A mesoscale phase-separated, tough gel material and its preparation method

Abstract

This invention discloses a mesoscale phase-separated, tough gel material, belonging to the field of functional polymer materials technology. The mesoscale phase-separated, tough gel material comprises island phase structures with sizes ranging from 0.1 to 5 micrometers and a continuous marine phase structure. The island phase structure is obtained by crosslinking a copolymer of a hydrophilic monomer and a pyridine-based organic ligand with metal ions, while the marine phase structure is polyurethane. Based on the island structure, the mesoscale phase-separated gel material exhibits abundant metal coordination and hydrogen bonding, giving the gel excellent resistance to loads and energy dissipation, and providing high tensile strength. This invention also discloses a method for preparing the above-mentioned mesoscale phase-separated, tough gel material. The method involves physical blending and solvent evaporation to prepare the mesoscale phase-separated, tough gel material. The synthesis operation is simple and has broad application prospects in flexible wearable devices, soft actuators, and artificial muscles.

Description

Technical Field

[0001] This invention belongs to the field of functional polymer materials technology, specifically relating to a mesoscale phase-separated strong and tough gel material and its preparation method. Background Technology

[0002] Hydrogels have significant applications in biomedicine, flexible electronics, and other fields. Many of these applications require hydrogels to withstand mechanical loads and resist fracture under static or cyclic loading conditions. To improve the fracture energy of these materials, various strategies have been developed and employed to enhance the mechanical properties of hydrogels, including: 1. Topological design, such as slip ring gels; 2. Introducing sacrificial bonds for energy dissipation, such as dual-network hydrogels; 3. Introducing higher-order structures, such as microphase separation structures and nanocrystalline domains. Among these, the microphase separation method effectively combines the advantages of both materials while introducing energy dissipation units, further improving the strength and fracture energy of the gel material. Therefore, the development of microphase separation methods is expected to play a positive role in improving the mechanical strength and fracture toughness of gels.

[0003] Phase separation is formed by the local aggregation of molecular chain segments. Block or random copolymers can stably produce bicontinuous phase-separated structures in the 5 nm to 100 nm range. For example, polyampholyte hydrogels formed by polymer-dense and sparse regions have achieved improved fatigue resistance. However, this nanoscale (microscale) phase separation cannot produce robust structures at scales much larger than the polymer itself. Furthermore, they face limitations in synthesis and polymer type. Phase-separated materials prepared by blending different polymers exhibit poor compatibility due to differences in the physical or chemical properties of the polymers, resulting in phase separation at the tens of micrometer scale. This macroscopic phase separation impairs the uniformity of the gel material's microstructure, hindering the improvement of mechanical properties.

[0004] Mesoscale phase-separated structures, ranging from hundreds of nanometers to several micrometers, can be more uniformly dispersed in materials, and their similar molecular structures promote the formation of a denser and more robust phase structure. This robust phase-separated structure provides the material with the ability to withstand loads and prevents crack initiation and propagation, thereby improving the material's fracture toughness. However, due to limitations in preparation methods, research on mesoscale phase-separated hydrogels remains lacking. Controlling the characteristic length scale of phase separation to prepare mesoscale phase-separated hydrogels is a current challenge.

[0005] Researchers have developed a variety of methods for preparing strong and tough hydrogels in the existing technology, and a relatively solid foundation has been established in the research of strong and tough integrated gel materials.

[0006] For example, the invention application with publication number CN118515902A discloses a tough composite hydrogel film, its preparation method and its application. The method uses biocompatible, biodegradable and non-toxic polyvinyl alcohol (PVA) and montmorillonite (MMT) as component units, and prepares a tough polyvinyl alcohol / montmorillonite (PVA / MMT) hydrogel through evaporation self-assembly technology. This composite hydrogel exhibits excellent mechanical properties and solves the problem of insufficient mechanical properties of tough hydrogels in the prior art.

