Epoxy Vitrimer material directionally regulated and controlled through phase separation engineering as well as preparation method and application of epoxy Vitrimer material

By inducing microphase separation through the polymerization of binary epoxy monomers and amine monomers, epoxy Vitrimer materials with homogeneous or island-like structures are formed, solving the problem of uncontrollable phase structure, achieving synergistic optimization of mechanical and luminescent properties, improving the mechanical stability and luminescent efficiency of the material, and extending the lifespan of optoelectronic devices.

CN120923738APending Publication Date: 2025-11-11ANHUI UNIVERSITY OF TECHNOLOGY
View PDF 0 Cites 0 Cited by

Patent Information

Application Number
CN202511069285.9
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2025-07-31
Publication Date
2025-11-11

AI Technical Summary

Technical Problem

In existing technologies, the phase structure of epoxy Vitrimer materials is uncontrollable, making it difficult to coordinate mechanical properties and luminescence properties. Traditional methods rely on catalysts, which leads to luminescence quenching. The phase interface mechanism is unclear, making it difficult to achieve the dual requirements of high mechanical stability and efficient luminescence.

Method used

By inducing microphase separation through the polymerization of binary epoxy monomers and amine monomers, homogeneous or island-like structures are formed. Dynamic covalent networks are constructed using precise control of reaction kinetics and thermodynamics to achieve nanoscale phase separation, avoiding the use of catalysts and enhancing the mechanical and luminescent properties of the materials.

Benefits of technology

The mechanical and luminescent properties of epoxy Vitrimer materials were synergistically optimized, improving the material's mechanical stability and luminescent efficiency. This solved the problem of aging and failure of traditional encapsulation materials, extended the lifespan of optoelectronic devices, and supported reuse.

✦ Generated by Eureka AI based on patent content.

Smart Images

  • Figure CN120923738A_ABST
    Figure CN120923738A_ABST
Patent Text Reader

Abstract

The invention discloses an epoxy Vitrimer material directionally regulated and controlled through phase separation engineering as well as a preparation method and application of the epoxy Vitrimer material, and belongs to the technical field of high-molecular polymers. According to the epoxy Vitrimer material, a binary epoxy monomer, a diamine monomer and a polyamine monomer are subjected to polymerization-induced microphase separation to form a homogeneous phase or sea-island structure, the molar ratio of amido to epoxy functional groups is 1: 1, and the amido functional groups provided by diamine and polyamine respectively account for 25-75%. In the sea-island structure, a polyamine high-crosslinking-density area forms an island phase, and diamine is a continuous phase. Directional construction of a phase structure is realized through a monomer adding sequence and temperature control, controllable preparation of a homogeneous phase and an island structure is realized by utilizing reaction kinetics and thermodynamics, and directional enhancement of mechanical properties and collaborative optimization of luminescent properties are realized by regulating and controlling nanoscale phase separation behaviors of a dynamic covalent network and a functional phase. No extra catalyst is needed, the problem of luminescence quenching is avoided, the self-repairing and recoverability of the material are improved, and the material has a good application prospect in the field of photoelectric devices such as LED packaging.
Need to check novelty before this filing date? Find Prior Art

Description

Technical Field

[0001] This invention relates to an epoxy Vitrimer material directionally controlled by phase separation engineering, its preparation method and application, belonging to the field of polymer technology. Background Technology

[0002] With the development of modern industry and technology, the application of polymer materials in daily life and industrial fields is becoming increasingly widespread. Among them, the epoxy Vitrimer dynamic covalent polymer network, with its unique topological rearrangement capability, shows great potential in the field of recyclable optoelectronic devices. Taking LED lighting as an example, although its high efficiency and energy-saving characteristics have established its position as a core light source, traditional encapsulation materials (such as epoxy resin or silicone) are prone to interface delamination, yellowing, or cracking under long-term thermal-photoaging, leading to device failure. Epoxy Vitrimer, through its reversible covalent network such as dynamic β-hydroxy ester bonds, not only inherits the excellent adhesion and optical transparency of traditional epoxy resin, but also achieves in-situ self-repair and reprocessing recycling of the encapsulation layer through topological rearrangement, significantly extending LED life and reducing electronic waste.

