CN116942921A - Magnesium-containing degradable injection hydrogel bone repair material and preparation method thereof - Google Patents
Magnesium-containing degradable injection hydrogel bone repair material and preparation method thereof Download PDFInfo
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- CN116942921A CN116942921A CN202310960872.1A CN202310960872A CN116942921A CN 116942921 A CN116942921 A CN 116942921A CN 202310960872 A CN202310960872 A CN 202310960872A CN 116942921 A CN116942921 A CN 116942921A
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- magnesium
- biodegradable
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- hydrogel
- repair material
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- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 title claims abstract description 113
- 229910052749 magnesium Inorganic materials 0.000 title claims abstract description 94
- 239000011777 magnesium Substances 0.000 title claims abstract description 94
- 210000000988 bone and bone Anatomy 0.000 title claims abstract description 80
- 239000000017 hydrogel Substances 0.000 title claims abstract description 73
- 239000000463 material Substances 0.000 title claims abstract description 65
- 238000002347 injection Methods 0.000 title claims abstract description 35
- 239000007924 injection Substances 0.000 title claims abstract description 35
- 238000002360 preparation method Methods 0.000 title claims abstract description 15
- 239000002245 particle Substances 0.000 claims abstract description 41
- 229920002988 biodegradable polymer Polymers 0.000 claims abstract description 28
- 239000004621 biodegradable polymer Substances 0.000 claims abstract description 28
- 229910052751 metal Inorganic materials 0.000 claims abstract description 28
- 239000002184 metal Substances 0.000 claims abstract description 28
- 239000012530 fluid Substances 0.000 claims abstract description 27
- 239000000843 powder Substances 0.000 claims abstract description 25
- 239000000243 solution Substances 0.000 claims abstract description 23
- UXVMQQNJUSDDNG-UHFFFAOYSA-L Calcium chloride Chemical compound [Cl-].[Cl-].[Ca+2] UXVMQQNJUSDDNG-UHFFFAOYSA-L 0.000 claims abstract description 21
- 235000013927 calcium gluconate Nutrition 0.000 claims abstract description 21
- 239000004227 calcium gluconate Substances 0.000 claims abstract description 21
- 229960004494 calcium gluconate Drugs 0.000 claims abstract description 21
- NEEHYRZPVYRGPP-UHFFFAOYSA-L calcium;2,3,4,5,6-pentahydroxyhexanoate Chemical compound [Ca+2].OCC(O)C(O)C(O)C(O)C([O-])=O.OCC(O)C(O)C(O)C(O)C([O-])=O NEEHYRZPVYRGPP-UHFFFAOYSA-L 0.000 claims abstract description 21
- IXPNQXFRVYWDDI-UHFFFAOYSA-N 1-methyl-2,4-dioxo-1,3-diazinane-5-carboximidamide Chemical compound CN1CC(C(N)=N)C(=O)NC1=O IXPNQXFRVYWDDI-UHFFFAOYSA-N 0.000 claims abstract description 18
- 235000010413 sodium alginate Nutrition 0.000 claims abstract description 18
- 239000000661 sodium alginate Substances 0.000 claims abstract description 18
- 229940005550 sodium alginate Drugs 0.000 claims abstract description 18
- 238000000034 method Methods 0.000 claims abstract description 10
- 238000003756 stirring Methods 0.000 claims abstract description 10
- 238000002156 mixing Methods 0.000 claims abstract description 8
- 239000000126 substance Substances 0.000 claims abstract description 8
- QORWJWZARLRLPR-UHFFFAOYSA-H tricalcium bis(phosphate) Chemical compound [Ca+2].[Ca+2].[Ca+2].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O QORWJWZARLRLPR-UHFFFAOYSA-H 0.000 claims description 15
- 239000002994 raw material Substances 0.000 claims description 13
- 239000007788 liquid Substances 0.000 claims description 10
- 238000010146 3D printing Methods 0.000 claims description 8
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 claims description 7
- 229960005069 calcium Drugs 0.000 claims description 7
- 229910052791 calcium Inorganic materials 0.000 claims description 7
- 239000011575 calcium Substances 0.000 claims description 7
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 claims description 6
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 claims description 6
- YMWUJEATGCHHMB-UHFFFAOYSA-N Dichloromethane Chemical compound ClCCl YMWUJEATGCHHMB-UHFFFAOYSA-N 0.000 claims description 6
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 6
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims description 6
- 229920001577 copolymer Polymers 0.000 claims description 6
- 238000005516 engineering process Methods 0.000 claims description 6
- 239000011259 mixed solution Substances 0.000 claims description 6
- 239000003960 organic solvent Substances 0.000 claims description 6
- 229910052725 zinc Inorganic materials 0.000 claims description 6
- 239000011701 zinc Substances 0.000 claims description 6
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 5
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 5
- 229910052709 silver Inorganic materials 0.000 claims description 5
- 239000004332 silver Substances 0.000 claims description 5
- JHIVVAPYMSGYDF-UHFFFAOYSA-N cyclohexanone Chemical compound O=C1CCCCC1 JHIVVAPYMSGYDF-UHFFFAOYSA-N 0.000 claims description 4
- 230000008014 freezing Effects 0.000 claims description 4
- 238000007710 freezing Methods 0.000 claims description 4
- 238000001291 vacuum drying Methods 0.000 claims description 4
- RYHBNJHYFVUHQT-UHFFFAOYSA-N 1,4-Dioxane Chemical compound C1COCCO1 RYHBNJHYFVUHQT-UHFFFAOYSA-N 0.000 claims description 3
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 3
- 239000002253 acid Substances 0.000 claims description 3
- 229910052742 iron Inorganic materials 0.000 claims description 3
- 229910052719 titanium Inorganic materials 0.000 claims description 3
- 239000010936 titanium Substances 0.000 claims description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 2
