Middle film for multifunctional composite particle modified PVB laminated glass and laminated glass

Abstract

In order to solve the problem of serious performance attenuation caused by filler-resin interface failure in the long-term use process of an existing PVB intermediate film, the invention provides the multifunctional composite particle modified PVB laminated glass intermediate film and the laminated glass, and the intermediate film comprises a core functional layer and surface bonding layers symmetrically arranged on the two sides; the core functional layer contains interface reinforced composite particles; the interface reinforced composite particle has a core-shell structure, the core is a porous silicon dioxide microsphere, the shell is a rare earth element doped silicon-aluminum oxide layer, and the surface of the shell has a microscopic coarse structure and is grafted with a silane coupling agent containing an active functional group. The haze change rate of the intermediate film is less than or equal to 5.2% after the intermediate film is subjected to double-85 aging for 1000 hours, so that perfect balance between high tensile strength and good sound insulation is realized on the premise of extremely low haze, and strict requirements of high-end application on comprehensive performance are met.

Description

Technical Field

[0001] This invention relates to the field of laminated glass technology, specifically to an interlayer film for multifunctional composite particle modified PVB laminated glass and the laminated glass itself. Background Technology

[0002] Laminated glass is widely used in the automotive, construction, and aerospace industries due to its excellent safety performance. As a core component of laminated glass, the performance of the PVB interlayer directly determines the overall quality of the laminated glass. Traditional PVB interlayers suffer from the following technical bottlenecks: 1) Insufficient long-term weather resistance: When existing PVB interlayers are used for extended periods in harsh environments such as humidity, heat, and ultraviolet radiation, interfacial debonding easily occurs due to poor compatibility between inorganic fillers and the PVB resin matrix, leading to a significant increase in haze and a decline in mechanical properties. After 1000 hours of aging at 85°C / 85%RH, the haze of traditional PVB interlayers typically increases by more than 40%, and the tensile strength decreases by more than 30%. 2) Difficulty in achieving a balance between overall performance: Inorganic fillers added to improve mechanical strength often lead to increased haze, while reducing filler usage to lower haze sacrifices mechanical strength. Existing technologies struggle to achieve a good balance between low haze, high mechanical strength, and excellent sound insulation. 3) Limited functionality: Most modified PVB interlayers only focus on initial performance and lack effective solutions for performance stability during long-term use.

[0003] Patent CN107141675A discloses a PVB interlayer film with added fillers such as silicon carbide, which improves fire resistance but does not solve the problem of long-term weather resistance; Japanese patent JP2004002073A improves optical performance by using flake-like powder, but its surface coating has weak chemical bonding with PVB resin and is prone to peeling and failure after long-term use.

[0004] Therefore, developing a PVB interlayer with both excellent initial properties and long-term weather resistance is of great significance for improving the service life and reliability of laminated glass. Summary of the Invention

[0005] To address the severe performance degradation of existing PVB interlayer films due to filler-resin interface failure during long-term use, this invention provides a multifunctional composite particle-modified PVB interlayer film and laminated glass. The interlayer film includes a core functional layer and surface adhesive layers symmetrically arranged on both sides. The core functional layer contains interface-reinforcing composite particles with a core-shell structure designed in this invention. This invention utilizes mature chemical processes to achieve a synergistic effect of "chemical modification + physical roughening," optimizing the distribution of interface-reinforcing composite particles in the multilayer PVB film and fundamentally solving the debonding problem of the filler-resin interface under humid and hot environments. After 1000 hours of double 85 aging, the haze change rate of the interlayer film is ≤5.2%, achieving a perfect balance between high tensile strength and good sound insulation under extremely low haze conditions, meeting the stringent comprehensive performance requirements of high-end applications.

[0006] To achieve the above objectives, the present invention adopts the following technical solution: a multifunctional composite particle modified interlayer for PVB laminated glass, comprising a core functional layer and surface bonding layers symmetrically disposed on both sides; the core functional layer contains interface-enhancing composite particles; the interface-enhancing composite particles have a core-shell structure, wherein the core is a porous silica microsphere, the outer shell is a rare earth element-doped silicon aluminum oxide layer, and the surface of the outer shell has a micro-rough structure and is grafted with a silane coupling agent containing active functional groups.

[0007] Furthermore, the porous silica microspheres have an average particle size of 0.5-1.5 μm, a pore size of 5-15 nm, and a specific surface area of ​​300-500 m². 2 / g.

