily focus on simple blending or surface coupling treatments, lacking designs that construct multi-scale synergistic networks at the molecular structure level. This makes it difficult to simultaneously optimize thermal conductivity, mechanical properties, and processing performance. In particular, the lack of effective interface control methods during the construction of thermal conduction pathways makes it difficult for fillers to form a continuous and efficient heat conduction network.

[0005] Therefore, there is an urgent need to provide a new nylon-based thermally conductive composite material. By synergistically modifying the structure of nylon resin and combining interface regulation and functional molecule interaction, a stable and continuous thermally conductive pathway can be constructed, thereby significantly improving thermal conductivity and maintaining good overall performance while reducing filler usage. Summary of the Invention

[0006] To overcome the problems of low thermal conductivity of nylon materials, decreased processing and mechanical properties due to high filler content, and high interfacial thermal resistance in the aforementioned background technologies, the present invention aims to provide a nylon-based thermally conductive composite material and its preparation method. The present invention constructs a synergistically modified nylon resin, introducing cage-like rigid nodes, dynamically reversible cross-linked structures, and intermolecular hydrogen bond networks into the nylon matrix to achieve ordered control of the nylon molecular chains. Simultaneously, it combines interfacial structure regulating components to perform surface effects on the thermally conductive filler and introduces small organic molecule functional regulators to enhance interfacial interactions, thereby constructing a continuous and stable thermally conductive pathway within the material. The present invention can construct a highly efficient and continuous thermally conductive network while reducing interfacial thermal resistance, thus significantly improving the material's thermal conductivity while maintaining mechanical and processing properties.

[0007] The objective of this invention can be achieved through the following technical solutions:

[0008] A nylon-based thermally conductive composite material comprises the following raw materials in parts by weight: 80-120 parts of synergistically modified nylon resin; 30-120 parts of thermally conductive filler; 5-30 parts of interface structure regulating component; 0.5-10 parts of organic small molecule functional regulator; 0.2-2 parts of antioxidant; 0.5-3 parts of lubricant; 0.5-5 parts of coupling agent; and 5-30 parts of deionized water. The synergistically modified nylon resin is formed by melt grafting nylon resin with octa(3-aminopropyl)silsesquioxane to construct cage-like rigid nodes, and introducing 3-deoxy-D-fructophenone to participate in dynamic condensation reaction to form a rearrangeable crosslinkable structure, while simultaneously constructing an intermolecular hydrogen bond synergistic network to achieve multi-scale structural synergistic modification.

[0009] Optionally, the synergistically modified nylon resin comprises the following raw materials in parts by weight: 80-120 parts of nylon resin; 2-10 parts of octa(3-aminopropyl)silsesquioxane; 0.5-6 parts of 3-deoxy-D-fructosone; 1-8 parts of tannic acid; 2-12 parts of 3-aminopropyltriethoxysilane; and 10-40 parts of deionized water.

[0010] Optionally, the preparation method of the synergistically modified nylon resin includes the following steps:

[0011] (1) Add octa(3-aminopropyl)silsesquioxane, tannic acid and 3-aminopropyltriethoxysilane to deionized water to react and obtain a pre-modified system;

[0012] (2) Add 3-deoxy-D-fructosone to the pre-modified system to react and obtain a synergistic modification intermediate;

[0013] (3) The nylon resin and the synergistic modification intermediate are melt-blended to obtain the synergistic modified nylon resin.

[0014] Optionally, the reaction conditions in step (1) are: temperature of 30-45℃, reaction time of 1.5-2.5h, stirring speed of 350-500r / min, and pH of the system of 8-9.

[0015] Optionally, the reaction conditions in step (2) are a temperature of 50-70°C, a reaction time of 3-4 h, and a pH of 6-7.

[0016] Optionally, the reaction conditions in step (3) are a melting temperature of 230-250°C, a screw speed of 100-130 r / min, and a melt blending time of 8-15 min.