- XDTMQSROBMDMFD-UHFFFAOYSA-N Cyclohexane Chemical compound C1CCCCC1 XDTMQSROBMDMFD-UHFFFAOYSA-N 0.000 claims description 2
- 229920002732 Polyanhydride Polymers 0.000 claims description 2
- 229920000954 Polyglycolide Polymers 0.000 claims description 2
- 229920001710 Polyorthoester Polymers 0.000 claims description 2
- 239000001506 calcium phosphate Substances 0.000 claims description 2
- 229910000389 calcium phosphate Inorganic materials 0.000 claims description 2
- 235000011010 calcium phosphates Nutrition 0.000 claims description 2
- 239000000378 calcium silicate Substances 0.000 claims description 2
- 229910052918 calcium silicate Inorganic materials 0.000 claims description 2
- OYACROKNLOSFPA-UHFFFAOYSA-N calcium;dioxido(oxo)silane Chemical compound [Ca+2].[O-][Si]([O-])=O OYACROKNLOSFPA-UHFFFAOYSA-N 0.000 claims description 2
- 229910052802 copper Inorganic materials 0.000 claims description 2
- 239000010949 copper Substances 0.000 claims description 2
- 229910052588 hydroxylapatite Inorganic materials 0.000 claims description 2
- 239000004310 lactic acid Substances 0.000 claims description 2
- XYJRXVWERLGGKC-UHFFFAOYSA-D pentacalcium;hydroxide;triphosphate Chemical compound [OH-].[Ca+2].[Ca+2].[Ca+2].[Ca+2].[Ca+2].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O XYJRXVWERLGGKC-UHFFFAOYSA-D 0.000 claims description 2
- 229920000747 poly(lactic acid) Polymers 0.000 claims description 2
- 239000002745 poly(ortho ester) Substances 0.000 claims description 2
- 229920002627 poly(phosphazenes) Polymers 0.000 claims description 2
- 229920001610 polycaprolactone Polymers 0.000 claims description 2
- 239000004632 polycaprolactone Substances 0.000 claims description 2
- 239000004633 polyglycolic acid Substances 0.000 claims description 2
- 239000004626 polylactic acid Substances 0.000 claims description 2
- 230000007547 defect Effects 0.000 abstract description 28
- 206010052428 Wound Diseases 0.000 abstract description 10
- 208000027418 Wounds and injury Diseases 0.000 abstract description 10
- 238000011049 filling Methods 0.000 abstract description 6
- 210000001519 tissue Anatomy 0.000 abstract description 6
- 238000000465 moulding Methods 0.000 abstract description 5
- 230000000740 bleeding effect Effects 0.000 abstract description 3
- 230000010478 bone regeneration Effects 0.000 abstract description 3
- 201000010099 disease Diseases 0.000 abstract description 3
- 208000037265 diseases, disorders, signs and symptoms Diseases 0.000 abstract description 3
- 230000001737 promoting effect Effects 0.000 abstract description 3
- 239000000203 mixture Substances 0.000 abstract 1
- 239000000499 gel Substances 0.000 description 11
- 229920000642 polymer Polymers 0.000 description 5
- 239000001110 calcium chloride Substances 0.000 description 4
- 229910001628 calcium chloride Inorganic materials 0.000 description 4
- 235000011148 calcium chloride Nutrition 0.000 description 4
- 238000007493 shaping process Methods 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- 238000010521 absorption reaction Methods 0.000 description 2
- 239000008280 blood Substances 0.000 description 2
- 210000004369 blood Anatomy 0.000 description 2
- 230000036772 blood pressure Effects 0.000 description 2
- 229960002713 calcium chloride Drugs 0.000 description 2
- 239000002131 composite material Substances 0.000 description 2
- 229940079593 drug Drugs 0.000 description 2
- 239000003814 drug Substances 0.000 description 2
- 238000000227 grinding Methods 0.000 description 2
- 239000000047 product Substances 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 238000007711 solidification Methods 0.000 description 2
- 230000008023 solidification Effects 0.000 description 2
- 208000006386 Bone Resorption Diseases 0.000 description 1
- BHPQYMZQTOCNFJ-UHFFFAOYSA-N Calcium cation Chemical compound [Ca+2] BHPQYMZQTOCNFJ-UHFFFAOYSA-N 0.000 description 1
- 208000002565 Open Fractures Diseases 0.000 description 1
- 206010031252 Osteomyelitis Diseases 0.000 description 1
- 208000001132 Osteoporosis Diseases 0.000 description 1
- 208000031737 Tissue Adhesions Diseases 0.000 description 1
- 230000003266 anti-allergic effect Effects 0.000 description 1
- 230000002924 anti-infective effect Effects 0.000 description 1
- 239000012227 artificial bone substitute Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000012620 biological material Substances 0.000 description 1
- 230000003592 biomimetic effect Effects 0.000 description 1
- 230000037182 bone density Effects 0.000 description 1
- 230000024279 bone resorption Effects 0.000 description 1
- 235000010410 calcium alginate Nutrition 0.000 description 1
- 239000000648 calcium alginate Substances 0.000 description 1
- 229960002681 calcium alginate Drugs 0.000 description 1
- 229910001424 calcium ion Inorganic materials 0.000 description 1
- OKHHGHGGPDJQHR-YMOPUZKJSA-L calcium;(2s,3s,4s,5s,6r)-6-[(2r,3s,4r,5s,6r)-2-carboxy-6-[(2r,3s,4r,5s,6r)-2-carboxylato-4,5,6-trihydroxyoxan-3-yl]oxy-4,5-dihydroxyoxan-3-yl]oxy-3,4,5-trihydroxyoxane-2-carboxylate Chemical compound [Ca+2].O[C@@H]1[C@H](O)[C@H](O)O[C@@H](C([O-])=O)[C@H]1O[C@H]1[C@@H](O)[C@@H](O)[C@H](O[C@H]2[C@H]([C@@H](O)[C@H](O)[C@H](O2)C([O-])=O)O)[C@H](C(O)=O)O1 OKHHGHGGPDJQHR-YMOPUZKJSA-L 0.000 description 1
- 230000007012 clinical effect Effects 0.000 description 1
- 230000015271 coagulation Effects 0.000 description 1
- 238000005345 coagulation Methods 0.000 description 1
- 238000013329 compounding Methods 0.000 description 1
- 230000006378 damage Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 238000012377 drug delivery Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 230000035876 healing Effects 0.000 description 1
- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 description 1
- 238000002513 implantation Methods 0.000 description 1
- 238000009776 industrial production Methods 0.000 description 1
- 208000014674 injury Diseases 0.000 description 1