[0003] The benzene ring, oxygen atoms, and carbonyl groups induce π-π, C=O…π, O…O, and O…C=O interactions through spatial electronic communication, forming clusters, which is termed cluster-triggered emission (CTE). The dipoles or transient dipoles present in these systems are the driving force for the generation of intramolecular spatial conjugation (TSC) and lead to cluster luminescence in the aggregated state.

[0004] In existing technologies, the mechanical properties (such as strength and toughness) and dynamic exchange activity of traditional vitrimers often exhibit an inherent contradiction, with one increasing and the other decreasing. Their single-phase structure makes it difficult to simultaneously meet the dual requirements of high mechanical stability and functionality (such as efficient luminescence) in devices. To address this, researchers have attempted to construct multifunctional composite materials through physical blending or chemical modification. However, the compatibility differences between different monomers easily induce uncontrolled phase separation during polymerization. Related literature reports that Kai Wu et al. (ACS Appl. Mater. Interfaces 2020, 12, 123) reported a one-pot reaction of bisphenol A type epoxy resin with cyclic carbonate-terminated polyurethane and polyamine. Due to differences in activity, asynchronous ring-opening crosslinking occurred, forming a soft-phase, hard-phase interpenetrating network structure, thus significantly improving performance. However, effective control of the phase structure is still not achieved, and the classical phase separation theory has not been used to explain it. Furthermore, the mechanism by which phase region size affects cluster luminescence remains unclear. The core challenge at present lies in the lack of a phase structure regulation mechanism: on the one hand, how to use the nucleation-growth mechanism to directionally construct island structures remains an unsolved problem; on the other hand, the structure-property relationship between micro and nano phase states and performance is not yet clear—the difference in spatial conjugation between different phase regions (such as dynamic bond-enriched phases and functional phases) will lead to the differentiation (enhancement or weakening) of local mechanical properties and the shift of electronic transition modes (n→σ-dominant region and n→π-dominant region), and how the above-mentioned micro-region structure affects the topological rearrangement dynamics and luminescence energy transfer efficiency of the dynamic cross-linked network still lacks quantitative correlation model support.

[0005] To address the issues of lack of controllable phase structure and difficulty in synergistically enhancing mechanical and luminescent properties in existing technologies, there is an urgent need to develop a composite material and its preparation method that can directionally regulate the mechanical and luminescent properties of epoxy vitrimer through nanoscale phase separation engineering. This method must overcome the challenges of catalytic quenching and unclear interfacial interaction mechanisms inherent in traditional methods. It aims to achieve fluorescence enhancement through the spatial confinement of intrinsic chromophores (such as ester bonds and hydroxyl groups) within the molecular chain via phase separation structures, thereby improving the long-term stability and luminescent efficiency of the material in optoelectronic device packaging. This approach has significant scientific and industrial value. Summary of the Invention

[0006] This invention aims to provide a directionally regulated epoxy vitrimer material and its preparation method to address the technical defects of existing technologies, such as uncontrollable phase structure, imbalance between mechanical and luminescent properties, and failure of optoelectronic devices. It offers a simple preparation method that regulates the nanoscale phase separation behavior of the dynamic covalent network and functional phase, achieving directional enhancement of mechanical properties and synergistic optimization of luminescent properties. This invention provides a directionally regulated epoxy vitrimer material through phase separation engineering, along with its preparation method and applications.

