CN115531591A - Intelligent electric heating dressing for temperature-controlled segmented drug delivery and preparation method thereof - Google Patents
Intelligent electric heating dressing for temperature-controlled segmented drug delivery and preparation method thereof Download PDFInfo
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- CN115531591A CN115531591A CN202211028002.2A CN202211028002A CN115531591A CN 115531591 A CN115531591 A CN 115531591A CN 202211028002 A CN202211028002 A CN 202211028002A CN 115531591 A CN115531591 A CN 115531591A
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- temperature
- microgel
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- sensitive
- dressing
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- 238000012377 drug delivery Methods 0.000 title claims description 16
- 238000002360 preparation method Methods 0.000 title claims description 15
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Images
Classifications
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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
- A61L15/00—Chemical aspects of, or use of materials for, bandages, dressings or absorbent pads
- A61L15/16—Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons
- A61L15/18—Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons containing inorganic materials
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61F—FILTERS IMPLANTABLE INTO BLOOD VESSELS; PROSTHESES; DEVICES PROVIDING PATENCY TO, OR PREVENTING COLLAPSING OF, TUBULAR STRUCTURES OF THE BODY, e.g. STENTS; ORTHOPAEDIC, NURSING OR CONTRACEPTIVE DEVICES; FOMENTATION; TREATMENT OR PROTECTION OF EYES OR EARS; BANDAGES, DRESSINGS OR ABSORBENT PADS; FIRST-AID KITS
- A61F13/00—Bandages or dressings; Absorbent pads
- A61F13/00051—Accessories for dressings
- A61F13/00063—Accessories for dressings comprising medicaments or additives, e.g. odor control, PH control, debriding, antimicrobic
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61F—FILTERS IMPLANTABLE INTO BLOOD VESSELS; PROSTHESES; DEVICES PROVIDING PATENCY TO, OR PREVENTING COLLAPSING OF, TUBULAR STRUCTURES OF THE BODY, e.g. STENTS; ORTHOPAEDIC, NURSING OR CONTRACEPTIVE DEVICES; FOMENTATION; TREATMENT OR PROTECTION OF EYES OR EARS; BANDAGES, DRESSINGS OR ABSORBENT PADS; FIRST-AID KITS
- A61F13/00—Bandages or dressings; Absorbent pads
- A61F13/02—Adhesive bandages or dressings
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61F—FILTERS IMPLANTABLE INTO BLOOD VESSELS; PROSTHESES; DEVICES PROVIDING PATENCY TO, OR PREVENTING COLLAPSING OF, TUBULAR STRUCTURES OF THE BODY, e.g. STENTS; ORTHOPAEDIC, NURSING OR CONTRACEPTIVE DEVICES; FOMENTATION; TREATMENT OR PROTECTION OF EYES OR EARS; BANDAGES, DRESSINGS OR ABSORBENT PADS; FIRST-AID KITS
- A61F13/00—Bandages or dressings; Absorbent pads
- A61F13/02—Adhesive bandages or dressings
- A61F13/0276—Apparatus or processes for manufacturing adhesive dressings or bandages
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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
- A61L15/00—Chemical aspects of, or use of materials for, bandages, dressings or absorbent pads
- A61L15/16—Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons
- A61L15/22—Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons containing macromolecular materials
- A61L15/28—Polysaccharides or their derivatives
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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
- A61L15/00—Chemical aspects of, or use of materials for, bandages, dressings or absorbent pads
- A61L15/16—Bandages, dressings or absorbent pads for physiological fluids such as urine or blood, e.g. sanitary towels, tampons
- A61L15/42—Use of materials characterised by their function or physical properties
- A61L15/44—Medicaments
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61F—FILTERS IMPLANTABLE INTO BLOOD VESSELS; PROSTHESES; DEVICES PROVIDING PATENCY TO, OR PREVENTING COLLAPSING OF, TUBULAR STRUCTURES OF THE BODY, e.g. STENTS; ORTHOPAEDIC, NURSING OR CONTRACEPTIVE DEVICES; FOMENTATION; TREATMENT OR PROTECTION OF EYES OR EARS; BANDAGES, DRESSINGS OR ABSORBENT PADS; FIRST-AID KITS
- A61F13/00—Bandages or dressings; Absorbent pads
- A61F2013/00361—Plasters
- A61F2013/00902—Plasters containing means
- A61F2013/00906—Plasters containing means for transcutaneous or transdermal drugs application
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02B—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO BUILDINGS, e.g. HOUSING, HOUSE APPLIANCES OR RELATED END-USER APPLICATIONS
- Y02B30/00—Energy efficient heating, ventilation or air conditioning [HVAC]
Landscapes
- Health & Medical Sciences (AREA)
- Engineering & Computer Science (AREA)
- General Health & Medical Sciences (AREA)
- Veterinary Medicine (AREA)
- Public Health (AREA)
- Life Sciences & Earth Sciences (AREA)
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- Chemical & Material Sciences (AREA)
- Heart & Thoracic Surgery (AREA)
- Vascular Medicine (AREA)
- Biomedical Technology (AREA)
- Hematology (AREA)
- Materials Engineering (AREA)
- Epidemiology (AREA)
- Manufacturing & Machinery (AREA)
- Medicinal Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Medicinal Preparation (AREA)
Abstract
The intelligent electric heating dressing comprises an electric heating conductive fabric, the electric heating conductive fabric is provided with a plurality of coating areas for independently controlling heating, each coating area is provided with a medicine dressing layer, each medicine dressing layer comprises a gel matrix, temperature-sensitive medicine-carrying microgel coated in the gel matrix and medicine solution loaded in the temperature-sensitive medicine-carrying microgel, and the types of the medicine solution loaded by the temperature-sensitive medicine-carrying microgel of different coating areas are different. The temperature-sensitive drug-loaded microgel can stimulate different areas to generate phase transformation, so that different drugs can be released according to the staged requirement of wound healing, the administration type, the dosage and the release time are controllable, the wound healing period is shortened, and the treatment effect is improved; and need not frequent change, effectively avoid changing the wound secondary infection that the dressing in-process arouses, it is very inconvenient for the patient to change dressings many times to and change dressings at every turn and probably increase the painful drawback of patient.