[0017] Optionally, the thermally conductive filler is a mixture of hexagonal boron nitride and spherical alumina in a mass ratio of 1:0.5 to 1:3; the interface structure regulating component is a mixture of octa(3-aminopropyl)silsesquioxane and tannic acid in a mass ratio of 1:1 to 1:4; the organic small molecule functional regulator is 1,10-o-phenanthroline; the antioxidant is a mixture of hindered phenolic antioxidant and phosphite antioxidant in a mass ratio of 1:0.5 to 1:2; the lubricant is a mixture of zinc stearate and polyethylene wax in a mass ratio of 1:0.5 to 1:2; and the coupling aid is a mixture of 3-aminopropyltriethoxysilane and vinyltrimethoxysilane in a mass ratio of 1:0.5 to 1:2.

[0018] Optionally, a method for preparing a nylon-based thermally conductive composite material includes the following steps:

[0019] S1, premix the thermally conductive filler with the interface structure regulating component to make the interface structure regulating component uniformly dispersed and act on the surface of the thermally conductive filler to obtain the surface-modified thermally conductive filler.

[0020] S2, the synergistically modified nylon resin is mixed with organic small molecule functional regulators, antioxidants, lubricants and coupling agents to obtain a uniform premix;

[0021] S3, surface-modified thermally conductive filler and premixed material are added to an extrusion device for melt blending, extrusion granulation, and nylon-based thermally conductive composite material is obtained.

[0022] Optionally, the reaction conditions for step S1 are a temperature of 40–80°C, a processing time of 1–3 h, and a stirring speed of 300–600 r / min; the reaction conditions for step S2 are a mixing temperature of 20–40°C, a mixing time of 10–30 min, and a stirring speed of 200–500 r / min.

[0023] Optionally, the reaction conditions for step S3 are: a melting temperature of 230–260°C, a screw speed of 80–150 r / min, and a melt blending time of 5–15 min.

[0024] The beneficial effects of this invention are:

[0025] This invention introduces octa(3-aminopropyl)silsesquioxane into the molecular structure of nylon resin to construct cage-like rigid nodes, and utilizes 3-deoxy-D-fructophenone to participate in dynamic condensation reactions to form rearrangeable crosslinkable structures. Simultaneously, it utilizes tannic acid to construct a multi-hydrogen bond synergistic network, enabling a stable multi-scale synergistic structural system within the nylon matrix. This significantly improves the degree of chain segment orientation and interfacial bonding strength while maintaining molecular chain flexibility. Furthermore, by using interfacial structure-regulating components to exert surface effects on the thermally conductive filler, and combining 1,10-o-phenanthroline to form coordination bridging and π-π interactions between the filler and the nylon matrix, it effectively reduces the interfacial thermal resistance between fillers and between the filler and the matrix, promotes efficient phonon transfer at the interface, and constructs a continuous and dense three-dimensional thermally conductive network structure. Therefore, it can significantly improve the thermal conductivity of the composite material with lower filler content, while avoiding the mechanical property degradation and processing difficulties caused by high filler content. This achieves a synergistic improvement in thermal conductivity, mechanical properties, and processing performance, demonstrating unexpected results superior to existing technologies. Attached Figure Description

[0026] The invention will now be further described with reference to the accompanying drawings.

[0027] Figure 1 This is a comparison of the infrared spectra of nylon resin and synergistically modified nylon resin. Detailed Implementation

[0028] The present invention will be further described below with reference to specific embodiments. However, the present invention is not limited to the following embodiments. Equivalent adjustments made without departing from the spirit and essence of the present invention should also be considered to fall within the protection scope of the present invention.

[0029] Example 1: The purpose of this example is to verify the basic thermal conductivity and processing properties of the material when the components and reaction conditions are in a low range.