- 230000001788 irregular Effects 0.000 description 1
- 230000007794 irritation Effects 0.000 description 1
- 238000005461 lubrication Methods 0.000 description 1
- 239000012567 medical material Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 229920005615 natural polymer Polymers 0.000 description 1
- 239000011664 nicotinic acid Substances 0.000 description 1
- 230000011164 ossification Effects 0.000 description 1
- 239000002861 polymer material Substances 0.000 description 1
- 230000008929 regeneration Effects 0.000 description 1
- 238000011069 regeneration method Methods 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 239000013589 supplement Substances 0.000 description 1
- 238000010998 test method Methods 0.000 description 1
- 230000017423 tissue regeneration Effects 0.000 description 1
- 230000008733 trauma Effects 0.000 description 1
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
- A61L27/00—Materials for grafts or prostheses or for coating grafts or prostheses
- A61L27/40—Composite materials, i.e. containing one material dispersed in a matrix of the same or different material
- A61L27/44—Composite materials, i.e. containing one material dispersed in a matrix of the same or different material having a macromolecular matrix
- A61L27/446—Composite materials, i.e. containing one material dispersed in a matrix of the same or different material having a macromolecular matrix with other specific inorganic fillers other than those covered by A61L27/443 or A61L27/46
-
- 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
- A61L27/40—Composite materials, i.e. containing one material dispersed in a matrix of the same or different material
- A61L27/44—Composite materials, i.e. containing one material dispersed in a matrix of the same or different material having a macromolecular matrix
- A61L27/46—Composite materials, i.e. containing one material dispersed in a matrix of the same or different material having a macromolecular matrix with phosphorus-containing inorganic fillers
-
- 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
- A61L27/54—Biologically active materials, e.g. therapeutic substances
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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
- A61L27/50—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
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B33—ADDITIVE MANUFACTURING TECHNOLOGY
- B33Y—ADDITIVE MANUFACTURING, i.e. MANUFACTURING OF THREE-DIMENSIONAL [3-D] OBJECTS BY ADDITIVE DEPOSITION, ADDITIVE AGGLOMERATION OR ADDITIVE LAYERING, e.g. BY 3-D PRINTING, STEREOLITHOGRAPHY OR SELECTIVE LASER SINTERING
- B33Y70/00—Materials specially adapted for additive manufacturing
- B33Y70/10—Composites of different types of material, e.g. mixtures of ceramics and polymers or mixtures of metals and biomaterials
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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
- A61L2300/00—Biologically active materials used in bandages, wound dressings, absorbent pads or medical devices
- A61L2300/10—Biologically active materials used in bandages, wound dressings, absorbent pads or medical devices containing or releasing inorganic materials
- A61L2300/102—Metals or metal compounds, e.g. salts such as bicarbonates, carbonates, oxides, zeolites, silicates
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- A—HUMAN NECESSITIES
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- 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
- A61L2300/00—Biologically active materials used in bandages, wound dressings, absorbent pads or medical devices
- A61L2300/40—Biologically active materials used in bandages, wound dressings, absorbent pads or medical devices characterised by a specific therapeutic activity or mode of action
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- 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
- A61L2400/00—Materials characterised by their function or physical properties
- A61L2400/04—Materials for stopping bleeding
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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
- A61L2400/00—Materials characterised by their function or physical properties
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- A—HUMAN NECESSITIES
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- A61L2430/00—Materials or treatment for tissue regeneration
- A61L2430/02—Materials or treatment for tissue regeneration for reconstruction of bones; weight-bearing implants
Abstract
The application discloses a magnesium-containing degradable injection hydrogel bone repair material and a preparation method thereof, wherein the method comprises the following steps: preparing a magnesium-containing biodegradable stent by adopting a biodegradable polymer, a biodegradable inorganic substance and metal magnesium powder; mixing a calcium chloride solution and a calcium gluconate solution, adding the mixture into sodium alginate powder, and stirring and mixing to obtain hydrogel fluid; the biodegradable magnesium-containing scaffold is crushed into biodegradable magnesium-containing particles with the particle size of 0.5-1.0 mm, the biodegradable magnesium-containing particles are added into the hydrogel fluid, and the biodegradable magnesium-containing injectable hydrogel bone repair material is obtained by stirring. The material is effectively used for limb non-bearing bone defect repair and alveolar bone defect repair, is used for injection filling of bone defects caused by wounds, diseases, operations and the like, does not need to cut random molding, plays a role in stopping bleeding and promoting bone regeneration at the bone defect part, can reduce running-in of the material and the defect wound, and prevents secondary pollution caused by adhesion of the material and tissue at the damaged part.