Description
Technical Field
The invention relates to the field of medical materials, in particular to an intelligent electric heating dressing for temperature-controlled segmented drug delivery and a preparation method thereof.
Background
The chronic wound refers to a wound which is not healed or has no healing tendency for more than 1 month due to the influence of external or internal factors, and comprises pressure sores, diabetic foot ulcers, lower limb arteriovenous ulcers and the like. With the increasing proportion of patients with chronic wounds in recent years, how to improve the curative effect of chronic wound treatment has become a great problem in the medical field.
The dressing is the most common means for nursing chronic wounds at present, can replace damaged skin to play a barrier role in a healing period, prevent the wounds from being polluted by the external environment, and provide an excellent healing environment. The gel dressing is a high polymer material consisting of a three-dimensional network structure, has high internal water content, good fitting property and excellent histocompatibility, can avoid secondary damage caused in the replacement process, and can absorb a small amount of tissue fluid exuded from a wound.
However, the healing of chronic wounds is a complex dynamic process involving the combined action of multiple drugs and growth factors, and the structure of the wound is complex, with different areas of the wound in different stages of healing. The gel dressing in the prior art is limited to passively releasing one to two active ingredients, but the periodic and regional requirements of chronic wound healing are ignored, dressings of different drug types need to be frequently replaced according to the wound healing condition (such as 1 to 2 days), multiple dressing changes bring great inconvenience to patients, the pain of the patients can be increased due to each dressing change, in addition, the treatment cost and the treatment period are increased, and the effect is poor.
Disclosure of Invention
Based on the above, the invention provides an intelligent temperature-controlled sectional-administration electrothermal dressing and a preparation method thereof, and aims to solve the technical problems that gel dressings in the prior art are limited to passively release one to two active ingredients, dressings of different drug types need to be frequently replaced according to the wound rehabilitation condition, and multiple dressing changes bring great inconvenience to patients and can increase the pain of the patients.
In order to achieve the purpose, the invention provides an intelligent electric heating dressing with temperature-control segmented drug delivery, which comprises an electric heating conductive fabric, wherein the electric heating conductive fabric is provided with a plurality of coating areas for independently controlling heating, each coating area is provided with a drug dressing layer, each drug dressing layer comprises a gel matrix, temperature-sensitive drug-loaded microgel coated in the gel matrix and drug solution loaded in the temperature-sensitive drug-loaded microgel, and the types of the drug solutions loaded by the temperature-sensitive drug-loaded microgels in different coating areas are different.
As a further preferable technical scheme of the invention, the medicine dressing layer is provided with a plurality of gel units which are distributed in an array manner, the thickness of each gel unit is 0.2-2mm, the diameter is 2-5mm, and the distance is 2-5mm.
As a further preferable technical scheme of the invention, an insulating partition area with the width of 1-5mm is reserved between the medicine dressing layers of different coating areas, and the insulating partition area is coated with a gel matrix without temperature-sensitive medicine-carrying microgel.
According to another aspect of the present invention, the present invention further provides a preparation method of the intelligent electrothermal dressing for temperature-controlled segmented drug delivery, wherein the method comprises the following steps:
s1, soaking a fabric into a dispersion liquid containing a carbon material, taking out the fabric, penetrating the fabric through a roller to realize pad dyeing, drying the fabric, and repeating the pad dyeing for a plurality of times to prepare a conductive fabric;
s2, adding two temperature-sensitive comonomers, sodium alginate, an initiator and an accelerator into the inorganic hectorite aqueous dispersion, polymerizing for 10-24 hours at room temperature, gradually dripping the obtained polymer into a calcium chloride aqueous solution to form spherical microgel, and regulating the molar ratio of the two temperature-sensitive comonomers to obtain the spherical microgel with different response temperatures; washing the spherical microgel with deionized water, filtering, freeze-drying, respectively putting the freeze-dried spherical microgel with different response temperatures into different drug solutions, and swelling for 12-24h to prepare various temperature-sensitive drug-loaded microgels loaded with different drug solutions;
and S3, adding an acrylamide monomer, an initiator and an accelerator into the inorganic hectorite aqueous dispersion to form a pre-polymerization solution, adding the temperature-sensitive drug-loaded microgel, coating the pre-polymerization solution on the surface of the conductive fabric, respectively corresponding the temperature-sensitive drug-loaded microgel loaded with different types of drug solutions to different coating areas, reacting for 8-24 hours at room temperature to enable the pre-polymerization solution to form a gel matrix coated with the temperature-sensitive drug-loaded microgel through a polymerization reaction, and finally obtaining the intelligent electrothermal dressing for temperature-controlled segmented drug delivery.
As a further preferable technical scheme of the present invention, in step S1, the fabric is a knitted, woven or non-woven fabric made of one or more fibers of cotton, nylon, polyphenylene sulfide or polypropylene; the carbon material is one or more of graphene oxide, carbon nano tubes, conductive carbon black or graphite; the mass fraction of the carbon material in the dispersion is 0.1-0.5wt.%, the solvent of the dispersion is a mixture of ethanol and water, and the volume ratio of ethanol to water is 1.
As a further preferable technical scheme of the invention, in the step S2, the two temperature-sensitive comonomers are 2-methyl-2-acrylic acid-2- (2-methoxyethoxy) ethyl ester and oligo-polyethylene glycol methyl ether methacrylate, the regulation and control of the response temperature of the spherical microgel are realized by regulating the molar ratio of the two, and the change range of the response temperature is 35-60 ℃.
