CN113427876A - Double-network hydrogel bionic intelligent skin and preparation method thereof - Google Patents
Double-network hydrogel bionic intelligent skin and preparation method thereof Download PDFInfo
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Abstract
The invention discloses a double-network hydrogel bionic intelligent skin and a preparation method thereof. The double-network hydrogel takes a three-dimensional network structure formed by polymerizing water-soluble monomer acrylamide and chemically crosslinking as a first network structure, and polymer chain segments which can be dispersed in water, namely carboxymethyl chitosan, pass through and Ag+Three formed by cross-linking through formation of coordination bondsThe dimension network structure is a second network structure, a photoinitiator and a cross-linking agent are added into a monomer aqueous solution containing acrylamide and carboxymethyl chitosan, a polymerization reaction is carried out to prepare hydrogel, the hydrogel is soaked in a silver nitrate solution to obtain double-network hydrogel, and finally, a dielectric layer is clamped by the two layers of double-network hydrogel to form a sandwich structure, so that the bionic intelligent skin is prepared. The double-network hydrogel bionic intelligent skin has excellent stretchability and rebound resilience, has good responsiveness to fine actions and large actions of a human body, and has wide application prospects in the field of flexible electronic devices.
Description
Technical Field
The invention belongs to the technical field of bionic materials, relates to a double-network hydrogel, and particularly relates to a double-network hydrogel bionic intelligent skin and a preparation method thereof.
Background
In recent years, flexible electronic devices with bionic function have become a research hotspot. However, there are fundamental differences in the working principles between conventional electronic devices and biological systems. The carriers in conventional electronic devices are holes and electrons whose paths are limited by the effective percolation network, and therefore the electronic conductivity of the device is susceptible to geometric distortions. In contrast, information transmission in biological systems relies on long-distance transport of ions, is insensitive to deformation of the relevant system, and has stable ionic conductivity. Inspired by biological systems, ion electronics is used as an emerging interdisciplinary technology based on complex ion control, and the selection range of the next-generation artificial intelligence material is greatly expanded. The hydrogel with a three-dimensional network structure can be used as an excellent ion conductor to transmit ions in a long distance.
The bionic intelligent skin device constructed based on the hydrogel provides a way for preparing the bionic intelligent skin, but compared with natural skin, the bionic intelligent skin device still lacks matched mechanical properties. The traditional widely used polyacrylamide hydrogel has limited mechanical properties, has the defects of low modulus, limited stretchability, easy fatigue and the like, and the breaking strain of the single-network polyacrylamide is only 80% (Advanced Materials,2003,15(14), 1155-1158). The breaking strain of the polyacrylamide-dodecyl glyceryl itaconate double-network hydrogel developed on the basis is improved to 2200%, but the breaking stress is small, and in the preparation process, the problems of solubility and dispersion uniformity of an amphiphilic monomer dodecyl glyceryl itaconate in water are involved, so that the preparation process presents certain complexity and uncontrollable property, and the mechanical behavior of the related hydrogel is further influenced (Macromolecules,2011,44(22), 8916-.
Disclosure of Invention
The invention aims to provide a double-network hydrogel bionic intelligent skin which is simple and easy to prepare and has good mechanical property and a preparation method thereof.
The technical scheme for realizing the purpose of the invention is as follows:
the double-network hydrogel bionic intelligent skin takes a three-dimensional network structure formed by polymerizing water-soluble monomer acrylamide and chemically crosslinking as a first network structure, and takes a three-dimensional network structure formed by crosslinking polymer chain segments carboxymethyl chitosan which can be dispersed in water and silver ions through coordination bonds formed by the carboxymethyl chitosan and the silver ions as a second network structure. The coordination bond in the second network structure is a dynamic reversible non-covalent bond, and can be broken under the condition of large deformation to effectively dissipate external stress, so that the effect of protecting the first network structure is achieved, and the double-network hydrogel bionic intelligent skin has good stretchability and resilience.
The preparation method of the double-network hydrogel bionic intelligent skin comprises the following steps:
(1) dispersing acrylamide and carboxymethyl chitosan in water to obtain a monomer aqueous solution;
(2) adding a photoinitiator and a crosslinking agent N, N-methylene bisacrylamide into a monomer aqueous solution, and carrying out polymerization reaction to obtain hydrogel A;
(3) soaking the hydrogel A in a silver nitrate solution to obtain a double-network hydrogel;
(4) and clamping the dielectric layer by using two layers of double-network hydrogel to form a sandwich structure, thereby preparing the bionic intelligent skin.
Preferably, in the step (1), the mass concentration of the acrylamide is 7.8 wt% -17.8 wt%, and the mass concentration of the carboxymethyl chitosan is 1.1 wt% -3.1 wt%.
