Multi-scale synergistically enhanced phenyl silicone rubber and preparation method thereof

Abstract

The invention discloses multi-scale synergistically enhanced phenyl silicone rubber and a preparation method thereof, and belongs to the technical field of phenyl silicone rubber, the multi-scale synergistically enhanced phenyl silicone rubber comprises the following components by weight: 70-90 parts of a gradient phenyl silicone rubber matrix, which is compounded by single phenyl silicone rubber and diphenyl silicone rubber according to a mass ratio of (1.5-2.5): 1; the core-shell structure dynamic crosslinking particles take SiO2 as a core and phenylsiloxane as a shell, and are modified by a KH550 silane coupling agent, and the mass ratio of the core to the shell is 1: (0.8-1.2); 5-8 parts of a graphene / fluorinated silicone rubber interpenetrating network, wherein the graphene / fluorinated silicone rubber interpenetrating network comprises 0.5-1.0 part of isocyanate functionalized graphene; 12 to 18 parts of fumed silica; 3-5 parts of a dynamic crosslinking auxiliary agent which is phenyl silicone oil containing ureido; 1.0 to 1.5 parts of vulcanizing agent; the diameter of the short carbon fiber is 5-10 [mu] m, and the length of the short carbon fiber is 50-100 [mu] m.

Description

TECHNICAL FIELD

[0001] The present application relates to the technical field of phenyl silicone rubber, in particular to a multi-scale synergistically reinforced phenyl silicone rubber and a preparation method thereof. BACKGROUND

[0002] Phenyl silicone rubber has excellent high and low temperature performance and damping characteristics due to the introduction of phenyl groups in the molecular chain, which destroys the regularity of the chain segment, and is widely used in vibration and noise reduction fields (a high-damping phenyl silicone rubber damping material and a preparation method thereof). However, the traditional phenyl silicone rubber has the following shortcomings:

[0003] (1) The damping temperature range is narrow (usually ≤100℃), which is difficult to meet the wide temperature range working condition requirements;

[0004] (2) Simply adding a heat-conducting filler will cause the damping performance to decrease;

[0005] (3) The oil resistance and mechanical strength are difficult to balance, which limits the application in harsh environments. SUMMARY

[0006] The technical problem to be solved by the present application is to provide a multi-scale synergistically reinforced phenyl silicone rubber and a preparation method thereof to solve the problems raised in the background.

[0007] In order to solve the above technical problems, the technical scheme of the present application is as follows:

[0008] A multi-scale synergistically reinforced phenyl silicone rubber, comprising the following components by weight:

[0009] 70-90 parts of a gradient phenyl silicone rubber matrix, which is compounded by mono-phenyl silicone rubber and di-phenyl silicone rubber at a mass ratio of (1.5-2.5):1;

[0010] 8-12 parts of core-shell structure dynamic crosslinking particles, which are modified by KH550 silane coupling agent and have SiO2 as the core and phenyl siloxane as the shell, with a core-shell mass ratio of 1:(0.8-1.2);

[0011] 5-8 parts of graphene / fluorosilicone rubber interpenetrating network, including 0.5-1.0 parts of isocyanate functionalized graphene;

[0012] 12-18 parts of fumed white carbon black;

[0013] 3-5 parts of a dynamic crosslinking aid, which is a phenyl silicone oil containing a urea group;

[0014] 1.0-1.5 parts of a vulcanizing agent;

[0015] 1-3 parts of short carbon fibers, which have a diameter of 5-10 microns and a length of 50-100 microns.

[0016] Preferably, the preparation method of the core-shell structure dynamic crosslinking particle comprises:

[0017] The SiO2 nanoparticles are dispersed in a mixture of ethanol and water, phenyl trimethoxysilane and KH550 silane coupling agent are added, the pH is adjusted to 4-5, and the reaction is carried out at a temperature of 50-60°C for 4-6h, and then dried at a temperature of 80°C and calcined at 300-350°C for 2h, wherein the molar ratio of phenyl trimethoxysilane to KH550 silane coupling agent is (5-8):1.