As a further preferred technical scheme of the present invention, in step S2, the inorganic hectorite aqueous dispersion is obtained by uniformly dispersing inorganic hectorite in deionized water, the total content of the two temperature-sensitive comonomers added is 5-20wt.% of the mass of the deionized water, the inorganic hectorite and sodium alginate are 0.5-3wt.% of the mass of the deionized water, the concentration of the calcium chloride aqueous solution is 2%, and the concentration of the drug solution is 0.1-2mg · mL -1 。
In a further preferred embodiment of the present invention, in step S2, the spherical microgel has a particle size of 50 to 200 μm after lyophilization.
As a further preferable technical scheme of the present invention, in step S3, the inorganic hectorite aqueous dispersion is obtained by uniformly dispersing inorganic hectorite in water, wherein the inorganic hectorite content is 5-20wt.% of the mass of water, the acrylamide monomer is 10-30wt.% of the mass of water, and the temperature-sensitive drug-loaded microgel is 10-40wt.% of the mass of the acrylamide monomer.
As a further preferable technical solution of the present invention, in steps S2 and S3, the initiator is one or more of potassium persulfate, ammonium persulfate, or sodium persulfate, and the accelerator is one or more of N, N' -tetramethylethylenediamine, or N, N-dimethylaniline, wherein: in the step S2, the dosage of the initiator is 1-10 wt% of the contents of the two temperature-sensitive comonomers, and in the step S3, the dosage of the initiator is 1-10 wt% of the contents of the acrylamide monomers; the dosage of the accelerator in the step S2 is 0.2-0.8% of the volume of the pre-polymerization liquid, and the dosage of the accelerator in the step S3 is 0.2-0.8% of the volume of the pre-polymerization liquid.
The intelligent electrothermal dressing with temperature-control segmented administration and the preparation method thereof adopt the technical scheme, and can achieve the following beneficial effects:
1) The advantages of the gel material are kept, a moist environment can be provided for wound recovery, exudative tissue fluid can be absorbed, necrotic tissues and toxins are eliminated, and meanwhile, the new tissues are not damaged;
2) The fabric is used as a substrate, so that the mechanical strength of the coated gel can be improved to a certain extent, the defect of poor mechanical property of the traditional gel dressing is overcome, and the service life of the dressing is prolonged;
3) The heating circuit formed after the fabric is tied and dyed is connected with an external power supply, and the temperature of the drug dressing layer is changed along with the change of the voltage, so that the temperature-sensitive drug-loaded microgel in different areas can be stimulated to generate phase transformation, different drugs can be released according to the stage requirements of wound healing, the drug administration type, the drug consumption and the release time are controllable, the wound healing period is further shortened, and the treatment effect is improved;
4) The intelligent electrothermal dressing adopts temperature control sectional administration, can be used for a long time, does not need frequent replacement, effectively avoids secondary wound infection caused in the dressing replacement process, avoids great inconvenience brought to patients by multiple times of dressing replacement and overcomes the defect that the pain of the patients can be increased by each time of dressing replacement, namely, the treatment cost is reduced to a certain extent; in addition, the dressing of the invention does not need external complex equipment, and is convenient to carry;
5) The intelligent electrothermal dressing prepared by the invention has relatively simple preparation process, does not involve complicated chemical reaction and conditions of high temperature, high pressure, organic solvent and the like in the process, and has no toxic or harmful effect on the environment.
Drawings
The invention is described in further detail below with reference to the drawings and the detailed description.
FIG. 1 is a schematic diagram of a gel coating method of the temperature-controlled sectional-administration intelligent electrothermal dressing of the invention;
FIG. 2 is a simplified flow chart of a method for preparing the intelligent electrothermal dressing for temperature-controlled and segmented drug delivery;
FIG. 3 is a graph showing the infrared images before and after energization of different coating modes and the temperature-time change curve of the drug dressing layer.
The objects, features and advantages of the present invention will be further explained with reference to the accompanying drawings.
Detailed Description
The invention will be further described with reference to the drawings and the detailed description. In the preferred embodiments, the terms "upper", "lower", "left", "right", "middle" and "a" are used for clarity of description only, and are not used to limit the scope of the invention, and the relative relationship between the terms and the terms is not changed or modified substantially without changing the technical content of the invention.
The invention provides an intelligent electric heating dressing for temperature-controlled segmented drug delivery, which comprises an electric heating conductive fabric, wherein the electric heating conductive fabric is provided with a plurality of coating areas for independently controlling heating, each coating area is provided with a drug dressing layer, each drug dressing layer comprises a gel matrix, temperature-sensitive drug-loaded microgel and drug solution, the temperature-sensitive drug-loaded microgel is coated in the gel matrix and is in a granular shape (the particle size is 50-200 mu m), the drug solutions are loaded in the temperature-sensitive drug-loaded microgel, and the types of the drug solutions loaded by the temperature-sensitive drug-loaded microgel in different coating areas are different.
Preferably, for the convenience of users and portability, the conductive fabric is further provided with an external power supply for providing electric energy for heating the conductive fabric, and the power supply can adopt a conventional portable charging power supply with the specification of less than 10000mAh and 12V, and of course, a storage battery can also be adopted. In order to realize intelligent control, the power supply is also provided with a controller which is used for controlling and adjusting the voltage output by the power supply and selecting a coating area needing electric heating.
The intelligent electric heating dressing and an external power supply are assembled into the intelligent electric heating dressing with temperature control and sectional administration, the electric heating fabric layer in a certain coating area is heated by applying voltage and is transmitted to the medicine dressing layer, and then the internal temperature-sensitive medicine-carrying microgel is stimulated to generate phase transformation to release corresponding loaded medicine; after the power supply is cut off, the temperature is reduced, and the drug release is stopped; by changing the position (coating area) and size of the applied voltage, another therapeutic drug can be released to the wound surface, and the effect of drug administration according to requirements can be achieved. In the heating process, the temperature rise range of the fabric layer is 50-75 ℃, because of certain heat loss in the transmission process, the temperature rise range of the medicine dressing layer is 40-65 ℃, and the temperature rise time is 60-300s.
