CN106581753A - Biological hydrogel for 3D printing of skin scaffold and preparation method of biological hydrogel - Google Patents
Biological hydrogel for 3D printing of skin scaffold and preparation method of biological hydrogel Download PDFInfo
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- CN106581753A CN106581753A CN201611221871.1A CN201611221871A CN106581753A CN 106581753 A CN106581753 A CN 106581753A CN 201611221871 A CN201611221871 A CN 201611221871A CN 106581753 A CN106581753 A CN 106581753A
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
- A61L27/00—Materials for grafts or prostheses or for coating grafts or prostheses
- A61L27/14—Macromolecular materials
- A61L27/22—Polypeptides or derivatives thereof, e.g. degradation products
- A61L27/24—Collagen
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
- A61L27/00—Materials for grafts or prostheses or for coating grafts or prostheses
- A61L27/14—Macromolecular materials
- A61L27/20—Polysaccharides
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
- A61L27/00—Materials for grafts or prostheses or for coating grafts or prostheses
- A61L27/50—Materials characterised by their function or physical properties, e.g. injectable or lubricating compositions, shape-memory materials, surface modified materials
- A61L27/52—Hydrogels or hydrocolloids
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
- A61L27/00—Materials for grafts or prostheses or for coating grafts or prostheses
- A61L27/50—Materials characterised by their function or physical properties, e.g. injectable or lubricating compositions, shape-memory materials, surface modified materials
- A61L27/58—Materials at least partially resorbable by the body
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
- A61L27/00—Materials for grafts or prostheses or for coating grafts or prostheses
- A61L27/50—Materials characterised by their function or physical properties, e.g. injectable or lubricating compositions, shape-memory materials, surface modified materials
- A61L27/60—Materials for use in artificial skin
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J3/00—Processes of treating or compounding macromolecular substances
- C08J3/24—Crosslinking, e.g. vulcanising, of macromolecules
- C08J3/246—Intercrosslinking of at least two polymers
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L1/00—Compositions of cellulose, modified cellulose or cellulose derivatives
- C08L1/02—Cellulose; Modified cellulose
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61L—METHODS OR APPARATUS FOR STERILISING MATERIALS OR OBJECTS IN GENERAL; DISINFECTION, STERILISATION OR DEODORISATION OF AIR; CHEMICAL ASPECTS OF BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES; MATERIALS FOR BANDAGES, DRESSINGS, ABSORBENT PADS OR SURGICAL ARTICLES
- A61L2430/00—Materials or treatment for tissue regeneration
- A61L2430/34—Materials or treatment for tissue regeneration for soft tissue reconstruction
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J2389/00—Characterised by the use of proteins; Derivatives thereof
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J2401/00—Characterised by the use of cellulose, modified cellulose or cellulose derivatives
- C08J2401/02—Cellulose; Modified cellulose
Abstract
The invention provides biological hydrogel for 3D printing of a skin scaffold and a preparation method of the biological hydrogel and belongs to the technical field of 3D printing. The biological hydrogel is prepared from 1%-15% of NCC (nano-crystalline cellulose), 65%-98% of collagen COL and 0.01%-20% of a cross-linking agent. The method comprises steps as follows: NCC, COL and the cross-linking agent are stirred uniformly with a solution blended process, and a modified collagen skin scaffold material is prepared after the components are completely cross-linked. According to the biological hydrogel for 3D printing of the skin scaffold and the preparation method of the biological hydrogel, NCC and COL are both natural high polymers and have good biocompatibility and biodegradability; NCC as reinforced filler has a combined action with the cross-linking agent, so that elongation at break, strength, toughness, heat resistance and other properties of modified collagen are improved, and additional value of plant fiber is also improved. The problem of poorer biocompatibility or insufficient mechanical property of a conventional 3D skin scaffold printing material is solved.
Description
Technical field
The invention belongs to 3D printing technique field, is related to a kind of biological hydrogel and its system for dermal scaffold 3D printing
Preparation Method, particularly relates to one kind and has biocompatibility, biodegradability, biological activity and meet dermal scaffold power
Learn composite of performance and preparation method thereof.
Background technology
Skin is the maximum organ of human body, and large area is externally exposed the skin histology moment of environment may sustain damage,
Ulcer is to cause the main cause that skin injury and function are lost wherein caused by burn, mechanical trauma and chronic disease, right
In any full thickness dermal with diameter greater than 4cm, human body all cannot completely be healed by itself.Organizational project in recent years
Its treatment that develops into of technology provides new approaches, becomes research in recent years focus.Organization engineering skin is referred to by by cell or carefully
Extracellular matrix or both combines the skin products of composition jointly.It is molded using low temperature moulding and model more, complex steps, each process
Precision is difficult to hold, and the support performance difference of making is very big, can not arbitrarily change the trend and hole of support, 3D printing technique
Appear as solve the above problems there is provided may.3D printer can precisely be printed according to default model, with molding it is rapid,
The advantages of sample standard, scale volume production, and the support of different scales can be printed by changing various parameters.3D printing skin
The material that support is used plays an important role in organization engineering skin structure, and the research and selection of timbering material are artificial skin
The important research content of skin, while also govern the development of 3D printing tissue engineering bracket.