Preferably, in the step (2), the mass concentration of the cross-linking agent N, N-methylene bisacrylamide is 0.02 wt% to 0.04 wt%.
Preferably, in the step (2), the photoinitiator is a photoinitiator conventionally used in the art, and the mass concentration of the photoinitiator is 0.03 wt% to 0.05 wt%.
Preferably, in the step (2), the polymerization reaction is performed by ultraviolet irradiation after the addition of the photoinitiator.
Preferably, in the step (3), the mass concentration of the silver nitrate is 1.7 wt% to 14.5 wt%.
Preferably, in the step (3), the soaking time is 1 +/-0.5 h, and more preferably 1 h.
Preferably, in step (4), the dielectric layer is a dielectric layer conventionally used in the art, such as polyethylene, polypropylene or polyacrylate film.
Compared with the prior art, the invention has the following advantages:
(1) the double-network hydrogel bionic intelligent skin has good mechanical property, high tensile strength (0.243MPa) and high toughness (9.544MJ m)-3) And good stretchability at high strain (600%);
(2) the double-network hydrogel bionic intelligent skin has good stimulation-response capability, can make good response to both fine activities and large-scale human body activities, and has the capability of being reused;
(3) the double-network hydrogel bionic intelligent skin is simple in process, does not involve the use of any organic solvent, and is easy to produce in large scale.
Drawings
FIG. 1 is a schematic structural diagram of a double-network hydrogel according to the present invention;
FIG. 2 shows different Ag+The stress-strain curve of the treated double-network hydrogel with concentration;
FIG. 3 is a diagram of a double-network hydrogel bionic intelligent skin;
FIG. 4 is a response curve of a double-network hydrogel bionic intelligent skin under different stimulation conditions;
FIG. 5 is a stress-strain curve of a double-network hydrogel prepared at different soaking times.
Detailed Description
The present invention will be described in more detail with reference to the following examples and the accompanying drawings.
The preparation method of the double-network hydrogel bionic intelligent skin comprises the following steps:
(1) dispersing acrylamide and carboxymethyl chitosan in deionized water, and stirring at the rotating speed of 1000-1200 rpm at 60 ℃ until a uniform and transparent monomer aqueous solution A is obtained;
(2) adding a photoinitiator Irgacure and a crosslinking agent N, N-methylene bisacrylamide into a monomer aqueous solution, and stirring at the rotating speed of 1000-1200 rpm at 60 ℃ until a uniform and transparent solution B is obtained; injecting the solution B into a glass mold with the interval of 500-1500 mu m, and polymerizing for 5-8 hours under the irradiation of ultraviolet light to obtain hydrogel A;
(3) soaking the hydrogel A in silver nitrate solution for 1 +/-0.5 hours to obtain double-network hydrogel;
(4) and clamping the dielectric layer by two layers of double-network hydrogel to form a sandwich structure, thereby constructing the capacitive bionic intelligent skin.
Example 1
(1) Dispersing 0.6g of acrylamide and 0.1g of carboxymethyl chitosan in 4mL of deionized water, and stirring at the rotating speed of 1200rpm at the temperature of 60 ℃ until a uniform and transparent monomer aqueous solution A is obtained;
(2) adding 0.0018g of photoinitiator Irgacure and 0.0012g of cross-linking agent N, N-methylene bisacrylamide into the aqueous monomer solution, and stirring at the rotating speed of 1200rpm at 60 ℃ until a uniform and transparent solution B is obtained; injecting the solution B into a glass mold with the interval of 1000 mu m, and polymerizing for 8 hours under the irradiation of ultraviolet light to obtain hydrogel A;
(3) and soaking the hydrogel A in a silver nitrate solution with the mass concentration of 1.7 wt% for 1 hour to obtain the double-network hydrogel.
The tensile stress-strain curve of the double-network hydrogel prepared in this example is shown in CS-PAM-Ag in FIG. 2+-1.7%.
Example 2
(1) Dispersing 0.6g of acrylamide and 0.1g of carboxymethyl chitosan in 4mL of deionized water, and stirring at the rotating speed of 1200rpm at the temperature of 60 ℃ until a uniform and transparent monomer aqueous solution A is obtained;
(2) adding 0.0018g of photoinitiator Irgacure and 0.0012g of cross-linking agent N, N-methylene bisacrylamide into the aqueous monomer solution, and stirring at the rotating speed of 1200rpm at 60 ℃ until a uniform and transparent solution B is obtained; injecting the solution B into a glass mold with the interval of 1000 mu m, and polymerizing for 8 hours under the irradiation of ultraviolet light to obtain hydrogel A;
(3) and soaking the hydrogel A in a silver nitrate solution with the mass concentration of 4.8 wt% for 1 hour to obtain the double-network hydrogel.
