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生物可降解聚酯/生物陶瓷3D打印骨组织工程支架研究进展

刘嗣聪 刘宏治 殷亚然

刘嗣聪, 刘宏治, 殷亚然. 生物可降解聚酯/生物陶瓷3D打印骨组织工程支架研究进展[J]. 复合材料学报, 2024, 41(4): 1672-1693. doi: 10.13801/j.cnki.fhclxb.20231211.002
引用本文: 刘嗣聪, 刘宏治, 殷亚然. 生物可降解聚酯/生物陶瓷3D打印骨组织工程支架研究进展[J]. 复合材料学报, 2024, 41(4): 1672-1693. doi: 10.13801/j.cnki.fhclxb.20231211.002
LIU Sicong, LIU Hongzhi, YIN Yaran. Research advances in 3D printed bone tissue engineering scaffolds based on biodegradable polyester/bioceramics[J]. Acta Materiae Compositae Sinica, 2024, 41(4): 1672-1693. doi: 10.13801/j.cnki.fhclxb.20231211.002
Citation: LIU Sicong, LIU Hongzhi, YIN Yaran. Research advances in 3D printed bone tissue engineering scaffolds based on biodegradable polyester/bioceramics[J]. Acta Materiae Compositae Sinica, 2024, 41(4): 1672-1693. doi: 10.13801/j.cnki.fhclxb.20231211.002

生物可降解聚酯/生物陶瓷3D打印骨组织工程支架研究进展

doi: 10.13801/j.cnki.fhclxb.20231211.002
基金项目: 国家自然科学基金项目(52373107;51573169);浙江省自然科学基金项目(LY15E030007);宁波市“3315计划”创新团队项目
详细信息
    通讯作者:

    刘宏治,博士,教授,硕士生导师,研究方向为纤维素纳米纤维(CNF)工业化制备、高值化应用和“绿色”、高性能聚乳酸(PLA)材料开发 E-mail: hzliu@iccas.ac.cn

  • 中图分类号: TB332

Research advances in 3D printed bone tissue engineering scaffolds based on biodegradable polyester/bioceramics

Funds: National Natural Science Foundation of China (52373107; 51573169); Zhejiang Provincial Natural Science Foundation of China (LY15E030007); Ningbo "3315 Innovative Team" Project
  • 摘要: 移植骨植入物是目前治疗骨缺损的公认有效手段之一。生物可降解聚酯/生物陶瓷复合材料结合了生物可降解聚酯的良好力学性能、可降解性能和生物陶瓷的成骨活性,为骨植入物材料提供了新的选择。骨组织工程通过模拟骨骼微环境,加速骨缺损修复。将生物可降解聚酯/生物陶瓷复合材料制备成骨组织工程支架,能进一步加快骨修复进程。3D打印技术的引入能使生物可降解聚酯/生物陶瓷骨组织工程支架的制备过程精确、可重复且具备高自由度,展现出了良好的发展前景。本文阐述了骨组织工程支架应具备的各项性能,总结了近年来国内外学者对生物可降解聚酯/生物陶瓷骨组织工程支架上述性能的改善策略,并展望未来该研究领域的发展方向。

     

  • 图  1  基于自然骨结构的骨植入物设计

    Figure  1.  Bone implant design based on natural bone structure

    BPE—Biodegradable polyester; BC—Bioceramics; ECM—Extracellular matrix

    图  2  支架制造技术示意图

    Figure  2.  Schematic illustrations of classical scaffold fabrication techniques

    Pgas—Current gas pressure; Pgas 0 —Equilibrium gas pressure

    图  3  各种3D打印工艺的示意图:(a) 熔融沉积建模/熔丝制造[17];(b) 扫描激光烧结[19];(c) 立体光刻打印[20];(d) 3D生物打印[21];(e) 熔融电写[22]