[0007] For example, invention application CN116925392A discloses a microphase-separated, tough hydrogel with excellent anti-swelling properties and its preparation method. By employing a solvent exchange-assisted microphase separation strategy, polyvinyl alcohol (PVA) and polyurethane (PU) are first dissolved in dimethyl sulfoxide (DMSO) to form a mixed solution. Then, through solvent exchange, DMSO is replaced by water, resulting in gelation. During gelation, PVA macromolecules aggregate and undergo physical cross-linking, while PU macromolecules undergo phase separation to form microspheres. These microspheres are uniformly distributed within the hydrogel and have strong hydrogen-bonded interactions with PVA. Phase separation increases the crystallinity of PVA, reduces the distance between adjacent crystal domains, and the rigid and stretchable PU microspheres and high crystallinity effectively improve the mechanical properties of the hydrogel. This invention has a simple preparation method, and the resulting hydrogel exhibits excellent mechanical properties, anti-swelling properties, and biocompatibility.

[0008] However, there are currently very few strong and tough gel materials prepared based on mesoscale phase separation, which makes it difficult to meet the needs of further practical applications. Summary of the Invention

[0009] To address the problems existing in the prior art, this invention proposes a mesoscale phase-separated, tough gel material and its preparation method. A polymer film with a mesoscale phase-separated structure is obtained through physical blending and solvent evaporation, and further coordination crosslinking with metal ions yields a mesoscale phase-separated gel material with excellent mechanical properties.

[0010] A mesoscale phase-separated, tough gel material comprising island phase structures with a size of 0.1–5 micrometers and a continuous marine phase structure;

[0011] The island phase structure is obtained by crosslinking of hydrophilic monomers and pyridine organic ligands with metal ions; the marine phase structure is polyurethane.

[0012] This invention is based on the formation of hydrophilic polymers from hydrophilic monomers and pyridine chelate ligand monomers. Metal ions exhibit excellent coordination ability with the hydrophilic polymers, and the strongly coordinated compounds formed through cross-linking exhibit island-phase structures with a size of 0.1–5 micrometers. These island-phase structures are uniformly distributed within a continuous marine structure, forming an island-like structure. The continuous marine structure contains abundant hydrogen bonding interactions, providing the gel material with high tensile strength and energy dissipation capacity. The metal coordination and hydrogen bonding interactions within the island-phase structure give the gel excellent resistance to loads and energy dissipation, resulting in superior mechanical properties for this mesoscale phase-separated, tough gel material.

[0013] Preferably, the mesoscale phase-separated, tough gel material exhibits a tensile strength of not less than 2.5 MPa and a toughness of not less than 20 MJ / m during stretching. 3 The fracture energy is not less than 5 kJ / m. 2 .

[0014] This invention also provides a method for preparing a mesoscale phase-separated, strong, and tough gel material, comprising the following steps:

[0015] (1) Dissolve pyridine chelating ligand monomers, sodium hydroxide, hydrophilic monomers and initiators in deionized water, and then prepare hydrophilic copolymers by thermally initiated free radical polymerization;

[0016] (2) Dissolve the hydrophilic copolymer in deionized water and stir until homogeneous to obtain precursor solution 1. Dissolve the polyurethane in an organic solution and stir until homogeneous to obtain precursor solution 2.

[0017] (3) Mix precursor solution 1 and precursor solution 2, stir until homogeneous to obtain a mixed solution, and then obtain a polymer film by solvent evaporation.

[0018] (4) Immerse the polymer film from step (3) in a solution containing metal ions to obtain a polymer hydrogel with mesoscale phase separation.

[0019] In the preparation process, a hydrophilic copolymer precursor solution and a polyurethane precursor solution are mixed, and a polymer film is obtained by solvent evaporation. Then, crosslinking with metal ions will form an island phase structure with a size of 0.1 to 5 micrometers. The final polymer hydrogel exhibits an island structure. When the tip stress is transmitted to the island phase structure, the propagation of cracks can be effectively prevented. This mesoscale phase separation is the main reason why the gel material has high tensile strength, toughness and fracture toughness.