[0007] To achieve the above objectives, the first technical objective of this invention is to provide an epoxy Vitrimer material that is directionally controlled through phase separation engineering. This material is formed by polymer-induced microphase separation of binary epoxy monomers and amine monomers to create a homogeneous or island-like phase-separated state. The binary epoxy monomers comprise 100% epoxy functional groups, with a molar ratio of amine functional groups to epoxy functional groups of 1:1. The amine monomers include diamine monomers and polyamine monomers, wherein the diamine monomers provide 25%–75% of the total amine functional groups, and the polyamine monomers provide 75%–25% of the total amine functional groups. When the island structure is formed, the high crosslinking density regions formed by the polyamine monomers constitute the island phase, and the regions formed by the diamine monomers constitute the continuous phase.

[0008] Preferably, the binary epoxy monomer is at least one selected from cyclohexane-1,2-dicarboxylic acid diglycidyl ester, resorcinol diglycidyl ether, 1,6-hexanediol diglycidyl ether, and epoxy-terminated polydimethylsiloxane.

[0009] Preferably, the diamine monomer is at least one selected from polyetheramine, amino-terminated polydimethylsiloxane, 1,4-cyclohexanediamine, and p-phenylenediamine.

[0010] Preferably, the polyamine monomer is at least one of tetraethylenepentamine, triethylenetetramine, and tri(2-aminoethyl)amine.

[0011] The second technical objective of the invention is to provide a method for preparing epoxy Vitrimer materials through phase separation engineering, characterized by achieving directional construction of the phase structure through monomer addition sequence and temperature control, comprising any one of the following steps:

[0012] S1. Synthesis of nano-homogeneous epoxy Vitrimer: Dicyclic epoxy monomers and diamine monomers are mixed uniformly and reacted at 80-100℃ for 2-4 h to obtain a uniform prepolymer. Then, polyamine monomers are added, stirred in an ice-water bath for 15-30 min, vacuum mixed in a vacuum degassing machine for 10-30 min, cured at room temperature for 24-48 h, and cured at 80-100℃ for 24-48 h to obtain a homogeneous epoxy Vitrimer material with no obvious phase separation.

[0013] S2. Synthesis of epoxy vitrimer with island structure and submicron island size: Diamine monomers and polyamine monomers were mixed at room temperature for 25-30 min, then a diepoxy monomer was added and stirred at room temperature for 20-30 min. The mixture was then vacuum mixed in a vacuum degassing machine for 10-30 min, cured at room temperature for 24-48 h, and then cured at 80-100℃ for 24-48 h to obtain epoxy vitrimer material with island structure and submicron island size.

[0014] S3. Synthesis of island-structured epoxy vitrimer with island phase size in the micrometer range: Dicyclic epoxy monomers and polyamine monomers are mixed evenly and reacted at 25-30℃ for 20-30 min to obtain a prepolymer. Then, diamine monomers are added, and the mixture is stirred in an ice-water bath for 15-30 min. The mixture is then vacuum mixed in a vacuum degassing machine for 10-30 min, cured at room temperature for 24-48 h, and then cured at 80-100℃ for 24-48 h to obtain an epoxy vitrimer material with an island structure and island phase size in the micrometer range.

[0015] The directionally controlled epoxy vitrimer material provided in this invention utilizes the rational use of raw materials such as binary epoxy monomers, diamine monomers, and polyamine monomers. By leveraging reaction kinetics and thermodynamics, homogeneous, island-structured epoxy vitrimers can be controllably prepared, filling a gap in the phase engineering field of epoxy vitrimer materials. Introducing rigid-flexible block or crystalline components into epoxy vitrimers can improve material toughness through stress dissipation mechanisms of dynamic bonds at the phase interface, while simultaneously enhancing luminescence efficiency through phase separation-induced chromophore spatial interaction effects. This solves the problem in existing technologies of how to achieve phase domain size control using polymerization-induced phase separation, which leads to the inability to guarantee the preparation of high-performance luminescent vitrimers and their application in light-emitting electronic devices. Polymerization-induced phase separation (PIMS) is used to develop unique nanostructures with highly useful morphologies through microphase separation of emerging block copolymers during polymerization. This provides a unique pathway for generating thermosetting polymers with well-defined nanostructures and microstructures.