    Figure  3.  A compilation/schematic of various 3D printing processes: (a) Fused deposition molding/fused filament fabrication[17]; (b) Selective laser sintering[19]; (c) Stereolithography[20]; (d) 3D bio-printing[21]; (e) Melt electrospinning writing[22]

    v—Vertical

    图  4  各类生物可降解聚酯的合成路径:(a) 聚乙醇酸(PGA);(b) 聚乳酸(PLA);(c) 聚己内酯(PCL);(d) 聚乳酸-乙醇酸(PLGA)

    Figure  4.  Synthetic paths of various biodegradable polyesters: (a) Poly(glycolic acid) (PGA); (b) Poly(lactide acid) (PLA); (c) Poly(e-caprolactone) (PCL); (d) Poly(lactide-co-glycolide) (PLGA)

    图  5  3D打印生物可降解聚酯/生物陶瓷骨组织工程支架的结构、性能及改进策略

    Figure  5.  Structure, properties and improvement strategies of 3D-printed biodegradable polyester/bioceramics bone tissue engineering scaffolds

    图  6  (a) 左旋聚乳酸(PLLA)/左旋聚乳酸改性羟基磷灰石(P-HA)支架的制备流程[27];(b) 熔融沉积建模(FDM)技术制备PLA-硬脂酸(SA)支架[29];(c) 扫描激光烧结(SLS)技术制备PLLA/氧化石墨烯(GO)@Si-HA复合材料支架[31];(d) PLA/PCL/聚(3-羟基丁酸-3-羟基戊酸) (PHBV)/锶取代纳米羟基磷灰石(Sr-nHA)复合材料支架的制备与表征[32]

    Figure  6.  (a) Preparation process of poly(L-lactide) (PLLA)/PLLA-modified HA nanoparticles (P-HA) scaffolds[27]; (b) Preparation of PLA-stearic acid (SA) scaffolds by fused deposition modeling (FDM) technique[29]; (c) Preparation of PLLA/graphene oxide (GO)@Si-HA by selected laser sintering (SLS) technique[31]; (d) Preparation and characterization of PLA/PCL/poly(-3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV)/Sr-nano-hydroxyapatite (Sr-nHA) composite scaffolds[32]

    TEOS—Ethyl silicate; D-HA—Poly-dopamine-coated HA nanoparticles; DMH—1, 6-diaminohexane; DA—Dopamine hydrochloride; MC3T3-E1—Mouse embryo osteoblast precursor cells

    图  7  聚乳酸-乙醇酸(PLGA)/β-磷酸三钙(β-TCP)/丹参酚酸B (SB)支架的制备流程与体内外表征[66]

    Figure  7.  Preparation process and in vitro and in vivo characterization of polylactic acid-co-polyglycolic acid (PLGA)/β-tricalcium phosphate (β-TCP)/salvianolic acid B (SB) scaffolds[66]

    OIM—Osteogenic induction medium; DMEM—Dulbecco's modified eagle medium; α-MEM—Minimum essential medium α

    图  8  (a1) PLA-胶原蛋白(Col)-米诺环素(MH)-柠檬酸-羟基磷灰石(cHA)支架的制备流程[46];(a2) PLA-Col、PLA-Col-MH、PLA-Col-MH-cHA支架表面形态[46];((b1)~(b3)) PLLA@HA@Ag颗粒的制备[47]

    Figure  8.  (a1) Preparation process of PLA-collagen (Col)-minocycline (MH)-citrate-hydroxyapatite (cHA) scaffolds[46]; (a2) Surface morphology of PLA-Col, PLA-Col-MH, and PLA-Col-MH-cHA scaffolds[46]; ((b1)-(b3)) Preparation of PLLA@HA@Ag particles[47]

    SBF—Simulated body fluid; hMSCs—Human mesenchymal stem cells; RUNX2—Runt-related transcription factor; OCN—Osteocalcin; OPN—Osteopontin