[0020] Sodium hydroxide forms salts or ionic compounds with pyridine chelating ligand monomers, increasing the solubility of the chelating ligand monomers. In addition, it undergoes thermally initiated free radical polymerization with hydrophilic monomers to obtain hydrophilic copolymers. The chelating ligands in the copolymers can complex with metal ions, which can improve the strength and stability of the gel band.

[0021] Preferably, the pyridine chelating ligand monomer is at least one selected from ureapyridine carboxylic acid, ureapyridine carboxylic acid ester, and pyridine carboxylic acid;

[0022] The hydrophilic monomer is at least one of acrylamide and acrylic acid.

[0023] Preferably, the molar ratio of the pyridine chelating ligand monomer to the hydrophilic monomer is 1 to 4:100.

[0024] More preferably, the molar ratio of the pyridine chelating ligand monomer to the hydrophilic monomer is 1 to 2:100.

[0025] Preferably, the initiator is ammonium persulfate or potassium persulfate.

[0026] By selecting a suitable initiator, free radicals can be induced to promote the polymerization reaction of monomer molecules, resulting in linear hydrophilic copolymers.

[0027] More preferably, in step (1), the initiator accounts for 1% to 2% of the mass percentage of the pyridine chelating ligand monomer, sodium hydroxide, hydrophilic monomer, and initiator.

[0028] In the preparation of gel materials, the content of initiator affects the degree of polymerization of polymers. Selecting initiators within the above-mentioned range for copolymer preparation can give hydrophilic copolymers suitable length and molecular weight.

[0029] Preferably, the thermally initiated free radical polymerization is carried out using an oil bath heating method, wherein the oil bath heating temperature is 60℃~80℃ and the oil bath heating time is at least 2 hours.

[0030] By selecting oil bath heating and controlling the variables of temperature and time, monomers are excited into monomer free radicals, which promotes the formation of hydrophilic copolymers.

[0031] Preferably, the hydrophilic copolymer accounts for 5% to 15% of the mass percentage of the hydrophilic copolymer and polyurethane.

[0032] Optionally, in steps (2) and (3), the stirring temperature is room temperature and the stirring time is at least 12 hours.

[0033] By adjusting the stirring time, the various solutes are mixed evenly in the solvent, which is then used to obtain polymer films via solvent evaporation.

[0034] Optionally, in step (2), the organic solution is a mixed solution of ethanol and deionized water, wherein the volume ratio of ethanol to water is 19:1.

[0035] Preferably, the solvent evaporation method includes pouring the uniformly stirred solution into a polytetrafluoroethylene mold, evaporating the solvent at room temperature to obtain a polymer film; wherein the solvent evaporation time at room temperature is at least 72 hours.

[0036] The solvent evaporation method evaporates water and organic solvents from the solvent, making the solution supersaturated. This provides sufficient driving force for the growth of polymer films. By adjusting the reaction time under constant temperature conditions to control the evaporation rate and thus the supersaturation of the solution, the resulting polymer film has uniform composition and a stable growth process, which can improve the stability of the gel material.

[0037] Preferably, the metal ion is at least one selected from zirconium ions, europium ions, terbium ions, and zinc ions.

[0038] More preferably, the concentration of the metal ions is 0.1 mol / L to 1 mol / L.

[0039] The present invention also provides the application of the mesoscale phase-separated tough gel material prepared by the above preparation method in flexible wearable devices, soft actuators and artificial muscles.

[0040] Compared with the prior art, the beneficial effects of the present invention are as follows:

[0041] (1) The continuous marine structure provides the gel material with high tensile strength and energy dissipation capacity. When the stretching degree is further increased, the island structure will deform accordingly, improving the tensile properties and toughness of the gel material.