[0016] The present invention also provides the application of the epoxy Vitrimer material, which is directionally controlled by phase separation engineering, in optoelectronic device packaging.

[0017] Compared with the prior art, the beneficial effects of the present invention are:

[0018] This invention achieves the controllable fabrication of homogeneous and submicron / micron-scale island structures in epoxy Vitrimer materials through the synergistic effects of binary epoxy monomers, diamines, and polyamines, utilizing precise control of reaction kinetics and thermodynamics. By directionally constructing a dynamic covalent network and achieving nanoscale phase separation of the functional phase, mechanical and luminescent properties are simultaneously optimized: the rigid-flexible block design combined with the stress dissipation mechanism of dynamic bonds at the phase interface enhances the tensile strength of the homogeneous structure; the phase separation-induced spatial confinement effect of fluorophores significantly improves luminescence efficiency. In the island structure, the spatial confinement of fluorophores within the nano / micron island phase enhances intramolecular spatial conjugation (TSC), improving the luminescence efficiency of aggregated clusters.

[0019] The phase structure can be directionally regulated by controlling the order of monomer addition and temperature, eliminating the need for catalysts and avoiding the luminescence quenching problem caused by traditional methods. This material combines high mechanical stability, self-healing ability, and excellent luminescence properties in optoelectronic devices such as LED packaging, solving the aging failure problem of traditional packaging materials, extending device life, and supporting recycling. Attached Figure Description

[0020] Figure 1 The images show the epoxy Vitrimer field emission scanning electron microscope images (scale bar 20 μm) of the nanophase, submicron phase, and micron phase prepared in Example 1 of this invention; wherein, (a) homogeneous structure, (b) island structure - submicron-level island phase, and (c) island structure - micron-level island phase.

[0021] Figure 2 The images show transmission electron microscopy (TEM) images of the nanophase, submicron phase, and micron phase of the epoxy Vitrimer material prepared in Example 1 of this invention; wherein, (a) homogeneous structure, (b) island structure - submicron-level island phase, and (c) island structure - micron-level island phase.

[0022] Figure 3 The infrared spectrum of Example 1 of the present invention shows that the epoxy characteristic peak at 913 cm⁻¹ and the NH stretching vibration peak at 3288 cm⁻¹ have both disappeared, indicating the formation of β-hydroxy ester bonds.

[0023] Figure 4 The tensile strength diagram of the epoxy Vitrimer material prepared in Example 1 of the present invention is shown; wherein, homogeneous structure: fracture strength 11.4 MPa; island structure - submicron island phase: fracture strength 2.3 MPa; island structure - micron island phase: fracture strength 1.9 MPa. Detailed Implementation

[0024] The technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention.

[0025] Example 1

[0026] According to the component amounts in Table 1 (based on the molar percentage of reactive functional groups): cyclohexane-1,2-dicarboxylic acid diglycidyl ester 100%, polyetheramine 25%, tetraethylenepentamine 75%;

[0027] (1) Synthesis of nano-homogeneous epoxy Vitrimer: Cyclohexane-1,2-dicarboxylic acid diglycidyl ester was mixed with polyetheramine and reacted at 80℃ for 3 h to obtain a homogeneous prepolymer. Then tetraethylenepentamine was added, stirred in an ice-water bath for 20 min, vacuum mixed in a vacuum degassing machine for 20 min, cured at room temperature for 24 h, and cured at 80~100℃ for 48 h to obtain nano-homogeneous epoxy Vitrimer material.

[0028] (2) Synthesis of epoxy Vitrimer with island structure and submicron island size: Polyetheramine and tetraethylenepentamine were mixed at room temperature for 20 min, then cyclohexane-1,2-dicarboxylic acid diglycidyl ester was added, stirred at room temperature for 20 min, vacuum mixed in a vacuum degassing machine for 20 min, cured at room temperature for 24 h, and cured at 80℃ for 48 h to obtain epoxy Vitrimer material with island structure and submicron island size;

[0029] (3) Synthesis of island-structured epoxy Vitrimer with island phase size in the micrometer range: Cyclohexane-1,2-dicarboxylic acid diglycidyl ester and tetraethylenepentamine were mixed evenly and reacted at 25°C for 30 min to obtain a prepolymer. Then, polyetheramine was added, and the mixture was stirred in an ice-water bath for 20 min. It was then vacuum mixed in a vacuum degassing machine for 20 min, cured at room temperature for 24 h, and cured at 80°C for 48 h to obtain an island-structured epoxy Vitrimer material with island phase size in the micrometer range.