    表  1  典型骨植入物材料性能对比

    Table  1.   Performance comparison of typical bone implant materials

    Types Advantages Drawbacks
    Natural bone implants Autogenous bone Osteogenic activity, biocompatibility Long surgery time and limited donor bone
    Homologous bone Wide range of materials, biocompatible Immune response, non-osteogenic activity,
    poor mechanical stability
    Metaphyseal bone Low cost, widely available, non-immunogenic Non-osteogenic activity
    Metals Tantalum, titanium, magnesium alloys Lightweight, high strength, good biocompatibility Complex production process, slow bone
    formation, non-degradable, stress masking
    Bioactive ceramics β-tricalcium phosphate
    (β-TCP)
    Similar composition with bone mineral, good degradability, osteogenic activity, compressive strength Mechanically brittle
    Bio-glass (BG)
    Hydroxyapatite (HA)
    Synthetic polymers Polyetheretherketone (PEEK) High strength, biocompatible, good plasticity Non-degradable
    Poly(lactic acid) (PLA) Plasticity, biocompatibility,
    biodegradability
    Insufficient mechanical properties, non-osteogenic activity
    Polycaprolactone (PCL)
    Polyglycolic acid (PGA)
    Polylactic acid-co-polyglycolic acid (PLGA)
    Composites PLA/HA Similar to natural bone matrix, good biocompatibility, good osteo-conductivity, low immune-genicity Demanding requirement in manufacture
    process
    下载: 导出CSV

    表  2  传统骨组织工程支架制备方法

    Table  2.   Preparation methods of bone tissue engineering scaffolds

    Preparation methods Preparation principles Advantages Drawbacks
    Electrospinning [9] Formation of fibers through the influence of an electric field, followed by deposition of the fibers
    to produce a highly porous structure
    Low cost Low connectivity of pores, irregularity, uncon-
    trollable pore size, low strength, poor repeatability
    Gas foaming[11] Gases grow inside the composite to form a three-dimensional porous polymer structure High porosity, small pore size, no use of organic solvents
    Solvent casting/particle leaching[12] Lyophilization to remove solvents from the polymer and filtration to obtain a porous structure Simple operation, controlled pore size
    and porosity
    Thermally induced phase separation[13] The polymer is dissolved in the solvent at a higher temperature and the porous structure is formed by lowering the temperature until the composite freezes inducing phase separation Good mechanical properties
    下载: 导出CSV

    表  3  3D打印骨组织工程支架制备方法

    Table  3.   Preparation methods of 3D printing bone tissue engineering scaffold

    3D printing type Working principle Advantage Drawback
    Fused deposition modeling/fused filament fabrication (FDM/FFF)[17] The polymer in its molten state is prepared as a filament and printed through the spinneret Inexpensive and durable, can be used with a wide range of materials Low resolution, anisotropic, nozzle may be clogged, support required
    Selected laser sintering
    (SLS)[19]
    Use of laser technology and heat curing Highly durable, easy to remove support material High equipment and material costs, easy to deform prints
    Stereolithography
    (SLA)[20]
    Laser beam scanning and hardening of
    UV-sensitive materials
    High print accuracy Short laser life and high cost
    3D-bioprinting[21] Pressurized syringe extrusion combined with UV curing Highly customizable Uneven micro-morphology
    Melt electrospinning writing (MEW)[22] Combining the advantages of electrostatic spinning and 3D printing Solvent-free, environmentally friendly and highly efficient Higher cost
    下载: 导出CSV

    表  4  典型生物可降解聚酯的性能对比

    Table  4.   Performance comparison of typical biodegradable polyesters

    Polyester type Density/(g·cm−3) Tensile strength/MPa Tensile modulus/GPa Tg/℃ Tm/℃ Biodegradation time/month
    PLA 1.25-1.27 27.6-50.0 1.00-3.45 50-60 12-16
    PLLA 1.24-1.30 15.5-150 2.7-4.14 55-65 170-200 >24
    PDLA 1.21-1.25 21-60 0.35-3.5 45-60 150-162
    PGA 1.50-1.71 60-99.7 6.0-7.0 35-45 220-233 6-12
    PCL 1.11-1.14 20.7-42 0.21-0.44 −60-−65 58-65 >24
    Notes: PLLA—Poly(L-lactide); PDLA—Poly(D-lactide); Tg—Glass transition temperature; Tm—Melting temperature.
    下载: 导出CSV