[0042] (2) Island phase structures with a size of 0.1 to 5 micrometers are uniformly distributed in the continuous marine phase structure. The island phase structure has excellent resistance to load and energy dissipation. When the tip stress is transmitted to the island phase structure, the crack propagation can be effectively prevented, which makes this mesoscale phase-separated gel material have high fracture energy.

[0043] (3) The present invention uses physical blending and solvent evaporation to prepare mesoscale phase separation tough gel materials, and the synthesis operation is simple.

[0044] (4) The mesoscale phase separation tough gel material provided by the present invention has broad application prospects in the fields of flexible wearable devices, soft actuators and artificial muscles. Attached Figure Description

[0045] Figure 1This is a schematic diagram of the internal structure of the mesoscale phase-separated tough gel material.

[0046] Figure 2 This is a scanning electron microscope image of the mesoscale phase-separated, tough gel material.

[0047] Figure 3 This is an optical image of a mesoscale phase-separated, tough gel material prepared in Example 1 lifting a weight.

[0048] Figure 4 The stress-strain curves of a mesoscale phase-separated, tough gel material during the tensile process.

[0049] Figure 5 Optical photographs of a notched, mesoscale phase-separated, tough gel material during the stretching process.

[0050] Figure 6 A schematic diagram of the mechanism for high fracture energy in mesoscale phase-separated tough gel materials. Detailed Implementation

[0051] To make the objectives, technical solutions, and advantages of this invention clearer, the invention will be further described and illustrated below with reference to examples. It should be understood that the specific embodiments described herein are for illustrative purposes only and are not intended to limit the invention. Operating methods not specifically specified in the following embodiments are generally performed under conventional conditions or as recommended by the manufacturer. The polyurethane used in the embodiments was purchased from AdvanSource Biomaterials, model HydroMed D3.

[0052] A schematic diagram of the structure of the mesoscale phase-separated material prepared in the examples is shown below. Figure 1 As shown.

[0053] Example 1

[0054] A method for preparing a mesoscale phase-separated, tough gel material includes the following steps:

[0055] (1) First, 0.2g of ureopyridine carboxylic acid monomer, 0.109g of sodium hydroxide, 4.8g of acrylamide and 0.1g of ammonium persulfate were dissolved in 50mL of deionized water and reacted in an oil bath at 70℃ for 5h to obtain a hydrophilic copolymer.

[0056] (2) Dissolve 0.1g of hydrophilic copolymer in 5.4mL of deionized water and stir at room temperature for 12h to obtain precursor solution 1; dissolve 0.9g of polyurethane in an organic solution consisting of 0.3mL of deionized water and 5.7mL of ethanol and stir at room temperature for 12h to obtain precursor solution 2.

[0057] (3) Mix the precursor solution 1 and precursor solution 2 prepared in step 2 and continue stirring for 12 hours to obtain a mixed solution.

[0058] (4) The mixed solution prepared in step (3) is dripped into a polytetrafluoroethylene mold (6×6cm) using a dropper. After the solvent evaporates at room temperature for 72 hours, a polymer film is obtained.

[0059] (5) Immerse the polymer film in a 0.1 mol / L zirconium tetrachloride solution for 15 min, and then transfer it to deionized water to remove free zirconium ions, thereby obtaining a phase-separated polymer hydrogel.

[0060] The phase-separated polymer hydrogel prepared in this embodiment has a mesoscale ocean-island phase separation structure, such as... Figure 2 As shown in the image. It is also capable of lifting objects weighing over 6000 times its own weight, such as... Figure 3 As shown in the figure. The hydrogel in Example 1 has a tensile strength of 3.3 MPa and a toughness of 28.8 MJ / m. -3 ,like Figure 3 As shown in the image. Optical photographs of the notched sample during the stretching process. Figure 5 As shown, the fracture energy is 13.7 kJ / m. -2 .