[0018] Preferably, the preparation method of the graphene / fluorosilicone rubber interpenetrating network comprises:

[0019] The modified graphene treated with diphenyl methane diisocyanate is mixed with fluorosilicone rubber at a mass ratio of 1:(8-12), and dicumyl peroxide is added, and pre-vulcanization is carried out at a temperature of 160-170°C for 8-10min to obtain.

[0020] Preferably, the preparation method of the modified graphene comprises:

[0021] The graphene oxide is reacted with vinyl triethoxysilane at a mass ratio of 10:(0.8-1.2), and then reacted with diphenyl methane diisocyanate to obtain.

[0022] A preparation method of the above-mentioned phenyl silicone rubber, comprising the following steps:

[0023] S1 Gradient matrix compounding:

[0024] The monophenyl silicone rubber and the diphenyl silicone rubber are mixed in an open mill for 5-8min, and fumed white carbon black and chopped carbon fibers are added and continue to mix for 15-20min;

[0025] S2 Dynamic network construction:

[0026] The core-shell structure dynamic crosslinking particle and the dynamic crosslinking aid are added, and the temperature is raised to 80-90°C, and mixed for 25-30min;

[0027] S3 Interpenetrating network compounding:

[0028] The graphene / fluorosilicone rubber interpenetrating network is added, the temperature is reduced to 80°C and maintained for 10min, then the temperature is continuously reduced to 60°C and maintained for 10min, then the temperature is continuously reduced to 40°C and maintained for 10min, and then the vulcanizing agent is added and thin passed 8-12 times;

[0029] S4 Vulcanization forming:

[0030] The first stage of vulcanization is carried out at 165-175℃ for 20-25 minutes, the second stage of vulcanization is carried out at 200-220℃ for 4-6 hours, and finally the vulcanization is carried out naturally to room temperature.

[0031] Preferably, the cooling rate in step S3 is controlled at 2-3 °C / min to ensure the synergistic construction of the dynamic hydrogen bond network and the covalent crosslinking network.

[0032] The above technical solution has the following beneficial effects:

[0033] Performance Synergy Breakthrough: Achieving a combination of damping (tanδ≥0.5) over a wide temperature range of -60℃ to 200℃, high thermal conductivity (1.65W / m·K), and oil resistance (volume change rate 3.8%), breaking through the performance bottleneck of traditional materials;

[0034] Structural innovation: The core-shell structure with dynamically cross-linked particles combines rigid support with dynamic hydrogen bonds for the first time, solving the trade-off between damping and strength;

[0035] Controllable process: Gradient cooling and step-by-step vulcanization processes ensure the coordinated construction of multi-scale networks, making them suitable for industrial production.

[0036] This invention provides a new technical route for multifunctional silicone rubber materials for high-end equipment through multi-scale structural design, which has significant economic value and social benefits. Detailed Implementation

[0037] The specific embodiments of the present invention will be further described below. It should be noted that these descriptions are for the purpose of aiding understanding the present invention, but do not constitute a limitation thereof. Furthermore, the technical features involved in the various embodiments of the present invention described below can be combined with each other as long as they do not conflict with each other.

[0038] To address the problem that the damping, thermal conductivity, and oil resistance properties of phenyl silicone rubber are difficult to improve synergistically in existing technologies, this invention proposes a multi-scale synergistic enhancement strategy. Through the organic combination of core-shell structured dynamic cross-linked particles, interpenetrating network construction, and gradient matrix compounding, a breakthrough in the comprehensive performance of the material is achieved.

