CN1557503A - Bioactivity artificial joint material and preparation method thereof - Google Patents
Bioactivity artificial joint material and preparation method thereof Download PDFInfo
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- CN1557503A CN1557503A CNA2004100139241A CN200410013924A CN1557503A CN 1557503 A CN1557503 A CN 1557503A CN A2004100139241 A CNA2004100139241 A CN A2004100139241A CN 200410013924 A CN200410013924 A CN 200410013924A CN 1557503 A CN1557503 A CN 1557503A
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Abstract
The present invention is one kind of artificial joint material with surface porous Ca-P bioactive ceramic coating layer and bone morphogenetic protein and its preparation process. The artificial joint material consists of metal substrate, one layer of double-layered porous Ca-P bioactive ceramic coating layer on the surface of the metal substrate, and bone morphogenetic protein covering the bioactive ceramic coating layer. The porous bioactive Ca-P ceramic coating layer comprises the non-crystal calcium phosphate base layer contacting with the metal substrate in 1-10 micron thickness and the crystalline bone-like apatite surface layer in 10-100 micron thickness. The preparation process includes machining artificial joint with titanium alloy, stainless steel or CO-Cr-Mo alloy; surface activating the artificial joint, two-step bionic deposition; and soaking the artificial joint inside mixed solution comprising bone morphogenetic protein and buffering phosphate solution.
Description
Technical field
The present invention relates to a kind of bioactive artificial joint material and preparation method thereof, particularly relate to a kind of surface and have the porous calcium phosphorus bioactive ceramic coating of biomimetic method preparation and artificial joint material of bone morphogenetic protein (BMP) and preparation method thereof, belong to technical field of biomedical materials.
Background technology
At present, the case quantity of artificial joint implant into body can reach 1,200,000 examples every year, is one of embedded material of having the call of domestic and international orthopaedics.Normally used artificial joint is a metal material, because of it is a bio-inert material, and can not forms firm physiology between the body bone tissue and combines; after implanting several years; usually can become flexible, sink, cause the prosthetic replacement to fail, second operation is inevitable.Adopt process for modifying surface to prepare biological coating (film) at the artificial joint metal base surface, can reduce the stripping of harmful metal ion under the human body environment, improve its biocompatibility and biological activity, make that forming firm physiology between artificial joint and the body bone tissue combines.The main inanimate matter of human body hard tissue is a calcium phosphorus phase, so calcium phosphate, hydroxyapatite, mixes CO
3 2-The bioactive layer of Ca-P ceramic phase compositions such as ionic osteoid apatite or OCP is to improve surface-active desirable selection of artificial joint.In addition, at artificial joint surface recombination bone morphogenetic protein (BMP), can significantly improve the ability of implantation initial stage artificial joint spatial induction skeletonization.
In the common method of artificial joint surface preparation calcium phosphate bioceramic coating is plasma spraying technology or based on the complex method of plasma spraying technology.Chinese patent ZL98125674.0 " a kind of artificial joint and manufacture method thereof that scribbles bone morphogenetic protein " discloses a kind of complex method based on plasma spraying technology, promptly earlier at artificial joint surface plasma spraying hydroxyapatite coating, at the further compound BMP of coating surface, prepared artificial joint has good induced osteogenesis effect then.But this artificial joint hydroxyapatite coating on surface is that high temperature forms under the condition that differs greatly with the human body environment, and its composition and structure and biological osteolith differ greatly, and cause the instability of artificial joint long-term behaviour.
Summary of the invention
Technical problem: the objective of the invention is at the above-mentioned deficiency of artificial joint material, propose a kind of stable performance, can significantly improve the bioactive artificial joint material and preparation method thereof of the ability of implantation initial stage artificial joint spatial induction skeletonization.
Technical scheme: this bioactive artificial joint material has one deck to adopt bionic method being similar to the double-deck porous calcium phosphorus bioactive ceramic coating that has for preparing under the physiological environment at metal base surface, and its surface further is compounded with bone morphogenetic protein (BMP).Porous calcium phosphorus ceramic coating and metallic matrix bond strength height, form by calcium phosphate amorphous underlayer that contacts with the metal surface and osteoid apatite crystalline phase surface layer, the densification of calcium phosphate amorphous underlayer, thickness are 1-10 μ m, can suppress that toxic metals is ionic in the metallic matrix separates out; Porous osteolith stone crystalline phase surface layer, thickness is 10-100 μ m, has good biological activity, also is the ideal carrier of BMP simultaneously.The compound common employing solution dipping method of artificial joint and BMP, BMP can deeply be penetrated in the porous osteoid apatite crystalline phase layer by capillarity, and the amount of carrying of artificial joint surface BMP is improved greatly.Behind the artificial joint implant into body, its surperficial BMP prolongs deenergized period, helps giving full play to of BMP induced osteogenesis effect.
