CN115678044B - Proton conductive organic hydrogel based on bovine serum albumin and preparation and application thereof - Google Patents
Proton conductive organic hydrogel based on bovine serum albumin and preparation and application thereof Download PDFInfo
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Abstract
The invention discloses a proton conductive organic hydrogel based on bovine serum albumin and preparation and application thereof, and belongs to the technical field of hydrogel preparation. The invention dissolves bovine serum albumin in a mixed solvent of 2, 2-trifluoroethanol and deionized water, then sequentially adds 2-mercaptoethanol, ethylenediamine and ethanol, and after stirring, stands still, and is soaked in glycerin after being washed by water, thus preparing the proton conductive organic hydrogel based on the bovine serum albumin. The protein-based biological proton hydrogel is composed of biological materials similar to skin components, such as protein, glycerol, water and the like, has excellent water retention capacity and biodegradability, and also has excellent freezing resistance, tensile property and transparency. The human body electro-physiological signal collecting device can be attached to the surface of the skin to collect high-quality human body electro-physiological signals for a long time (up to 9 days), and can be used for electrocardiograph, electromyogram monitoring and human-computer interaction control systems based on human body activities.
Description
Technical Field
The invention belongs to the technical field of hydrogel preparation, and particularly relates to a proton conductive organic hydrogel based on bovine serum albumin, and preparation and application thereof.
Background
Human-machine interfaces are an important medium for human-machine interaction, and attention has been paid in recent years. Because of skin-like mechanical properties and sensing functions, artificial electronic skin has great potential in medical monitoring and personal electronics, and is also expected to be used for developing next-generation human-machine fusion interfaces. Human skin is composed mainly of proteins, lipids, water, etc., while most artificial skin is made of synthetic polymers, metals, or carbon materials. The fusion of artificial skin with the human body is to a large extent limited by the different composition of the existing artificial skin and biological tissue materials.
The natural conductive protein hydrogel has similar material composition and physiological characteristics to human tissues, and is a potential candidate material for artificial skin of a man-machine fusion interface. In addition, proton conduction in conductive proteins is also similar to the principle of human skin sensing based on the Grotthus mechanism, i.e., protons are transported in a hydrated state along a hydrogen bond network by adjacent water molecules. However, the current conductive protein hydrogels have a key problem of easy water loss, which severely deteriorates proton conductivity thereof in several hours under the naked environment, preventing practical application thereof. Thus, there is a current urgent need to develop a natural electrically conductive protein hydrogel with reliable water-retaining ability, good biocompatibility and biodegradability, but it is still an unresolved challenge.
Disclosure of Invention
Aiming at the defects of the prior art, the invention provides a proton-conducting organic hydrogel of bovine serum albumin, and preparation and application thereof. Compared with the existing hydrogel, the albumin-based proton-conducting organic hydrogel is made of biological materials similar to skin components, such as protein, glycerol, water and the like, has excellent water retention capacity, biocompatibility and biodegradability, and also has excellent freezing resistance, tensile property and transparency. It can collect high-quality human body electrophysiological signals for a long time (up to 9 days), and can be used for electrocardiograph, electromyographic physiological signal monitoring and human-computer interaction control system based on human body activities.
In order to achieve the above object, the present invention provides the following solutions:
the invention aims at providing a preparation method of a proton-conducting organic hydrogel based on bovine serum albumin, which comprises the following steps: dissolving bovine serum albumin in a mixed solvent of 2, 2-trifluoroethanol and deionized water, then adding 2-mercaptoethanol, fully stirring, adding ethylenediamine and ethanol, stirring, standing, washing with water, and soaking in glycerol to obtain the proton-conducting organic hydrogel based on bovine serum albumin.
Further, the mass ratio of the mixed solvent of the bovine serum albumin, the 2, 2-trifluoroethanol and the deionized water is 1-2:8-10, and the mass ratio of the 2, 2-trifluoroethanol to the deionized water is 3-5:1.
Further, the mass volume ratio of the bovine serum albumin to the 2-mercaptoethanol to the ethylenediamine to the ethanol is 1-2 g:0.4-0.5 mL:0.3-0.5 mL.