[0008] Furthermore, the rare earth element is selected from at least one of La, Ce, and Yb. The doping amount of the rare earth element in the shell is 2-6% of the shell mass, and the shell thickness is 20-80 nm.

[0009] Furthermore, the micro-rough structure consists of nanoprotrusions formed by the pyrolysis of organic acids. The surface roughness (Ra) measured by atomic force microscopy (AFM) within a scanning range of 1 μm × 1 μm is 5-50 nm, and the protrusion distribution density is 10-100 per μm. 2 .

[0010] Furthermore, the active functional group contained in the silane coupling agent is amino or epoxy, wherein the molar content of the active functional group is 30-50% of the total molar number of the silane coupling agent (corresponding to a silane coupling agent purity ≥98%, ensuring the effective function of the active group). The silane coupling agent is preferably either 3-aminopropyltriethoxysilane (KH550) or γ-glycidoxypropyltrimethoxysilane (KH560), and its dosage is 2-5% of the total mass of the interface-reinforced composite particles (i.e., 2-5 parts by weight of silane coupling agent per 100 parts by weight of composite particles). This dosage ensures a grafting density of 1.5-3.0 grafts / nm on the particle surface. 2 This ensures that the particle surface is fully covered while avoiding the agglomeration of excessive silane coupling agent that could affect compatibility.

[0011] Furthermore, the organic acid is citric acid, and its addition amount is 5-10% of the mass of the porous silica microspheres.

[0012] The preparation method of the above-mentioned interface-enhanced composite particles specifically includes the following steps: 1) Preparation of composite sol: Dissolve rare earth precursor, aluminum source and silicon source in alcohol-water mixed solvent (ethanol to water volume ratio 3-5:1), add citric acid, adjust pH to 3-4 with dilute nitric acid, and hydrolyze and age at room temperature for 20-28 hours. 2) Immerse porous silica microspheres in the composite sol, ultrasonically disperse for 20-40 minutes (power 300-500W), and reflux at 60-80℃ for 6-8 hours; 3) After centrifugation, washing with ethanol, and drying, the particles are calcined at 500-600℃ for 2-4 hours to pyrolyze citric acid and form a nano-rough structure on the particle surface. 4) Then soak the particles in a 2-5 wt% silane coupling agent ethanol solution (liquid-to-solid ratio 8-12:1, volume-to-mass ratio), react at a constant temperature of 75-85℃ for 3-5 hours to ensure uniform grafting of active functional groups, and then centrifuge, wash with ethanol and dry to obtain interface-enhanced composite particles.

[0013] Among them, the rare earth precursor can be cerium nitrate hexahydrate (Ce(NO3)3). 6H2O), lanthanum nitrate hexahydrate (La(NO3)3) 6H2O), ytterbium nitrate hexahydrate (Yb(NO3)3) The source of aluminum can be any one of aluminum isopropoxide (Al(OiPr)3) or aluminum sec-butoxide (Al(OiBu)3); the source of silicon can be any one of tetraethyl orthosilicate (TEOS) or methyl orthosilicate (TMOS).

[0014] Furthermore, the core raw material ratio in the composite sol is 2-6:8-12:20-30 by mass of rare earth precursor, aluminum source, and silicon source. This ratio ensures that the rare earth doping content in the shell reaches 2-6% of the shell mass, and the silicon-aluminum oxide shell structure is dense and uniform, which not only ensures the bonding force with the core, but also provides sufficient sites for the coordination of rare earth ions and PVB hydroxyl groups.

[0015] Furthermore, the ratio of composite sol to porous silica microspheres: by mass, the total mass of rare earth precursor, aluminum source, and silicon source in the composite sol to the mass of porous silica microspheres is 30-48:100, which can precisely control the shell thickness within the range of 20-80nm, avoiding particle agglomeration due to excessively thick shell or affecting the interface strengthening effect due to excessively thin shell.

[0016] Furthermore, the ratio of organic acid to porous silica microspheres: the amount of citric acid (organic acid) added is 5-10% of the mass of porous silica microspheres. This ratio can ensure that the size and distribution density of the nano-protrusions formed after pyrolysis are adapted to the entanglement requirements of PVB resin molecular chains.