The plurality of coating areas which can independently control heating can be randomly arranged on the conductive fabric according to requirements, such as left-right or up-down arrangement, or a plurality of areas are arranged side by side, a plurality of areas are arranged in concentric rings, a plurality of areas are sequentially arranged around a certain point, and the like, wherein fig. 1 shows the distribution condition of four coating areas (areas I-IV) on the conductive fabric in one example.
The coating structure of the medicine dressing layer in the coating area can adopt the following modes, namely plane coating, vertical coating, parallel coating and array coating, wherein the plane coating means that the medicine dressing layer is an integral body (a in figure 3), the vertical coating means that the medicine dressing layer is transversely arranged in parallel in a strip shape (b in figure 3), the parallel coating means that the medicine dressing layer is longitudinally arranged in parallel in a strip shape (c in figure 3), and the array coating means that the medicine dressing is distributed in a dot matrix form by a plurality of gel units (d in figure 3). The infrared images and the gel layer temperature-time change curves before and after the above four coating structures were powered on, as shown in fig. 3. In the process of coating the drug dressing layer, since the fabric has certain pores, the pre-polymerization solution can permeate into the fabric, and form a reinforcing network after polymerization, which affects the conductive path of the fabric to a certain extent and weakens the electrothermal effect of the fabric, as can be seen from fig. 3, the surface temperature of the drug dressing layer in planar coating is slowly raised and lowered, and the vertical and parallel coating modes are the next time, so that the array coating effect is optimal. By comparing the changes of the gel surface temperature in the modes of plane, vertical, parallel or array coating, the array coating has relatively minimum influence on the resistance of the fabric, and the response temperature of the internal microgel can be reached relatively quickly.
In a specific implementation, the drug dressing layer has a plurality of gel units, the gel units are distributed in an array form (dot matrix coating structure), the thickness of each gel unit is 0.2-2mm, the diameter is 2-5mm, and the distance is 2-5mm, the array distribution is shown in figure 1, each circle in the figure is a coated gel matrix (gel unit) coated with temperature-sensitive drug-loaded microgel, and different slashes in the circle represent different types of drug solutions loaded by the temperature-sensitive drug-loaded microgel.
Preferably, an insulation partition area with the width of 1-5mm is reserved between the medicine dressing layers of different coating areas, and the insulation partition area is coated with a gel matrix without temperature-sensitive medicine-carrying microgel, so that not only is the regional medicine release realized, but also the influence of the gel on a conductive path and an electrothermal effect in the fabric can be reduced.
As shown in fig. 2, the invention also provides a preparation method of the intelligent electrothermal dressing for temperature-controlled segmented drug delivery, which comprises the following steps:
step S1, soaking the fabric in dispersion liquid of a carbon-containing material, taking out the fabric, penetrating the fabric through a roller to realize pad dyeing, drying the fabric, repeating the pad dyeing for a plurality of times, and loading the carbon-containing material in the fabric to form a heating circuit so as to prepare the conductive fabric.
In the step S1, the fabric is a knitted, woven or non-woven fabric formed by one or more fibers of cotton, nylon, polyphenylene sulfide or polypropylene; the carbon material is one or more of Graphene Oxide (GO), carbon Nano Tube (CNT), conductive carbon black or graphite; the mass fraction of the carbon material in the dispersion is 0.1-0.5wt.%, the solvent of the dispersion is a mixture of ethanol and water, and the volume ratio of ethanol to water is 1.
When the carbon material is graphene oxide, repeated pad dyeing is followed by reduction treatment, and the reduction treatment is carried out by taking a mixed solution of hydriodic acid (HI) and glacial acetic acid (HAc) as a reducing agent, and reacting for 10 hours at the temperature of 90 ℃ according to the volume ratio of HI to HAc = 2.
Specifically, the conductive fabric is provided with a plurality of coating areas for independently controlling heat generation, and the different coating areas are required to be insulated, and the following operations can be realized: the regions between adjacent coated regions are not impregnated with the dispersion of carbonaceous material when the fabric is first soaked, even though the fabric between adjacent coated regions does not contain carbonaceous material; different coating areas are respectively connected with an external power supply through wires, and independent control of heating can be realized.
S2, adding two temperature-sensitive comonomers, sodium alginate (Alg), an initiator and an accelerator into inorganic hectorite (clay) water dispersion, polymerizing for 10-24 hours at room temperature, gradually dripping the obtained polymer into calcium chloride water solution to form spherical microgel, and adjusting the molar ratio of the two temperature-sensitive comonomers to obtain the spherical microgel with different response temperatures; washing the spherical microgel with deionized water, filtering, freeze-drying, respectively putting the freeze-dried spherical microgel with different response temperatures into different drug solutions, and swelling for 12-24h to prepare the multiple temperature-sensitive drug-loaded microgels loaded with different drug solutions.
In the step S2, the two temperature-sensitive comonomers are 2-methyl-2-acrylic acid-2- (2-methoxyethoxy) ethyl ester (MEO) 2 MA，M n ＝188g·mol -1 ) And oligoethylene glycol methyl ether methacrylate (OEGMA, M) n ＝475g·mol -1 ) The adjustment of the molar ratio of the two components realizes the adjustment and control of the response temperature of the spherical microgel, and the response temperature changesThe chemical range is 35-60 ℃.
The inorganic hectorite aqueous dispersion is obtained by uniformly dispersing inorganic hectorite in deionized water, the total content of two temperature-sensitive comonomers is 5-20 wt% of the mass of the deionized water, the inorganic hectorite and sodium alginate are 0.5-3 wt% of the mass of the deionized water, and the concentration of a calcium chloride aqueous solution is 2%.
