Hydrolytic Degradation of Porous Crosslinked Poly(ε-Caprolactone) Synthesized by High Internal Phase Emulsion Templating
Hydrolytic Degradation of Porous Crosslinked Poly(ε-Caprolactone) Synthesized by High Internal Phase Emulsion Templating
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DOI：
10.3390/polym12081849
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发表时间：
2020-08-01
期刊：
影响因子：
5
通讯作者：
Hakkarainen, Minna
中科院分区：
文献类型：
--
作者：
Erdal, Nejla Benyahia;Lando, Gabriela Albara;Hakkarainen, Minna
采用高内聚乳液（HIPE）技术制备了多孔聚己内酯（PCL）支架材料。以双（ε -己内酯-4-基）（BCY）为交联剂。通过改变交联密度和分散相体积分数，研究这些参数对37℃和60℃水解降解的潜在影响。不同水解次数后，对剩余固体样品进行傅里叶变换红外光谱（FTIR）和扫描电镜（SEM）分析。采用激光解吸电离-质谱法（LDI-MS）分析老化水溶液中的降解产物。正如预期的那样，温度对降解过程和降解产物释放的影响是显著的。FTIR分析也显示了温度效应，在60℃水解70天后，羟基吸收带的强度显著增加，表明聚合物链发生了明显的断裂。LDI-MS分析证实了低聚物的释放范围从二聚体到六聚体。产物形态相似，但相对/ z信号强度随时间、温度和交联密度的增加而增加，表明产物释放量较大。后者可能是由于结晶度随交联剂用量的增加而降低所致。在老化过程中，支架失去了多孔结构和形态。交联密度越高，支架保持原有多孔结构和形态的时间越长。
Porous poly(epsilon-caprolactone) (PCL) scaffolds were fabricated using the high internal polymerization emulsion (HIPE) technique. Bis(epsilon-caprolactone-4-yl) (BCY) was utilized as crosslinker. The crosslinking density and the volume fraction of the dispersed phase were varied in order to study the potential effect of these parameters on the hydrolytic degradation at 37 degrees C and 60 degrees C. After different hydrolysis times the remaining solid samples were analyzed by Fourier transform infrared spectroscopy (FTIR) and scanning electron microscopy (SEM), while the degradation products in the aqueous aging solutions were analyzed by laser desorption ionization-mass spectrometry (LDI-MS). The effect of temperature on the degradation process and release of degradation products was, as expected, significant. The temperature effect was also shown by FTIR analysis that displayed a pronounced increase in the intensity of the hydroxyl-group absorption band after 70 days of hydrolysis at 60 degrees C indicating significant cleavage of the polymer chains. LDI-MS analysis proved the release of oligomers ranging from dimers to hexamers. The product patterns were similar, but the relativem/zsignal intensities increased with increasing time, temperature and crosslinking density, indicating larger amounts of released products. The latter is probably due to the decreasing degree of crystallinity as a function of amount of crosslinker. The porous structure and morphology of the scaffolds were lost during the aging. The higher the crosslinking density, the longer the scaffolds retained their original porous structure and morphology.