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Ultrahigh-water-content biocompatible gelatin-based hydrogels: Toughened through micro-sized dissipative morphology as an effective strategy
Biomaterials Advances ( IF 7.9 ) Pub Date : 2020-11-27 , DOI: 10.1016/j.msec.2020.111750
M. Sheikhi , F. Rafiemanzelat , L. Moroni , M. Setayeshmehr

Fabrication of simultaneously robust and superabsorbent gelatin-based hydrogels for biomedical applications still remains a challenge due to lack of locally dissipative points in the presence of large water content. Here, we apply a synthesis strategy through which water absorbency and energy dissipative points are separated, and toughening mechanism is active closely at the crack tip. For this, gelatin-based microgels (GeMs) were synthesized in a way that concentrated supramolecular interactions were present to increase the energy necessary to propagate a macroscopic crack. The microgels were interlocked to each other via both temporary hydrophobic associations and permanent covalent crosslinks, in which the sacrificial binds sustained the toughness due to the mobility of the junction zones and particles sliding. However, chemical crosslinking points preserved the integrity and fast recoverability of the hydrogel. Hysteresis increased strongly with increasing supramolecular interactions within the network. The prepared hydrogels showed energy loss and swelling ratio up to 3440 J. m−3 and 830%, respectively, which was not achievable with conventional network fabrication methods. The microgels were also assessed for their in vivo biocompatibility in a rat subcutaneous pocket assay. Results of hematoxylin and eosin (H&E) staining demonstrated regeneration of the tissue around the scaffolds without incorporation of growth factors. Also, vascularization within the scaffolds was observed after 4 weeks implantation. These results indicate that our strategy is a promising method to manipulate those valuable polymers, which lose their toughness and applicability with increasing their water content.



中文翻译:

超高含水量的生物相容性明胶基水凝胶:通过微细的耗散形态进行增韧是一种有效的策略

用于生物医学的同时坚固耐用和超吸收性的明胶基水凝胶的制造仍然是一个挑战,因为在存在大量水的情况下缺乏局部耗散点。在这里,我们采用一种合成策略,通过该策略将吸水率和耗能点分开,并且增韧机理在裂纹尖端处非常活跃。为此,合成了基于明胶的微凝胶(GeMs),其方式是存在浓缩的超分子相互作用,以增加传播宏观裂纹所需的能量。这些微凝胶通过暂时的疏水缔合和永久的共价交联而彼此互锁,其中牺牲性结合由于连接区的移动性和颗粒滑动而保持了韧性。然而,化学交联点保留了水凝胶的完整性和快速的可回收性。磁滞随着网络内超分子相互作用的增加而强烈增加。制备的水凝胶显示能量损失和溶胀比高达3440 J. m-3和830%,这是常规网络制造方法无法实现的。还通过大鼠皮下口袋试验评估了微凝胶的体内生物相容性。苏木精和曙红(H&E)染色的结果表明,支架周围的组织再生而未掺入生长因子。同样,植入4周后观察到支架内的血管形成。这些结果表明,我们的策略是处理这些有价值的聚合物的有前途的方法,这些有价值的聚合物会随着水含量的增加而失去其韧性和适用性。

更新日期:2020-12-06
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