Description
Technical Field
The application relates to the technical field of bone repair, in particular to a magnesium-containing degradable injection hydrogel bone repair material and a preparation method thereof.
Background
With the progress of science and technology, medical level is continuously improved, medical materials are increasingly and widely paid attention to, wherein artificial bone substitute materials are utilized for repairing, and bone defect substitution becomes a research focus in the field of medical orthopaedics. Research into various materials and tissue engineering bones has been greatly advanced, and different materials all show strong bone defect repair capability. With the development of biological material science and technology, the performance and clinical effect of the artificial bone repair material are increasingly improved, and the product is gradually known and accepted by more and more clinicians, so that the artificial bone repair material is used in the filling and regeneration repair of various clinical bone defects.
Hydrogel backbones are generally formed by polymeric polymers with a three-dimensional network of water in the interior, such that the entire gel backbone has a fluid character similar to a biological tissue structure that is filled with water in a large amount. Due to the local softness, wetted surface and bionic knot loosening characteristics of the hydrogel, the irritation to biological tissues can be remarkably avoided, so that the biocompatibility is improved. Injectable hydrogels have been widely used in drug delivery and tissue repair engineering due to their unique physicochemical properties, such as unique hydrophilic, water retention and biomimetic properties, good biocompatibility, specific hydrodynamic properties, and multiple environmental responsivity. Based on natural polymer materials, the injectable polymer hydrogel is synthesized, and the structure and the performance of the injectable polymer hydrogel can be finely regulated and controlled to meet the treatment requirement. In particular to a multifunctional responsive gel which has controllable degradability, good biocompatibility and repeatability, is easy to process and realize industrial production and has great clinical application potential.
In recent years, commercialized artificial bone materials are used as biological medicines and tissue engineering medicines, new vitality is injected, but the artificial bone materials are materials with a certain mechanical supporting strength, and when the artificial bone materials are implanted into a bone defect position, in order to ensure that the implanted materials are attached to wounds, the materials are often required to be cut and irregular bone defect positions are ground down, so that the implantation of the repaired materials is complete, and the operation process is complex. Open fracture bone defects caused by trauma often lead to bone infections, and it is necessary to develop anti-infective, more convenient to use bone repair materials for repairing bone defects.
Disclosure of Invention
In order to solve the defects in the prior art, the application provides the magnesium-containing degradable injection hydrogel bone repair material and the preparation method thereof, the 3D printing technology is used for preparing biodegradable polymer/biodegradable inorganic matter/metal magnesium powder according to a certain proportion, the injectable hydrogel material consisting of sodium alginate, calcium chloride and calcium gluconate is used as a carrier to bear the magnesium-containing degradable bone repair material so as to realize the composite degradable injection hydrogel bone repair material of hydrogel and degradable bone repair material, the magnesium-containing degradable injection hydrogel bone repair material is effectively used for limb non-bearing bone defect repair and alveolar bone defect repair, the injection filling of bone defects caused by wounds, diseases, operations and the like is not needed, the effect of stopping bleeding and promoting bone regeneration at the bone defect position is also achieved, various problems existing in the traditional artificial bone grafting treatment method can be solved, such as increasing blood volume and maintaining blood pressure, filling wounds and random shaping, reducing material and defect wound running-in, preventing the material from adhering to tissue at the damaged position and the like, the porous support bone repair material and gel composite property and application are effectively used, and more secondary pollution is provided for clinical demands.
The application aims to achieve the aim, and the aim is achieved by the following technical scheme:
a magnesium-containing degradable injection hydrogel bone repair material, which comprises the following components:
a magnesium-containing biodegradable particle, the magnesium-containing biodegradable particle comprising: biodegradable polymer, biodegradable inorganic matter and metal magnesium powder;
a hydrogel fluid, the hydrogel fluid comprising: calcium chloride solution, calcium gluconate solution and sodium alginate powder.