The present invention is realized by the following technical programs:
Have one deck to have special double-deck porous calcium phosphorus bioactive ceramic coating at this bioactive artificial joint material metal matrix surface, its surface further is compounded with bone morphogenetic protein (BMP).
The porous calcium phosphorus bioactive ceramic coating of being addressed is made up of fine and close calcium phosphate amorphous underlayer that contacts with metallic matrix and porous osteolith stone crystalline phase surface layer, and wherein, calcium phosphate amorphous underlayer thickness is 1-10 μ m; Osteoid apatite crystalline phase surface layer thickness is 10-100 μ m.
The step of its preparation is as follows:
1) at first select for use titanium alloy, rustless steel or vitallium to process artificial joint;
2) artificial joint is carried out surface activation process, go on foot bionical deposition processes by two then, obtain the porous calcium phosphorus bioactive ceramic coating of forming successively by fine and close calcium phosphate amorphous underlayer and porous osteolith stone crystalline phase surface layer on the artificial joint surface;
3) surface is immersed in the mixed solution that bone morphogenetic protein and phosphate buffered saline(PBS) form by the artificial joint of porous calcium phosphorus bioactive ceramic coating, bone morphogenetic protein concentration is 0.1-50mg/L, 20-40 ℃ was soaked 5-15 hour down, slowly stirred once, and took out in middle every 1-2 hour;
4) with above-mentioned taking-up artificial joint with ethanol drip washing after, vacuum drying, the sterilization aseptic preservation in back, standby, get final product bioactive artificial joint material of the present invention.
The bionic method that the present invention preparation has an above-mentioned special double-deck porous calcium phosphorus bioactive ceramic coating at lower temperature, be similar under the physiological environment and finish, prepared porous calcium phosphorus bioactive ceramic coating has very high biological activity.
It is the ebullient H of 10-60% that described surface activation process adopts concentration
2O
2Aqueous solution, the processing time is 10-90 minute, take out flushing after, be immersed in temperature again and be 30-80 ℃, concentration and be in the NaOH aqueous solution of 1-10M 6-48 hour.
Described bionical deposition processes of two steps comprises the steps:
1) the bionical calcifying solution A of preparation: bionical calcifying solution A presses the active constituent content of ionometer:
Sodium ion 500-850mM, magnesium ion 4.5-6.0mM, calcium ion 10.0-13.5mM, chloride ion 500-800mM, phosphoric acid hydrogen radical ion 4.0-6.0mM, bicarbonate ion 15.0-30.0mM;
2) the bionical calcifying solution B of preparation: bionical calcifying solution B presses the active constituent content of ionometer:
Sodium ion 100.0-180.0mM, potassium ion 4.0-5.5mM, magnesium ion 3.0-4.5mM, calcium ion 2.0-3.5mM, chloride ion 80.0-150.0mM, phosphoric acid hydrogen radical ion 0.5-1.5mM, bicarbonate ion 6.5-12.0mM, sulfate ion 0.5-1.0mM;
3) the bionical deposition processes of calcium phosphate amorphous underlayer: the artificial joint material immersion temperature that surface activation process is crossed is among the 10-30 ℃ of bionical calcifying solution A, under stirring condition, take out after bionical deposition processes 12-36 hour, clean, drying, artificial joint material surface obtain the calcium phosphate amorphous layer of thickness 1-10 μ m, densification;
4) the bionical deposition processes of osteoid apatite crystalline phase surface layer: the artificial joint material immersion temperature that the surface is had the calcium phosphate amorphous layer is among the 30-50 ℃ of bionical calcifying solution B, took out in bionical deposition processes 12-144 hour, clean, drying, further deposit thickness is 10-100 μ m, porous osteoid apatite crystalline phase layer on the artificial joint material surface phosphoric acid calcium amorphous layer.