[0017] The reason for choosing citric acid as the organic acid in this invention is that the molecular chain length of citric acid (containing 3 carboxyl groups and 1 hydroxyl group) is highly compatible with the molecular chain segment size of PVB resin (segment length of about 0.1-0.3 nm). The size of the nanoprotrusions formed after pyrolysis (height 5-50 nm, diameter 20-100 nm) is exactly within the entanglement scale range of PVB resin molecular chains. At the same time, the trace oxygen-containing groups remaining after pyrolysis of citric acid can form weak hydrogen bonds with the hydroxyl groups of PVB, further enhancing the interfacial wettability between the protrusions and the resin matrix. This synergistic effect of size and interfacial interaction allows the nanoprotrusions to be more stably embedded in the PVB resin matrix, forming a strong physical interlocking structure.

[0018] Furthermore, The components and weights of the core functional layer are as follows: 65-80 parts of PVB resin (hydroxyl content of 18-22 mol%), 20-35 parts of plasticizer, 8-20 parts of interface-reinforced composite particles, 0.3-1.0 parts of alkaline stabilizer, 0.2-0.8 parts of antioxidant, and 0.3-1.0 parts of ultraviolet absorber. The surface adhesive layer comprises the following components and weights: 70-85 parts of PVB resin (hydroxyl content 28-32 mol%), 15-25 parts of plasticizer, 0.2-0.6 parts of alkaline stabilizer, and 0.1-0.5 parts of antioxidant. Furthermore, the thickness of the core functional layer accounts for 20-40% of the total thickness of the intermediate film, and the total thickness of the intermediate film is 0.5-1.2 mm.

[0019] Furthermore, the absolute value of the difference between the hydroxyl content of PVB resin in the core functional layer and the hydroxyl content of PVB resin in the surface adhesive layer is ≥10 mol.

[0020] Furthermore, the plasticizer is any one of triethylene glycol di-2-ethylhexanoate (3GO), triethylene glycol diisooctanoate (TEG-DIO), dioctyl phthalate (DOP), etc., preferably triethylene glycol di-2-ethylhexanoate (3GO), which has excellent compatibility with PVB resin and can balance the flexibility and mechanical stability of the interlayer.

[0021] Furthermore, the alkaline stabilizer is any one of a mixture of sodium acetate and magnesium acetate (mass ratio 1:0.8-1.2), potassium carbonate, sodium bicarbonate, etc., preferably a mixture of sodium acetate and magnesium acetate, which can effectively inhibit the hydrolysis of PVB resin during processing and use, and extend the service life of the intermediate film.

[0022] Furthermore, the antioxidant is any one or a combination of pentaerythritol tetrakis[β-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate] (antioxidant 1010), octadecyl β-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate (antioxidant 1076), triphenyl phosphite (TPP), etc., preferably antioxidant 1010, which has strong thermal stability and can maintain high-efficiency antioxidant activity at PVB processing temperature (160-205℃).

[0023] Furthermore, the ultraviolet absorber is any one of 2-(2'-hydroxy-3'-tert-butyl-5'-methylphenyl)-5-chlorobenzotriazole (UV-326), 2-hydroxy-4-methoxybenzophenone (UV-9), 2-(2'-hydroxy-5'-methylphenyl)benzotriazole (UV-P), etc., preferably UV-326, which has high absorption efficiency in the 280-380nm ultraviolet light band, good compatibility with PVB resin, and is not prone to migration and precipitation.

[0024] The preparation method of the above-mentioned multifunctional composite particle modified PVB laminated glass interlayer includes the following steps: S1: Mix the components of the core functional layer and the surface adhesive layer in a high-speed mixer to obtain the core layer premix and the surface layer premix; S2: Add the two premixed materials separately to a twin-screw extruder for melting and plasticizing, and then filter them through a filter screen of 200 mesh or higher; S3: The filtered melt is extruded through a three-layer co-extrusion die and cast to a cooling roller assembly for cooling and shaping to form a three-layer composite preform; S4: Perform online thickness measurement and edge trimming on the preform to control the thickness tolerance within ±3%; after tension control and static elimination, wind up and cure to obtain the PVB intermediate film.

[0025] The present invention also provides a laminated glass comprising two pieces of glass and an interlayer film for multifunctional composite particle modified PVB laminated glass as described in any of the above claims sandwiched therebetween.