The magnesium-containing degradable injection hydrogel bone repair material comprises the following components in parts by mass:
40-66 parts of the magnesium-containing biodegradable particles, 100 parts of the hydrogel fluid, and by way of example, 40 parts, 41 parts, 42 parts, 43 parts, 44 parts, 45 parts, 46 parts, 47 parts, 48 parts, 49 parts, 50 parts, 51 parts, 52 parts, 53 parts, 54 parts, 55 parts, 56 parts, 57 parts, 58 parts, 59 parts, 60 parts, 61 parts, 62 parts, 63 parts, 64 parts, 65 parts, 66 parts of the magnesium-containing biodegradable particles.
The magnesium-containing biodegradable particles comprise the following raw materials in parts by mass: 50-85 parts of biodegradable polymer, 10-35 parts of biodegradable inorganic matter and 2-20 parts of metal magnesium powder; exemplary, 50 parts, 53 parts, 55 parts, 57 parts, 60 parts, 62 parts, 65 parts, 68 parts, 70 parts, 71 parts, 75 parts, 78 parts, 80 parts, 83 parts, 85 parts of biodegradable inorganic substances 10 parts, 12 parts, 15 parts, 17 parts, 20 parts, 22 parts, 25 parts, 28 parts, 30 parts, 31 parts, 32 parts, 35 parts, 2 parts, 3 parts, 4 parts, 5 parts, 6 parts, 7 parts, 8 parts, 9 parts, 10 parts, 11 parts, 12 parts, 13 parts, 14 parts, 15 parts, 16 parts, 17 parts, 18 parts, 19 parts, 20 parts of metal magnesium powder.
The hydrogel fluid comprises the following raw materials: 1-10 parts of calcium chloride solution, 10-25 parts of calcium gluconate solution and 60-90 parts of sodium alginate powder. Exemplary, 1 part, 2 parts, 3 parts, 4 parts, 5 parts, 6 parts, 7 parts, 8 parts, 9 parts, 10 parts, 11 parts, 12 parts, 13 parts, 14 parts, 15 parts, 16 parts, 17 parts, 18 parts, 19 parts, 20 parts, 21 parts, 22 parts, 23 parts, 24 parts, 25 parts, 60 parts, 62 parts, 65 parts, 68 parts, 70 parts, 73 parts, 75 parts, 78 parts, 80 parts, 82 parts, 85 parts, 87 parts, 90 parts of sodium alginate powder.
The particle diameter of the magnesium-containing biodegradable particles is 0.5 mm to 1.0 mm, and exemplary, the particle diameter of the magnesium-containing biodegradable particles may be 0.5 mm, 0.6 mm, 0.7 mm, 0.8 mm, 0.9 mm, or the magnesium-containing biodegradable particles may be mixed particles of any particle diameter between 0.5 mm to 1.0 mm.
The biodegradable polymer is one or more of polyglycolic acid-lactic acid copolymer, polylactic acid, polyglycolic acid, polycaprolactone, polyorthoester, polyanhydride, polyphosphazene and polyamino acid, which are mixed according to any proportion.
The biodegradable inorganic matter comprises one or more of alpha-tricalcium phosphate, beta-tricalcium phosphate, hydroxyapatite, calcium phosphate and calcium silicate which are mixed in any proportion.
The magnesium-containing biodegradable particles further comprise 1-15 parts of doped metal powder according to parts by weight, wherein the doped metal powder is 1 part, 2 parts, 3 parts, 4 parts, 5 parts, 6 parts, 7 parts, 8 parts, 9 parts, 10 parts, 11 parts, 12 parts, 13 parts, 14 parts and 15 parts, the doped metal powder is one or more of copper, zinc, silver, iron, calcium and titanium, and the doped metal powder is a combination of silver, zinc and calcium; or a combination of zinc, silver, iron; or a combination of zinc, silver, calcium, titanium.
The biodegradable particles containing magnesium are molded into the biodegradable stent containing magnesium by adopting a 3D printing technology at the temperature of minus 180 ℃ to minus 20 ℃, and then the biodegradable stent containing magnesium is obtained after being crushed.