The initiator is one or more of potassium persulfate (KPS), ammonium Persulfate (APS) or sodium persulfate (NaPS), the accelerator is one or more of N, N, N ', N' -Tetramethylethylenediamine (TEMED) or N, N-dimethylaniline, the dosage of the initiator is 1-10 wt% of the content of the two temperature-sensitive comonomers, and the dosage of the accelerator is 0.2-0.8% of the volume of the pre-polymerization liquid.
The medicinal solution can be one or more of healing promoting substance solutions with hemostatic, antibacterial or antiinflammatory effects, and has concentration of 0.1-2 mg/mL -1 。
The polymer formed by two temperature-sensitive comonomers is gradually and gradually extruded into a calcium chloride aqueous solution through an injection needle to form spherical microgel, the size of the spherical microgel can be changed by changing the type of the injection needle, and the particle size of the microgel after freeze-drying is 50-200 mu m. The drug loading capacity of the spherical microgel is limited by the size of the microgel, and the spherical microgel with different sizes has different drug loading energies, so that the dispersing capacities in the pre-polymerization liquid are different, and in practical application, the size of the spherical microgel can be reasonably selected according to the requirement of the actual drug loading amount per unit area so as to meet the use requirement.
In the step, the water in the microgel is removed by adopting a freeze-drying operation method, so that the subsequent storage and drug loading are facilitated.
And S3, adding an acrylamide monomer (AAm), an initiator and an accelerator into an inorganic hectorite (clay) water dispersion to form a pre-polymerization solution, adding temperature-sensitive drug-loaded microgel, coating the pre-polymerization solution on the surface of the conductive fabric, respectively corresponding the temperature-sensitive drug-loaded microgel loaded with different types of drug solutions to different coating areas, reacting for 8-24 hours at room temperature to enable the pre-polymerization solution to form a gel matrix coated with the temperature-sensitive drug-loaded microgel through a polymerization reaction, and finally obtaining the intelligent electric heating dressing with temperature-controlled sectional administration.
In the step S3, the inorganic hectorite aqueous dispersion is obtained by uniformly dispersing inorganic hectorite in water, wherein the inorganic hectorite accounts for 5-20 wt% of the water, the acrylamide monomer accounts for 10-30 wt% of the water, and the temperature-sensitive drug-loaded microgel accounts for 10-40 wt% of the acrylamide monomer.
The initiator is one or more of potassium persulfate, ammonium persulfate or sodium persulfate, the accelerator is one or more of N, N, N ', N' -tetramethylethylenediamine or N, N-dimethylaniline, the using amount of the initiator is 1-10 wt% of the monomer content of acrylamide, and the using amount of the accelerator is 0.2-0.8% of the volume of the prepolymer liquid.
In order to further understand the technical scheme of the present invention, the technical scheme of the preparation method of the present invention is further detailed below by specific examples.
Example 1
(1) Preparing a conductive fabric: adding 1g of Carbon Nanotube (CNT) powder into a mixed solvent of 900g of water and 100g of ethanol (EtOH), and carrying out pre-stirring for 0.5h and ultrasonic treatment for 1h to obtain 0.1wt.% of dispersion liquid; soaking the cut all-cotton knitted fabric in a dispersion liquid, taking out the all-cotton knitted fabric, then passing through a roller to enable the liquid to penetrate into the fabric, and removing residual liquid; drying and repeatedly pad-dyeing for 30 times to prepare the CNT coated all-cotton knitted fabric (conductive fabric) with good conductivity for later use, wherein the conductive fabric is provided with four coating areas (areas I-IV) which independently control heating.
(2) Preparing the drug-loaded microgel: 0.05g of inorganic hectorite (clay) is uniformly dispersed in 10g of deionized water, and 0.119g of oligoethylene glycol monomethyl ether methacrylate (OEGMA) and 0.381g of 2-methyl-2-acrylic acid-2- (2-methoxyethoxy) ethyl ester (MEO) are added in sequence 2 MA), 0.1g sodium alginate (Alg), 0.02g potassium persulfate (KPS) and 20. Mu.L N, N, N ', N' -Tetramethylethylenediamine (TEMED) were polymerized at room temperature for 10 hours, and then extruded dropwise into CaCl 2 In the water solution, spherical microgel with response temperature of about 35 ℃ is obtained; then adjusting the molar ratio of the two comonomers to obtain spherical microgel with response temperatures of about 37 ℃, 40 ℃ and 42 ℃ in sequence; washing the spherical microgel with deionized waterRemoving unreacted monomers, crosslinking agents and the like for multiple times; filtering, freeze-drying, and respectively adding the obtained four spherical microgels into 1 mg/mL -1 Cefazolin, curcumin, insulin and 0.1 mg/mL -1 Swelling the vascular endothelial growth factor solution for 24h to obtain four temperature-sensitive drug-loaded microgels respectively loaded with four different drug solutions.
(3) Preparation of the dressing: adding 0.5g of clay into 10g of deionized water, and uniformly stirring to obtain a dispersion liquid with the mass fraction of 5 wt.%; then adding 1g of acrylamide monomer (AAm), 0.04g of KPS and 30 mu L of TEMED to prepare a prepolymerization solution, dividing the prepolymerization solution into four parts, respectively adding 0.1g of the prepared four temperature-sensitive drug-loaded microgels to prepare coating solutions, respectively coating the coating solutions (shown in figure 1) wrapping 4 temperature-sensitive drug-loaded microgels on areas I-IV of the conductive fabric, and reacting for 8 hours at room temperature to obtain a final product; wherein the areas of the regions are consistent and are 20 × 20mm 2 Coating liquid is distributed in a punctiform array manner for coating, the diameter of each coating point is 3mm, and the adjacent distance is 3mm; the interval between adjacent coating areas is 1mm, and the thickness of the pre-polymerization liquid coated with the temperature-sensitive medicine-carrying microgel is 0.5mm.
