CN1944495A - Water gel containing natural high molecule and its radiation preparing method - Google Patents
Water gel containing natural high molecule and its radiation preparing method Download PDFInfo
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- CN1944495A CN1944495A CN200610113539.3A CN200610113539A CN1944495A CN 1944495 A CN1944495 A CN 1944495A CN 200610113539 A CN200610113539 A CN 200610113539A CN 1944495 A CN1944495 A CN 1944495A
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- Medicinal Preparation (AREA)
- Materials For Medical Uses (AREA)
Abstract
The present invention provides one kind of water gel containing natural high molecular material and its preparation process. The water gel has cross-linking degree of 70-95 % and water absorption of 500-80000 %, and contains natural high molecular material or its derivative selected from chitin, chitin derivative, chitosan, chitosan derivative, carrageenin, etc. The water gel may have synthetic high molecular material, inorganic filler, cross-linking sensitizer, medicine and other assistant added. It is prepared through radiation cross-linking, with the radiation dosage being 10-40 kGy. The water gel of the present invention has high water absorption, high flexibility, good medicine slow releasing performance, and may be used in wound dressing, etc.
Description
Technical field
The present invention relates to hydrogel, relate in particular to a kind of water gel containing natural high molecule and preparation method thereof.This hydrogel is applicable to but is not limited to biomedical materials field.
Background technology
Hydrogel is a kind of macromolecular material that is similar to vital tissues, it by in water, not dissolving but the macromolecule network and the water of swellable form, because of it has performances such as formability, water absorbability, film-forming properties, cohesiveness, thermal capacity be big, multiple fields such as widespread use food, medicine.One of important use of medical aquogel is as wound dressing, this wound dressing that is applicable to the protecting wound surface of wound, burn and operative incision is compared with traditional dressing such as gauze has lot of advantages, be described as " desirable dressing ", these advantages comprise: (1) is transparent, tough, flexible; (2) abundant absorbed body fluid and prevent its loss; (3) can effectively shield bacterium; (4) good but be of value to skin growth with adhering skin; (5) can allow oxygen penetration apply film and arrive wound surface, accelerating wound healing; (6) but embedding medicinal; (7) material is transparent thereby can observe the wound healing process at any time; (8) can prevent that the wound hypertrophy from forming scabbing; (9) inviscid to wound, thereby removal/replacing is applied film and can not damaged newborn epidermis easily; (10) no antigen reaction; (11) no anaphylaxis; (12) store easily and use.
Application number is that the open text (CN1616116A) of 200410066999.6 Chinese patent application provides a kind of and is made up of Polyvinylpyrolidone (PVP), polyvinyl alcohol, radiation sensitive agent, softening agent, pH regulator agent and water, with the crosslinked hydrogel wound dressing that forms of cobalt-60 radiosterilize.Claims of this technology and all embodiment show that its wound dressing is is main base material with polyvinyl alcohol, produce for convenience and the irradiation two procedures between transportation, before the irradiation moulding, increased freezing process.The hydrogel of polyvinyl alcohol base material can pass through circulating frozen-freezing process and generate the better physical gel of intensity, but the water absorbing properties of polyvinyl alcohol hydrogel is not ideal, and it is opaque with the freezing method preparation gel to be become, and causes water-absorbent further to reduce.In addition, the radiation processing technology that this invention provides is not satisfactory, and radiation sensitive agent, softening agent, the pH regulator agent adopted in its prescription are all unfavorable to the radiation crosslinking of gel, cause the degree of crosslinking of product in the embodiment all to be lower than 45%.So the hydrogel intensity of low crosslinking degree is inevitable bad, and a large amount of colloidal sol and transudate are blended in clinically and perhaps can produce many problems.