The preparation method of the magnesium-containing degradable injection hydrogel bone repair material comprises the following steps:
preparation of a biodegradable stent containing magnesium: dissolving a biodegradable polymer in an organic solvent to form a biodegradable polymer solution; adding biodegradable inorganic matters into biodegradable polymer solution to form homogeneous liquid, adding metal magnesium powder into the homogeneous liquid, and stirring at normal temperature for 5-30 hours to obtain mixed liquid, wherein the mixed liquid is exemplified by stirring at normal temperature for 10 hours, 15 hours, 20 hours and 25 hours; the mixed solution is formed into a magnesium-containing biodegradable stent blank by 3D printing under the low temperature condition of minus 180 ℃ to minus 20 ℃, and the mixed solution can be formed into a magnesium-containing biodegradable stent blank by 3D printing under the low temperature conditions of minus 180 ℃, minus 170 ℃, minus 160 ℃, minus 150 ℃, minus 140 ℃, minus 130 ℃, minus 120 ℃, minus 110 ℃, minus 100 ℃, minus 90 ℃, minus 80 ℃, minus 70 ℃, minus 60 ℃, minus 50 ℃, minus 45 ℃, minus 40 ℃, minus 35 ℃, minus 30 ℃, minus 25 ℃ and minus 20 ℃; 3D printing can be performed by adopting low-temperature rapid forming equipment, and the precooling temperature of a forming working cavity of the equipment is between-180 ℃ and-20 ℃; freezing and storing the magnesium-containing biodegradable stent blank for 5-40 hours at the temperature of minus 180 ℃ to minus 20 ℃ and then vacuum drying for 5-30 days at the vacuum condition of 40-55 ℃ to obtain the magnesium-containing biodegradable stent; illustratively, the freezing is carried out at a temperature of-45℃for 35 hours; vacuum drying at 45deg.C for 25 days to obtain biodegradable stent containing magnesium.
Mixing a calcium chloride solution and a calcium gluconate solution, adding sodium alginate powder, and stirring and mixing to obtain hydrogel fluid;
the biodegradable stent containing magnesium is crushed into biodegradable particles containing magnesium, then added into hydrogel fluid, and stirred at normal temperature to obtain the bone repair material of the biodegradable injection hydrogel containing magnesium.
The preparation of the biodegradable stent containing magnesium further comprises the addition of doped metal powder, wherein the doped metal powder and the metal magnesium powder are added into homogeneous phase liquid together.
The organic solvent is at least one of 1, 4-dioxane, acetonitrile, cyclohexane, acetone, glycol, cyclohexanone and dichloromethane.
Compared with the prior art, the application has the beneficial effects that:
1. the application combines biodegradable polymer/biodegradable inorganic matter/magnesium powder/hydrogel fluid into the same bone repair material to prepare the magnesium-containing degradable injection hydrogel bone repair material, which can be directly injected and implanted into a bone defect position without further grinding the autologous bone at the bone defect position, thereby ensuring the integrity of the autologous bone to the maximum extent, and reducing the lubrication and adhesion of the hydrogel and further damage caused by grinding the defect wound.
2. The magnesium-containing degradable injection hydrogel bone repair material has certain adhesion before solidification, can be well anastomosed with a bone defect part, is adhered to an autologous bone and is not easy to fall off, is adhered to the autologous bone for shaping after solidification, and can be used for well improving the adhesion between the material and the autologous bone defect part and promoting bone generation and bone healing.
3. According to the application, the biodegradable polymer/biodegradable inorganic matter/magnesium powder/is prepared into the magnesium-containing biodegradable scaffold and crushed by a 3D printing technology under a low temperature condition, the injectable hydrogel material consisting of sodium alginate, calcium chloride and calcium gluconate is taken as a carrier to bear the magnesium-containing degradable high polymer bone repair particles so as to realize the bone repair material compounded by the hydrogel and the magnesium-containing degradable high polymer bone repair particles, so that the prepared magnesium-containing degradable injectable hydrogel bone repair material is effectively used for limb non-bearing bone defect repair and alveolar bone defect repair, is used for injection filling of bone defects caused by wounds, diseases, operations and the like, does not need to cut random molding, stops bleeding and promotes bone regeneration at the bone defect position, can solve various problems in the traditional artificial bone grafting treatment method, such as increasing blood volume and maintaining blood pressure, filling wounds and random shaping, reducing material and defect wound running-in, preventing secondary pollution caused by tissue adhesion of the material and the damaged position, expands the properties and gel compounding and other properties and application, and provides more choices for clinical requirements.
4. The hydrogel fluid comprises 1-10 parts of calcium chloride solution, 10-25 parts of calcium gluconate solution and 60-90 parts of sodium alginate powder, and the three components are matched with biodegradable particles containing magnesium, so that the problem of inconvenient injection caused by too fast fixation of the hydrogel in clinic can be relieved, the operation time is striven for, and the delay and the retraction of the hydrogel coagulation time can provide a certain remedy time for patients in clinical application to a certain extent so as to realize the maximum utilization rate of the product; the calcium gluconate can also supplement calcium ions so as to promote bone resorption and bone formation, and has antiallergic effect; the calcium chloride with a certain concentration is added into the sodium alginate to make the gel become brittle, which directly influences the tensile strength of the gel, and the absorption rate of the gel is reduced because the incomplete calcium alginate in the gel has low water holding capacity due to the too compact network structure on the surface of the gel, and the addition of the calcium gluconate can improve the brittleness of the coagulated hydrogel, so that the internal network structure is evacuated to increase the absorption rate of the gel; on the other hand, the calcium can be cooperated with calcium chloride to replace calcium needed by human body with sodium alginate to form a crosslinked gel system, thereby increasing bone density and treating osteoporosis.
Drawings
FIG. 1 is a physical view of biodegradable particles containing magnesium with a particle diameter of 0.5 mm to 1.0 mm according to the present application.
Detailed Description
The application will be further described with reference to specific examples. It is to be understood that these examples are illustrative of the present application and are not intended to limit the scope of the present application. Further, it will be understood that various changes and modifications may be made by those skilled in the art after reading the teachings of the application, and such equivalents are intended to fall within the scope of the application as defined by the claims.