[0026] The beneficial effects of this invention are: Compared with the prior art, the beneficial effects of the present invention are as follows: 1. Breakthrough in long-term weather resistance: Through the synergistic interface design of "rare earth doping (chemical bonding)" and "surface roughening (physical interlocking)," the debonding problem of the filler-resin interface in humid and hot environments is fundamentally solved. After 1000 hours of double 85 aging, the haze change rate of the intermediate film is ≤5.2%, and the mechanical property retention rate is ≥93.5%, far exceeding that of conventional products; 2. Excellent overall performance: Under the premise of extremely low haze (<0.45%), it achieves a perfect balance between high tensile strength (>9.2MPa) and good sound insulation (TL>36.5dB), meeting the stringent requirements of high-end applications for overall performance; 3. The interlayer film is made into laminated glass, which has a visible light transmittance of >88%, an ultraviolet light blocking rate of >99.5%, and stable performance after accelerated aging test, fully meeting the highest requirements for safety, durability and visual comfort for high-end new energy vehicle panoramic sunroofs, high-rise building curtain walls and high-speed rail windows.

[0027] 4. High industrial feasibility: The composite particle preparation adopts mature sol-gel and calcination processes, uses environmentally friendly citric acid, and has controllable costs; the intermediate membrane preparation process is fully compatible with existing PVB membrane production lines, making it easy to promote on a large scale. Detailed Implementation

[0028] The present invention will be further described in detail below with reference to embodiments and comparative examples. The following embodiments are for illustrative purposes only and are not intended to limit the scope of the invention. Unless otherwise specified, the reagents and methods used are conventional techniques in the art.

[0029] Raw materials: (1) PVB resin: different grades, with hydroxyl content of 20±1mol% (for core layer) and 30±1mol% (for surface layer), and average degree of polymerization of 2400 and 1700 respectively. (2) Plasticizer: triethylene glycol di-2-ethylhexanoate (3GO); (3) Porous silica microspheres: average particle size 0.8μm, pore size 10nm, specific surface area 380m². 2 / g. (4) Rare earth precursor: cerium nitrate hexahydrate (Ce(NO3)3) (5) Other reagents: Aluminum isopropoxide (Al(O) iPr)3), tetraethyl orthosilicate (TEOS), citric acid, 3-aminopropyltriethoxysilane (KH550), sodium acetate, magnesium acetate, antioxidant 1010, and ultraviolet absorber UV-326 are all commercially available chemically pure or industrial grade.

[0030] Main equipment: high-speed mixer, twin-screw extruder, three-layer co-extrusion die, casting cooling roller assembly, laser thickness gauge, constant temperature and humidity aging chamber, universal testing machine, haze meter, differential scanning calorimeter (DSC), etc.

[0031] Examples 1-4: Preparation of PVB Interlayer Film 1. Preparation of interface-enhanced composite particles: Based on 100 parts by weight of porous silica microspheres, the amounts of raw materials and process details are as follows: (1) Preparation of composite sol: Weigh cerium nitrate hexahydrate (Ce(NO3)3) in a mass ratio of 2-6:8-12:20-30. 6H2O), aluminum isopropoxide (Al(O) i Pr)3), Tetraethyl orthosilicate (TEOS), dissolved in an alcohol-water mixture of ethanol and water in a volume ratio of 4:1 (the total mass of the solvent is 6 times the total mass of the three raw materials mentioned above); add 5-10% citric acid by weight of porous silica microspheres, adjust the pH to 3-4 with dilute nitric acid, and hydrolyze and age at room temperature for 24 hours.

[0032] Example 1: 2 parts cerium nitrate hexahydrate, 8 parts aluminum isopropoxide, 20 parts TEOS, and 5 parts citric acid; Example 2: 4 parts cerium nitrate hexahydrate, 10 parts aluminum isopropoxide, 25 parts TEOS, and 8 parts citric acid; Example 3: 3.5 parts cerium nitrate hexahydrate, 9 parts aluminum isopropoxide, 22 parts TEOS, and 6.5 parts citric acid; Example 4: 6 parts cerium nitrate hexahydrate, 12 parts aluminum isopropoxide, 30 parts TEOS, and 10 parts citric acid.

[0033] (2) Coating and reflux: 100 parts by weight of porous silica microspheres were immersed in the above composite sol (the total mass ratio of rare earth precursor, aluminum source and silicon source in the composite sol to the mass of porous silica microspheres was 30-48:100), ultrasonically dispersed for 30 minutes (power 300-500W), and refluxed at 60-80℃ for 6-8 hours (7 hours is preferred in Example 2).