Chinese patent ZL 00107403.2 (CN1121876C) has introduced raw material and has been selected from methacrylic acid-β hydroxyl ethyl ester, acrylate, polyvinylpyrrolidone, polyvinyl alcohol, polyoxyethylene, polyoxyethylene glycol, with electron beam or gamma-radiation radiation crosslinking form, water ratio is 75-95%, degree of crosslinking is 75-95%, water-intake rate is hydrogel of 200-400% and preparation method thereof, this hydrogel and air-permeable envelope, separate-type paper are composited and are the wound dressing goods.This invention is the early stage technology of aquogel type wound dressing research and development, similar technology is gone into operation in a plurality of countries such as China, Japan, Poland, but popularization along with this product, the patient is to intensity, the snappiness of goods, especially water-retaining capacity is had higher requirement, and related prescription and the technology of this invention can't satisfy these requirements.
Summary of the invention
The object of the invention be to provide a kind of have high water-retaining capacity and speed, better gel-strength and biocompatibility, the hydrogel formulation that is specially adapted to medical science and beauty treatment fields and synthesis technique arranged.
Hydrogel of the present invention mainly contains 3～20% natural polymer or derivatives thereof by weight, and 0～15% synthetic macromolecule, and 80～95% water make through radiation crosslinking.The degree of crosslinking of this hydrogel is 70～95%, water-intake rate is 500～80000%, and described natural polymer or derivatives thereof can be selected from one or more in the following polymer: chitin and chitin derivativ are (as carboxymethyl chitin, propyloic chitin etc.), chitosan and chitosan derivatives are (as cm-chitosan, carboxyetbyl chitosan etc.), carrageenin and carboxymethyl carrageenin, derivatived cellulose is (as carboxymethyl cellulose, hydroxypropylcellulose, Vltra tears etc.), starch and starch derivative (carboxymethyl starch etc.), sodium alginate, melon glue and carboxymethyl melon glue, collagen protein, hyaluronic acid etc.Described synthetic macromolecule can be selected from one or more in methacrylic acid-β hydroxyl ethyl ester, acrylate, polyvinylpyrrolidone, polyvinyl alcohol, polyoxyethylene, the polyoxyethylene glycol etc.
Can also add mineral filler, crosslinking sensitizer, and other auxiliary agent such as medicine as required.Wherein, mineral filler can be selected from gac, white carbon black, polynite, carbon nanotube etc., and addition is no more than 10% of hydrogel gross weight; Crosslinking sensitizer can be selected from N, N-dimethyl bisacrylamide, Ethylene glycol dimethacrylate etc., and its usage quantity is no more than 3% (weight) of macromolecular material (comprising natural polymer and synthetic macromolecule); Other auxiliary agent comprises sanitas, wetting Agent for Printing Inks, the medicine that adds according to the clinical treatment needs and the component that helps drug release etc., for example have the effective constituent of Chinese medicine pseudo-ginseng, the root of Dahurain angelica of antisepsis and anti-inflammation, analgesic activity and BSP etc., and medicines such as the special efficacy that is usually used in broad spectrum antibiotic that wound disposes or hospital and provides is burnt, scalded, wound.Usually the content of antimicrobial drug in hydrogel that adds is 0.1～1% (weight), and other medicines content is 1～5% (weight).
Hydrogel of the present invention adopts electron beam or gamma-radiation radiation crosslinking to form by with natural polymer or derivatives thereof, synthetic macromolecule, water and other component blend then.Concrete preparation technology comprises the steps:
(1) with natural polymer or derivatives thereof, synthetic macromolecule, components such as mineral filler of adding under the necessary situation and crosslinking sensitizer mix with water under heating or room temperature condition, adopt technology such as high-speed stirring, evacuation and centrifugal degassing that each component is mixed in case of necessity;
(2) mixed solution is packed;
(3) radiation crosslinking;
(4) the fixed postprocessing working procedures according to product-use is as drying, pulverizing, can etc.
If need to add mineral filler, can also realize the uniform distribution of nano grade inorganic filler in hydrogel substrate with the original position composite methods in step (1).
If this hydrogel cuts the dress box, and then packs as wound dressing after step (2) is coated base materials such as non-woven fabrics, air-permeable envelope with mixed solution.Use for convenience, before cutting or packing, can attach separate-type paper or stripping film, before this wound dressing is affixed on the affected part, this film is thrown off in the one side that does not attach base material.
Step (3) can adopt dosage be 10～40kGy the cobalt source (
60The Co gamma-radiation) or rumbatron (electron beam) irradiation, can also adopt the method for ultraviolet light irradiation.