[0061] Example 2

[0062] The preparation steps of Example 2 are the same as those of Example 1, except that the molar ratio of pyridine chelating ligand and hydrophilic monomer is changed from 1:100 to 2:100. Specifically, 0.4g of ureidopyridine carboxylic acid monomer, 0.218g of sodium hydroxide, 4.8g of acrylamide and 0.1g of ammonium persulfate are dissolved in 50mL of deionized water.

[0063] Example 3

[0064] The preparation steps of Example 3 are the same as those of Example 1, except that the molar ratio of pyridine chelating ligand and hydrophilic monomer is changed from 1:100 to 4:100. Specifically, 0.8g of ureidopyridine carboxylic acid monomer, 0.436g of sodium hydroxide, 4.8g of acrylamide, and 0.1g of ammonium persulfate are dissolved in 50mL of deionized water.

[0065] Example 4

[0066] The preparation steps of Example 4 are the same as those of Example 1, except that the mass percentage of the hydrophilic copolymer in the polymer composed of the hydrophilic copolymer and polyurethane is changed from 10% to 5%. Specifically, 0.05g of hydrophilic copolymer is dissolved in 5.4mL of deionized water and stirred at room temperature for 12h to obtain precursor solution 1; 0.95g of polyurethane is added to a mixed solvent of 0.3mL of deionized water and 5.7mL of ethanol and stirred at room temperature for 12h to obtain precursor solution 2.

[0067] Example 5

[0068] The preparation steps of Example 5 are the same as those of Example 1, except that the mass percentage of the hydrophilic copolymer in all polymer components is changed from 10% to 15%. Specifically, 0.15g of the hydrophilic copolymer is dissolved in 5.4mL of deionized water and stirred at room temperature for 12h; 0.85g of polyurethane is added to a mixed solvent of 0.3mL of deionized water and 5.7mL of ethanol and stirred at room temperature for 12h.

[0069] Example 6

[0070] The preparation steps of Example 6 are the same as those of Example 1, except that the metal ions are changed from zirconium ions to europium ions. Specifically, the polymer film is immersed in a 0.1M europium nitrate solution for 15 minutes, and then transferred to deionized water to remove free europium ions, resulting in a phase-separated polymer hydrogel.

[0071] Example 7

[0072] The preparation steps of Example 7 are the same as those of Example 1, except that the metal ions are changed from zirconium ions to terbium ions. Specifically, the polymer film is immersed in a 0.1M terbium nitrate solution for 15 minutes, and then transferred to deionized water to remove free terbium ions, thereby obtaining a phase-separated polymer hydrogel.

[0073] Example 8

[0074] The preparation steps of Example 8 are the same as those of Example 1, except that the hydrophilic monomer is changed from acrylamide to acrylic acid. Specifically, 0.2g of ureidopyridine carboxylic acid monomer, 0.109g of sodium hydroxide, 4.9g of acrylic acid and 0.1g of ammonium persulfate are dissolved in 50mL of deionized water and reacted in an oil bath at 70°C for 5h to obtain a hydrophilic copolymer.

[0075] Example 9

[0076] The preparation steps of Example 9 are the same as those of Example 1, except that the pyridine chelating ligand monomer is changed from ureidopyridine carboxylic acid monomer to pyridine carboxylic acid monomer. Specifically, 0.13g of pyridine carboxylic acid monomer, 0.109g of sodium hydroxide, 4.8g of acrylamide and 0.1g of ammonium persulfate are dissolved in 50mL of deionized water and reacted in an oil bath at 70℃ for 5h to obtain a hydrophilic copolymer.

[0077] Example 10

[0078] The preparation steps of Example 10 are the same as those of Example 1, except that the metal ion concentration is changed from 0.1 mol / L to 0.5 mol / L. Specifically, the polymer film is immersed in a 0.5 mol / L zirconium tetrachloride solution for 15 min, and then transferred to deionized water to remove free zirconium ions, thereby obtaining a phase-separated polymer hydrogel.