[0039] A multi-scale synergistically reinforced phenyl silicone rubber comprises, by weight, the following components: 70-90 parts of gradient phenyl silicone rubber matrix, 8-12 parts of core-shell structured dynamic crosslinked particles, 5-8 parts of graphene / fluorosilicone rubber interpenetrating network, 12-18 parts of fumed silica, 3-5 parts of dynamic crosslinking aid, 1.0-1.5 parts of vulcanizing agent, and 1-3 parts of chopped carbon fiber; specifically as follows:

[0040] The gradient phenyl silicone rubber matrix consists of 70-90 parts, composed of monophenyl silicone rubber and diphenyl silicone rubber in a mass ratio of (1.5-2.5):1; wherein the monophenyl silicone rubber has a phenyl content of 15-20 mol%, and the diphenyl silicone rubber has a phenyl content of 25-30 mol%. Specifically, the monophenyl silicone rubber has a phenyl content of 15 mol% or 20 mol%, and the diphenyl silicone rubber has a phenyl content of 25 mol% or 30 mol%. The gradient phenyl silicone rubber matrix comprises 70 parts. Alternatively, 90 parts of monophenyl silicone rubber and diphenyl silicone rubber can be mixed in a mass ratio of 1.5:1 or 2.5:1, or even 2:1. Monophenyl silicone rubber (15-20 mol% phenyl) provides damping performance in the low-temperature range (-60 to -20°C), while diphenyl silicone rubber (25-30 mol% phenyl) provides damping performance in the high-temperature range (0 to 200°C). By mixing them in a mass ratio of 2:1, the glass transition temperature ranges overlap, forming a wide-temperature damping platform from -60 to 200°C.

[0041] Wide-temperature-range damping performance and process realization of monophenyl and diphenyl silicone rubber composites

[0042] By compounding monophenyl silicone rubber (15-20 mol% phenyl) and diphenyl silicone rubber (25-30 mol% phenyl) in a mass ratio of 2:1, a wide temperature range damping plateau of -60 to 200℃ can theoretically be formed through the overlapping effect of their glass transition temperature ranges.

[0043] The specific process parameters are recommended as follows:

[0044] Mixing process: Internal mixer temperature 50-80℃, time 20-40 minutes, speed 30-90 rpm

[0045] The vulcanization process includes a first-stage vulcanization: vulcanizing at 160–170°C and 10–20 MPa for 10–20 minutes, and a second-stage vulcanization: vulcanizing at 200–220°C for 2–4 hours.

[0046] The overlapping mechanism of glass transition temperatures (Tg): Monophenyl silicone rubber (15–20 mol% phenyl) has a Tg of approximately -106 °C, exhibiting a damping peak in the range of -60 to -20 °C; diphenyl silicone rubber (25–30 mol% phenyl) has a Tg of approximately -40 to -20 °C, with its damping peak covering the high-temperature range of 0–200 °C. When the two are compounded in a 2:1 ratio, through the synergistic effect of molecular chain segment movement, the Tg ranges can shift from -106 °C and -40 °C of the single component to intermediate temperatures and overlap, forming a continuous damping plateau.

[0047] The core-shell structure of the dynamically cross-linked particles consists of 8 to 12 parts, with SiO2 as the core and phenylsiloxane as the shell, modified by KH550 silane coupling agent, and the core-shell mass ratio is 1:(0.8 to 1.2). Specifically, the number of core-shell structure of the dynamically cross-linked particles is 8 or 12 parts, with SiO2 as the core and phenylsiloxane as the shell, and the core-shell mass ratio is 1:0.8 or 1:1.2.

[0048] Structural design of core-shell dynamically cross-linked particles: SiO2 core (particle size 200-300nm) provides rigid support, phenylsiloxane shell (containing 5-8 mol% hydroxyl groups) introduces dynamic hydrogen bonding sites; compatibility with the matrix is ​​improved by using KH550 silane coupling agent (3-5% of particle mass);

[0049] Mechanism of action: Under the action of external force, the hydrogen bonds formed between the hydroxyl groups of the shell phenylsiloxane and the matrix are reversibly broken and recombined, dissipating energy while inhibiting molecular chain slippage;

[0050] The graphene / fluorosilicone rubber interpenetrating network comprises 5 to 8 parts, including 0.5 to 1.0 parts of isocyanate-functionalized graphene. Specifically, the graphene / fluorosilicone rubber interpenetrating network comprises 5 or 8 parts, wherein the graphene / fluorosilicone rubber interpenetrating network includes 0.5 or 1 part of isocyanate-functionalized graphene.

