CN112354019A - Preparation method of pH-driven artificial muscle flexible composite material - Google Patents

Preparation method of pH-driven artificial muscle flexible composite material Download PDF

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Publication number
CN112354019A
CN112354019A CN202011200018.8A CN202011200018A CN112354019A CN 112354019 A CN112354019 A CN 112354019A CN 202011200018 A CN202011200018 A CN 202011200018A CN 112354019 A CN112354019 A CN 112354019A
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artificial muscle
composite material
fibers
preparing
flexible composite
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CN112354019B (en
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李群
刘佳璇
张世超
何爽
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Tianjin University of Science and Technology
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Tianjin University of Science and Technology
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    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L27/00—Materials for grafts or prostheses or for coating grafts or prostheses
    • A61L27/50—Materials characterised by their function or physical properties, e.g. injectable or lubricating compositions, shape-memory materials, surface modified materials
    • A61L27/56—Porous materials, e.g. foams or sponges
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L27/00—Materials for grafts or prostheses or for coating grafts or prostheses
    • A61L27/14—Macromolecular materials
    • A61L27/18—Macromolecular materials obtained otherwise than by reactions only involving carbon-to-carbon unsaturated bonds
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L27/00—Materials for grafts or prostheses or for coating grafts or prostheses
    • A61L27/14—Macromolecular materials
    • A61L27/20—Polysaccharides
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L27/00—Materials for grafts or prostheses or for coating grafts or prostheses
    • A61L27/50—Materials characterised by their function or physical properties, e.g. injectable or lubricating compositions, shape-memory materials, surface modified materials
    • D—TEXTILES; PAPER
    • D01—NATURAL OR MAN-MADE THREADS OR FIBRES; SPINNING
    • D01D—MECHANICAL METHODS OR APPARATUS IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS
    • D01D5/00—Formation of filaments, threads, or the like
    • D01D5/0007—Electro-spinning
    • D01D5/0015—Electro-spinning characterised by the initial state of the material
    • D01D5/003—Electro-spinning characterised by the initial state of the material the material being a polymer solution or dispersion
    • D—TEXTILES; PAPER
    • D01—NATURAL OR MAN-MADE THREADS OR FIBRES; SPINNING
    • D01D—MECHANICAL METHODS OR APPARATUS IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS
    • D01D5/00—Formation of filaments, threads, or the like
    • D01D5/28—Formation of filaments, threads, or the like while mixing different spinning solutions or melts during the spinning operation; Spinnerette packs therefor
    • D01D5/30—Conjugate filaments; Spinnerette packs therefor
    • D—TEXTILES; PAPER
    • D01—NATURAL OR MAN-MADE THREADS OR FIBRES; SPINNING
    • D01F—CHEMICAL FEATURES IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS; APPARATUS SPECIALLY ADAPTED FOR THE MANUFACTURE OF CARBON FILAMENTS
    • D01F1/00—General methods for the manufacture of artificial filaments or the like
    • D01F1/02—Addition of substances to the spinning solution or to the melt
    • D01F1/10—Other agents for modifying properties
    • D—TEXTILES; PAPER
    • D01—NATURAL OR MAN-MADE THREADS OR FIBRES; SPINNING
    • D01F—CHEMICAL FEATURES IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS; APPARATUS SPECIALLY ADAPTED FOR THE MANUFACTURE OF CARBON FILAMENTS
    • D01F6/00—Monocomponent artificial filaments or the like of synthetic polymers; Manufacture thereof
    • D01F6/88—Monocomponent artificial filaments or the like of synthetic polymers; Manufacture thereof from mixtures of polycondensation products as major constituent with other polymers or low-molecular-weight compounds
    • D01F6/94—Monocomponent artificial filaments or the like of synthetic polymers; Manufacture thereof from mixtures of polycondensation products as major constituent with other polymers or low-molecular-weight compounds of other polycondensation products
    • D—TEXTILES; PAPER
    • D02—YARNS; MECHANICAL FINISHING OF YARNS OR ROPES; WARPING OR BEAMING
    • D02G—CRIMPING OR CURLING FIBRES, FILAMENTS, THREADS, OR YARNS; YARNS OR THREADS
    • D02G3/00—Yarns or threads, e.g. fancy yarns; Processes or apparatus for the production thereof, not otherwise provided for
    • D02G3/02—Yarns or threads characterised by the material or by the materials from which they are made
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L2400/00—Materials characterised by their function or physical properties
    • A61L2400/12—Nanosized materials, e.g. nanofibres, nanoparticles, nanowires, nanotubes; Nanostructured surfaces
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L2400/00—Materials characterised by their function or physical properties
    • A61L2400/16—Materials with shape-memory or superelastic properties
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
    • A61L2430/00—Materials or treatment for tissue regeneration
    • A61L2430/30—Materials or treatment for tissue regeneration for muscle reconstruction
    • D—TEXTILES; PAPER
    • D10—INDEXING SCHEME ASSOCIATED WITH SUBLASSES OF SECTION D, RELATING TO TEXTILES
    • D10B—INDEXING SCHEME ASSOCIATED WITH SUBLASSES OF SECTION D, RELATING TO TEXTILES
    • D10B2201/00—Cellulose-based fibres, e.g. vegetable fibres
    • D10B2201/20—Cellulose-derived artificial fibres
    • D10B2201/22—Cellulose-derived artificial fibres made from cellulose solutions
    • D—TEXTILES; PAPER
    • D10—INDEXING SCHEME ASSOCIATED WITH SUBLASSES OF SECTION D, RELATING TO TEXTILES
    • D10B—INDEXING SCHEME ASSOCIATED WITH SUBLASSES OF SECTION D, RELATING TO TEXTILES
    • D10B2331/00—Fibres made from polymers obtained otherwise than by reactions only involving carbon-to-carbon unsaturated bonds, e.g. polycondensation products
    • D10B2331/10—Fibres made from polymers obtained otherwise than by reactions only involving carbon-to-carbon unsaturated bonds, e.g. polycondensation products polyurethanes