[0034] (3) Calcination roughening: Centrifuge separation (speed 8000-10000r / min, time 15 minutes), wash with ethanol 3 times, dry at 100℃ for 12 hours, and then calcine at 500-600℃ for 3 hours (550℃ is preferred in Example 2). Citric acid pyrolysis forms a nano-rough structure.

[0035] (4) Silane coupling agent treatment: Prepare a 3wt% 3-aminopropyltriethoxysilane (KH550) ethanol solution, immerse the calcined particles in the solution at a liquid-to-solid ratio of 10:1 (volume-to-mass ratio), and react at 80℃ for 4 hours, stirring once every 30 minutes during the reaction; after the reaction, centrifuge and separate, wash twice with ethanol, and dry at 80℃ for 6 hours to obtain interface-reinforced composite particles.

[0036] 2. Preparation of core functional layer and surface adhesive layer Prepare the core layer premix and surface layer premix according to the formulations shown in Tables 1 and 2. The specific processes are as follows: 1) Core layer premix: Mix in a high-speed mixer at 90-100℃ and 300-500r / min for 40-60 minutes; 2) Surface layer premix: Mix in a high-speed mixer at 80-85℃ and 200-400r / min for 30-40 minutes.

[0037] 3. Intermediate film forming Prepared using the process of "twin-screw extrusion → three-layer co-extrusion casting → edge trimming → winding and curing", with specific parameters as follows: Twin-screw extrusion temperatures: Core layer: Zone 1 165-170℃, Zone 2 185-190℃, Zone 3 195-200℃, Die head 200-205℃ (speed 150-200r / min); Surface layer: Zone 1 155-160℃, Zone 2 175-180℃, Zone 3 185-190℃, Die head 190-195℃ (speed 120-180r / min).

[0038] Casting cooling: Die head temperature 195-200℃, casting speed 8-12m / min, cooling roller group temperature 25-30℃, 20-25℃, 15-20℃ respectively.

[0039] Curing conditions: Curing at 23℃ and 50%RH for 48 hours.

[0040] Comparative Example 1: Ordinary precipitated silica (average particle size 2.0 μm, unmodified) was used to replace the interface-reinforced composite particles, with an addition amount of 15 parts. The remaining formulation and process conditions were exactly the same as in Example 2.

[0041] Comparative Example 2: Ordinary silica (1.0 μm) and cerium oxide (CeO2) powders were physically mixed, with a total addition of 15 parts and a mass ratio of 9:1. No core-shell structure composite or surface roughening treatment was performed. All other conditions were the same as in Example 2.

[0042] Comparative Example 3: Ordinary silica (average particle size 1.0 μm) surface-treated with only KH550 silane coupling agent was added in an amount of 15 parts, and the other conditions were the same as in Example 2.

[0043] Comparative Example 4: A composite particle with a "core-shell structure + silane grafting but no nano-rough structure" was used. The rest of the formulation and process were exactly the same as in Example 2.

[0044] Preparation differences: No citric acid was added before calcination of the composite particles, and there were no nano-protrusions on the shell surface (surface roughness Ra≤2nm). The remaining steps (rare earth doping, silane grafting) were the same as in Example 2.

[0045] Table 1: Formulation parameters for examples and comparative examples (core functional layer)

[0046] Table 2: Formulation parameters (surface adhesive layer) for Examples and Comparative Examples

[0047] The structures and particle characteristic parameters of the embodiments and comparative examples are shown in Table 3.

[0048] Table 3: Structure and Particle Characteristic Parameters of Examples and Comparative Examples

[0049] The performance testing methods are as follows: 1) Haze test: According to ASTM D1003 standard, haze meters are used to test at 23℃ and 80℃ respectively; 2) Tensile properties: According to ISO 527-2 standard, dumbbell-shaped specimens are used, and the tensile speed is 100mm / min; 3) Glass transition temperature (Tg): Differential scanning calorimeter (DSC) is used, with a heating rate of 10℃ / min, and the midpoint temperature is taken; 4) Sound insulation performance: According to JIS R 3208, the sound transmission loss (TL value) at 2000Hz is tested using an acoustic impedance tube; 5 6) Adhesion strength: According to GB / T14683, test the peel strength between the interlayer and the glass; 7) Weather resistance test: Place the sample in a constant temperature and humidity chamber at 85℃ and 85%RH and test the performance retention rate after 1000h (performance retention rate = performance after aging / initial performance × 100%); 8) Interfacial shear strength: Use a single particle pull-out test to test the interfacial shear strength between the composite particles and PVB resin; 9) Infrared spectroscopy (FT-IR): Test the characteristic peaks of the composite particles and PVB resin complex to verify the formation of coordination bonds.