[0030] The performance of the raw materials and the obtained product in Example 1 was analyzed, such as... Figures 1-4 As shown.

[0031] like Figure 1 As shown in (a), the material prepared in Example 1 exhibits a uniform phase structure with no obvious phase separation domain, indicating that a homogeneous structure was successfully obtained. Figure 1(b) Uniformly dispersed island phases (bright areas) with sizes ranging from 100 to 500 nm are embedded in a continuous phase (dark areas), confirming the acquisition of submicron island structures; Figure 1 (c) The island phase size is shown to be 1-5 μm, confirming the acquisition of micron-sized island structures.

[0032] like Figure 2 As shown in (a), the material prepared in Example 1 exhibits a uniform electronic contrast distribution and no obvious phase interface or phase domain structure, indicating that a homogeneous structure was successfully obtained. Figure 2 (b) The uniformly dispersed dark island phase (high cross-linking density phase) with a size of 100-500 nm is embedded in a light-colored continuous phase, confirming the acquisition of a submicron island structure; Figure 2 (c) The island phase size is shown to be 1-5 μm, confirming the acquisition of a micron-sized island structure. This result directly corroborates the mechanism by which the monomer addition order directionally regulates the phase structure type and scale through the nanoscale phase interface morphology.

[0033] Figure 3 The results showed that the NH stretching vibration peak at 3288 cm⁻¹ and the epoxy group characteristic peak at 913 cm⁻¹ completely disappeared after the reaction. At the same time, a strong absorption peak attributable to C=O in the β-hydroxy ester bond was observed near 1730 cm⁻¹. This fully demonstrates that the epoxy group reacted with the amino group to form a dynamic covalent cross-linked network (β-hydroxy ester bond), and the target epoxy Vitrimer material was successfully synthesized.

[0034] Figure 4 The stress-strain curves show that the tensile strength of the homogeneous structure (11.4 MPa) is significantly higher than that of the two island structures (submicron: 2.3 MPa; micron: 1.9 MPa). Analysis indicates that introducing long-chain polyetheramines first, followed by crosslinking with short-chain tetraethylenepentamine, yields a nearly homogeneous system. However, if highly reactive short-chain amines are introduced first for crosslinking, and then long-chain amines are added, island structures will nucleate and grow during polymerization.

[0035] Example 2

[0036] Compared with Example 1, except that the specific raw materials of the directional controlled epoxy Vitrimer material have the same component amounts (by the molar percentage of the reactive functional groups) of 100% resorcinol diglycidyl ether, 25% polyetheramine, and 75% tetraethylenepentamine, everything else is the same.

[0037] Example 3

[0038] Compared with Example 1, except that the specific raw materials of the directional controlled epoxy Vitrimer material have the same component amounts (in terms of the molar percentage of the reactive functional groups) of 1,6-hexanediol diglycidyl ether 100%, amino-terminated polydimethylsiloxane 25%, and triethylenetetramine 75%, everything else is the same.

[0039] Example 4

[0040] Compared with Example 1, the only difference is that the specific raw materials of the directional controlled epoxy Vitrimer material have the same component amounts (in terms of the molar percentage of the reactive functional groups) of 100% epoxy-terminated polydimethylsiloxane, 25% hexamethylenediamine, and 75% tris(2-aminoethyl)amine.