[0030] S1, 80 parts of nylon resin, 2 parts of octa(3-aminopropyl)silsesquioxane, 1 part of tannic acid, and 2 parts of 3-aminopropyltriethoxysilane were added to 10 parts of deionized water and reacted at 30°C, 350 r / min, and pH 8 for 1.5 h to obtain a pre-modified system; then 0.5 parts of 3-deoxy-D-fructosone were added and reacted at 50°C and pH 6 for 3 h to obtain a synergistic modification intermediate; finally, the above synergistic modification intermediate was melt-blended with nylon resin and treated at 230°C, 100 r / min, and 8 min to obtain a synergistically modified nylon resin;

[0031] S2, 30 parts of hexagonal boron nitride and 15 parts of spherical alumina were mixed at a mass ratio of 1:0.5, and 5 parts of interface structure regulating component were added for premixing. The mixture was then treated at 40℃ and 300r / min for 1h to obtain surface-modified thermally conductive filler.

[0032] S3, the synergistically modified nylon resin obtained in step S1 is mixed with 0.5 parts of 1,10-o-phenanthroline, 0.2 parts of antioxidant, 0.5 parts of lubricant and 0.5 parts of coupling agent, and mixed at 20°C and 200 r / min for 10 min. Then, the surface-modified thermally conductive filler obtained in step S2 is added, and the mixture is extruded and granulated at 230°C, 80 r / min screw speed and 5 min melt blending time to obtain nylon-based thermally conductive composite material.

[0033] Example 2: The purpose of this example is to verify that the overall performance of the material is optimal when the components and reaction conditions are within a moderate range.

[0034] S1, 100 parts of nylon resin, 6 parts of octa(3-aminopropyl)silsesquioxane, 4 parts of tannic acid, and 7 parts of 3-aminopropyltriethoxysilane were added to 25 parts of deionized water and reacted at 35°C, 400 r / min, and pH 8.5 for 2 h to obtain a pre-modified system; then 3 parts of 3-deoxy-D-fructosone were added and reacted at 60°C and pH 6.5 for 3.5 h to obtain a synergistic modification intermediate; finally, the above synergistic modification intermediate was melt-blended with nylon resin and treated at 240°C, 110 r / min, and 10 min to obtain a synergistically modified nylon resin; Figure 1 Infrared spectroscopy comparison shows that the unmodified nylon resin at 3300 cm⁻¹... -1 A relatively obvious NH stretching vibration absorption peak exists at 1650 cm⁻¹, but after modification, this peak becomes significantly broader and stronger, indicating that the hydrogen bonding interaction in the system is significantly enhanced; at 1650 cm⁻¹ -1 The C=O absorption peak near the molecular chain shows a certain degree of peak shape change, indicating that the chemical environment around the molecular chain has changed; at the same time, at 1100 cm⁻¹... -1and 1050cm -1 The appearance of new absorption peaks nearby, corresponding to Si-O-Si and Si-OC structures, proves the successful construction of the silicon-oxygen network; at 1600 cm⁻¹ -1 Enhanced absorption in the vicinity indicates the introduction of aromatic structures; in summary, this demonstrates that synergistic modification has successfully formed a multi-scale network structure in the nylon molecular structure.

[0035] S2, 70 parts of hexagonal boron nitride and 70 parts of spherical alumina were mixed at a mass ratio of 1:1, and 15 parts of interface structure regulating component were added for premixing. The mixture was then treated at 60℃ and 450r / min for 2h to obtain surface-modified thermally conductive filler.

[0036] S3. The synergistically modified nylon resin obtained in step S1 is mixed with 5 parts of 1,10-o-phenanthroline, 1 part of antioxidant, 2 parts of lubricant and 2.5 parts of coupling agent. The mixture is mixed for 20 min at 30°C and 350 r / min stirring speed. Then, the surface-modified thermally conductive filler obtained in step S2 is added. The mixture is extruded and granulated at 245°C, 120 r / min screw speed and 10 min melt blending time to obtain nylon-based thermally conductive composite material.

[0037] Example 3: The purpose of this example is to verify the limit of improvement in the thermal conductivity of the material when the components and reaction conditions are in a high range.