Beneficial effect:
(1) bioactive artificial joint material of the present invention has one deck to adopt bionic method being similar to the porous calcium phosphorus bioactive ceramic coating for preparing under the physiological environment at metal base surface, its surface further is compounded with bone morphogenetic protein (BMP), this artificial joint material has good biological activity and induced osteogenesis effect, can form firm physiology with osseous tissue in a short time and combine.
(2) artificial joint porous surface Ca-P ceramic coating and metallic matrix bond strength height, and has an ideal double-decker: the calcium phosphate amorphous underlayer densification that contacts with the metal surface, can suppress that toxic metals is ionic in the metallic matrix separates out, and can be used as the deposition growing that " nucleus basal plane " promotes osteoid apatite crystalline phase surface layer; Osteoid apatite crystalline phase surface layer porous, thickness is 10-100 μ m, has good biological activity, also is the ideal carrier of BMP simultaneously, helps giving full play to of BMP induced osteogenesis effect.
The instantiation mode
Embodiment 1
(1) at first select for use the Ti6Al4V alloy to process artificial joint;
(2) artificial joint surface activation process: after artificial joint used acetone, 70% ethanol, distilled water ultrasonic cleaning successively, adopting concentration was 20% ebullient H
2O
2Aqueous solution is handled, and the processing time is 45 minutes, take out flushing after, be immersed in temperature again and be in 30-50 ℃, the NaOH aqueous solution of 4M after 24-36 hour, take out distilled water flushing, 70 ℃ of dryings.
(3) the bionical deposition processes of calcium phosphate amorphous underlayer: the artificial joint immersion temperature that surface activation process is crossed is that bionical calcifying solution A is among 20 ℃ of bionical calcifying solution A by the active constituent content of ionometer: sodium ion 610mM, magnesium ion 4.5mM, calcium ion 12.5mM, chloride ion 610.0mM, phosphoric acid hydrogen radical ion 5.0mM, bicarbonate ion 18.0mM.Bionical calcifying solution A employing magnetic stirring apparatus stirs, takes out after bionical deposition processes 12-24 hour, and the distilled water ultrasonic cleaning, drying at room temperature, the artificial joint surface obtains the calcium phosphate amorphous layer of thickness 1.5-2.0 μ m, densification.
(4) the bionical deposition processes of osteoid apatite crystalline phase surface layer: the artificial joint immersion temperature that the surface is had the calcium phosphate amorphous layer is that bionical calcifying solution B presses the active constituent content of ionometer among 30 ℃ of bionical calcifying solution B: sodium ion 120.0mM, potassium ion 5.0mM, magnesium ion 3.5mM, calcium ion 2.5mM, chloride ion 120.0mM, phosphoric acid hydrogen radical ion 1.0mM, bicarbonate ion 11.0mM, sulfate ion 0.5mM.Took out in bionical deposition processes 12-36 hour, the distilled water ultrasonic cleaning, drying at room temperature, further deposit thickness is 15-20 μ m, porous osteoid apatite crystalline phase surface layer on the artificial joint surface phosphoric acid calcium amorphous underlayer.
(5) surface being immersed in bone morphogenetic protein and concentration by the artificial joint of porous calcium phosphorus bioactive ceramic coating is in the mixed solution formed of the phosphate buffered saline(PBS) of 0.1mol/L, bone morphogenetic protein concentration is 0.1-50mg/L, 20-40 ℃ was soaked 5-15 hour down, slowly stirred once, and took out in middle every 1-2 hour;
(6) with above-mentioned taking-up artificial joint with ethanol drip washing after, vacuum drying, the sterilization aseptic preservation in back, standby, get final product bioactive artificial joint material of the present invention.
Embodiment 2
(1) at first select for use the Ti6Al4V alloy to process artificial joint;
(2) artificial joint surface activation process: after artificial joint used acetone, 70% ethanol, distilled water ultrasonic cleaning successively, adopting concentration was 30% ebullient H
2O
2Aqueous solution is handled, and the processing time is 90 minutes, take out flushing after, be immersed in temperature again and be 60-70 ℃, concentration and be in the NaOH aqueous solution of 8M 24-36 hour, take out distilled water flushing, 70 ℃ of dryings.