If powder, the sponge-gel of the special water-retaining capacity of preparation can directly be used or invest on the porous substrate after step (4) be with gel drying, pulverizing and use.
If preparation paste hydrogel can be sterilized after step (4) is with the gel can, also carry out irradiation after (2) can set by step, the crosslinked of sample and one step of sterilization are finished.
Hydrogel of the present invention has higher water-absorbent, snappiness preferably, and medicine is had sustained release performance preferably.Because the natural polymer or derivatives thereof is polyelectrolyte, thereby these hydrogels that contain natural polymer of synthetic have pH, electricity, temperature sensitivity etc., and purposes is widely arranged.In addition, because chitosan and derivative thereof have germ resistance, the hydrogel that contains chitosan and derivative thereof also has anti-microbial activity.
Hydrogel of the present invention adopts the method for pure natural polymer or natural polymer and synthetic macromolecule radiation crosslinking in the aqueous solution, can make the hydrogel water-intake rate bring up to tens even hundred times, especially the rate of water absorption at initial stage improves greatly, can effectively absorb wound fluid, and then quicken wound healing.In addition, be that base material synthetic hydrogel also has better biocompatibility and Biodegradable with natural polymer, the hydrogel that contains chitosan and derivative thereof also has anti-microbial activity, is a kind of material of environment-friendly type.
With the hydrogel of method of radiating preparation because pure, the good biocompatibility of system is especially suitable for use as medical material.Because the diversity and the preparation method of component of the present invention have better controllability, not only can prepare membranaceous hydrogel according to the present invention, can also be prepared into shapes such as microcapsule, paste, sponge, powder, thereby have better absorption, adsorptive power, this concerning hydrogel as extremely crucial the purposes such as pharmaceutical carrier, slow-releasing system and blood, tissue juice absorbing material.Except that medical material, hydrogel of the present invention can also be developed serial cosmetics, as facial mask, beauty-care gel etc.
Embodiment
Embodiment 1
After polyvinyl alcohol/carboxyetbyl chitosan/water mixed with 10/3/87 weight ratio, inject the encapsulation of mould final vacuum, use electron beam irradiation 25kGy, the hydrogel that obtains has germ resistance, water-intake rate is 20000%, reached swelling equilibrium in 2 hours, and tensile strength is compared with pure polyvinyl alcohol gel with elongation at break and is all improved more than 1 times.
Embodiment 2
After polyvinylpyrrolidone/carboxymethyl cellulose/water mixed with 5/5/90 weight ratio, inject the encapsulation of mould final vacuum, with gamma-radiation irradiation 25kGy, the hydrogel that obtains has ideal intensity, does not have bubble, and water-intake rate is 10000%.
Embodiment 3
After carboxymethyl cellulose/gac/water mixed with 15/5/80 weight ratio, inject the encapsulation of mould final vacuum, with gamma-radiation irradiation 25kGy, the hydrogel intensity that contains inorganic materials that obtains is compared with pure carboxymethyl cellulose (CMC) hydrogel and is improved more than 2 times, do not have bubble, and water-retaining capacity is suitable with pure CMC hydrogel.
Embodiment 4
The solution that will prepare by embodiment 1-3 component, after injecting the bottom and being placed with the polyester container of polyethylene breathable film, the top attaches the polyester film post heat-seal, cross-linking radiation forms the membrane-like wound dressing.
Embodiment 5
After polyvinylpyrrolidone/amylopectin/water and broad spectrum antibiotic mixed with the 3/15/81.9/0.1 weight ratio, seal after being filled to plastics tubing, forming water-intake rate with gamma-radiation irradiation 15kGy is 200 times paste hydrogel.
Embodiment 6
Hydroxypropylcellulose/linking agent/water is mixed with the 10/0.3/94.7 weight ratio, coat on the composite membrane of air-permeable envelope and non-woven fabrics, the opposite side of composite membrane attaches one deck separate-type paper, cut the final vacuum encapsulation, use gamma-radiation irradiation 40kGy subsequently, obtain flexibility, ventilation property, the good slim wound dressing of water-absorbent.