[0038] S1, 120 parts of nylon resin, 10 parts of octa(3-aminopropyl)silsesquioxane, 8 parts of tannic acid, and 12 parts of 3-aminopropyltriethoxysilane were added to 40 parts of deionized water and reacted at 45°C, 500 r / min, and pH 9 for 2.5 h to obtain a pre-modified system; then 6 parts of 3-deoxy-D-fructosone were added and reacted at 70°C and pH 7 for 4 h to obtain a synergistic modification intermediate; finally, the above synergistic modification intermediate was melt-blended with nylon resin and treated at 250°C, 130 r / min, and 15 min to obtain a synergistically modified nylon resin;

[0039] S2, 120 parts of hexagonal boron nitride and 360 parts of spherical alumina were mixed at a mass ratio of 1:3, and 30 parts of interface structure regulating component were added for premixing. The mixture was then treated at 80℃ and 600r / min for 3h to obtain surface-modified thermally conductive filler.

[0040] S3, the synergistically modified nylon resin obtained in step S1 is mixed with 10 parts of 1,10-o-phenanthroline, 2 parts of antioxidant, 3 parts of lubricant and 5 parts of coupling agent, and mixed at 40°C and 500 r / min for 30 min. Then, the surface-modified thermally conductive filler obtained in step S2 is added, and the mixture is extruded and granulated at 260°C, 150 r / min screw speed and 15 min melt blending time to obtain nylon-based thermally conductive composite material.

[0041] Comparative Example 1: The purpose of this comparative example is to verify the influence of the cage-like rigid node structure on thermal conductivity and interface stability.

[0042] S1. 100 parts of nylon resin, 4 parts of tannic acid, and 7 parts of 3-aminopropyltriethoxysilane were added to 25 parts of deionized water and reacted at 35°C, 400 r / min, and pH 8.5 for 2 h to obtain a pre-modified system. Subsequently, 3 parts of 3-deoxy-D-fructosone were added and reacted at 60°C and pH 6.5 for 3.5 h to obtain a modified intermediate. Finally, the above modified intermediate was melt-blended with nylon resin and treated at 240°C, 110 r / min, and 10 min to obtain a single-modified nylon resin.

[0043] S2, 70 parts of hexagonal boron nitride and 70 parts of spherical alumina were mixed at a mass ratio of 1:1, and 15 parts of interface structure regulating component were added for premixing. The mixture was then treated at 60℃ and 450r / min for 2h to obtain surface-modified thermally conductive filler.

[0044] S3. The single modified nylon resin obtained in step S1 is mixed with 5 parts of 1,10-o-phenanthroline, 1 part of antioxidant, 2 parts of lubricant and 2.5 parts of coupling agent. The mixture is mixed for 20 min at 30°C and 350 r / min stirring speed. Then the surface modified thermally conductive filler obtained in step S2 is added. The mixture is extruded and granulated at 245°C, 120 r / min screw speed and 10 min melt blending time to obtain nylon-based thermally conductive composite material.

[0045] Comparative Example 2: The purpose of this comparative example is to verify the influence of the dynamic reversible cross-linking structure on the continuity of the heat conduction path and the overall performance of the material.

[0046] S1, 100 parts of nylon resin, 6 parts of octa(3-aminopropyl)silsesquioxane, 4 parts of tannic acid, and 7 parts of 3-aminopropyltriethoxysilane were added to 25 parts of deionized water and reacted at 35°C, 400 r / min, and pH 8.5 for 2 h to obtain a pre-modified system; without adding 3-deoxy-D-fructophenone, the above system was directly melt-blended with nylon resin and treated at 240°C, 110 r / min, and 10 min to obtain a single-modified nylon resin;

[0047] S2, 70 parts of hexagonal boron nitride and 70 parts of spherical alumina were mixed at a mass ratio of 1:1, and 15 parts of interface structure regulating component were added for premixing. The mixture was then treated at 60℃ and 450r / min for 2h to obtain surface-modified thermally conductive filler.