Effect verification: the prepared intelligent electric heating dressing and an external power supply are assembled into the intelligent electric heating dressing for temperature control segmented drug delivery, when the output voltage is 8V, the temperature of the fabric layer is measured to be about 46 ℃, after 80s, the temperature of the drug dressing layer is increased to 35 ℃, and the temperature-sensitive drug-loaded microgel in the region I immediately undergoes phase transformation and releases loaded drugs; after the preset time, applying 9V voltage to the area II, stabilizing the temperature of the drug dressing layer to about 38 ℃, enabling the temperature-sensitive drug-loaded microgel of the area II to reach the critical phase transition temperature, and responding to the stimulus to release another drug; by analogy, targeted quantitative and timed administration can be realized.
Example 2
(1) Preparing a conductive fabric: taking 250g of 1wt.% GO dispersion and 500g of H 2 Mixing O and 250g of EtOH, and carrying out pre-stirring for 0.5h and ultrasonic treatment for 1h to obtain 0.25wt.% of dispersion liquid; soaking the cut PPS woven fabric in the dispersion liquid, and then passing through a roller to enable the liquid to penetrate into the fabric and remove residual liquid; after drying and pad dyeing for 35 times, pressAccording to the volume ratio of HI: HAc =2, a reducing agent is prepared and fully immersed in the fabric, and the reducing agent reacts for 10 hours in an environment at 90 ℃ to prepare rGO-coated PPS woven fabric (conductive fabric) with good conductivity for standby, and the conductive fabric is provided with four coating areas (areas I-IV) capable of independently controlling heat generation.
(2) Preparing a drug-loaded microgel: 0.1g of clay was uniformly dispersed in 10g of deionized water, and 0.274g of OEGMA and 0.726g of MEO were added in that order 2 MA, 0.2g of Alg, 0.04g of KPS and 30. Mu.L of TEMED, and after polymerization at room temperature for 12 hours, it was extruded dropwise onto CaCl 2 In the water solution, spherical microgel with response temperature of about 37 ℃ is obtained; then adjusting the molar ratio of the two comonomers to obtain spherical microgel with response temperatures of 40 ℃, 42 ℃ and 45 ℃ in sequence; washing the spherical microgel for many times by deionized water to remove unreacted monomers, cross-linking agents and the like; filtering, freeze-drying, and respectively adding the obtained four spherical microgels into 1.2 mg/mL -1 Cefazolin, vancomycin, insulin and 0.2 mg/mL -1 Swelling the vascular endothelial growth factor solution for 24h to obtain four temperature-sensitive drug-loaded microgels respectively loaded with four different drug solutions.
(3) Preparation of the dressing: adding 1g of clay into 10g of deionized water, and uniformly stirring to obtain a dispersion liquid with the mass fraction of 10wt.%; then adding 2g of monomer AAm, 0.08g of KPS and 30 mu L of TEMED to prepare prepolymerization liquid, dividing the prepolymerization liquid into four parts, respectively adding 0.4g of the prepared four temperature-sensitive drug-loaded microgels to prepare coating liquids, respectively coating the coating liquids (shown in figure 1) wrapping the 4 temperature-sensitive drug-loaded microgels in the areas I-IV of the conductive fabric, and reacting at room temperature for 10 hours to obtain a final product; wherein the areas of the regions are consistent and are 20 × 20mm 2 Coating liquid is distributed in a punctiform array for coating, the diameter of each coating point is 2mm, and the adjacent distance is 2mm; the interval between adjacent coating areas is 2mm, and the thickness of the pre-polymerization liquid coated with the temperature-sensitive drug-loaded microgel is 0.8mm.
Effect verification: the prepared dressing and an external power supply are assembled into the intelligent electric heating dressing for temperature control segmented administration, when the output voltage is 8V, the temperature of a fabric layer is measured to be about 48 ℃, the temperature of a medicine dressing layer is increased to 37 ℃ after 90s, and the temperature-sensitive medicine-carrying microgel in the area I immediately undergoes phase transition and releases loaded medicine; after the preset time, applying 9V voltage to the area II, stabilizing the temperature of the drug dressing layer by about 40 ℃, enabling the temperature-sensitive drug-loaded microgel of the area II to reach the critical phase transition temperature, and responding to the stimulus to release another drug; by analogy, targeted quantitative and timed administration can be realized.
Example 3
(1) Preparing a conductive fabric: adding 800g H into 4g of conductive carbon black powder 2 Pre-stirring for 0.5h and performing ultrasonic treatment for 1h in a mixed solvent of O and 200g of EtOH to obtain 0.4wt.% of dispersion liquid; soaking the cut nylon knitted fabric in the dispersion liquid, and then passing through a roller to ensure that the liquid penetrates into the fabric and remove residual liquid; drying and pad dyeing are carried out for 40 times repeatedly, carbon black coating nylon knitted fabrics (conductive fabrics) with good conductivity are prepared for standby, and the conductive fabrics are provided with four coating areas (areas I-IV) which independently control heating.
(2) Preparing the drug-loaded microgel: 0.2g of clay was uniformly dispersed in 10g of deionized water, and 0.535g of OEGMA and 0.965g of MEO were added in that order 2 MA, 0.2g Alg, 0.09g APS and 50. Mu.L dimethylaniline, polymerized at room temperature for 14h and then extruded dropwise onto CaCl 2 Obtaining spherical microgel with response temperature of about 40 ℃ in aqueous solution; then adjusting the molar ratio of the two comonomers to obtain microgel with response temperatures of 42 ℃, 45 ℃ and 48 ℃ in sequence; washing with deionized water for several times to remove unreacted monomer, crosslinking agent, etc.; filtering, freeze-drying, and respectively adding 4 microgels into 1.5 mg/mL -1 Vancomycin, curcumin, insulin or 0.3 mg/mL -1 Swelling the vascular endothelial growth factor solution for 24h to obtain four temperature-sensitive drug-loaded microgels respectively loaded with four different drug solutions.