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  • Health & Medical Sciences (AREA)
  • Chemical & Material Sciences (AREA)
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  • Dispersion Chemistry (AREA)
  • Manufacturing & Machinery (AREA)
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  • Yarns And Mechanical Finishing Of Yarns Or Ropes (AREA)
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Abstract

The invention provides a preparation method of a pH-driven artificial muscle flexible composite material, and belongs to the field of preparation of artificial muscle flexible materials. The method is basically characterized in that wood fibers with high beating degree and length-diameter ratio are used for phosphorylation modification to enable pH sensitive groups to be generated on the surfaces of the fibers, and the wood fibers are compounded with base material polyurethane in solutions with different pH values to generate reversible formation and disappearance of hydrogen bond networks so as to control the shape fixation and recovery of the material, and finally the artificial muscle material with pH response performance is prepared. The development of the material is to convert cheap high-strength polymer fibers into artificial muscle fibers which meet or exceed the performance of skeletal muscles of mammals, so as to provide millions of reversible contractions and over 50 percent of stretching strokes, quickly improve heavy load, improve the response speed of the artificial muscle material and reduce the application cost of the artificial muscle fibers.

Description

Preparation method of pH-driven artificial muscle flexible composite material
Spin out, spin out and feel
Technical Field
The invention belongs to the field of preparation of artificial muscle flexible composite materials, and particularly relates to a preparation method of a pH-driven artificial muscle flexible composite material taking cellulose nanofibers as a composite functional body.
Background
Artificial muscle flexible materials are a general term for a class of materials or devices that can reversibly contract, expand, bend or rotate within a member as a result of an external stimulus (e.g., pressure, voltage, current, temperature, light, humidity, magnetic force, etc.). To date, different driving methods of flexible materials (e.g., silicone rubber, shape memory alloys, dielectric elastomers, hydrogels, etc.) have been widely studied for their respective advantages. For example, light-driven artificial muscle material shows great advantage in free manipulation in a non-contact manner, and humidity-driven artificial muscle material can extract energy from ambient humidity changes to drive shape changes. However, these drives are limited and slow, and the current solution to the response speed lag is the key to the application of artificial muscle materials.
Shape Memory Polyurethane (SMPU) is a thermoplastic block high molecular polymer, the molecular backbone usually consisting of a reversible phase and a stationary phase. To achieve the shape memory effect, SMPU is designed to contain amorphous or semi-crystalline soft phase and hard segment structures. The hard segment is equivalent to a network fixed node of the material and can be a physical or chemical cross-linking, a supermolecular complex or an interpenetrating network; the soft phase is similar to a transition switch and can be a percolation network structure composed of glass transition, crystallization transition, liquid crystal transition, photosensitive groups, supermolecular units and nano fillers. The shape memory of SMPU is influenced by the type and content of hard segment, the type and relative molecular mass of soft segment, cross-linking agent, filler doping and the like. The research of the shape memory polymer of which the nano-filler is used as a change-over switch is novel and practical, but the nano-filler is mainly used in the polyurethane filling material at present by adopting direct thermal drive or indirect electromagnetic drive thermal induction and the like, and the reports on the aspect of pH drive are less.