The 3D biometric print materials of skin tissue engineering are divided into synthetic material and the big class of natural macromolecular material two.People
Geosynthetics include polyactide, PHA, Merlon, polylactic acid, polyglycolic acid etc..Synthetic material has
Have good mechanical property and plasticity, easy printing shaping, but cause inflammation around more its catabolite, biocompatibility compared with
Difference.Natural macromolecular material includes collagen, shitosan, cellular matrix etc..Natural polymer has good biocompatibility, life
Biodegradable and biological activity, can preferably induce the self-recovery of compromised skin.But natural macromolecular material mechanical property
Can be poor, and in vivo degradation speed is too fast in the presence of various enzymes, support has caved in when cambium does not also grow good.Cause
This, finds a kind of material with good biocompatibility, biodegradability, biological activity and mechanical property particularly important.
Once solving the problem of materials of 3D printing dermal scaffold, the technology is by the treatment for quickly applying to skin injury.
The content of the invention
The purpose of the present invention is the deficiency existed for above-mentioned prior art, the invention provides a kind of be used for dermal scaffold
Biological hydrogel of 3D printing and preparation method thereof, can slow down degradation speed of the collagen in human body, can further improve biology
The mechanical property and stability of hydrogel.
The technical scheme is that：A kind of biological hydrogel for dermal scaffold 3D printing, it is characterised in that described
Biological hydrogel is made up of the raw material of following solid masses percentage composition：NCC (nano-celluloses) 1～15%, COL (collagen) 65
～98%, cross-linking agent 0.01%～20%.
The cross-linking agent is any one in genipin, heparin sulfate, glutaraldehyde.
Described COL refers to the mixing of I type, II type or both.
The NCC is isolated from natural plant fibre or Microcrystalline Cellulose, a diameter of 1～20nm of NCC, length
For 100～1500nm.
A kind of preparation method of the biological hydrogel for dermal scaffold 3D printing, it is characterised in that including following operation
Step：
(1) solvent is prepared：Using the one kind in aqueous acetic acid, hexafluoroisopropanol, the alkane of Isosorbide-5-Nitrae-dioxy six or arbitrarily several mixing；
(2) NCC, COL are placed in the solvent of step 1 and are blended, blending temperature is 1～25 DEG C, the blending time is 6～48h,
NCC-COL blended liquids are obtained after 200～2000rpm of mixing speed；
(3) in NCC-COL blended liquids cross-linking agent being added in step 2,1～4h, stirring speed are stirred under the conditions of 1～25 DEG C
200～2000rpm of degree, 4 DEG C stand overnight and treat that its is full cross-linked, obtain the enhanced cross-linking modified collagen protein biology water-settings of NCC
Glue；
(4) obtained biological hydrogel is carried out under the conditions of 1～10 DEG C sterile storage.
Beneficial effects of the present invention are：
(1) NCC used in the present invention from many natural plants, agricultural waste material, or can pass through from from Microcrystalline Cellulose
Conventional chemical processes are obtained, and improve the surcharge of Plant fiber；
(2) NCC used in the present invention is 1～20nm of diameter, 100～1500nm of length, and so little particle diameter is more convenient for from 3D
Extrude in shower nozzle；
(3) NCC used in the present invention and collagen have good biodegradability and biocompatibility, additionally, collagen is used
Make dermal scaffold material and there is good biological activity；
(4) collagen is carried out using cross-linking agent cross-linking modified, the mechanical strength of collagen itself can be improved, and improve the steady of collagen
It is qualitative, degradation speed of the collagen in human body can be slowed down；
(5) NCC as strengthen packing material, because its own high aspect ratio and high Young's modulus can further improve Biological water
The mechanical property of gel.
Specific embodiment
Below by embodiment, the present invention is further illustrated：
Specific embodiment 1
(1) the solid masses percentage composition of each raw material：NCC2%, COL (I type) 97%, heparin sulfate 1%；
(2) solvent for being used is the aqueous acetic acid of 0.5mol/L, and solute gross mass is 2 with the mass ratio of solvent：98；
(3) NCC and COL is blended 10h in 4 DEG C, and mixing speed 1000rpm adds afterwards 4 DEG C of blending 1h of heparin sulfate, stands overnight；
(4) 1 DEG C of sterile storages are standby.