Embodiment 7
After amylopectin/carboxymethyl cellulose/water mixed with 3/5/92 weight ratio, under the condition of continuously stirring, use electron accelerator irradiation 30kGy, obtain thick solution, with vacuum spray drying legal system powdered.
Embodiment 8
Vltra tears/water is mixed with 20/80 weight percent, behind gamma-radiation irradiation 20kGy, make microgel with traditional microcapsule preparation technology, embedding content is the suitable medicine of 3% (weight), one or more medicines as the effective constituent and the BSP of Chinese medicine pseudo-ginseng, the root of Dahurain angelica, be dried then, sterilize, make medicine controlled releasing system with pH and temperature sensitivity.
The foregoing description the cited case has embodied aim of the present invention, promptly adjust hydrogel formulation and technology by different purposes, have good water absorbent rate, rate of water absorption, ventilation property, biocompatibility, aseptic with preparation, further can have the medical aquogel that snappiness, germ resistance, environmental stimulus responsiveness etc. help wound healing or disease treatment.Be not limited only to the foregoing description but the present invention protects, any modification of making according to spirit of the present invention all belongs to protection category of the present invention.
Claims (10)
1. hydrogel contains by weight 3～20% natural polymer or derivatives thereof, 0～15% synthetic macromolecule and 80～95% water, makes through radiation crosslinking; The degree of crosslinking of this hydrogel is 70～95%, and water-intake rate is 5～800 times; Described natural polymer or derivatives thereof is selected from one or more in the following polymer: chitin, carboxymethyl chitin, propyloic chitin, chitosan, cm-chitosan, carboxyetbyl chitosan, carrageenin, carboxymethyl carrageenin, carboxymethyl cellulose, hydroxypropylcellulose, Vltra tears, starch, carboxymethyl starch, sodium alginate, melon glue, carboxymethyl melon glue, collagen protein, hyaluronic acid; Described synthetic macromolecule is selected from one or more in methacrylic acid-β hydroxyl ethyl ester, acrylate, polyvinylpyrrolidone, polyvinyl alcohol, polyoxyethylene, the polyoxyethylene glycol.
2. hydrogel as claimed in claim 1 is characterized in that, described hydrogel is that gamma-radiation or the crosslinking electron beam irradiation of 10～40kGy forms by dosage.
3. hydrogel as claimed in claim 1 is characterized in that, also contains in the following material one or more in the described hydrogel: mineral filler, crosslinking sensitizer and other auxiliary agent.
4. hydrogel as claimed in claim 3 is characterized in that described mineral filler is selected from one or more in gac, white carbon black, polynite, the carbon nanotube, and its content is no more than 10% of hydrogel gross weight.
5. hydrogel as claimed in claim 3 is characterized in that described crosslinking sensitizer is N, N-dimethyl bisacrylamide and/or Ethylene glycol dimethacrylate, and its content is no more than 3% of macromolecular material weight.
6. hydrogel as claimed in claim 3 is characterized in that, described other auxiliary agent is selected from sanitas, wetting Agent for Printing Inks, medicine and helps the component of drug release.
7. hydrogel as claimed in claim 6, it is characterized in that, described medicine is that content is the antimicrobial drug of 0.1～1% (weight), and/or content is the Chinese medicine pseudo-ginseng with antisepsis and anti-inflammation, analgesic activity of 1～5% (weight), the effective constituent of the root of Dahurain angelica and one or more medicines in the BSP.
8. the preparation method of the described hydrogel of arbitrary claim in the claim 1～7, each component and the water of described hydrogel are mixed under heating or room temperature condition, pack then and carry out radiation crosslinking, carry out corresponding postprocessing working procedures according to product-use at last.
9. hydrogel preparation method as claimed in claim 8 is characterized in that, uses
60The electron beam that Co gamma-radiation or rumbatron produce carries out radiation, and dosage is 10～40kGy.
10. hydrogel wound dressing is made up of non-woven fabrics and/or air-permeable envelope base material and hydrogel layer, and wherein hydrogel is the described hydrogel of arbitrary claim in the claim 1～7.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
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