    表  5  文献报道的FDM打印制备的PLA/HA复合材料骨组织工程支架力学性能

    Table  5.   Mechanical properties of PLA/HA bone tissue engineering scaffolds prepared by FDM printing reported in the literature

    Preparation method Compositions Pore size/μm Scaffold mechanical properties
    Compressive
    strength/MPa
    Compressive
    modulus/MPa
    Tensile strength/MPa Tensile modulus/MPa
    Adding
    surfactants
    PLA[27] 800 3.13
    PLA/PDA-HA[27] 800 4.00
    PLLA[28] 44.02±6.85 43±0.09
    PLLA/30HA[28] 29.68±1.92 45.54±0.11
    PLLA/50HA[28] 14.22±0.63 44.32±0.10
    PLA[29] 200 45 56
    PLA/SA-HA[29] 200 45 7
    Adding other additives PLA[30] 1200 31.34±0.16 598.09±15.24
    PLA/3WS/3HA[30] 1200 32.15±0.44 506.01±3.52
    PLA/3WS/8HA[30] 1200 26.83±0.08 721.97±18.27
    PLA/3WS/15HA[30] 1200 35.72±0.97 883.22±12.32
    PLA/8WS/3HA[30] 1200 27.58±1.08 723.80±10.23
    PLA/15WS/3HA[30] 1200 23.36±0.48 680.90±1.93
    PLLA[31] 12.1 118
    PLLA/GO[31] 18.5 240
    PLLA/GO@Si-HA[31] 22.4 280
    PLLA[32] 800 26.43
    PLLA/PCL/PHBV/
    2.5Sr-nHA[32]
    800 32.57
    Notes: PDA—Polydopamine; WS—Walnut shell.
    下载: 导出CSV

    表  6  不同孔隙形状与孔径的3D打印PLA/HA骨组织工程支架的力学性能[33]

    Table  6.   Mechanical properties of 3D printed PLA/HA bone tissue engineering scaffolds with different pore shapes and pore diameters[33]

    Sample Compress strength/MPa Elastic modulus/MPa Poisson's ratio Density/(g·cm−3)
    Cube-1 5.48 125 0.31 2.9
    Cube-2 6.20 136 0.32 2.9
    Cylinder-1 6.52 190 0.31 2.9
    Cylinder-2 6.70 204 0.33 2.9
    Hexgonal-1 7.20 350 0.34 2.9
    Hexgonal-2 7.55 410 0.35 2.9
    下载: 导出CSV

    表  7  文献报道的生物可降解聚酯/生物陶瓷骨组织工程支架性能参数

    Table  7.   Performance parameters of biodegradable polyester/bioceramic bone tissue engineering scaffolds prepared reported in the literatures

    Biomaterial Mixing mass ratio (Polyester :
    Bioceramic)
    Bioceramic particle size Production method Porosity/% Pore size/
    μm
    Elastic modulus Compressive strength/MPa Ref.
    PLA+HA 90:10 50 μm FFF 58 450 [75]
    PLA+CaP coating Uncoated FDM 49.93±5.28 (0.512±0.24) GPa 20.50±1.95 [84]
    98:2 49.09±3.2 (0.510±0.11) GPa 31.18±4.85
    PLA+n-HA 80:20 FDM 70±2.23 (10.12±1.24) GPa 31.18±4.86 [81]
    PLLA+β-TCP 100:0 250 μm 3D bioplotter ~62 100 258±102 [85]
    90:10 18.22±2.67
    70:30 31.18±4.86
    PLA+AW 70%AW+30%MD Powder (50:50) 55% (90 μm)
    15% (0-53 μm)
    AW-binder jetting/sintering
    PLA-FFF
    AW disks 41.85%±
    0.94%
    PLA 60%
    [86]
    PLA+HA 85:15 (2.1±0.4) μm MDS 60±1.5 500±20 [87]
    PLA+OCP 40:60 MEB 500 1 [70]
    PLA+n-HA 100:0 50-80 nm FDM ~50 ~35 [88]
    90:10 ~29
    80:20 ~28
    70:30 ~25
    60:40 ~23
    50:50 ~17
    PLA+n-HA 100:0 (75±20) nm FDM 300-400 35.41±2.07 [89]
    50:50 17.80±1.92
    PLLA+n-HA 100:0 50-80 nm FDM 60 (43±0.09) MPa 44.02±6.85 [28]
    70:30 (45.54±0.11) MPa 29.68±1.92
    50:50 (44.31±0.10) MPa 14.22±0.20
    PLA+HA 70:30 50 μm 3D bioplotter 60 500 [90]
    PLA+n-HA 90:10 (63±1.5) nm FDM 26.4 292±1.8 23.36±0.48 [91]
    PLA+HA 85:15 (2.1±1) μm MDS 60 500 [82]
    PLA+HA FDM [82]
    Notes: AW—Apatite-wollastonite; MD—Maltodexrin; OCP—Octacalcium phosphate; MDS—Mini-deposition system; MEB—Micro-extrusion biopinting.
    下载: 导出CSV