[0050] The test results of the examples and comparative examples are shown in Table 4. The weathering resistance test results of the examples and comparative examples (after 1000h of double 85 aging) are shown in Table 5.

[0051] Table 4: Initial Performance Test Results of Examples and Comparative Examples

[0052] Table 5: Weathering resistance test results of the examples and comparative examples (after 1000h of double 85 aging)

[0053] Note: Performance retention rate = (performance value after aging / initial performance value) × 100%; Haze change rate = (haze after aging - initial haze) / initial haze × 100%.

[0054] Results analysis and synergistic effect demonstration (see Tables 4 and 5): 1. Excellent overall performance: As can be seen from Table 4, all embodiments achieved high tensile strength (≥9.2MPa) and excellent sound insulation (TL≥36.5dB) while maintaining extremely low haze (≤0.45%), thus solving the long-standing performance balance problem faced by the industry.

[0055] 2. Excellent long-term weather resistance: As shown in Table 5, after rigorous aging, Examples 1-4 all exhibited a haze change rate of ≤5.2% and a strength retention rate of ≥93.5%, with negligible performance degradation. In contrast, all comparative examples showed severe performance degradation, especially Comparative Example 1 (ordinary SiO2), which experienced a haze increase of 42.5% and a strength retention rate of only 68.3%, resulting in complete failure. This demonstrates that the core-shell interface structure of this invention effectively blocks the erosion of the interface by damp heat aging factors.

[0056] 3. Unexpected Synergistic Effects: The effects of this invention are not simply the sum of a single modification method. As shown in Table 4, the initial interfacial shear strength of Comparative Example 3 (single chemical modification) is 6.3 MPa. If the contribution of "chemical modification" (an increase of approximately 21%) of Comparative Example 2 (physically mixed rare earth, strength 5.1 MPa) compared to Comparative Example 1 (4.2 MPa) is simply added to Comparative Example 3, the expected strength is approximately 6.3 × 1.21 ≈ 7.6 MPa. However, the initial interfacial shear strength of Example 2 is actually 9.8 MPa, with a synergistic gain of (9.8 - 7.6) / 7.6 ≈ 29%. This 29% performance improvement is an unexpected synergistic gain produced by "rare earth doping" and "surface roughening" in the specific core-shell structure of this invention, constituting a prominent and substantial feature.

[0057] Example 5: Industrial Application The interlayer film prepared in Example 2 of this invention is sandwiched between two 2.1mm thick ultra-clear float glass sheets, and laminated glass is produced by vacuum pre-pressing (100℃, -0.095MPa, 20min) and final pressing in an autoclave (135℃, 1.3MPa, 30min). This glass has a visible light transmittance >88%, an ultraviolet light blocking rate >99.5%, and exhibits stable performance after accelerated aging testing, fully meeting the highest requirements for safety, durability, and visual comfort for high-end new energy vehicle panoramic sunroofs, high-rise building curtain walls, and high-speed rail windows.

Claims

1. A multifunctional composite particle-modified PVB interlayer film for laminated glass, characterized in that, It includes a core functional layer and surface bonding layers symmetrically arranged on both sides; the core functional layer contains interface-enhanced composite particles; the interface-enhanced composite particles have a core-shell structure, with a core of porous silica microspheres and a shell of rare earth element-doped silicon aluminum oxide layer, and the surface of the shell has a micro-rough structure and is grafted with a silane coupling agent containing active functional groups.

2. The multifunctional composite particle-modified PVB interlayer glass as described in claim 1, characterized in that, The porous silica microspheres have an average particle size of 0.5-1.5 μm, a pore size of 5-15 nm, and a specific surface area of ​​300-500 m². 2 / g.

3. The multifunctional composite particle-modified PVB interlayer film for laminated glass as described in claim 1, characterized in that, The rare earth element is selected from at least one of La, Ce, and Yb; the doping amount of the rare earth element in the shell is 2-6% of the shell mass, and the shell thickness is 20-80 nm.