[0048] S3. The single modified nylon resin obtained in step S1 is mixed with 5 parts of 1,10-o-phenanthroline, 1 part of antioxidant, 2 parts of lubricant and 2.5 parts of coupling agent. The mixture is mixed for 20 min at 30°C and 350 r / min stirring speed. Then the surface modified thermally conductive filler obtained in step S2 is added. The mixture is extruded and granulated at 245°C, 120 r / min screw speed and 10 min melt blending time to obtain nylon-based thermally conductive composite material.

[0049] Comparative Example 3: The purpose of this comparative example is to verify the effect of organic small molecule functional regulators on interfacial thermal resistance and thermal conductivity.

[0050] S1, 100 parts of nylon resin, 6 parts of octa(3-aminopropyl)silsesquioxane, 4 parts of tannic acid, and 7 parts of 3-aminopropyltriethoxysilane were added to 25 parts of deionized water and reacted at 35°C, 400 r / min, and pH 8.5 for 2 h to obtain a pre-modified system; then 3 parts of 3-deoxy-D-fructosone were added and reacted at 60°C and pH 6.5 for 3.5 h to obtain a synergistic modification intermediate; finally, the above synergistic modification intermediate was melt-blended with nylon resin and treated at 240°C, 110 r / min, and 10 min to obtain a synergistically modified nylon resin;

[0051] S2, 70 parts of hexagonal boron nitride and 70 parts of spherical alumina were mixed at a mass ratio of 1:1, and 15 parts of interface structure regulating component were added for premixing. The mixture was then treated at 60℃ and 450r / min for 2h to obtain surface-modified thermally conductive filler.

[0052] S3, the synergistically modified nylon resin obtained in step S1 is mixed with 1 part antioxidant, 2 parts lubricant and 2.5 parts coupling agent, and mixed at 30°C and 350 r / min for 20 min. Then the surface-modified thermally conductive filler obtained in step S2 is added, and the mixture is extruded and granulated at 245°C, 120 r / min screw speed and 10 min melt blending time to obtain nylon-based thermally conductive composite material.

[0053] Performance testing:

[0054] 1. Thermal conductivity test method

[0055] The nylon-based thermally conductive composite materials obtained in the examples and comparative examples were injection molded into flat samples with dimensions of 100mm×100mm×2mm. These samples were then dried in a vacuum drying oven at 80℃ for 24 hours to remove adsorbed moisture. The thermal diffusivity of the material at 25℃ was measured using a laser flash thermal conductivity meter, while the specific heat capacity was measured using a differential scanning calorimeter, and the density was determined using the Archimedes method. Thermal conductivity was calculated based on the formula: thermal diffusivity equals thermal diffusivity multiplied by specific heat capacity multiplied by density. Each sample was tested three times, and the average value was taken to ensure the accuracy and repeatability of the data.

[0056] 2. Mechanical property testing methods

[0057] The composite materials obtained in the examples and comparative examples were injection molded into standard dumbbell-shaped tensile specimens and tested according to GB / T1040 standard. The tensile test was conducted on an electronic universal testing machine at a tensile rate of 50 mm / min, a test temperature of 23℃, and a relative humidity of 50%. At the same time, notched impact specimens with dimensions of 80 mm × 10 mm × 4 mm were prepared and subjected to cantilever beam impact test according to GB / T1843 standard at a test temperature of 23℃. Each group of specimens consisted of no less than 5 specimens, and the average value was taken as the final result to evaluate the strength and toughness of the material.

[0058] 3. Interfacial thermal resistance testing method

[0059] The composite materials obtained in the examples and comparative examples were processed into uniform sheets with a thickness of 2 mm and tested in a steady-state thermal conductivity testing device. A stable heat flow was established by applying a constant temperature difference of about 20°C on both sides of the sample. The overall thermal conductivity of the material was recorded, and the composite system was theoretically calculated using the Maxwell-Eucken model. The interfacial thermal resistance between the filler and the nylon matrix was obtained by inverting the deviation between the experimental and theoretical values. Each group of samples was tested three times and the average value was taken to evaluate the effect of interfacial structure regulation and the influence of organic small molecules on interfacial heat transfer performance.