[0079] Example 11

[0080] The preparation steps of Example 11 are the same as those of Example 1, except that the metal ion concentration is changed from 0.1 mol / L to 1 mol / L. Specifically, the polymer film is immersed in a 1 mol / L zirconium tetrachloride solution for 15 min, and then transferred to deionized water to remove free zirconium ions, thereby obtaining a phase-separated polymer hydrogel.

[0081] Comparative Example 1

[0082] The preparation steps of Comparative Example 1 are the same as those of Example 1, except that the mass percentage of the hydrophilic copolymer in the polymer composed of the hydrophilic copolymer and polyurethane is changed from 10% to 20%. Specifically, 0.2 g of the hydrophilic copolymer is dissolved in 5.4 mL of deionized water and stirred at room temperature for 12 h to obtain precursor solution 1; 0.8 g of polyurethane is dissolved in an organic solution composed of 0.3 mL of deionized water and 5.7 mL of ethanol and stirred at room temperature for 12 h to obtain precursor solution 2.

[0083] Comparative Example 2

[0084] The preparation steps of Comparative Example 2 are the same as those of Example 1, except that the mass percentage of the hydrophilic copolymer in the polymer composed of the hydrophilic copolymer and polyurethane is changed from 10% to 30%. Specifically, 0.3g of the hydrophilic copolymer is dissolved in 5.4mL of deionized water and stirred at room temperature for 12h to obtain precursor solution 1; 0.7g of polyurethane is dissolved in an organic solution composed of 0.3mL of deionized water and 5.7mL of ethanol and stirred at room temperature for 12h to obtain precursor solution 2.

[0085] Comparative Example 3

[0086] The preparation steps of Comparative Example 3 are the same as those of Example 1, except that the polymer film is immersed in deionized water to reach swelling equilibrium, resulting in a phase-separated polymer hydrogel.

[0087] Detection Example 1

[0088] like Figure 3 , Figure 4 and Figure 5 As shown, the mechanical properties of the phase-separated polymer hydrogels prepared in each embodiment and comparative example were tested by stress-strain curves from weight lifting and tensile tests and notched sample tensile tests. Table 1 shows the results of tensile strength, toughness and fracture energy of each embodiment and comparative example.

[0089] Table 1

[0090]

[0091]

[0092] The results show that the mesoscale phase-separated strong and tough gel material has the characteristics of high tensile strength, high toughness and high fracture toughness, with a tensile strength of not less than 2.5 MPa and a toughness of not less than 20 MJ / m. -3 The fracture energy is not less than 5 kJ / m. -2 .

[0093] This mesoscale phase-separated gel material, with its high tensile strength and high toughness, exhibits excellent tensile properties and toughness when subjected to external tensile forces. The polyurethane-based marine phase provides high tensile strength and energy dissipation capacity due to the abundant hydrogen bond interactions within it. As the degree of stretching increases further, the island phase structure deforms accordingly, which also provides toughness to the material. Therefore, this mesoscale phase-separated tough gel material exhibits excellent tensile properties and toughness.

[0094] like Figure 6 As shown, based on these excellent mechanical properties, a schematic diagram of the corresponding fracture toughness mechanism is given. When the notched material is subjected to tension, the mesoscale island phase structure is uniformly distributed in the marine phase structure. The metal coordination and hydrogen bonding in the island phase structure give it excellent resistance to load and energy dissipation. Therefore, when the tip stress is transmitted to the island phase structure, the crack propagation can be effectively prevented, making this mesoscale phase-separated gel material have high fracture energy.