Before the embodiments of the application are explained in further detail, it is to be understood that the application is not limited in its scope to the particular embodiments described below; it is also to be understood that the terminology used in the examples of the application is for the purpose of describing particular embodiments only, and is not intended to limit the scope of the application. Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this application belongs. The test methods in the following examples, in which specific conditions are not noted, are generally conducted under conventional conditions or under conditions recommended by the respective manufacturers. In addition to the specific methods, devices, materials used in the embodiments, any methods, devices, and materials of the prior art similar or equivalent to those described in the embodiments of the present application may be used to practice the present application according to the knowledge of one skilled in the art and the description of the present application.
Example 1
The magnesium-containing degradable injection hydrogel bone repair material comprises the following components in parts by mass:
45 parts of the magnesium-containing biodegradable particles and 100 parts of the hydrogel fluid; the magnesium-containing biodegradable particles comprise the following raw materials in parts by mass: 55 parts of biodegradable polymer, 20 parts of biodegradable inorganic matter and 10 parts of metal magnesium powder; the hydrogel fluid comprises the following raw materials: 5 parts of calcium chloride solution (the mass percentage concentration of the calcium chloride solution is 5%), 15 parts of calcium gluconate solution (the mass percentage concentration of the calcium gluconate solution is 25%) and 70 parts of sodium alginate powder. The biodegradable polymer is polylactic acid-glycolic acid copolymer (PLGA), and the biodegradable inorganic substance is beta-tricalcium phosphate (beta-TCP).
The preparation method of the magnesium-containing degradable injection hydrogel bone repair material comprises the following steps:
preparation of a biodegradable stent containing magnesium: the biodegradable polymer is dissolved in an organic solvent, wherein the organic solvent is 1, 4-dioxane, and a biodegradable polymer solution is formed; adding biodegradable inorganic matters into biodegradable polymer solution, stirring to form homogeneous liquid, adding metal magnesium powder into the homogeneous liquid, and stirring at normal temperature for 10 hr to obtain mixed solution; after the biodegradable inorganic matters are crushed, the metal magnesium powder is used after passing through a 200-400 mesh screen, the mixed solution is 3D printed and molded into a magnesium-containing biodegradable bracket blank by adopting low-temperature rapid molding equipment under the low-temperature condition of minus 50 ℃, and the molding working cavity of the low-temperature rapid molding equipment is precooled to minus 50 ℃; freezing and storing the biodegradable bracket blank containing magnesium at the temperature of-45 ℃ for 35 hours; vacuum drying at 45deg.C for 25 days to obtain biodegradable stent containing magnesium.
Mixing a calcium chloride solution and a calcium gluconate solution, adding sodium alginate powder, and stirring and mixing to obtain hydrogel fluid;
the biodegradable stent containing magnesium is crushed into biodegradable particles containing magnesium, then added into hydrogel fluid, and stirred at normal temperature to obtain the bone repair material of the biodegradable injection hydrogel containing magnesium.
Example 2
The magnesium-containing degradable injection hydrogel bone repair material comprises the following components in parts by mass: 45 parts of the magnesium-containing biodegradable particles and 100 parts of the hydrogel fluid; the magnesium-containing biodegradable particles comprise the following raw materials in parts by mass: 62 parts of biodegradable polymer, 15 parts of biodegradable inorganic matter and 12 parts of metal magnesium powder; the hydrogel fluid comprises the following raw materials: 5 parts of calcium chloride solution (the mass percentage concentration of the calcium chloride solution is 5%), 15 parts of calcium gluconate solution (the mass percentage concentration of the calcium gluconate solution is 25%) and 70 parts of sodium alginate powder. The biodegradable polymer is polylactic acid-glycolic acid copolymer (PLGA), and the biodegradable inorganic substance is beta-tricalcium phosphate (beta-TCP).
The preparation method is identical to example 1.
Example 3
The magnesium-containing degradable injection hydrogel bone repair material comprises the following components in parts by mass: 45 parts of the magnesium-containing biodegradable particles and 100 parts of the hydrogel fluid; the magnesium-containing biodegradable particles comprise the following raw materials in parts by mass: 78 parts of biodegradable polymer, 18 parts of biodegradable inorganic matters and 8 parts of metal magnesium powder; the hydrogel fluid comprises the following raw materials: 5 parts of calcium chloride solution (the mass percentage concentration of the calcium chloride solution is 5%), 20 parts of calcium gluconate solution (the mass percentage concentration of the calcium gluconate solution is 25%), and 80 parts of sodium alginate powder. The biodegradable polymer is polylactic acid-glycolic acid copolymer (PLGA), and the biodegradable inorganic substance is beta-tricalcium phosphate (beta-TCP).
The preparation method is identical to example 1.