[0060] 4. Thermal stability test method

[0061] Take 5-10 mg of the composite material samples obtained in the examples and comparative examples, and test them using a thermogravimetric analyzer under a nitrogen protective atmosphere with a flow rate of 50 mL per minute. The heating rate is 10 °C per minute, and the test temperature range is 30-700 °C. Record the temperature at which the material loses 5% of its mass and the temperature corresponding to the maximum decomposition rate. Compare and analyze the thermal decomposition behavior of different samples to evaluate the effect of the synergistic modified structure on improving the thermal stability of the material.

[0062] Table 1. Performance test results of nylon-based thermally conductive composite materials

[0063] sample Thermal conductivity W / m·K Tensile strength (MPa) <![CDATA[Interfacial thermal resistance × 10 -8 m 2 ·K / W]]> Thermal decomposition temperature (°C) Example 1 1.85 62.3 3.8 368 Example 2 2.76 78.5 2.1 402 Example 3 2.35 70.2 2.9 390 Comparative Example 1 1.42 55.6 5.6 350 Comparative Example 2 1.58 58.9 4.9 358 Comparative Example 3 1.67 60.1 4.3 362

[0064] As shown in Table 1, there are significant differences between the examples and the comparative examples in terms of thermal conductivity, mechanical properties, interfacial thermal resistance, and thermal stability. Specifically, the thermal conductivity of Example 2 reaches 2.76 W / m·K, significantly higher than that of Examples 1 and 3, and also much higher than that of the comparative examples, indicating that under moderate component ratios and reaction conditions, the internal thermal conductivity pathways of the material are most well-developed. In contrast, the thermal conductivity of Comparative Examples 1 to 3 is significantly reduced, indicating that the lack of key synergistic modified structures leads to discontinuous thermal conductivity pathways, thus affecting the overall thermal conductivity efficiency.

[0065] From the perspective of mechanical properties, the tensile strength of Example 2 is 78.5 MPa, which is significantly better than that of other examples and all comparative examples. This shows that the synergistic effect of cage-like rigid nodes, dynamic cross-linking structure and hydrogen bond network not only did not weaken the mechanical properties of the material, but also achieved an enhancement effect. In contrast, the comparative examples lacked a complete synergistic modification structure and had weak interfacial bonding, resulting in a significant decrease in material strength.

[0066] Regarding interfacial thermal resistance, Example 2 exhibits the lowest interfacial thermal resistance, at only 2.1 × 10⁻⁶. -8 m 2 The K / W ratio indicates that the interfacial bonding between the filler and the nylon matrix is ​​the tightest, resulting in the lowest thermal conductivity resistance. In contrast, the interfacial thermal resistance of each comparative example is significantly increased, especially in comparative example 1, indicating that the lack of a cage-like structure or dynamic network will significantly increase interfacial scattering, thereby reducing thermal conductivity efficiency.

[0067] Regarding thermal stability, the thermal decomposition temperature of Example 2 reached 402℃, which is higher than that of other examples and all comparative examples, indicating that the synergistic modified structure can effectively improve the thermal stability of the material; while the comparative examples have relatively low thermal stability due to incomplete structure and are prone to thermal decomposition.

[0068] In summary, this invention achieves simultaneous improvement in thermal conductivity, mechanical properties, and thermal stability by constructing a multi-scale synergistic modification structure. Among all embodiments, Embodiment 2 exhibits the best overall performance, fully demonstrating the effectiveness and superiority of this technical solution.

Claims

1. A nylon-based thermally conductive composite material, characterized in that, The composite material comprises the following raw materials in parts by weight: 80-120 parts of synergistically modified nylon resin; 30-120 parts of thermally conductive filler; 5-30 parts of interface structure regulating component; 0.5-10 parts of organic small molecule functional regulator; 0.2-2 parts of antioxidant; 0.5-3 parts of lubricant; 0.5-5 parts of coupling agent; and 5-30 parts of deionized water. The synergistically modified nylon resin is formed by melt grafting nylon resin with octa(3-aminopropyl)silsesquioxane to construct cage-like rigid nodes, and introducing 3-deoxy-D-fructophenone to participate in dynamic condensation reaction to form a rearrangeable crosslinkable structure, while simultaneously constructing an intermolecular hydrogen bond synergistic network to achieve multi-scale structural synergistic modification.