Claims

1. A mesoscale phase-separated, strong, and tough gel material, characterized in that, This includes island-like structures ranging in size from 0.1 to 5 micrometers and continuous marine structures; The island-phase structure is obtained by crosslinking of hydrophilic monomers and pyridine organic ligands with metal ions. The marine structure is polyurethane; The method for preparing the mesoscale phase-separated, tough gel material includes the following steps: (1) Dissolve pyridine chelating ligand monomers, sodium hydroxide, hydrophilic monomers and initiators in deionized water, and then prepare hydrophilic copolymers by thermally initiated free radical polymerization; (2) Dissolve the hydrophilic copolymer in deionized water and stir until homogeneous to obtain precursor solution 1. Dissolve the polyurethane in an organic solution and stir until homogeneous to obtain precursor solution 2. (3) Mix precursor solution 1 and precursor solution 2, stir until homogeneous to obtain a mixed solution, and then obtain a polymer film by solvent evaporation. (4) Immerse the polymer film from step (3) in a solution containing metal ions to obtain a polymer hydrogel with mesoscale phase separation; The pyridine chelating ligand monomer is at least one of ureapyridine carboxylic acid, ureapyridine carboxylic acid ester, and pyridine carboxylic acid. The hydrophilic monomer is at least one of acrylamide and acrylic acid; The mass percentage of the hydrophilic copolymer in the hydrophilic copolymer and polyurethane is 5% to 15%.

2. The mesoscale phase-separated, tough gel material according to claim 1, characterized in that, The aforementioned mesoscale phase-separated, tough gel material exhibits a tensile strength of not less than 2.5 MPa and a toughness of not less than 20 MJ / m during stretching. -3 The fracture energy is not less than 5 kJ / m. -2 .

3. The method for preparing the mesoscale phase-separated, strong and tough gel material according to claim 1, characterized in that, Includes the following steps: (1) Dissolve pyridine chelating ligand monomers, sodium hydroxide, hydrophilic monomers and initiators in deionized water, and then prepare hydrophilic copolymers by thermally initiated free radical polymerization; (2) Dissolve the hydrophilic copolymer in deionized water and stir until homogeneous to obtain precursor solution 1. Dissolve the polyurethane in an organic solution and stir until homogeneous to obtain precursor solution 2. (3) Mix precursor solution 1 and precursor solution 2, stir until homogeneous to obtain a mixed solution, and then obtain a polymer film by solvent evaporation. (4) Immerse the polymer film from step (3) in a solution containing metal ions to obtain a polymer hydrogel with mesoscale phase separation; The pyridine chelating ligand monomer is at least one of ureapyridine carboxylic acid, ureapyridine carboxylic acid ester, and pyridine carboxylic acid. The hydrophilic monomer is at least one of acrylamide and acrylic acid; The mass percentage of the hydrophilic copolymer in the hydrophilic copolymer and polyurethane is 5% to 15%.

4. The method for preparing the mesoscale phase-separated, strong and tough gel material according to claim 3, characterized in that, The molar ratio of the pyridine chelating ligand monomer to the hydrophilic monomer is 1~4:

100.

5. The method for preparing the mesoscale phase-separated, strong and tough gel material according to claim 3, characterized in that, The initiator is ammonium persulfate or potassium persulfate, and the initiator accounts for 1% to 2% of the mass percentage of the pyridine chelating ligand monomer, sodium hydroxide, hydrophilic monomer and initiator.

6. The method for preparing the mesoscale phase-separated, strong and tough gel material according to claim 3, characterized in that, The thermally initiated free radical polymerization is carried out using an oil bath heating method, wherein the oil bath heating temperature is 60 ℃~80 ℃ and the oil bath heating time is at least 2 h.

7. The method for preparing the mesoscale phase-separated, strong and tough gel material according to claim 3, characterized in that, The solvent evaporation method includes pouring a well-stirred mixed solution into a polytetrafluoroethylene mold, evaporating the solvent at room temperature to obtain a polymer film; wherein the solvent evaporation time at room temperature is at least 72 h.

8. The method for preparing the mesoscale phase-separated, strong and tough gel material according to claim 3, characterized in that, The metal ion is at least one of zirconium ion, europium ion, terbium ion, and zinc ion, and the concentration of the metal ion is 0.1 mol / L to 1 mol / L.

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