[0041] Example 5

[0042] Compared with Example 1, except that the specific raw materials of the directional controlled epoxy Vitrimer material have the same component amounts (by the molar percentage of the reactive functional groups) of cyclohexane-1,2-dicarboxylic acid diglycidyl ester 100%, 1,4-cyclohexanediamine 25%, and triethylenetetramine 75%, everything else is the same.

[0043] Example 6

[0044] Compared with Example 1, except that the specific raw materials of the directional controlled epoxy Vitrimer material have the same component amounts (in terms of the molar percentage of the reactive functional groups) of 100% epoxy-terminated polydimethylsiloxane, 25% 1,4-cyclohexanediamine, and 75% tris(2-aminoethyl)amine, all other aspects are the same.

[0045] Comparative Example 1

[0046] According to the component amounts in Table 1 (based on the molar percentage of reactive functional groups): cyclohexane-1,2-dicarboxylic acid diglycidyl ester 100%, amino-terminated polydimethylsiloxane 25%, tetraethylenepentamine 75%;

[0047] (1) Synthesis of nanophase epoxy Vitrimer: Cyclohexane-1,2-dicarboxylic acid diglycidyl ester was mixed with amino-terminated polydimethylsiloxane and reacted at 80℃ for 3 h to obtain a homogeneous prepolymer. Tetraethylenepentamine was added, and the mixture was stirred in an ice-water bath for 20 min. It was then vacuum mixed in a vacuum degassing machine for 20 min, cured at room temperature for 24 h, and cured at 80-100℃ for 48 h to obtain a mixture with uneven phase separation.

[0048] (2) Synthesis of submicron phase epoxy Vitrimer: Polydimethylsiloxane and tetraethylenepentamine were mixed at room temperature for 25 min, then cyclohexane-1,2-dicarboxylic acid diglycidyl ester was added, stirred at room temperature for 20 min, vacuum mixed in a vacuum degassing machine for 20 min, cured at room temperature for 24 h, and cured at 80℃ for 48 h to obtain a mixture of submicron phases.

[0049] (3) Synthesis of micron-phase epoxy Vitrimer: Cyclohexane-1,2-dicarboxylic acid diglycidyl ester and tetraethylenepentamine were mixed evenly and reacted at 25°C for 30 min to obtain a prepolymer. Polydimethylsiloxane was then added, and the mixture was stirred in an ice-water bath for 20 min. It was then vacuum mixed in a vacuum degassing machine for 20 min, cured at room temperature for 24 h, and cured at 80°C for 48 h to obtain a micron-phase mixture.

[0050] Comparative Example 2

[0051] According to the component amounts in Table 1 (based on the molar percentage of the reactive functional groups): resorcinol bisglycidyl ether 100%, amino-terminated polydimethylsiloxane 25%, tetraethylenepentamine 75%;

[0052] (1) Synthesis of nanophase epoxy Vitrimer: Resorcinol bisglycidyl ether and polydimethylsiloxane were mixed evenly and reacted at 80℃ for 3 h to obtain a uniform prepolymer. Then tetraethylenepentamine was added, stirred in an ice-water bath for 20 min, vacuum mixed in a vacuum degassing machine for 20 min, cured at room temperature for 24 h, and cured at 80-100℃ for 48 h to obtain a mixture of nanophases.

[0053] (2) Synthesis of submicron phase epoxy Vitrimer: Polydimethylsiloxane and tetraethylenepentamine were mixed at room temperature for 20 min, then resorcinol bisglycidyl ether was added, stirred at room temperature for 20 min, vacuum mixed in a vacuum degassing machine for 20 min, cured at room temperature for 24 h, and cured at 80℃ for 48 h to obtain a mixture of submicron phases.

[0054] (3) Synthesis of micron-phase epoxy Vitrimer: Resorcinol diglycidyl ether and tetraethylenepentamine were mixed evenly and reacted at 25°C for 30 min to obtain a prepolymer. Polydimethylsiloxane was then added, stirred in an ice-water bath for 20 min, vacuum mixed in a vacuum degassing machine for 20 min, cured at room temperature for 24 h, and cured at 80°C for 48 h to obtain a micron-phase mixture.