    表  8  文献报道的生物可降解聚酯/生物陶瓷骨组织工程支架的体内测试方案

    Table  8.   In vivo testing protocols for biodegradable polyester/bioceramic bone tissue engineering scaffoldsreported in the literatures

    Biomaterial groups Animal Sample size Defect CSD Empty control Groups Bone metabolisms substances Sacrifice weeks Main findings Ref.
    PLA/HA Rat wistar
    300 g
    4 m/o
    1/2 female
    1/2 male
    24 Calvarial bone circular bilateral defect diameter 5.5 mm Yes Yes Empty (n=8)
    Bio-oss (n=8)
    PLA (n=8)
    PLA/HA (n=8)
    PLA/HA+DPSC (n=8)
    PLA/HA+ECM
    (n=8)
    DPSC
    ECM
    8 w Osteogenic capacity is comparable to
    bio-oss.
    [75]
    PLA/CaP Rat wistar
    300-400 g
    45 Calvarial bone circular unilateral defect diameter 8 mm Yes No PLA (n=15)
    PLA/CaP (n=15)
    PLA/CaP+rhBMP-2 (n=15)
    rhBMP-2 1 m, 3 m and 6 m Promoting new bone formation after 6 months without rhBMP-2. [84]
    PLA/
    n-HA
    Rat sprague-dawley
    280-320 g weight
    12-13 w/o male
    126 Calvarial bone
    circular unilateral defect
    diameter 6 mm
    No Yes Empty (n=24)
    PLA/n-HA (n=24)
    PLA/n-HA+EMF
    (n=24)
    PLA/n-HA+EMF+
    BMSCs
    (n=24)
    BMSCs
    sinusoidal EMF;
    15 Hz, 1 mT
    4 h/day
    4 w and 12 w PLA/HA/BMSCs scaffolds with EMF exposure present the best bone integration among all the groups. [81]
    PLLA/β-TCP Rat sprague-dawley
    320-350 g
    8 w/o
    90 Calvarial bone circular unilateral defect
    diameter 5 mm
    No No PLLA (n=15)
    PLLA/TCP10 (n=15)
    PLLA/TCP30 (n=15)
    PLLA+
    MG-63 (n=15)
    PLLA/TCP10+
    MG-63 (n=15)
    PLLA/TCP30+
    MG-63 (n=15)
    MG-63 4 w, 8 w and 12 w Higher bone regeneration rate in those animals with higher percent of TCP and after adding of MG-63 to the scaffolds. [85]
    PLA/AW Rat sprague-dawley
    350 g
    adult
    male
    15 Calvarial bone circular unilateral defect diameter 8 mm Yes No PLA discs (n=3)
    AW discs (n=6)
    AW/PLA discs (n=6)
    12 w AW/PLA scaffold shows highest formed new bone. [86]
    PLA/HA Rat sprague-dawley
    300-350 g
    8 w/o
    male
    32 Calvarial bone
    circular unilateral defect
    diameter 5 mm
    No Yes 3DP PLA/HA (n=8)
    β-TCP (n=8)
    DBM (n=8)
    Black control (n=8)
    4 w and 8 w The percentage of new bone area in 3DP PLA/HA scaffolds was larger than in DBM and control groups but less than β-TCP groups. [87]
    PLA/OCP Rat
    6-8 w/o
    Calvarial bone
    circular unilateral defect
    diameter 5 mm
    No Yes La 8 w The scaffolds enhanced bone defect regeneration in vivo. 0.2La-OCP/PLA scaffolds are significantly more likely to enhance bone defect regeneration in vivo than other groups. [70]
    PLA/n-HA Rabbit
    New Zealand
    white
    2-3 kg, male
    18 Femoral Diaphysis