Specific embodiment 2
(1) the solid masses percentage composition of each raw material：NCC6%, COL (I type and II type mix) 92%, heparin sulfate 4%；
(2) solvent for being used is the mass ratio of the mixed liquor of hexafluoroisopropanol and aqueous acetic acid, solute gross mass and solvent
For 4：96；
(3) NCC and COL is blended 12h in 8 DEG C, and mixing speed 800rpm adds afterwards 4 DEG C of blending 2h of heparin sulfate, stands overnight；
(4) 4 DEG C of sterile storages are standby.
Specific embodiment 3
(1) the solid masses percentage composition of each raw material：NCC 10%, COL (I type and II type mix) 82%, heparin sulfate 8%；
(2) solvent for being used is the quality of the mixed liquor of the alkane of Isosorbide-5-Nitrae-dioxy six and aqueous acetic acid, solute gross mass and solvent
Than for 7：93；
(3) NCC and COL is blended 24h in 12 DEG C, and mixing speed 800rpm adds afterwards 12 DEG C of blending 2h of heparin sulfate, stood
Night；
(4) 6 DEG C of sterile storages are standby.
Specific embodiment 4
(1) the solid masses percentage composition of each raw material：NCC 10%, COL (I type and II type mix) 82%, genipin 8%；
(2) solvent for being used is the aqueous acetic acid of 0.5mol/L, and solute gross mass is 2 with the mass ratio of solvent：98；
(3) NCC and COL is blended 15h in 14 DEG C, and mixing speed 800rpm adds afterwards 14 DEG C of blending 2h of heparin sulfate, stood
Night；
(4) 2 DEG C of sterile storages are standby.
Specific embodiment 5
(1) the solid masses percentage composition of each raw material：NCC 10%, COL (I type and II type mix) 82%, genipin 8%；
(2) solvent for being used is the mass ratio of the mixed liquor of hexafluoroisopropanol and aqueous acetic acid, solute gross mass and solvent
For 8：92；
(3) NCC and COL is blended 12h in 8 DEG C, and mixing speed 600rpm adds afterwards 8 DEG C of blending 2h of heparin sulfate, stands overnight；
(4) 3 DEG C of sterile storages are standby.
Specific embodiment 6
(1) weight/mass percentage composition of each raw material：NCC6%, COL (I type and II type mix) 91%, glutaraldehyde 3%；
(2) solvent for being used be hexafluoroisopropanol, the alkane of Isosorbide-5-Nitrae-dioxy six and aqueous acetic acid mixed liquor, solute gross mass with it is molten
The mass ratio of agent is 15：85；
(3) NCC and COL is blended 12h in 8 DEG C, and mixing speed 600rpm adds afterwards 8 DEG C of blending 2h of heparin sulfate, stands overnight；
(4) 5 DEG C of sterile storages are standby.
Specific embodiment 7
(1) weight/mass percentage composition of each raw material：NCC 4%, COL (I type and II type mix) 86%, glutaraldehyde 10%；
(2) solvent for being used be hexafluoroisopropanol, the alkane of Isosorbide-5-Nitrae-dioxy six and aqueous acetic acid mixed liquor, solute gross mass with it is molten
The mass ratio of agent is 10：90；
(3) NCC and COL is blended 12h in 6 DEG C, and mixing speed 500rpm adds afterwards 6 DEG C of blending 2h of heparin sulfate, stands overnight；
(4) 7 DEG C of sterile storages are standby.
The biological hydrogel of preparation is made into cylindrical, is highly 12mm, a diameter of 20mm, 25 DEG C of temperature is relatively wet
Mechanical property such as following table under the conditions of degree 50%：
| Title | Compression failure intensity |
| Pure collagen hydrogels | 1.9Kpa |
| The gained biological hydrogel of specific embodiment one | 18.4KPa |
| The gained biological hydrogel of specific embodiment two | 20.1KPa |
| The gained biological hydrogel of specific embodiment three | 19.6KPa |
| The gained biological hydrogel of specific embodiment four | 17.2KPa |
| The gained biological hydrogel of specific embodiment five | 22.3KPa |
| The gained biological hydrogel of specific embodiment six | 15.7KPa |
| The gained biological hydrogel of specific embodiment seven | 18.9KPa |
Claims (5)
1. a kind of biological hydrogel for dermal scaffold 3D printing, it is characterised in that the biological hydrogel is by following solid
The raw material composition of weight/mass percentage composition：NCC 1～15%, COL 65～98%, cross-linking agent 0.01%～20%.
2. a kind of biological hydrogel for dermal scaffold 3D printing according to claim 1, it is characterised in that：The friendship
Connection agent is any one in genipin, heparin sulfate, glutaraldehyde.
3. a kind of biological hydrogel for dermal scaffold 3D printing according to claim 1, it is characterised in that：Described
COL refers to the mixing of I type, II type or both.