[0055] Comparative Example 3

[0056] According to the component amounts in Table 1 (based on the molar percentage of the reactive functional groups): 1,6-hexanediol diglycidyl ether 100%, p-phenylenediamine 25%, triethylenetetramine 75%;

[0057] (1) Synthesis of nanophase epoxy Vitrimer: 1,6-hexanediol diglycidyl ether and p-phenylenediamine were mixed evenly and reacted at 80℃ for 3 h to obtain a uniform prepolymer. Triethylenetetramine was then added, stirred in an ice-water bath for 20 min, vacuum mixed in a vacuum degassing machine for 20 min, cured at room temperature for 24 h, and cured at 80-100℃ for 48 h to obtain a mixture of nanophases.

[0058] (2) Synthesis of submicron phase epoxy Vitrimer: p-phenylenediamine and triethylenetetramine were mixed at room temperature for 20 min, then 1,6-hexanediol diglycidyl ether was added, stirred at room temperature for 20 min, vacuum mixed in a vacuum degassing machine for 20 min, cured at room temperature for 24 h, and cured at 80℃ for 48 h to obtain a mixture of submicron phases.

[0059] (3) Synthesis of micron-phase epoxy Vitrimer: 1,6-hexanediol diglycidyl ether and triethylenetetramine were mixed evenly and reacted at 25°C for 30 min to obtain a prepolymer. Then p-phenylenediamine was added, and the mixture was stirred in an ice-water bath for 20 min. It was then vacuum mixed in a vacuum degassing machine for 20 min, cured at room temperature for 24 h, and cured at 80°C for 48 h to obtain a micron-phase mixture.

[0060] The component amounts for each of the above embodiments are shown in Table 1 below.

[0061] Table 1. Component dosage for each embodiment (molar percentage of functional groups of each monomer, %)

[0062]

[0063] The epoxy Vitrimer materials obtained in the above embodiments were subjected to strength tests and mechanical properties tests on a universal testing machine. The results are shown in Table 2 below.

[0064] Table 2. Performance test results of epoxy Vitrimer materials prepared in each embodiment.

[0065]

[0066] As shown in Table 2, the highly reactive short-chain tetraethylenepentamine preferentially crosslinks with epoxy resin, making it difficult for long-chain amines to enter the system, resulting in poor compatibility and the formation of macroscopically separated submicron and micron phases. Macroscopic phase separation leads to a clear interface between the two phases but weak bonding forces. Dynamic bonds are excessively concentrated in one phase, potentially becoming brittle fracture points due to a lack of dynamic bonds. Under external forces, interface slippage or debonding easily occurs, significantly reducing mechanical properties. In contrast, a homogeneous structure without significant phase separation dramatically increases the interfacial area between the two phases, and the molecular chains at the interface are more tightly entangled. Stress can be efficiently transferred through chemical bonds / van der Waals forces. The movement of polymer chain segments within the micro-region is geometrically constrained, increasing the orientation and packing density of the molecular chains, thereby enhancing local modulus and strength.

[0067] The epoxy Vitrimer materials prepared in the above embodiments and comparative examples were tested on a fluorescence spectrophotometer, and the results are shown in Table 3 below.

[0068] Table 3. Fluorescence performance test results of epoxy Vitrimer materials prepared in each example.

[0069]

[0070] As shown in Table 3, in island structures (especially when the island phase size is large, such as submicron or micron), phase separation may lead to the enrichment of fluorophores in specific phase regions (such as island phases or continuous phases). This spatial confinement effect and the influence of phase region size on light scattering / reflection can enhance aggregation-induced emission, thereby significantly improving the fluorescence intensity of the material. The fluorescence intensity of the submicron island structure in Comparative Example 3 is as high as 7603, far exceeding that of its corresponding homogeneous structure (4464). It should be noted that the specific value of fluorescence intensity is also significantly affected by the luminescent properties of the monomers themselves.