(3) Preparation of the dressing: adding 1.5g of clay into 10g of deionized water, and uniformly stirring to obtain a dispersion liquid with the mass fraction of 15 wt.%; then 3g of monomer AAm, 0.18g of APS and 50 mu L of dimethylaniline are added to prepare prepolymerization liquid, the prepolymerization liquid is divided into four parts, 0.9g of the four prepared temperature-sensitive drug-carrying microgels are respectively added, and coating liquids wrapping 4 temperature-sensitive drug-carrying microgels are respectively coated in areas I-IV of the conductive fabric(shown in figure 1), reacting for 12 hours at room temperature to obtain a final product; wherein the areas of the regions are uniform and are 30 × 30mm 2 Coating liquid is distributed in a punctiform array manner for coating, the diameter of each coating point is 4mm, and the adjacent distance is 4mm; the interval between adjacent coating areas is 3mm, and the thickness of the pre-polymerization liquid coated with the temperature-sensitive medicine-carrying microgel is 1mm.
Effect verification: the prepared dressing and an external power supply are assembled into the intelligent electric heating dressing for temperature control segmented drug delivery, when the output voltage is 7V, the temperature of a fabric layer is measured to be about 50 ℃, the temperature of a drug dressing layer is increased to 40 ℃ after 100s, and the temperature-sensitive drug-loaded microgel in the area I immediately undergoes phase transition and releases loaded drugs; after the preset time, applying 9V voltage to the region II, stabilizing the temperature of the drug dressing layer to about 42 ℃, enabling the temperature-sensitive drug-loaded microgel in the region II to reach the critical phase transition temperature, and responding to the stimulus to release another drug; by analogy, targeted quantitative dosing can be achieved.
Example 4
(1) Preparing a conductive fabric: adding 500g H into 5g graphite powder 2 Pre-stirring for 0.5h and performing ultrasonic treatment for 1h in a mixed solvent of O and 500g of EtOH to obtain 0.5wt.% of dispersion liquid; soaking the cut PP non-woven fabric in the dispersion liquid, and then passing through a roller to enable the liquid to penetrate into the fabric and remove residual liquid; after drying and repeated pad dyeing for 45 times, the graphite coating PP non-woven fabric (conductive fabric) with good conductivity is prepared for standby, and the conductive fabric is provided with four coating areas (areas I-IV) which independently control heating.
(2) Preparing the drug-loaded microgel: 0.3g of clay was uniformly dispersed in 10g of deionized water, and 0.804g of OEGMA and 1.196g of MEO were added in this order 2 MA, 0.3g of Alg, 0.2g of NaPS and 60. Mu.L of dimethylaniline, which were polymerized at room temperature for 24 hours, were extruded dropwise into CaCl 2 Obtaining spherical microgel with response temperature of about 42 ℃ in aqueous solution; then adjusting the molar ratio of the two comonomers to obtain microgel with response temperatures of about 45 ℃, 48 ℃ and 50 ℃ in sequence; washing with deionized water for several times to remove unreacted monomer, crosslinking agent, etc.; filtering, freeze-drying, and respectively adding 4 microgels into 2 mg. ML -1 Cefazolin, curcumin, insulin or 0.1mg·mL -1 Swelling the epidermal cell growth factor solution for 24 hours to obtain four temperature-sensitive drug-loaded microgels respectively loaded with four different drug solutions.
(3) Preparation of the dressing: adding 2g of clay into 10g of deionized water, and uniformly stirring to obtain a solution with the mass fraction of 20 wt.%; then adding 3g of monomer AAm, 0.3g of NaPS and 60 mu L of dimethylaniline to prepare a prepolymerization solution, dividing the prepolymerization solution into four parts, respectively adding 1.0g of the four prepared temperature-sensitive drug-loaded microgels, respectively coating solutions (shown in figure 1) wrapping 4 temperature-sensitive drug-loaded microgels on the areas I-IV of the conductive fabric, and reacting at room temperature for 24h to obtain a final product; wherein the areas of the regions are consistent and 40 × 40mm 2 Coating liquid is distributed in a punctiform array manner for coating, the diameter of each coating point is 5mm, and the adjacent distance is 5mm; the interval between adjacent coating areas is 4mm, and the thickness of the pre-polymerization liquid coated with the temperature-sensitive drug-loaded microgel is 1.5mm.
Effect verification: the prepared dressing and an external power supply are assembled into the intelligent electric heating dressing for temperature control segmented drug delivery, when the output voltage is 6V, the temperature of a fabric layer is measured to be about 54 ℃, the temperature of a drug dressing layer is increased to 43 ℃ after 80s, and the sensitive drug-loaded microgel in the area I immediately undergoes phase transition and releases loaded drugs; after the preset time, 8V voltage is applied to the area II, the temperature of the drug dressing layer is stabilized by about 45 ℃, the sensitive drug-loaded microgel of the area II reaches the critical phase transition temperature, and another drug is released in response to stimulation; by analogy, targeted quantitative and timed administration can be realized.
The conductive fabric provided by the invention has a plurality of coating areas which independently control heating, the phase-change temperatures of the temperature-sensitive drug-loaded microgel in different coating areas are different, and the types of loaded drug solutions are different, in practical application, when temperature-controlled sectional administration is carried out, temperature control is carried out in sequence according to the increasing condition of the phase-change temperatures of the temperature-sensitive drug-loaded microgels, wherein the temperature-sensitive drug-loaded microgels at lower temperatures firstly release drugs, and the temperature-sensitive drug-loaded microgels at higher temperatures release drugs after being heated.