The tensile stress-strain curve of the double-network hydrogel prepared in this example is shown in CS-PAM-Ag in FIG. 2+-4.8%.
Example 3
(1) Dispersing 0.6g of acrylamide and 0.1g of carboxymethyl chitosan in 4mL of deionized water, and stirring at the rotating speed of 1200rpm at the temperature of 60 ℃ until a uniform and transparent monomer aqueous solution A is obtained;
(2) adding 0.0018g of photoinitiator Irgacure and 0.0012g of cross-linking agent N, N-methylene bisacrylamide into the aqueous monomer solution, and stirring at the rotating speed of 1200rpm at 60 ℃ until a uniform and transparent solution B is obtained; injecting the solution B into a glass mold with the interval of 1000 mu m, and polymerizing for 8 hours under the irradiation of ultraviolet light to obtain hydrogel A;
(3) and soaking the hydrogel A in a silver nitrate solution with the mass concentration of 8.3 wt% for 1 hour to obtain the double-network hydrogel.
The tensile stress-strain curve of the double-network hydrogel prepared in this example is shown in CS-PAM-Ag in FIG. 2+-8.3%.
Example 4
(1) Dispersing 0.6g of acrylamide and 0.1g of carboxymethyl chitosan in 4mL of deionized water, and stirring at the rotating speed of 1200rpm at the temperature of 60 ℃ until a uniform and transparent monomer aqueous solution A is obtained;
(2) adding 0.0018g of photoinitiator Irgacure and 0.0012g of cross-linking agent N, N-methylene bisacrylamide into the monomer aqueous solution, and stirring at the rotating speed of 1200rpm at 60 ℃ until a uniform and transparent solution B is obtained; injecting the solution B into a glass mold with the interval of 1000 mu m, and polymerizing for 8 hours under the irradiation of ultraviolet light to obtain hydrogel A;
(3) and soaking the hydrogel A in a silver nitrate solution with the mass concentration of 10.6 wt% for 1 hour to obtain the double-network hydrogel.
The tensile stress-strain curve of the double-network hydrogel prepared in this example is shown in CS-PAM-Ag in FIG. 2+-10.6%.
Example 5
(1) Dispersing 0.6g of acrylamide and 0.1g of carboxymethyl chitosan in 4mL of deionized water, and stirring at the rotating speed of 1200rpm at the temperature of 60 ℃ until a uniform and transparent monomer aqueous solution A is obtained;
(2) adding 0.0018g of photoinitiator Irgacure and 0.0012g of cross-linking agent N, N-methylene bisacrylamide into the aqueous monomer solution, and stirring at the rotating speed of 1200rpm at 60 ℃ until a uniform and transparent solution B is obtained; injecting the solution B into a glass mold with the interval of 1000 mu m, and polymerizing for 8 hours under the irradiation of ultraviolet light to obtain hydrogel A;
(3) and soaking the hydrogel A in a silver nitrate solution with the mass concentration of 14.5 wt% for 1 hour to obtain the double-network hydrogel.
The tensile stress-strain curve of the double-network hydrogel prepared in this example is shown in CS-PAM-Ag in FIG. 2+-14.5%.
As shown in FIG. 2, the tensile stress-strain curves of the double-network hydrogel obtained by soaking in silver nitrate solutions with different concentrations are approximately the same, and all the curves show that the stress gradually increases along with the increase of the strain, and the stress rapidly decreases after the peak value is reached. The hydrogel obtained after soaking in 8.3 wt% silver nitrate for 1 hr has the best mechanical properties, high tensile strength (0.243MPa), and high toughness (9.544MJ m)-3) And good stretchability at high strain (600%).
Application example
A physical map of the double-network hydrogel bionic intelligent skin is shown in fig. 3. Preparing a double-network hydrogel (CS-PAM-Ag) with a regular shape and an area smaller than that of the VHB adhesive tape+) The two pieces of conductive copper adhesive tapes are wrapped between the two pieces of adhesive tapes to form a sandwich structure, and the two pieces of conductive copper adhesive tapes are adhered to two ends of the hydrogel to obtain the double-network hydrogel bionic intelligent skin. And respectively testing the response of the double-network hydrogel bionic intelligent skin under different stimuli. As can be seen from FIG. 4, the double-network hydrogel bionic intelligent skin canIn response to three different deformation stimuli, compression, tension and torsion. The response curve of each mechanical stimulus has fewer peaks, the response curve is smoother, and has signal responses of different degrees along with the change of the stimulus degree, thereby showing the high reliability and sensitivity of the double-network hydrogel bionic intelligent skin.
