Shape memory polymer (SMP) scaffolds with improved self-fitting properties.
Shape memory polymer (SMP) scaffolds with improved self-fitting properties.
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DOI：
10.1039/d0tb02987d
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发表时间：
2021-05-14
期刊：
影响因子：
--
通讯作者：
Grunlan MA
中科院分区：
文献类型：
--
作者：
Pfau MR;McKinzey KG;Roth AA;Graul LM;Maitland DJ;Grunlan MA
用交联线性聚（ε-己内酯）-二丙烯酸酯（PCL-DA, Mn ~10 kg/mol）和线性聚（l -乳酸）（PLLA, Mn ~15 kg/mol） [75/25 wt%]制备的“自拟合”形状记忆聚合物（SMP）支架与PCL-DA支架对照相比，具有良好的力学性能和更快的降解速率。然而，它们治疗不规则颅颌面（CMF）骨缺损的潜力受到其相对较高的安装温度（Tfit ~55℃；与PCL的Tm相关）的限制，在支架的压合过程中需要形状恢复（即膨胀）和随后的形状固定，这可能对周围组织有害。此外，在制造过程中，浇铸在熔融盐模板上的溶剂型前驱体溶液的粘度会限制支架的尺寸。因此，在这项工作中，类似的半ipn SMP支架也由四臂星型pcl -四酸酯（star-PCL-TA） （Mn ~10 kg/mol）和星型plla （Mn ~15 kg/mol）形成。为了评估星形聚合物结构的影响，制备了四种半ipn组合物：线性- pcl - da /线性- plla （L/L）、线性- pcl - da /星形- plla （L/S）、星形- pcl - ta /线性- plla （S/L）和星形- pcl - ta /星形- plla （S/S）。还制备了两种PCL对照：LPCL（即100%线性-PCL- da）和SPCL（即100%星形-PCL- ta）。S/S半ipn支架表现出特别理想的性能。除了达到较低的组织安全Tfit（~45°C）外，它还表现出最快的降解速度，预计更有利于新组织的浸润。S/S半ipn支架在Tfit处施加的径向膨胀压力大于LPCL，有望增强骨整合和力学稳定性。S/S半ipn大分子溶液的特性粘度也降低了，从而可以制备更大的支架样品。
“Self-fitting” shape memory polymer (SMP) scaffolds prepared as semi-interpenetrating networks (semi-IPNs) with crosslinked linear-poly(ε-caprolactone)-diacrylate (PCL-DA, Mn ~10 kg/mol) and linear-poly(L-lactic acid) (PLLA, Mn ~15 kg/mol) [75/25 wt%] exhibited robust mechanical properties and accelerated degradation rates versus a PCL-DA scaffold control. However, their potential to treat irregular craniomaxillofacial (CMF) bone defects is limited by their relatively high fitting temperature (Tfit ~55 °C; related to the Tm of PCL) required for shape recovery (i.e. expansion) and subsequent shape fixation during press fitting of the scaffold, which can be harmful to surrounding tissue. Additionally, the viscosity of the solvent-based precursor solutions, cast over a fused salt template during fabrication, can limit scaffold size. Thus, in this work, analogous semi-IPN SMP scaffolds were also formed with a 4-arm star-PCL-tetracryalate (star-PCL-TA) (Mn ~10 kg/mol) and star-PLLA (Mn ~15 kg/mol). To assess the impact of a star-polymer architecture, four semi-IPN compositions were prepared: linear-PCL-DA/linear-PLLA (L/L), linear-PCL-DA/star-PLLA (L/S), star-PCL-TA/linear-PLLA (S/L) and star-PCL-TA/star-PLLA (S/S). Two PCL controls were also prepared: LPCL (i.e. 100% linear-PCL-DA) and SPCL (i.e. 100% star-PCL-TA). The S/S semi-IPN scaffold exhibited particularly desirable properties. In addition to achieving a lower, tissue-safe Tfit (~45 °C), it exhibited the fastest rate of degradation which is anticipated to more favourably permit neotissue infiltration. The radial expansion pressure exerted by the S/S semi-IPN scaffold at Tfit was greater than that of LPCL, which is expected to enhance osseointegration and mechanical stability. The intrinsic viscosity of the S/S semi-IPN macromer solution was also reduced such that larger scaffold specimens could be prepared.
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