Example 4
The magnesium-containing degradable injection hydrogel bone repair material comprises the following components in parts by mass: 45 parts of the magnesium-containing biodegradable particles and 100 parts of the hydrogel fluid; the magnesium-containing biodegradable particles comprise the following raw materials in parts by mass: 78 parts of biodegradable polymer, 18 parts of biodegradable inorganic matters and 12 parts of metal magnesium powder; the hydrogel fluid comprises the following raw materials: 10 parts of calcium chloride solution (the mass percentage concentration of the calcium chloride solution is 5%), 15 parts of calcium gluconate solution (the mass percentage concentration of the calcium gluconate solution is 25%) and 60 parts of sodium alginate powder. The biodegradable polymer is polylactic acid-glycolic acid copolymer (PLGA), and the biodegradable inorganic substance is beta-tricalcium phosphate (beta-TCP).
The preparation method is identical to example 1.
Example 5
A magnesium-containing degradable injection hydrogel bone repair material, which is different from example 4 in that the material also comprises 5 parts of doped metal powder, 3 parts of zinc and 3 parts of calcium.
Example 6
A magnesium-containing degradable injection hydrogel bone repair material, which is different from example 4 in that the biodegradable polymer is polyamino acid and the biodegradable inorganic substance is alpha-tricalcium phosphate.
Claims (10)
1. The degradable injection hydrogel bone repair material containing magnesium is characterized by comprising the following components:
a magnesium-containing biodegradable particle, the magnesium-containing biodegradable particle comprising: biodegradable polymer, biodegradable inorganic matter and metal magnesium powder;
a hydrogel fluid, the hydrogel fluid comprising: calcium chloride solution, calcium gluconate solution and sodium alginate powder.
2. The magnesium-containing degradable injection hydrogel bone repair material according to claim 1, which is characterized by comprising the following components in parts by mass:
40-66 parts of magnesium-containing biodegradable particles and 100 parts of hydrogel fluid;
the magnesium-containing biodegradable particles comprise the following raw materials in parts by mass: 50-85 parts of biodegradable polymer, 10-35 parts of biodegradable inorganic matter and 2-20 parts of metal magnesium powder;
the hydrogel fluid comprises the following raw materials in parts by mass: 1-10 parts of calcium chloride solution, 10-25 parts of calcium gluconate solution and 60-90 parts of sodium alginate powder.
3. The magnesium-containing biodegradable injection hydrogel bone repair material of claim 1, wherein the magnesium-containing biodegradable particles have a particle size of 0.5 mm to 1.0 mm.
4. The magnesium-containing degradable injection hydrogel bone repair material of claim 1, wherein the biodegradable polymer is one or more of polyglycolic acid-lactic acid copolymer, polylactic acid, polyglycolic acid, polycaprolactone, polyorthoester, polyanhydride, polyphosphazene, polyamino acid, mixed in any ratio.
5. The magnesium-containing degradable injection hydrogel bone repair material of claim 1, wherein the biodegradable inorganic substance comprises one or more of α -tricalcium phosphate, β -tricalcium phosphate, hydroxyapatite, calcium phosphate, and calcium silicate mixed in any ratio.
6. The magnesium-containing degradable injection hydrogel bone repair material according to claim 1, wherein the raw materials of the magnesium-containing biodegradable particles comprise 1-15 parts of doped metal powder in parts by mass, and the doped metal powder is one or more of copper, zinc, silver, iron, calcium and titanium mixed in any proportion.
7. The magnesium-containing biodegradable injection hydrogel bone repair material according to claim 1, wherein the magnesium-containing biodegradable particles are formed into a magnesium-containing biodegradable scaffold by a 3D printing technology at a temperature of-180 ℃ to-20 ℃, and then the magnesium-containing biodegradable scaffold is crushed.
8. The method for preparing the magnesium-containing degradable injection hydrogel bone repair material according to any one of claims 1 to 7, comprising the following steps:
preparation of a biodegradable stent containing magnesium: dissolving a biodegradable polymer in an organic solvent to form a biodegradable polymer solution; adding biodegradable inorganic matters into biodegradable polymer solution to form homogeneous liquid, adding metal magnesium powder into the homogeneous liquid, and stirring at normal temperature for 5-30 hours to obtain mixed solution; the mixed solution is formed into a magnesium-containing biodegradable bracket blank by 3D printing under the low temperature condition of minus 180 ℃ to minus 20 ℃; freezing and storing the magnesium-containing biodegradable stent blank for 5-40 hours at the temperature of minus 180 ℃ to minus 20 ℃ and then vacuum drying for 5-30 days at the vacuum condition of 40-55 ℃ to obtain the magnesium-containing biodegradable stent;
mixing a calcium chloride solution and a calcium gluconate solution, adding sodium alginate powder, and stirring and mixing to obtain hydrogel fluid;
the biodegradable stent containing magnesium is crushed into biodegradable particles containing magnesium, then added into hydrogel fluid, and stirred at normal temperature to obtain the bone repair material of the biodegradable injection hydrogel containing magnesium.
9. The method for preparing a biodegradable injectable hydrogel bone repair material containing magnesium according to claim 8, wherein the preparation of the biodegradable scaffold containing magnesium further comprises adding a doped metal powder, wherein the doped metal powder is added into a homogeneous liquid together with the metal magnesium powder.
10. The method for preparing a magnesium-containing degradable injection hydrogel bone repair material according to claim 8, wherein the organic solvent is at least one of 1, 4-dioxane, acetonitrile, cyclohexane, acetone, ethylene glycol, cyclohexanone and dichloromethane.
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