    circular
    No No PLA (n=9)
    PLA/n-HA30%
    (n=9)
    4 w, 8 w and 12 w [88]
    PLA/n-HA Rabbit
    New Zealand
    white
    2-3 kg, male
    Femoral Diaphysis circular unilateral defect
    diameter 5 mm
    No No 1 m, 2 m and 3 m The increasing incorporation of n-HA doesn't affect significantly the overall mechanical strength in a limited range (0%-30%), but it really enhances the osteogenesis in vivo. [89]
    PLLA/n-HA Rabbit
    New Zealand
    white
    2-3 kg, male
    9 Diaphysis left
    Radius
    segmental
    unilateral defect
    15 mm
    Yes No PLLA (n=3)
    PLLA/30%n-HA (n=3)
    PLLA/50%n-HA (n=3)
    4 w The new bone growth of the PLLA/50%n-HA composite material is significantly higher than that of the PLA group. [28]
    PLA/HA Rabbit
    New Zealand
    white
    (2.5±0.25) kg, 6 m/o
    36 Diaphysis left
    Radius
    segmental
    unilateral defect
    15 mm
    Yes No ICBG+IM (n=9)
    PLA/HA (n=9)
    IM+PLA/HA (n=9)
    IM+PLA/HA +eBM (n=9)
    eBM
    ICBG
    IMemb
    4 w, 12 w and 16 w The PLLA/50%n-HA has shown a preferable capability of bone regeneration, compared with the PLLA/30%n-HA specimens than the PLLA ones. [90]
    PLA/n-HA Rabbit
    New Zealand
    white
    (4.2±0.18) kg, 6 m/o
    3 Distal right Femur circular unilateral defect
    diameter 5 mm and depth
    10-13 mm
    No No PLA/HA (n=3) 4 w, 8 w and 12 w The IM combined with 3D-printed PLA-HA scaffold and eBM has a bigger efficiency for treatment of large bone defects than the PLA-HA and the IM/PLA-HA groups, and similar to the IM/ICBG group. [91]
    PLA/HA Rabbit
    New Zealand
    white
    (2.5±0.2) kg, 6 m/o
    24 Tibial diaphysis Periosteum
    cuboid shaped periosteal pockets 10 mm in length and 7.5 mm in diameter
    No Experimental group:
    PLA/HA+BMSCs with blood vessel
    Control group:
    PLA/HA+BMSCs without blood vessel
    BMSCs 4 w and
    8 w
    In vivo trials confirmed that the printed PLA/n-HA scaffold can enhance osteogenesis and osteo conductivity. It was showing bone formation within the femoral defect at 4, 8 and 12 weeks, and no inflammation signs. [82]
    Notes: m/o—Months old; w/o—Weeks old; IM—Intramuscular injection; IV—Intravenous injection; BMSCs—Bone marrow mesenchymal stem cells; DBM—Demineralized bone marrow; La—Lanthanum; eBM—Enhanced bone marrow; ICBG—Iliac crest bone graft; IMemb—Induced membranes; w—Weeks; m—Months; DPSC—Dental pulp stem cells; ECM—Extracellular matrix; rhBMP-2—Recombinant human protein; EMF—Electromagneticfields; MG63—Human osteoblast-like cell; 3DP—3D printing; n—Sample size; CSD—Critical-sized defect.
    下载: 导出CSV
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  • 收稿日期:  2023-10-07
  • 修回日期:  2023-11-16
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