[0071] The above description is merely a preferred embodiment of the present invention, but the scope of protection of the present invention is not limited thereto. Any equivalent substitutions or modifications made by those skilled in the art within the scope of the technology disclosed in the present invention, based on the technical solution and inventive concept of the present invention, should be covered within the scope of protection of the present invention.

Claims

1. An epoxy Vitrimer material directionally controlled by phase separation engineering, characterized in that: Phase-separated materials with homogeneous or island-like structures are formed by polymerization-induced microphase separation of binary epoxy monomers and amine monomers. The binary epoxy monomers comprise 100% epoxy functional groups, with a molar ratio of 1:1 between the total amount of amino functional groups and the total amount of epoxy functional groups. The amine monomers include binary amine monomers and polyamine monomers, wherein the amino functional groups provided by the binary amine monomers account for 25% to 75% of the total amount of amino functional groups, and the remainder is provided by the polyamine monomers. When the island structure is formed, the high crosslinking density regions formed by the polyamine monomers constitute the island phase, and the regions formed by the binary amine monomers constitute the continuous phase.

2. The epoxy Vitrimer material directionally controlled by phase separation engineering according to claim 1, characterized in that: The binary epoxy monomer is at least one of cyclohexane-1,2-dicarboxylic acid diglycidyl ester, resorcinol diglycidyl ether, 1,6-hexanediol diglycidyl ether, and epoxy-terminated polydimethylsiloxane.

3. The epoxy Vitrimer material directionally controlled by phase separation engineering according to claim 1, characterized in that: The diamine monomer is at least one of polyetheramine, amino-terminated polydimethylsiloxane, 1,4-cyclohexanediamine, and p-phenylenediamine.

4. The epoxy Vitrimer material directionally controlled by phase separation engineering according to claim 1, characterized in that: The polyamine monomer is at least one of tetraethylenepentamine, triethylenetetramine, and tri(2-aminoethyl)amine.

5. A method for preparing epoxy Vitrimer materials as described in any one of claims 1 to 4, characterized in that, Oriented construction of phase structures is achieved through monomer addition sequence and temperature control, including any of the following steps: S1. Synthesis to form a homogeneous structure: The binary epoxy monomer and the diamine monomer are mixed evenly and reacted at 80~100 ℃ for 2~4 h to obtain the prepolymer; after adding the polyamine monomer, the mixture is stirred in an ice-water bath for 15~30 min, mixed evenly, and then degassed under vacuum for 10~30 min; cured at room temperature for 24~48 h, and then cured at 80~100 ℃ for 24~48 h to obtain the homogeneous epoxy Vitrimer material; S2. Synthesis of epoxy Vitrimer material with island structure and submicron island size: Diamine monomers and polyamine monomers are mixed at room temperature for 25-30 min, then the diepoxide monomer is added and stirred at room temperature for 20-30 min. After mixing evenly, vacuum degassing is performed for 10-30 min. The mixture is then cured at room temperature for 24-48 h, and then cured at 80-100℃ for 24-48 h to obtain epoxy Vitrimer material with island structure and submicron island size. S3. Synthesis of epoxy Vitrimer material with island structure and island phase size in the micrometer range: Binary epoxy monomers and polyamine monomers are mixed and reacted at 25~30℃ for 20~30 min to obtain a prepolymer; after adding the diamine monomer, the mixture is stirred in an ice-water bath for 15~30 min, and after mixing evenly, it is degassed under vacuum for 10~30 min; it is cured at room temperature for 24~48 h, and then cured at 80~100℃ for 24~48 h to obtain epoxy Vitrimer material with island structure and island phase size in the micrometer range.

6. The application of epoxy Vitrimer materials directionally controlled by phase separation engineering according to any one of claims 1 to 4 in optoelectronic device packaging.

7. The application of epoxy vitrimer material directionally controlled by phase separation engineering according to claim 6 in optoelectronic device packaging, characterized in that: The optoelectronic device is packaged as an LED lamp package.