[0051] Graphene / fluorosilicone rubber interpenetrating networks include:

[0052] Modified graphene: Covalent crosslinking with fluorosilicone rubber is achieved through isocyanate functionalization;

[0053] Double cross-linked network: Graphene sheets construct thermally conductive pathways, while fluorosilicone rubber segments provide an oil-resistant barrier; the network density is controlled at 2.5-3.5 × 10⁻⁶. -4 mol / cm 3 ;

[0054] Fumed silica 12 to 18 parts, specifically, the amount of fumed silica is 12 or 18 parts;

[0055] 3 to 5 parts of dynamic crosslinking aid, which is urea-containing phenyl silicone oil; specifically, the amount of dynamic crosslinking aid is 3 or 5 parts.

[0056] 1.0 to 1.5 parts of vulcanizing agent; specifically, the amount of vulcanizing agent is 1 part or 1.5 parts.

[0057] The short-cut carbon fibers consist of 1 to 3 parts, with a diameter of 5 to 10 μm and a length of 50 to 100 μm. Specifically, the number of short-cut carbon fibers is 1 or 3 parts, with a diameter of 5 μm or 10 μm and a length of 50 μm or 100 μm.

[0058] Multi-scale synergistic effects include:

[0059] Nanoscale: Dynamic hydrogen bond network of core-shell particles enhances damping performance;

[0060] Micrometer scale: Short-cut carbon fibers (aspect ratio 10-20) bridge core-shell particles to construct a thermally conductive network;

[0061] Macroscale: Interpenetrating networks and gradient matrix synergistically regulate modulus stability.

[0062] The preparation methods for core-shell structured dynamically cross-linked particles include:

[0063] SiO2 nanoparticles were dispersed in a mixture of ethanol and water, and phenyltrimethoxysilane and KH550 silane coupling agent were added. The pH was adjusted to 4-5, and the mixture was reacted at 50-60℃ for 4-6 hours. After drying at 80℃, the mixture was calcined at 300-350℃ for 2 hours. The molar ratio of phenyltrimethoxysilane to KH550 silane coupling agent was (5-8):1.

[0064] Specifically, the preparation methods for core-shell structured dynamically cross-linked particles include:

[0065] SiO2 nanoparticles were dispersed in a mixture of ethanol and water, and phenyltrimethoxysilane and KH550 silane coupling agent were added. The pH was adjusted to between 4 and 5, and the mixture was reacted at 50°C or 60°C for 4 h or 6 h. After drying at 80°C, the mixture was calcined at 300°C or 350°C for 2 h. The molar ratio of phenyltrimethoxysilane to KH550 silane coupling agent was 5:1 or 8:1.

[0066] The preparation methods for graphene / fluorosilicone rubber interpenetrating networks include:

[0067] The modified graphene treated with diphenylmethane diisocyanate was mixed with fluorosilicone rubber at a mass ratio of 1:(8-12), and dicumyl peroxide was added. The mixture was then pre-vulcanized at 160-170°C for 8-10 minutes to obtain the product.

[0068] Specifically, the preparation methods of graphene / fluorosilicone rubber interpenetrating networks include:

[0069] Modified graphene treated with diphenylmethane diisocyanate was mixed with fluorosilicone rubber at a mass ratio of 1:8 or 1:12, wherein the fluorosilicone rubber contained 0.3-0.5 mol% vinyl groups, specifically 0.3 mol% or 0.5 mol%. Dicumyl peroxide was added, and the mixture was pre-vulcanized at 160-170°C for 8-10 minutes. The amount of dicumyl peroxide added was 1.2-1.5% of the mass of the fluorosilicone rubber, specifically 1.2% or 1.5% of the mass of the fluorosilicone rubber.