Cellulose Nanofibers (CNF) refer to cellulose materials with a one-dimensional space of nanometer width, which are extracted from abundant plant biomass resources and are inexpensive to produce. The cellulose nanofiber has special forms, properties and functions different from those of petroleum-based or inorganic nano materials, and has an almost perfect crystal structure, wherein cellulose chains are closely arranged and have strong hydrogen bond interaction, so that the cellulose nanofiber has the characteristics of high strength, high elastic modulus (100-200 GPa) and large specific surface area (25 nm-0.2-2 mu m). In recent years, CNF has been widely used in fillers for polymer nanocomposites. Polymer nanocomposites with a percolating network of nanofibrils can be readily prepared by mixing modified cellulose nanofibrils with a polymer, the nanofibrils 'closing' the hydrogen bonding self-interaction of surface hydroxyl groups through competing hydrogen bonds with the polymer. When induced by different pH conditions, the interactions between nanofibrils and polymer are "opened up" and they combine into a percolating network. This strong interaction between the structure and the nanofibrils maximizes stress transfer and thus overall modulus.
The current problems of expandability and cost of the flexible material of the artificial muscle limit the application of the material of the artificial muscle. Therefore, the characteristics of good ductility, easy weaving, high strength, low cost and the like of natural plant fibers are utilized, the material obtains a hydrogen bond network structure capable of being reversibly formed through modification and compounding, the network structure can be rapidly formed and disappeared in different acid-base solutions, a plurality of strands of composite yarns are obtained through the electrostatic spinning of the material, highly twisted fibers can spontaneously form spiral structures, the spiral structures provide obvious telescopic driving, and therefore the pH-driven artificial muscle flexible composite material is developed, the application range of the artificial muscle material is expanded through the development of the material, and a new path is opened for the preparation of the artificial muscle material.
Disclosure of Invention
The invention mainly solves the technical problems that: aiming at the problems of slow drive responsiveness and limited drive mode of the current artificial muscle material, the pH drive type artificial muscle flexible composite material is prepared by utilizing the characteristics that natural plant fibers have high strength and large specific surface area and the high porosity is caused by nanometer or micron-sized gaps of a fiber laminated structure, and the drive performance and the response performance of the natural plant fibers can be improved. The basic characteristic is that polyurethane is used as a base material, and a huge hydrogen bond network structure can be formed between the polyurethane and the cellulose nanofiber through the composite phosphorylation modification, so that the shape of the material is driven to change under different acid-base stimulation.
The technical problem to be solved by the invention is implemented by the following technical scheme:
(1) preparation of phosphorylated modified cellulose nanofibers: adding 1-5 g of oven-dried natural fiber, 10-80 g of urea and 1-10 g of phosphoric acid into a DMF solution, heating to 125 ℃ under the protection of nitrogen, and reacting for 4 hours; filtering and washing the product with sodium hydroxide solution for 3 times; and precipitating the washed product for 3 times by using methanol, then centrifuging and dispersing to transfer the fiber from the suspension to anhydrous acetone, centrifuging and dispersing again to transfer the fiber from the anhydrous acetone to carbon tetrachloride, and freeze-drying to obtain the cellulose nanofiber after phosphorylation modification.
(2) Preparing a composite material functional body: respectively mixing 5-20 g of cellulose nano-fiber prepared in the step (1) with 45-100 g of caprolactone monomer, slowly adding 2-6 wt% of stannous octoate under the protection of nitrogen, and reacting at a certain temperature for more than 12 h; and soaking and extracting the product in dichloromethane for 48h, removing self-polymerization and unreacted monomers, and freeze-drying to obtain the functional body of the composite material.