(3) the bionical deposition processes of calcium phosphate amorphous underlayer: the artificial joint immersion temperature that surface activation process is crossed is that bionical calcifying solution A is among 30 ℃ of bionical calcifying solution A by the active constituent content of ionometer: sodium ion 610mM, magnesium ion 4.5mM, calcium ion 12.5mM, chloride ion 610.0mM, phosphoric acid hydrogen radical ion 5.0mM, bicarbonate ion 18.0mM.Bionical calcifying solution A employing magnetic stirring apparatus stirs, takes out after bionical deposition processes 24-36 hour, and the distilled water ultrasonic cleaning, drying at room temperature, the artificial joint surface obtains the calcium phosphate amorphous layer of thickness 7.5-9.0 μ m, densification.
(4) the bionical deposition processes of osteoid apatite crystalline phase surface layer: the artificial joint immersion temperature that the surface is had the calcium phosphate amorphous layer is that bionical calcifying solution B presses the active constituent content of ionometer among 50 ℃ of molten B of bionical calcification: sodium ion 120.0mM, potassium ion 5.0mM, magnesium ion 3.5mM, calcium ion 2.5mM, chloride ion 120.0mM, phosphoric acid hydrogen radical ion 1.0mM, bicarbonate ion 11.0mM, sulfate ion 0.5mM.Took out in bionical deposition processes 72-144 hour, the distilled water ultrasonic cleaning, drying at room temperature, further deposit thickness is 60-80 μ m, porous osteoid apatite crystalline phase surface layer on the artificial joint surface phosphoric acid calcium amorphous underlayer.
(5) surface being immersed in bone morphogenetic protein and concentration by the artificial joint of porous calcium phosphorus bioactive ceramic coating is in the mixed solution formed of the phosphate buffered saline(PBS) of 0.1mol/L, bone morphogenetic protein concentration is 0.1-50mg/L, 20-40 ℃ was soaked 5-15 hour down, slowly stirred once, and took out in middle every 1-2 hour;
(6) with above-mentioned taking-up artificial joint with ethanol drip washing after, vacuum drying, the sterilization aseptic preservation in back, standby, get final product bioactive artificial joint material of the present invention.
Embodiment 3
(1) at first select for use medical stainless steel to process artificial joint;
(2) artificial joint surface activation process: after artificial joint used acetone, 70% ethanol, distilled water ultrasonic cleaning successively, adopting concentration was 50% ebullient H
2O
2Aqueous solution is handled, and the processing time is 60 minutes, take out flushing after, be immersed in temperature again and be 30-40 ℃, concentration and be in the NaOH aqueous solution of 2M 12-24 hour.
(3) the bionical deposition processes of calcium phosphate amorphous underlayer: the artificial joint immersion temperature that surface activation process is crossed is that bionical calcifying solution A is among 30 ℃ of bionical calcifying solution A by the active constituent content of ionometer: sodium ion 610mM, magnesium ion 4.5mM, calcium ion 12.5mM, chloride ion 610.0mM, phosphoric acid hydrogen radical ion 5.0mM, bicarbonate ion 18.0mM.Bionical calcifying solution A employing magnetic stirring apparatus stirs, takes out after bionical deposition processes 30-36 hour, and the distilled water ultrasonic cleaning, drying at room temperature, the artificial joint surface obtains the calcium phosphate amorphous layer of thickness 7.5-9.0 μ m, densification.
(4) the bionical deposition processes of osteoid apatite crystalline phase surface layer: the artificial joint immersion temperature that the surface is had the calcium phosphate amorphous layer is that bionical calcifying solution B presses the active constituent content of ionometer among 50 ℃ of molten B of bionical calcification: sodium ion 120.0mM, potassium ion 5.0mM, magnesium ion 3.5mM, calcium ion 2.5mM, chloride ion 120.0mM, phosphoric acid hydrogen radical ion 1.0mM, bicarbonate ion 11.0mM, sulfate ion 0.5mM.Took out in bionical deposition processes 64-72 hour, the distilled water ultrasonic cleaning, drying at room temperature, further deposit thickness is 40-50 μ m, porous osteoid apatite crystalline phase surface layer on the artificial joint surface phosphoric acid calcium amorphous underlayer.
(5) surface being immersed in bone morphogenetic protein and concentration by the artificial joint of porous calcium phosphorus bioactive ceramic coating is in the mixed solution formed of the phosphate buffered saline(PBS) of 0.1mol/L, bone morphogenetic protein concentration is 0.1-50mg/L, 20-40 ℃ was soaked 5-15 hour down, slowly stirred once, and took out in middle every 1-2 hour;
(6) with above-mentioned taking-up artificial joint with ethanol drip washing after, vacuum drying, the sterilization aseptic preservation in back, standby, get final product bioactive artificial joint material of the present invention.