[0070] The preparation methods for modified graphene include:

[0071] The graphene oxide is reacted with vinyltriethoxysilane at a mass ratio of 10:(0.8-1.2), and then reacted with diphenylmethane diisocyanate to obtain the product.

[0072] Specifically, the preparation method of modified graphene includes: reacting graphene oxide with vinyltriethoxysilane at a mass ratio of 10:0.8 or 10:1.2, and then reacting it with diphenylmethane diisocyanate. The molar ratio of NCO to OH in the diphenylmethane diisocyanate is 1.5 to 2.0:1, specifically 1.5:1 or 2:1.

[0073] A method for preparing the above-mentioned phenyl silicone rubber includes the following steps:

[0074] S1 gradient matrix blending:

[0075] Mix monophenyl silicone rubber and diphenyl silicone rubber in a two-roll mill for 5-8 minutes, add fumed silica and chopped carbon fibers, and continue mixing for 15-20 minutes; specifically, mix monophenyl silicone rubber and diphenyl silicone rubber in a two-roll mill for 5 or 8 minutes, with the roller temperature being 50-60°C, add fumed silica and chopped carbon fibers, and continue mixing for 15 or 20 minutes.

[0076] S2 dynamic network construction:

[0077] Add core-shell structured dynamic crosslinking particles and dynamic crosslinking aids, raise the temperature to 80-90℃, and mix for 25-30 minutes. Specifically, after adding core-shell structured dynamic crosslinking particles and dynamic crosslinking aids, raise the temperature to 80℃ or 90℃ and mix for 25 minutes or 30 minutes.

[0078] S3 interpenetrating network composite:

[0079] Add a graphene / fluorosilicone rubber interpenetrating network, lower the temperature to 80℃ and hold for 10 minutes, then continue to lower the temperature to 60℃ and hold for 10 minutes, then continue to lower the temperature to 40℃ and hold for 10 minutes, then add a vulcanizing agent and pass through the tube 8 to 12 times.

[0080] Specifically, a graphene / fluorosilicone rubber interpenetrating network is added. If the temperature in the previous step is 80°C, it is held at 80°C for 10 minutes. If the temperature is 90°C, it is lowered to 80°C and held for 10 minutes. Then, the temperature is lowered to 60°C and held for 10 minutes. The temperature is then lowered to 40°C and held for 10 minutes. Then, a vulcanizing agent is added, and the process is repeated 8 or 12 times. The cooling rate is between 2 and 3°C / min, specifically 2°C / min or 3°C / min, to ensure the synergistic construction of the dynamic hydrogen bond network and the covalent crosslinking network.

[0081] S4 vulcanization molding:

[0082] The first stage of vulcanization is carried out at 165-175℃ for 20-25 minutes, the second stage of vulcanization is carried out at 200-220℃ for 4-6 hours, and finally the vulcanization is allowed to cool naturally to room temperature.

[0083] Specifically, a first-stage vulcanization is performed at 165℃ or 175℃ for 20 or 25 minutes, followed by a second-stage vulcanization at 200℃ or 220℃ for 4 or 6 hours, and finally, the mixture is allowed to cool naturally to room temperature.

[0084] Performance Synergy Breakthrough: Achieving a combination of damping (tanδ≥0.5) over a wide temperature range of -60℃ to 200℃, high thermal conductivity (1.65W / m·K), and oil resistance (volume change rate 3.8%), breaking through the performance bottleneck of traditional materials;

[0085] Structural innovation: The core-shell structure with dynamically cross-linked particles combines rigid support with dynamic hydrogen bonds for the first time, solving the trade-off between damping and strength;

[0086] Controllable process: Gradient cooling and step-by-step vulcanization processes ensure the coordinated construction of multi-scale networks, making them suitable for industrial production.

[0087] This invention, through multi-scale structural design, provides a new technical route for multifunctional silicone rubber materials used in high-end equipment, and has significant economic value and social benefits.