(3) Preparing a pH driving type artificial muscle flexible composite material: adding the product obtained in the step (2) and matrix polyurethane into a DMF solution according to a certain proportion, and stirring for 6 hours at room temperature to fully disperse fibers in the polyurethane; preparing composite fibers from the solution through an electrostatic spinning device, then over-twisting 2-10 strands of unwound fiber composite materials into yarns under the constant load of 0.5N by adopting a motor, and carrying out vacuum drying at 60 ℃ for 12 hours to obtain the pH-driven artificial muscle flexible composite material.
The natural cellulose is a wood fiber material with larger length-diameter ratio and higher beating degree.
The polyurethane is a segmented thermoplastic linear copolymer, the soft segment is polyester or polyether polyol, the relative molecular mass is 1000-2000, and the content is 40-80 wt%.
In the composite material functional body, the reaction temperature for preparation is 125-140 ℃.
In the composite material, the phosphorylation modified cellulose nano-fiber: the mass ratio of the polyurethane is (1-2) to (4-5).
Compared with the prior art, the invention has the following advantages:
(1) the invention utilizes the structural characteristics of easy weaving, high strength, high porosity and the like of natural plant fibers, obtains a hydrogen bond network structure capable of being reversibly formed by modification and compounding, performs deprotonation in an acid solution to fix the temporary shape of the material, and develops a pH-driven artificial muscle flexible composite material by the property that the hydrogen bond structure is damaged to recover the shape in an alkaline solution, and the development of the material expands the application scope of artificial muscles.
(2) The invention selects polyurethane with larger elastic modulus as the substrate, and the shrinkage effect of the cellulose nano-fibrils can be followed without hindering the driving. Meanwhile, the combination of CNF and polyurethane can amplify the shrinkage and stability of the material, the shrinkage and load are high in the same time, and the shape memory performance is excellent.
(3) The cost of the artificial muscle flexible material prepared by the invention is lower. The material is mainly prepared by compounding common polyurethane and biomass resource cellulose, and has the advantages of wide raw material source, simple method and lower cost compared with other artificial muscle materials.
Detailed Description
The best mode for carrying out the invention is described in further detail below by way of specific examples.
[ example 1 ]
Respectively adding 3g of oven-dried wood fiber, 32g of urea and 5g of phosphoric acid into a 150ml of DMF solution, heating the mixture in a three-neck flask to 125 ℃, and reacting for 4 hours under the protection of nitrogen; filtering and washing the product with sodium hydroxide solution and methanol for 3 times, centrifuging, dispersing, transferring the fiber from the suspension to anhydrous acetone and carbon tetrachloride in turn, and freeze-drying to obtain the fiber. Respectively mixing 4g of phosphorylated modified cellulose nano-fiber with 45g of caprolactone monomer, slowly adding 4 wt% of stannous octoate under the protection of nitrogen, and reacting for more than 12h at a certain temperature; and soaking and extracting the product in dichloromethane for 48h, removing self-polymerization and unreacted monomers, and freeze-drying to obtain the functional body of the composite material. Adding 1g of the product and 9g of polyurethane into DMF to prepare a 10 wt% solution; stirring for 6h at room temperature to fully disperse the fibers in the polyurethane; preparing composite fibers from the solution through an electrostatic spinning device, then over-twisting 2-10 strands of unwound fiber composite materials into yarns under the constant load of 0.5N by adopting a motor, and drying the yarns in vacuum at 60 ℃ for 12 hours to obtain the pH-driven artificial muscle flexible composite material.
[ example 2 ]
The test procedure for a pH-driven artificial muscle flexible composite material prepared by the method described in the first embodiment is as follows:
soaking the material prepared by the method of the first embodiment in a solution with pH of 13 for 20 min;
stretching the material treated in the step (1) and spraying a solution with the pH value of 1;
and (3) spraying the material treated in the step (2) with a solution with the pH value of 13 again.