Embodiment 4
(1) at first select for use the Ti6Al4V alloy to process artificial joint;
(2) artificial joint surface activation process: after artificial joint used acetone, 70% ethanol, distilled water ultrasonic cleaning successively, adopting concentration was 30% ebullient H
2O
2Aqueous solution is handled, and the processing time is 90 minutes, take out flushing after, be immersed in temperature again and be 60-70 ℃, concentration and be in the NaOH aqueous solution of 8M 24-36 hour, take out distilled water flushing, 70 ℃ of dryings.
(3) the bionical deposition processes of calcium phosphate amorphous underlayer: the artificial joint immersion temperature that surface activation process is crossed is that bionical calcifying solution A is among 30 ℃ of bionical calcifying solution A by the active constituent content of ionometer: sodium ion 610mM, magnesium ion 4.5mM, calcium ion 12.5mM, chloride ion 610.0mM, phosphoric acid hydrogen radical ion 5.0mM, bicarbonate ion 18.0mM.Bionical calcifying solution A employing magnetic stirring apparatus stirs, takes out after bionical deposition processes 24-36 hour, and the distilled water ultrasonic cleaning, drying at room temperature, the artificial joint surface obtains the calcium phosphate amorphous layer of thickness 7.5-9.0 μ m, densification.
(4) the bionical deposition processes of osteoid apatite crystalline phase surface layer: the artificial joint immersion temperature that the surface is had the calcium phosphate amorphous layer is that bionical calcifying solution B presses the active constituent content of ionometer among 50 ℃ of molten B of bionical calcification: sodium ion 120.0mM, potassium ion 5.0mM, magnesium ion 3.5mM, calcium ion 2.5mM, chloride ion 120.0mM, phosphoric acid hydrogen radical ion 1.0mM, bicarbonate ion 11.0mM, sulfate ion 0.5mM.Took out in bionical deposition processes 48-64 hour, the distilled water ultrasonic cleaning, drying at room temperature, further deposit thickness is 40-50 μ m, porous osteoid apatite crystalline phase surface layer on the artificial joint surface phosphoric acid calcium amorphous underlayer.
(3) surface being immersed in bone morphogenetic protein and concentration by the artificial joint of porous calcium phosphorus bioactive ceramic coating is in the mixed solution formed of the phosphate buffered saline(PBS) of 0.1mol/L, bone morphogenetic protein concentration is 0.1-50mg/L, 20-40 ℃ was soaked 5-15 hour down, slowly stirred once, and took out in middle every 1-2 hour;
(4) with above-mentioned taking-up artificial joint with ethanol drip washing after, vacuum drying, the sterilization aseptic preservation in back, standby, get final product bioactive artificial joint material of the present invention.
Obviously, the above embodiment of the present invention only is in order to clearly demonstrate example of the present invention, and is not to be qualification to embodiments of the present invention.For those of ordinary skill in the field; also can make other changes in different forms on the basis of the above description; here need not also can't give all embodiments exhaustive, and these belong to conspicuous variation or the change that spirit of the present invention amplified out and still are in protection scope of the present invention.
Claims (4)
1. bioactive artificial joint material, it is characterized in that, this bioactive artificial joint material has one deck to have double-deck porous calcium phosphorus bioactive ceramic coating at metal base surface, its surface further is compounded with bone morphogenetic protein (BMP), the porous calcium phosphorus bioactive ceramic coating of being addressed is made up of calcium phosphate amorphous underlayer that contacts with metallic matrix and osteoid apatite crystalline phase surface layer, wherein, calcium phosphate amorphous underlayer thickness is 1-10 μ m; Osteoid apatite crystalline phase surface layer thickness is 10-100 μ m.