[0088] Example 1

[0089] A method for preparing the above-mentioned phenyl silicone rubber includes the following steps:

[0090] Step 1: Preparation of dynamically cross-linked particles with core-shell structure

[0091] 10g of SiO2 nanoparticles were dispersed in 100mL of ethanol-water mixture (volume ratio 3:1), 8g of phenyltrimethoxysilane and 0.8g of KH550 were added, the pH was adjusted to 4.5 with hydrochloric acid, and the reaction was carried out at 55℃ for 5h. After washing, the product was calcined at 320℃ for 2h to obtain core-shell particles.

[0092] Step 2: Preparation of Modified Graphene

[0093] 1) 1g of graphene oxide was dispersed in 100ml of LDMF, and 0.1g of vinyltriethoxysilane was added. The mixture was stirred at room temperature for 12h.

[0094] 2) Add 0.15g of diphenylmethane diisocyanate, react at 75℃ for 14h, and freeze-dry to obtain isocyanate-functionalized graphene.

[0095] Step 3: Preparation of graphene / fluorosilicone rubber interpenetrating network

[0096] Mix 0.8g of modified graphene with 8g of fluorosilicone rubber (vinyl content 0.4mol%), add 0.1g of dicumyl peroxide, pre-vulcanize at 165℃ for 9min, pulverize and set aside.

[0097] Step 4: Phenyl silicone rubber composite molding

[0098] 1) Monophenyl silicone rubber (20 parts) and diphenyl silicone rubber (10 parts) were mixed in a two-roll mill for 6 minutes, and fumed silica (15 parts) and chopped carbon fiber (2 parts) were added and mixed for 18 minutes.

[0099] 2) Add core-shell particles (10 parts) and ureoylphenyl silicone oil (4 parts), heat to 85℃, and mix for 28 minutes;

[0100] 3) Add an interpenetrating network (6 parts), gradually cool to 40℃, add a diphenyl sulfide agent (1.2 parts), and pass through a thin tube 10 times;

[0101] 4) First stage vulcanization at 170℃ for 22 min, second stage vulcanization at 210℃ for 5 h, to obtain the finished product.

[0102] The phenyl silicone rubber prepared according to the above method was tested for the following results:

[0103] Damping performance: loss factor 0.52 to 0.78 at -60℃ to 200℃, shear modulus 3.5 to 28.6 MPa;

[0104] Thermal conductivity: 1.65 W / m·K;

[0105] Oil resistance: Volume change rate at 120℃ for 75 hours (using No. 3 standard oil) is 3.8%, and tensile strength retention rate is 92%.

[0106] Mechanical properties: tensile strength 14.2 MPa, elongation at break 358%.

[0107] Comparative Example 1 (Coreless / Shell-less Particles)

[0108] The loss factor is 0.35 to 0.51 (-60℃ to 200℃), which proves the effect of dynamic hydrogen bond network on damping.

[0109] Comparative Example 2 (No Interpenetrating Networks)

[0110] With a volume change rate of 11.2% and a thermal conductivity of 0.87 W / m·K, the oil resistance and thermal conductivity synergistic effect of the graphene / fluorosilicone rubber network is verified.

[0111] Comparative Example 3 (Single Phenyl Content)

[0112] The loss factor is less than 0.3 below -40℃, indicating the regulatory effect of the gradient composite system on a wide temperature range.

[0113] The preparation of core-shell structured dynamic cross-linked particles can be achieved by adjusting the amount of phenyltrimethoxysilane (6-10g) to control the shell thickness (20-50nm). The damping performance is optimal when the shell thickness is 30nm.

[0114] With the optimization of interpenetrating networks, the thermal conductivity and oil resistance are balanced when the amount of modified graphene is 0.8 parts; excessive amount will lead to agglomeration.

[0115] For vulcanization process parameters, the optimal temperature for the two-stage vulcanization is 210℃. Temperatures below 200℃ will result in incomplete dynamic cross-linking, while temperatures above 220℃ will cause urea decomposition.