2. The nylon-based thermally conductive composite material according to claim 1, characterized in that, The synergistically modified nylon resin comprises the following raw materials in parts by weight: 80-120 parts nylon resin; 2-10 parts octa(3-aminopropyl)silsesquioxane; 0.5-6 parts 3-deoxy-D-fructosone; 1-8 parts tannic acid; 2-12 parts 3-aminopropyltriethoxysilane; and 10-40 parts deionized water.

3. A nylon-based thermally conductive composite material according to claim 1 or 2, characterized in that, The preparation method of the synergistically modified nylon resin includes the following steps: (1) Add octa(3-aminopropyl)silsesquioxane, tannic acid and 3-aminopropyltriethoxysilane to deionized water to react and obtain a pre-modified system; (2) Add 3-deoxy-D-fructosone to the pre-modified system to react and obtain a synergistic modification intermediate; (3) The nylon resin and the synergistic modification intermediate are melt-blended to obtain the synergistic modified nylon resin.

4. The nylon-based thermally conductive composite material according to claim 3, characterized in that, The reaction conditions for step (1) are: temperature of 30-45℃, reaction time of 1.5-2.5h, stirring speed of 350-500r / min, and pH of the system of 8-9.

5. The nylon-based thermally conductive composite material according to claim 3, characterized in that, The reaction conditions for step (2) are a temperature of 50-70°C, a reaction time of 3-4 hours, and a pH of 6-7.

6. The nylon-based thermally conductive composite material according to claim 3, characterized in that, The reaction conditions for step (3) are: melting temperature of 230-250°C, screw speed of 100-130 r / min, and melting and blending time of 8-15 min.

7. The nylon-based thermally conductive composite material according to claim 1, characterized in that, The thermally conductive filler is a mixture of hexagonal boron nitride and spherical alumina in a mass ratio of 1:0.5 to 1:3; the interface structure regulating component is a mixture of octa(3-aminopropyl)silsesquioxane and tannic acid in a mass ratio of 1:1 to 1:4; the organic small molecule functional regulator is 1,10-o-phenanthroline; the antioxidant is a mixture of hindered phenolic antioxidant and phosphite antioxidant in a mass ratio of 1:0.5 to 1:2; the lubricant is a mixture of zinc stearate and polyethylene wax in a mass ratio of 1:0.5 to 1:2; and the coupling aid is a mixture of 3-aminopropyltriethoxysilane and vinyltrimethoxysilane in a mass ratio of 1:0.5 to 1:

2.

8. A method for preparing a nylon-based thermally conductive composite material, characterized in that, The preparation method includes the following steps: S1, premix the thermally conductive filler with the interface structure regulating component to make the interface structure regulating component uniformly dispersed and act on the surface of the thermally conductive filler to obtain the surface-modified thermally conductive filler. S2, the synergistically modified nylon resin is mixed with organic small molecule functional regulators, antioxidants, lubricants and coupling agents to obtain a uniform premix; S3, surface-modified thermally conductive filler and premixed material are added to an extrusion device for melt blending, extrusion granulation, and nylon-based thermally conductive composite material is obtained.

9. The method for preparing a nylon-based thermally conductive composite material according to claim 8, characterized in that, The reaction conditions for step S1 are a temperature of 40–80°C, a processing time of 1–3 h, and a stirring speed of 300–600 r / min; the reaction conditions for step S2 are a mixing temperature of 20–40°C, a mixing time of 10–30 min, and a stirring speed of 200–500 r / min.

10. The method for preparing a nylon-based thermally conductive composite material according to claim 8, characterized in that, The reaction conditions for step S3 are: a melting temperature of 230–260°C, a screw speed of 80–150 r / min, and a melt blending time of 5–15 min.