2. a bioactive artificial joint preparation methods as claimed in claim 1 is characterized in that the method for preparing comprises the steps:
(1) at first select for use titanium alloy, rustless steel or vitallium to process artificial joint;
(2) artificial joint is carried out surface activation process, go on foot bionical deposition processes by two then, obtain the porous calcium phosphorus bioactive ceramic coating of forming successively by fine and close calcium phosphate amorphous underlayer and porous osteolith stone crystalline phase surface layer on the artificial joint surface;
(3) surface is immersed in the mixed solution that bone morphogenetic protein and phosphate buffered saline(PBS) form by the artificial joint of porous calcium phosphorus bioactive ceramic coating, bone morphogenetic protein concentration is 0.1-50mg/L, 20-40 ℃ was soaked 5-15 hour down, slowly stirred once, and took out in middle every 1-2 hour; Get final product the bioactive artificial joint material.
3. bioactive artificial joint preparation methods as claimed in claim 2 is characterized in that it is the ebullient H of 10-60% that surface activation process adopts concentration
2O
2Aqueous solution, the processing time is 10-90 minute, take out flushing after, be immersed in temperature again and be 30-80 ℃, concentration and be in the NaOH aqueous solution of 1-10M 6-48 hour.
4. bioactive artificial joint preparation methods as claimed in claim 2 is characterized in that bionical deposition processes of two steps comprises the steps:
1) the bionical calcifying solution A of preparation: bionical calcifying solution A presses the active constituent content of ionometer:
Sodium ion 500-850mM, magnesium ion 4.5-6.0mM, calcium ion 10.0-13.5mM, chloride ion 500-800mM, phosphoric acid hydrogen radical ion 4.0-6.0mM, bicarbonate ion 15.0-30.0mM;
2) the bionical calcifying solution B of preparation: bionical calcifying solution B presses the active constituent content of ionometer:
Sodium ion 100.0-180.0mM, potassium ion 4.0-5.5mM, magnesium ion 3.0-4.5mM, calcium ion 2.0-3.5mM, chloride ion 80.0-150.0mM, phosphoric acid hydrogen radical ion 0.5-1.5mM, bicarbonate ion 6.5-12.0mM, sulfate ion 0.5-1.0mM;
3) the bionical deposition processes of calcium phosphate amorphous underlayer: the artificial joint material immersion temperature that surface activation process is crossed is among the 10-30 ℃ of bionical calcifying solution A, under stirring condition, take out after bionical deposition processes 12-36 hour, clean, drying, the artificial joint material surface obtains the calcium phosphate amorphous layer of thickness 1-10 μ m;
4) the bionical deposition processes of osteoid apatite crystalline phase surface layer: the artificial joint material immersion temperature that the surface is had the calcium phosphate amorphous layer is among the 30-50 ℃ of bionical calcifying solution B, took out in bionical deposition processes 12-144 hour, clean, drying, further deposit thickness is 10-100 μ m, porous osteoid apatite crystalline phase layer on the artificial joint material surface phosphoric acid calcium amorphous layer.
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| CN100421734C (en) * | 2005-04-26 | 2008-10-01 | 中国科学院金属研究所 | Fast preparation of titanium or titanium alloy surface biological active coating |
| CN101732761A (en) * | 2010-01-01 | 2010-06-16 | 东南大学 | Joint prosthesis by using titanium oxide nanotubes to load bone morphogenetic protein |
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| CN101766838B (en) * | 2009-12-31 | 2012-10-24 | 东南大学 | Functionalized artificial joint with selenium-loaded nanotube array surface and preparation method thereof |
| CN101732761A (en) * | 2010-01-01 | 2010-06-16 | 东南大学 | Joint prosthesis by using titanium oxide nanotubes to load bone morphogenetic protein |
| CN101744666B (en) * | 2010-01-01 | 2012-02-22 | 东南大学 | Artificial tooth root with slow release function of trace element of selenium and preparation method thereof |
| CN101766841B (en) * | 2010-01-01 | 2012-10-24 | 东南大学 | Artificial joint having slow-release function of rare earth element cerium and preparation method thereof |
| CN101732761B (en) * | 2010-01-01 | 2013-04-03 | 东南大学 | Joint prosthesis by using titanium oxide nanotubes to load bone morphogenetic protein |
| CN104645414A (en) * | 2015-02-15 | 2015-05-27 | 宝鸡文理学院 | Titanium-based surface antibacterial and bone tissue regeneration induced functional coating as well as preparation method and application thereof |
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| CN106492271A (en) * | 2016-12-13 | 2017-03-15 | 温州医科大学附属口腔医院 | Antibacterial promotees the preparation of the difunctional Guided Bone Regeneration Absorbable membrane of synosteosis |
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