Claims (4)

1. A preparation method of a pH driving type artificial muscle flexible composite material is characterized by comprising the following preparation steps:
(1) preparation of phosphorylated modified cellulose nanofibers: adding 1-5 g of absolutely dry natural fibers, 8-100 g of urea and 1-10 g of phosphoric acid into a DMF solution according to a certain proportion, heating and reacting for 4 hours under the protection of nitrogen; filtering and washing the product with sodium hydroxide solution for 3 times; and precipitating the washed product for 3 times by using methanol, then centrifuging and dispersing to transfer the fiber from the suspension to anhydrous acetone, centrifuging and dispersing again to transfer the fiber from the anhydrous acetone to carbon tetrachloride, and freeze-drying to obtain the cellulose nanofiber after phosphorylation modification.
(2) Preparing a composite material functional body: respectively mixing 5-20 g of cellulose nano-fiber prepared in the step (1) with 45-100 g of caprolactone monomer, slowly adding 2-6 wt% of stannous octoate under the protection of nitrogen, and reacting at a certain temperature for more than 12 h; and soaking and extracting the product in dichloromethane for 48h, removing self-polymerization and unreacted monomers, and freeze-drying to obtain the functional body of the composite material.
(3) Preparing a pH driving type artificial muscle flexible composite material: adding the product obtained in the step (2) and matrix polyurethane into a DMF solution according to a certain proportion, and stirring for 6 hours at room temperature to fully disperse fibers in the polyurethane; preparing composite fibers from the solution through an electrostatic spinning device, then over-twisting 2-10 strands of unwound fiber composite materials into yarns under the constant load of 0.5N by adopting a motor, and carrying out vacuum drying at 60 ℃ for 12 hours to obtain the pH-driven artificial muscle flexible composite material.
2. The method for preparing pH-driven artificial muscle flexible composite material according to claim 1, wherein the natural cellulose is wood fiber material with large length-diameter ratio and high beating degree. The polyurethane is a segmented thermoplastic linear copolymer, the soft segment is polyester or polyether polyol, the relative molecular mass is 1000-2000, and the content is 40-80 wt%.
3. The method for preparing the pH-driven artificial muscle flexible composite material as claimed in claim 1, wherein the reaction temperature for preparing the composite functional body is 125-140 ℃.
4. The method for preparing the pH-driven artificial muscle flexible composite material as claimed in claim 1, wherein the mass ratio of the phosphorylated modified cellulose nanofibers to the polyurethane is (1-2) to (4-5).
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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113073394A (en) * 2021-03-29 2021-07-06 浙江理工大学 Thermal driving type twisted artificial muscle composite fiber and preparation method thereof
CN114263038A (en) * 2021-12-16 2022-04-01 常州大学 Preparation method of PH response artificial muscle with carbon fiber as substrate
CN115737911A (en) * 2022-12-16 2023-03-07 华南理工大学 High-toughness bone repair composite material and preparation method thereof

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN105440296A (en) * 2015-01-14 2016-03-30 湖南工业大学 High-strength cellulose-based nanocomposite temperature and pH dual stimuli-responsive gel and preparation method thereof
CN109826015A (en) * 2019-01-30 2019-05-31 广西大学 Temperature sensitive/pH the double-bang firecracker of one kind answers intelligent nano fibrous material and its preparation method and application

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN105440296A (en) * 2015-01-14 2016-03-30 湖南工业大学 High-strength cellulose-based nanocomposite temperature and pH dual stimuli-responsive gel and preparation method thereof
CN109826015A (en) * 2019-01-30 2019-05-31 广西大学 Temperature sensitive/pH the double-bang firecracker of one kind answers intelligent nano fibrous material and its preparation method and application

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113073394A (en) * 2021-03-29 2021-07-06 浙江理工大学 Thermal driving type twisted artificial muscle composite fiber and preparation method thereof
CN113073394B (en) * 2021-03-29 2022-03-18 浙江理工大学 Thermal driving type twisted artificial muscle composite fiber and preparation method thereof
CN114263038A (en) * 2021-12-16 2022-04-01 常州大学 Preparation method of PH response artificial muscle with carbon fiber as substrate
CN114263038B (en) * 2021-12-16 2024-05-28 常州大学 Preparation method of PH response artificial muscle with carbon fiber as substrate
CN115737911A (en) * 2022-12-16 2023-03-07 华南理工大学 High-toughness bone repair composite material and preparation method thereof

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