Although specific embodiments of the present invention have been described above, it will be appreciated by those skilled in the art that these are merely examples and that many variations or modifications may be made to the embodiments without departing from the principles and spirit of the invention, the scope of which is defined in the appended claims.
Claims (10)
1. The intelligent electric heating dressing is characterized by comprising an electric heating conductive fabric, wherein the electric heating conductive fabric is provided with a plurality of independently controlled heating coating areas, each coating area is provided with a medicine dressing layer, each medicine dressing layer comprises a gel matrix, temperature-sensitive medicine-carrying microgel coated in the gel matrix and medicine solution loaded in the temperature-sensitive medicine-carrying microgel, and the different medicine solutions loaded by the temperature-sensitive medicine-carrying microgel in the coating areas are different in types.
2. The intelligent electrothermal dressing according to claim 1, wherein the drug dressing layer comprises a plurality of gel units, the gel units are distributed in an array, the thickness of each gel unit is 0.2-2mm, the diameter of each gel unit is 2-5mm, and the distance between the gel units is 2-5mm.
3. The intelligent electrothermal dressing according to claim 1, wherein insulation partitions with a width of 1-5mm are reserved between the drug dressing layers of different coating areas, and the insulation partitions are coated with a gel matrix without temperature-sensitive drug-loaded microgel.
4. The preparation method of the intelligent electrothermal dressing for temperature-controlled segmented drug delivery according to any one of claims 1 to 3, characterized by comprising the following steps:
s1, soaking a fabric into a dispersion liquid containing a carbon material, taking out the fabric, penetrating the fabric through a roller to realize pad dyeing, drying the fabric, and repeating the pad dyeing for a plurality of times to prepare a conductive fabric;
s2, adding two temperature-sensitive comonomers, sodium alginate, an initiator and an accelerator into the inorganic hectorite aqueous dispersion, polymerizing for 10-24 hours at room temperature, gradually dripping the obtained polymer into a calcium chloride aqueous solution to form spherical microgel, and regulating the molar ratio of the two temperature-sensitive comonomers to obtain the spherical microgel with different response temperatures; washing the spherical microgel with deionized water, filtering, freeze-drying, respectively putting the freeze-dried spherical microgel with different response temperatures into different drug solutions, and swelling for 12-24h to prepare various temperature-sensitive drug-loaded microgels loaded with different drug solutions;
and S3, adding an acrylamide monomer, an initiator and an accelerator into the inorganic hectorite aqueous dispersion to form a pre-polymerization solution, adding the temperature-sensitive drug-loaded microgel, coating the pre-polymerization solution on the surface of the conductive fabric, respectively corresponding the temperature-sensitive drug-loaded microgel loaded with different types of drug solutions to different coating areas, reacting for 8-24 hours at room temperature to enable the pre-polymerization solution to form a gel matrix coated with the temperature-sensitive drug-loaded microgel through a polymerization reaction, and finally obtaining the intelligent electrothermal dressing for temperature-controlled segmented drug delivery.
5. The method for preparing intelligent electrothermal dressing according to claim 4, wherein in step S1, the fabric is a knitted, woven or non-woven fabric made of one or more fibers selected from cotton, nylon, polyphenylene sulfide or polypropylene; the carbon material is one or more of graphene oxide, carbon nano tubes, conductive carbon black or graphite; the mass fraction of the carbon material in the dispersion is 0.1-0.5wt.%, the solvent of the dispersion is a mixture of ethanol and water, and the volume ratio of ethanol to water is 1.
6. The method for preparing intelligent electrothermal dressing according to claim 4, wherein in step S2, the two temperature-sensitive comonomers are 2-methyl-2-acrylic acid-2- (2-methoxyethoxy) ethyl ester and oligoethylene glycol methyl ether methacrylate, and the response temperature of the spherical microgel is adjusted by adjusting the molar ratio of the two comonomers, and the change range of the response temperature is 35-60 ℃.
7. The intelligent electrothermal dressing for temperature-controlled segmented drug delivery according to claim 4The preparation method is characterized in that in the step S2, the inorganic hectorite aqueous dispersion is obtained by uniformly dispersing inorganic hectorite in deionized water, the total content of the two temperature-sensitive comonomers added is 5-20wt.% of the mass of the deionized water, the inorganic hectorite and the sodium alginate are 0.5-3wt.% of the mass of the deionized water, the concentration of the calcium chloride aqueous solution is 2 percent, and the concentration of the medicinal solution is 0.1-2 mg/mL -1 。
8. The method for preparing intelligent electrothermal dressing according to claim 4, wherein in step S2, the size of the lyophilized spherical microgel particles is 50-200 μm.
9. The method for preparing an intelligent electrothermal dressing through temperature-controlled segmented drug delivery according to claim 4, wherein in step S3, the inorganic hectorite aqueous dispersion is obtained by uniformly dispersing inorganic hectorite in water, the content of the inorganic hectorite is 5-20 wt% of the mass of the water, the content of the acrylamide monomer is 10-30 wt% of the mass of the water, and the content of the temperature-sensitive drug-loaded microgel is 10-40 wt% of the mass of the acrylamide monomer.
10. The method for preparing intelligent electrothermal dressing according to any one of claims 4 to 9, wherein in steps S2 and S3, the initiator is one or more of potassium persulfate, ammonium persulfate or sodium persulfate, and the accelerator is N, N ’ ,N ’ One or more of tetramethylethylenediamine or N, N-dimethylaniline,
wherein: in the step S2, the dosage of the initiator is 1-10 wt% of the contents of the two temperature-sensitive comonomers, and in the step S3, the dosage of the initiator is 1-10 wt% of the contents of the acrylamide monomers; the dosage of the accelerator in the step S2 is 0.2-0.8% of the volume of the pre-polymerization liquid, and the dosage of the accelerator in the step S3 is 0.2-0.8% of the volume of the pre-polymerization liquid.
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