4. a kind of biological hydrogel for dermal scaffold 3D printing according to claim 1, it is characterised in that：It is described
NCC is isolated from natural plant fibre or Microcrystalline Cellulose, a diameter of 1～20nm of NCC, length is 100～
1500nm。
5. a kind of a kind of preparation method of the biological hydrogel for dermal scaffold 3D printing as claimed in claim 1, it is special
Levy and be, including following operating procedure：
(1) solvent is prepared：Using the one kind in aqueous acetic acid, hexafluoroisopropanol, the alkane of Isosorbide-5-Nitrae-dioxy six or arbitrarily several mixing；
(2) NCC, COL are placed in the solvent of step 1 and are blended, blending temperature is 1～25 DEG C, the blending time is 6～48h,
NCC-COL blended liquids are obtained after 200～2000rpm of mixing speed；
(3) in NCC-COL blended liquids cross-linking agent being added in step 2,1～4h, stirring speed are stirred under the conditions of 1～25 DEG C
200～2000rpm of degree, 4 DEG C stand overnight and treat that its is full cross-linked, obtain the enhanced cross-linking modified collagen protein biology water-settings of NCC
Glue；
(4) obtained biological hydrogel is carried out under the conditions of 1～10 DEG C sterile storage.
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| Application Number | Priority Date | Filing Date | Title |
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| CN201611221871.1A CN106581753A (en) | 2016-12-27 | 2016-12-27 | Biological hydrogel for 3D printing of skin scaffold and preparation method of biological hydrogel |
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|---|---|---|---|
| CN201611221871.1A CN106581753A (en) | 2016-12-27 | 2016-12-27 | Biological hydrogel for 3D printing of skin scaffold and preparation method of biological hydrogel |
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107998451A (en) * | 2018-01-30 | 2018-05-08 | 扬州大学 | A kind of 3D printing preparation method of skin tissue engineering scaffold and the vitro cytotoxicity test method of the stent |
| CN108114324A (en) * | 2018-01-30 | 2018-06-05 | 扬州大学 | A kind of vitro cytotoxicity test method for the method and the stent that skin tissue engineering scaffold is prepared based on 3D biometric print technologies |
| CN109758608A (en) * | 2019-01-17 | 2019-05-17 | 广东省生物工程研究所（广州甘蔗糖业研究所） | Printable composite hydrogel and preparation method and application with high tenacity |
| CN111031792A (en) * | 2017-06-01 | 2020-04-17 | Ucl商业有限公司 | Low temperature preservation |
| CN113018517A (en) * | 2021-03-29 | 2021-06-25 | 深圳市创想三维科技有限公司 | 3D printing skin stent and preparation method and application thereof |
| WO2022069772A1 (en) | 2020-10-02 | 2022-04-07 | Viscofan, S.A. | Collagen ink for 3d printing |
| CN114306750A (en) * | 2021-12-08 | 2022-04-12 | 扬州大学 | H-CNC multi-orientation coaxial artificial blood vessel and preparation method thereof |
| CN115845133A (en) * | 2022-12-26 | 2023-03-28 | 深圳钧兴生物科技有限公司 | Collagen-based biological printing material and preparation method thereof |
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Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111031792A (en) * | 2017-06-01 | 2020-04-17 | Ucl商业有限公司 | Low temperature preservation |
| CN107998451A (en) * | 2018-01-30 | 2018-05-08 | 扬州大学 | A kind of 3D printing preparation method of skin tissue engineering scaffold and the vitro cytotoxicity test method of the stent |
| CN108114324A (en) * | 2018-01-30 | 2018-06-05 | 扬州大学 | A kind of vitro cytotoxicity test method for the method and the stent that skin tissue engineering scaffold is prepared based on 3D biometric print technologies |
| CN109758608A (en) * | 2019-01-17 | 2019-05-17 | 广东省生物工程研究所（广州甘蔗糖业研究所） | Printable composite hydrogel and preparation method and application with high tenacity |
| WO2022069772A1 (en) | 2020-10-02 | 2022-04-07 | Viscofan, S.A. | Collagen ink for 3d printing |
| CN113018517A (en) * | 2021-03-29 | 2021-06-25 | 深圳市创想三维科技有限公司 | 3D printing skin stent and preparation method and application thereof |
| CN114306750A (en) * | 2021-12-08 | 2022-04-12 | 扬州大学 | H-CNC multi-orientation coaxial artificial blood vessel and preparation method thereof |
| CN114306750B (en) * | 2021-12-08 | 2022-08-26 | 扬州大学 | H-CNC multi-orientation coaxial artificial blood vessel and preparation method thereof |
| CN115845133A (en) * | 2022-12-26 | 2023-03-28 | 深圳钧兴生物科技有限公司 | Collagen-based biological printing material and preparation method thereof |
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Application publication date: 20170426 |