Further, the solution was cast on a glass plate before the standing for 5 hours.
Further, the flushing is to flush with deionized water for 2-3 times; the soaking is to soak in glycerin for 10-40 min.
The second object of the invention is to provide a proton-conducting organic hydrogel based on bovine serum albumin prepared by the preparation method.
The invention further aims to provide an application of the proton conducting organic hydrogel based on bovine serum albumin in electrocardiograph and electromyography monitoring and intelligent robot control systems.
The invention has the beneficial effects that:
(1) The proton-conducting organic hydrogel based on bovine serum albumin has excellent freezing resistance, no obvious peak value is found in the temperature range of-80-50 ℃, and the proton-conducting organic hydrogel has certain freezing resistance even at the extremely low temperature of-80 ℃.
(2) The proton-conducting organic hydrogel based on bovine serum albumin is prepared from biological materials such as protein, glycerol, water and the like, so that the whole proton-conducting organic hydrogel based on bovine serum albumin is biodegradable. The proton-conducting organic hydrogel based on bovine serum albumin provided by the invention can be completely degraded after being soaked in trypsin solution for 48 hours, and the protein-based biological proton hydrogel provided by the invention has good biocompatibility and biodegradability.
(3) The proton-conducting organic hydrogel based on bovine serum albumin has reliable water retention performance, and the organic solvent glycerol is introduced into the outermost layer of the hydrogel to retain water by a simple solvent replacement strategy, so that the proton-conducting organic hydrogel has long-term water retention capability of 9 days in an open environment.
(4) The protein-based biological proton hydrogel provided by the invention takes bovine serum albumin as a raw material, the bovine serum albumin has natural proton conductivity, and the proton conductive organic hydrogel based on the bovine serum albumin can collect high-quality human electrophysiological signals for a long time (up to 9 days), can be used for electrocardiograph, electromyogram physiological signal monitoring and human-computer interaction control systems based on human activities, and opens up a new opportunity for developing a next-generation human-computer fusion interface.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings that are needed in the embodiments will be briefly described below, and it is obvious that the drawings in the following description are only some embodiments of the present invention, and other drawings can be obtained according to these drawings without inventive effort for a person skilled in the art.
FIG. 1 is a graph showing the weight change of the proton-conducting organic hydrogel based on bovine serum albumin prepared by immersing in glycerol for various times in proof example 2;
FIG. 2 is an electrocardiogram of the human body measured with the proton conducting organic hydrogel based on bovine serum albumin of verification example 3 (example 1);
FIG. 3 is an electromyography of human body measured in verification example 4 using the proton conductive organic hydrogel based on bovine serum albumin of example 1;
FIG. 4 is a flow chart of validation example 4 of a bovine serum albumin based proton conducting organic hydrogel (example 1) for synchronous control of a robotic arm.
Detailed Description
The present invention will be described in further detail with reference to examples for better understanding of the technical scheme of the present invention to those skilled in the art.
Example 1
1.46g of bovine serum albumin is dissolved in 9g of mixed solvent of 2, 2-trifluoroethanol and deionized water (the mass ratio of the 2, 2-trifluoroethanol to the deionized water is 4:1), after stirring to form a clear solution, 0.48mL of 2-mercaptoethanol is added, and the solution becomes turbid gradually during stirring. Then 0.44mL of ethylenediamine EDA and 0.44mL of ethanol were added and the solution was changed to a clear solution again after continuous stirring. Then casting the solution on a glass plate, evaporating and standing the solution for 5 hours to form a large film, and washing the film with deionized water for 2 to 3 times. Subsequently, the film was immersed in glycerol for 20min to obtain a proton-conducting organic hydrogel based on bovine serum albumin.
Example 2
1g of bovine serum albumin is dissolved in 8g of mixed solvent of 2, 2-trifluoroethanol and deionized water (the mass ratio of the 2, 2-trifluoroethanol to the deionized water is 5:1), after stirring to form clear solution, 0.4mL of 2-mercaptoethanol is added, and the solution is gradually turbid during stirring. Then 0.3mL of ethylenediamine EDA and 0.3mL of ethanol were added and the mixture was continuously stirred and changed to a clear solution again. Then casting the solution on a glass plate, evaporating and standing the solution for 5 hours to form a large film, and washing the film with deionized water for 2 to 3 times. Subsequently, the film was immersed in glycerol for 10min to obtain a proton-conducting organic hydrogel based on bovine serum albumin.