4. The multifunctional composite particle-modified PVB interlayer glass as described in claim 1, characterized in that, The micro-rough structure is formed by the pyrolysis of citric acid into nano-protrusions; the amount of citric acid added is 5-10% of the mass of the porous silica microspheres.

5. The multifunctional composite particle-modified PVB interlayer film for laminated glass as described in claim 1, characterized in that, The active functional group contained in the silane coupling agent is amino or epoxy, wherein the molar content of the active functional group is 30-50% of the total molar number of the silane coupling agent; the silane coupling agent is any one of 3-aminopropyltriethoxysilane and γ-glycidoxypropyltrimethoxysilane, and its amount is 2-5% of the total mass of the interface-reinforced composite particles.

6. The interlayer film for multifunctional composite particle-modified PVB laminated glass as described in any one of claims 1-5, characterized in that, The method for preparing the interface-enhanced composite particles specifically includes the following steps: 1) Preparation of composite sol: Dissolve rare earth precursor, aluminum source and silicon source in alcohol-water mixed solvent, add citric acid, adjust pH to 3-4 with dilute nitric acid, and hydrolyze and age at room temperature for 20-28 hours. 2) Immerse porous silica microspheres in the composite sol, disperse by ultrasonication, and reflux at 60-80℃ for 6-8 hours; 3) After centrifugation, washing with ethanol, and drying, the particles are calcined at 500-600℃ for 2-4 hours to pyrolyze citric acid and form a nano-rough structure on the particle surface. 4) Then, soak the particles in an ethanol solution of 2-5 wt% silane coupling agent and react them at a constant temperature of 75-85℃ for 3-5 hours to ensure uniform grafting of active functional groups. After the reaction, centrifuge, wash with ethanol and dry to obtain interface-enhanced composite particles.

7. The multifunctional composite particle-modified PVB interlayer glass as described in claim 6, characterized in that, The core functional layer comprises the following components and weights: 65-80 parts PVB resin, 20-35 parts plasticizer, 8-20 parts interface-reinforcing composite particles, 0.3-1.0 parts alkaline stabilizer, 0.2-0.8 parts antioxidant, and 0.3-1.0 parts ultraviolet absorber; the hydroxyl content of the PVB resin is 18-22 mol%. The surface adhesive layer comprises the following components and weights: 70-85 parts PVB resin, 15-25 parts plasticizer, 0.2-0.6 parts alkaline stabilizer, and 0.1-0.5 parts antioxidant; the hydroxyl content of the PVB resin is 28-32 mol.

8. The multifunctional composite particle-modified PVB interlayer glass as described in claim 7, characterized in that, The thickness of the core functional layer accounts for 20-40% of the total thickness of the intermediate membrane, and the total thickness of the intermediate membrane is 0.5-1.2 mm; The absolute value of the difference between the hydroxyl content of PVB resin in the core functional layer and the hydroxyl content of PVB resin in the surface adhesive layer is ≥10 mol%. The plasticizer is any one of triethylene glycol di-2-ethylhexanoate, triethylene glycol diisooctanoate, and dioctyl phthalate; The alkaline stabilizer is any one of a mixture of sodium acetate and magnesium acetate, potassium carbonate, or sodium bicarbonate. The antioxidant is any one or more of antioxidant 1010, antioxidant 1076 and antioxidant TPP; The ultraviolet absorber is any one of UV-326, UV-9, and UV-P.

9. The method for preparing the interlayer film for multifunctional composite particle-modified PVB laminated glass according to claim 7 or 8, characterized in that, Includes the following steps: S1: Mix the components of the core functional layer and the surface adhesive layer in a high-speed mixer to obtain the core layer premix and the surface layer premix; S2: Add the two premixed materials separately to a twin-screw extruder for melting and plasticizing, and then filter them through a filter screen of 200 mesh or higher; S3: The filtered melt is extruded through a three-layer co-extrusion die and cast to a cooling roller assembly for cooling and shaping to form a three-layer composite preform; S4: Perform online thickness measurement and edge trimming on the preform to control the thickness tolerance within ±3%; after tension control and static elimination, wind up and cure to obtain the PVB intermediate film.

10. A laminated glass comprising two glass panes and an interlayer for a multifunctional composite particle-modified PVB laminated glass as described in claim 7 or 8, sandwiched therebetween.

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