Comparative example 1
(1) Dispersing 0.6g of acrylamide and 0.1g of carboxymethyl chitosan in 4mL of deionized water, and stirring at the rotating speed of 1200rpm at the temperature of 60 ℃ until a uniform and transparent monomer aqueous solution A is obtained;
(2) adding 0.0018g of photoinitiator Irgacure and 0.0012g of cross-linking agent N, N-methylene bisacrylamide into the aqueous monomer solution, and stirring at the rotating speed of 1200rpm at 60 ℃ until a uniform and transparent solution B is obtained; injecting the solution B into a glass mold with the interval of 1000 mu m, and polymerizing for 8 hours under the irradiation of ultraviolet light to obtain hydrogel A;
(3) the hydrogel A was soaked in a silver nitrate solution with a mass concentration of 8.3 wt% for 3 hours.
The tensile stress-strain curve of the double-network hydrogel prepared in this comparative example is shown in FIG. 5. As can be seen from FIG. 5, the excessively long soaking time causes the toughness and stretchability of the hydrogel to be reduced, and the hydrogel is not suitable for being used as a conductive matrix to manufacture the double-network hydrogel bionic intelligent skin.
Comparative example 2
(1) Dispersing 0.6g of acrylamide and 0.1g of carboxymethyl chitosan in 4mL of deionized water, and stirring at the rotating speed of 1200rpm at the temperature of 60 ℃ until a uniform and transparent monomer aqueous solution A is obtained;
(2) adding 0.0018g of photoinitiator Irgacure and 0.0012g of cross-linking agent N, N-methylene bisacrylamide into the aqueous monomer solution, and stirring at the rotating speed of 1200rpm at 60 ℃ until a uniform and transparent solution B is obtained; injecting the solution B into a glass mold with the interval of 1000 mu m, and polymerizing for 8 hours under the irradiation of ultraviolet light to obtain hydrogel A;
(3) the hydrogel A was soaked in a silver nitrate solution with a mass concentration of 8.3 wt% for 0.5 hour.
Experimental results show that the hydrogel is seriously adhered to a sample with the soaking time of less than 1h, and the later-stage packaging processing is not facilitated.
Claims (10)
1. The preparation method of the double-network hydrogel bionic intelligent skin is characterized by comprising the following steps:
(1) dispersing acrylamide and carboxymethyl chitosan in water to obtain a monomer aqueous solution;
(2) adding a photoinitiator and a crosslinking agent N, N-methylene bisacrylamide into a monomer aqueous solution, and carrying out polymerization reaction to obtain hydrogel A;
(3) soaking the hydrogel A in a silver nitrate solution to obtain a double-network hydrogel;
(4) and clamping the dielectric layer by using two layers of double-network hydrogel to form a sandwich structure, thereby preparing the bionic intelligent skin.
2. The method according to claim 1, wherein in the step (1), the mass concentration of acrylamide is 7.8 wt% to 17.8 wt%, and the mass concentration of carboxymethyl chitosan is 1.1 wt% to 3.1 wt%.
3. The preparation method according to claim 1, wherein in the step (2), the mass concentration of the crosslinking agent N, N-methylene bisacrylamide is 0.02 wt% to 0.04 wt%.
4. The method according to claim 1, wherein in the step (2), the mass concentration of the photoinitiator is 0.03 wt% to 0.05 wt%.
5. The method according to claim 1, wherein in the step (2), the polymerization is carried out by ultraviolet irradiation after the addition of the photoinitiator.
6. The preparation method according to claim 1, wherein in the step (3), the mass concentration of the silver nitrate is 1.7 wt% to 14.5 wt%.
7. The method according to claim 1, wherein the soaking time in step (3) is 1 ± 0.5 h.
8. The method according to claim 1, wherein in the step (3), the soaking time is 1 hour.
9. The method according to claim 1, wherein in step (4), the dielectric layer is a polyethylene, polypropylene or polyacrylate film.
10. The double-network hydrogel bionic intelligent skin prepared by the preparation method according to any one of claims 1 to 9.
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| CN114523685A (en) * | 2022-01-28 | 2022-05-24 | 华南理工大学 | Flame-retardant rapid software driver based on shape memory effect and preparation method and application thereof |
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| CN108676118A (en) * | 2018-05-30 | 2018-10-19 | 雷周玥 | A kind of preparation method of Multifunctional polyelectrolyte hydrogel bionic intelligence skin |
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| CN109232921A (en) * | 2018-09-06 | 2019-01-18 | 宁波大学 | A kind of preparation method of triplicated network hydrogel |
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