Example 3
2g of bovine serum albumin is dissolved in 10g of mixed solvent of 2, 2-trifluoroethanol and deionized water (the mass ratio of the 2, 2-trifluoroethanol to the deionized water is 3:1), after stirring to form clear solution, 0.5mL of 2-mercaptoethanol is added, and the solution is gradually turbid during stirring. Then 0.5mL of ethylenediamine EDA and 0.5mL of ethanol were added and the mixture was continuously stirred and changed to a clear solution again. Then casting the solution on a glass plate, evaporating and standing the solution for 5 hours to form a large film, and washing the film with deionized water for 2 to 3 times. Subsequently, the film was immersed in glycerol for 40min to obtain a proton-conducting organic hydrogel based on bovine serum albumin.
Verification example 1
(1) Anti-freeze performance test: the heat flow change during cooling and heating was tested for bovine serum albumin-based proton conducting organic hydrogels (example 1) and control samples without glycerol using Differential Scanning Calorimetry (DSC) at a temperature in the range of-80 to 50 ℃. The control sample exhibited a spike during cooling at-12℃due to the corresponding phase change, indicating that the control sample had to be frozen below-12 ℃. Whereas the proton-conducting organic hydrogel based on bovine serum albumin of example 1 showed no significant peaks over the entire temperature range, indicating that it has excellent freezing resistance even at very low temperatures of-80 ℃.
(2) Biodegradability: the proton-conducting organic hydrogel based on bovine serum albumin is entirely made of biological materials such as protein, glycerol and water, so the entire hydrogel is biodegradable. The proton-conducting organic hydrogel based on bovine serum albumin (example 1) having a thickness of 0.2mm was immersed in a trypsin solution, and the immersed portion thereof was completely degraded after 48 hours, indicating that the proton-conducting organic hydrogel based on bovine serum albumin of the present invention has excellent biodegradability.
Verification example 2
Based on example 1, the weight change curve of the proton-conducting organic hydrogel based on bovine serum albumin prepared by immersing in glycerol for different times was measured, and the water retention capacity thereof was studied, and the results are shown in fig. 1. The control sample without glycerol had a sharp drop in weight to 41.4% after 1 day of storage at 20 ℃. As the soaking time increased from 10min to 40min, the residual weight of the proton-conducting organic hydrogel based on bovine serum albumin (example 1) increased from 71.1% to 95.1% after 9d storage, and the proton-conducting organic hydrogel based on bovine serum albumin remained 82.3% of the original weight after 20min soaking, indicating good water retention.
Verification example 3
The proton-conducting organic hydrogel based on bovine serum albumin of example 1 was used for electrocardiographic monitoring:
firstly, sterilizing skin of a part attached to a human body by using alcohol cotton, respectively attaching the proton conductive organic hydrogel based on bovine serum albumin of the embodiment 1 to the left wrist and the right ankle, then connecting the proton conductive organic hydrogel based on bovine serum albumin with an electrocardio signal monitor, wherein the electrocardio signal monitor is provided with three signal acquisition lines, respectively connecting red and green signal acquisition lines to the proton conductive organic hydrogel based on bovine serum albumin of the left wrist and the right wrist, connecting a black signal acquisition line to the proton conductive organic hydrogel based on bovine serum albumin of the right ankle, and finally outputting by control software to realize electrocardio signal monitoring, and fig. 2 is an electrocardiogram of the human body measured by using the proton conductive organic hydrogel based on bovine serum albumin of the embodiment 1.