[0116] The embodiments of the present invention have been described in detail above, but the present invention is not limited to the described embodiments. For those skilled in the art, various changes, modifications, substitutions, and variations can be made to these embodiments without departing from the principles and spirit of the present invention, and these variations still fall within the protection scope of the present invention.

Claims

1. A multi-scale synergistically reinforced phenyl silicone rubber, characterized in that, The following components are included in parts by weight: The gradient phenyl silicone rubber matrix consists of 70-90 parts, which are compounded from monophenyl silicone rubber and diphenyl silicone rubber in a mass ratio of (1.5-2.5):

1. Eight to twelve parts of core-shell structured dynamic cross-linked particles, wherein the core-shell structured dynamic cross-linked particles have SiO2 as the core and phenylsiloxane as the shell, and are modified by KH550 silane coupling agent, with a core-shell mass ratio of 1:(0.8 to 1.2). 5-8 parts of graphene / fluorosilicone rubber interpenetrating network, including 0.5-1.0 parts of isocyanate-functionalized graphene; 12-18 parts of fumed silica; 3-5 parts of dynamic crosslinking aid, which is urea-containing phenyl silicone oil; 1.0 to 1.5 parts of vulcanizing agent; One to three parts of chopped carbon fibers, wherein the chopped carbon fibers have a diameter of 5 to 10 μm and a length of 50 to 100 μm.

2. The phenyl silicone rubber according to claim 1, characterized in that, The method for preparing the core-shell structured dynamically cross-linked particles includes: SiO2 nanoparticles were dispersed in a mixture of ethanol and water, and phenyltrimethoxysilane and KH550 silane coupling agent were added. The pH was adjusted to 4-5, and the mixture was reacted at 50-60℃ for 4-6 hours. After drying at 80℃, the mixture was calcined at 300-350℃ for 2 hours. The molar ratio of phenyltrimethoxysilane to KH550 silane coupling agent was (5-8):

1.

3. The phenyl silicone rubber according to claim 1, characterized in that, The preparation method of the graphene / fluorosilicone rubber interpenetrating network includes: The modified graphene treated with diphenylmethane diisocyanate was mixed with fluorosilicone rubber at a mass ratio of 1:(8-12), and dicumyl peroxide was added. The mixture was then pre-vulcanized at 160-170°C for 8-10 minutes.

4. The phenyl silicone rubber according to claim 3, characterized in that, The method for preparing the modified graphene includes: The graphene oxide is reacted with vinyltriethoxysilane at a mass ratio of 10:(0.8-1.2), and then reacted with diphenylmethane diisocyanate to obtain the product.

5. A method for preparing phenyl silicone rubber as described in any one of claims 1-4, characterized in that, Includes the following steps: S1 gradient matrix blending: Mix monophenyl silicone rubber and diphenyl silicone rubber in a two-roll mill for 5-8 minutes, add fumed silica and chopped carbon fibers, and continue mixing for 15-20 minutes. S2 dynamic network construction: Add core-shell structured dynamic crosslinking particles and dynamic crosslinking aids, raise the temperature to 80-90℃, and mix for 25-30 minutes; S3 interpenetrating network composite: Add a graphene / fluorosilicone rubber interpenetrating network, lower the temperature to 80℃ and hold for 10 minutes, then continue to lower the temperature to 60℃ and hold for 10 minutes, then continue to lower the temperature to 40℃ and hold for 10 minutes, then add a vulcanizing agent and pass through the tube 8 to 12 times. S4 vulcanization molding: The first stage of vulcanization is carried out at 165-175℃ for 20-25 minutes, the second stage of vulcanization is carried out at 200-220℃ for 4-6 hours, and finally the vulcanization is carried out naturally to room temperature.

6. The preparation method according to claim 5, characterized in that, In step S3, the cooling rate is controlled at 2–3 °C / min to ensure the synergistic construction of the dynamic hydrogen bond network and the covalent crosslinking network.