Verification example 4
The proton-conducting organic hydrogel based on bovine serum albumin of example 1 was used in a human activity-based control system with high precision electrophysiological signal acquisition capability:
based on the proton conductive organic hydrogel based on bovine serum albumin, an intelligent robot control system consisting of a signal acquisition unit, a voltage comparator and a data processing microcontroller is further developed. Two proton-conducting organic hydrogels based on bovine serum albumin are attached to the upper arm of the user to collect electromyographic signals, as follows: the electromyographic signal monitor has three signal acquisition lines, the yellow-green signal acquisition lines are respectively connected to the proton conductive organic hydrogel based on bovine serum albumin on the upper arm of the user, the red signal acquisition lines are connected to the proton conductive organic hydrogel based on bovine serum albumin on the back of the hand, and finally the electromyographic signal monitoring can be realized through the output of control software, and fig. 3 is an electromyography of a human body measured by using the hydrogel of embodiment 1. When the arms of the user perform straightening and bending actions, the electromyographic signals received from the proton-conducting organic hydrogel based on bovine serum albumin are converted into control commands in real time by the microcontroller. A flow chart of the human arm straightening/bending electromyography signals recorded by the proton conducting organic hydrogel based on the bovine serum albumin for synchronously controlling the mechanical arm is shown as figure 4, which shows that the proton conducting organic hydrogel based on the bovine serum albumin can successfully control the mechanical arm to perform straightening and bending actions corresponding to the human arm.
The above embodiments are only illustrative of the preferred embodiments of the present invention and are not intended to limit the scope of the present invention, and various modifications and improvements made by those skilled in the art to the technical solutions of the present invention should fall within the protection scope defined by the claims of the present invention without departing from the design spirit of the present invention.
Claims (7)
1. A preparation method of a proton-conducting organic hydrogel based on bovine serum albumin is characterized by comprising the following steps: the method comprises the following steps: dissolving bovine serum albumin in a mixed solvent of 2, 2-trifluoroethanol and deionized water, then adding 2-mercaptoethanol, fully stirring, adding ethylenediamine and ethanol, stirring, standing, washing with water, and soaking in glycerol to obtain the proton-conducting organic hydrogel based on bovine serum albumin.
2. The preparation method according to claim 1, wherein the mass ratio of the bovine serum albumin to the mixed solvent of 2, 2-trifluoroethanol and deionized water is 1-2:8-10, and the mass ratio of the 2, 2-trifluoroethanol to the deionized water is 3-5:1.
3. The preparation method according to claim 1, wherein the mass-volume ratio of the bovine serum albumin, the 2-mercaptoethanol, the ethylenediamine and the ethanol is 1-2 g:0.4-0.5 ml:0.3-0.5 mL.
4. The method of claim 1, wherein the solution is cast onto a glass plate prior to the resting for a period of 5 hours.
5. The method according to claim 1, wherein the rinsing is performed 2 to 3 times with deionized water; the soaking is to soak in glycerin for 10-40 min.
6. A proton-conducting organic hydrogel based on bovine serum albumin prepared by the method of any one of claims 1 to 5.
7. Use of the bovine serum albumin-based proton-conducting organic hydrogel according to claim 6 in electrocardiographic, electromyographic physiological electrical signal monitoring and intelligent robotic control systems.
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| CN114213673A (en) * | 2021-12-27 | 2022-03-22 | 湖南工业大学 | Preparation method of polypyrrole-modified bovine serum albumin, protein conductive hydrogel and preparation method and application thereof |
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Patent Citations (5)
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| CN104487103A (en) * | 2012-05-15 | 2015-04-01 | 泰克尼恩研究和发展基金有限公司 | Fiber-reinforced hydrogel composites and methods of forming fiber-reinforced hydrogel composites |
| CN105189532A (en) * | 2012-12-31 | 2015-12-23 | 新加坡科技研究局 | Self-assembled ultrashort peptides hydrogels for wound healing, skin care and cosmetics applications |
| CN105837861A (en) * | 2016-04-03 | 2016-08-10 | 苏鑫 | Composite natural polymer gel material |
| CN110078944A (en) * | 2019-05-17 | 2019-08-02 | 长春工业大学 | The preparation method of tough protein-based hydrogels is glued in a kind of Low-temperature antifreeze conduction self-healing |
| CN114213673A (en) * | 2021-12-27 | 2022-03-22 | 湖南工业大学 | Preparation method of polypyrrole-modified bovine serum albumin, protein conductive hydrogel and preparation method and application thereof |
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