Bioinspired baroplastic glycosaminoglycan sealants for soft tissues
Bioinspired baroplastic glycosaminoglycan sealants for soft tissues
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DOI：
10.1016/j.actbio.2019.01.040
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发表时间：
2019-03-15
影响因子：
9.7
通讯作者：
Pashkuleva, Iva
中科院分区：
文献类型：
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作者：
Costa, Rui R.;da Costa, Diana Soares;Pashkuleva, Iva
我们描述仿生粘合剂的灵感来自海洋胶制造的沙堡蠕虫。采用Zeta电位滴定法优化了聚赖氨酸（PLL）与不同硫酸化程度的糖胺聚糖（GAG）-肝素（HEP）、硫酸软骨素（CS）和透明质酸（HA）-之间形成稳定的复合物的条件。这些PLL/GAG复合物通过压塑性加工被转化为具有受控水含量和密度的紧凑的PLL复合物（coPEC）。旋转剪切测试表明，含有硫酸化GAG（HEP或CS）的coPEC具有固体样性质，而基于HA的复合物形成高度水合的粘性样网络。分别使用聚苯乙烯和兔皮在干燥和湿润状态下测试所产生的coPEC的剪切强度（归一化搭接剪切强度）。在干燥状态下，粘合剂表现出数百kPa量级的搭接剪切强度，其中coPLL/FIEP和coPLL/CS比coPLL/HA强约1.5倍。在湿润状态下，所有coPEC密封家兔皮肤并恢复超过60%的完整皮肤的伸长能力，其中coPLL/HA提供最坚固的粘附（约85%伸长恢复）。我们证明，这是由于更高的水分数，提高了湿标本之间的粘合，展示了潜在的上级机械恢复对受伤tissues.Statement的重要性在水和潮湿的存在下，具有足够的粘合强度的医用密封剂的发展仍然是一个巨大的挑战。我们目前的糖胺聚糖（GAG）作为生物材料的组装具有较强的粘附强度，在生理条件下的软组织的气压塑料。具有粘性特性的气压塑料是通过一种温和的组装过程产生的，该组装过程是基于树脂的络合和压实。这些材料表现为多功能密封剂：由于GAG的硫酸化程度不同，它们的粘度可以根据干燥或潮湿的样品进行调整。这些密封剂对L929细胞无细胞毒性，并使受损皮肤恢复大量天然弹性：它们保留了生物软组织典型的J形应力/应变机械反应。(C)2019 Acta Materialia Inc.由爱思唯尔有限公司出版。保留所有权利。
We describe biomimetic adhesives inspired by the marine glues fabricated by the sandcastle worm. The formation of stable polyelectrolyte complexes between poly-L-lysine (PLL) and glycosaminoglycans (GAGs) with different sulfation degree - heparin (HEP), chondroitin sulfate (CS) and hyaluronic acid (HA) - is optimized by zeta-potential titrations. These PLL/GAG complexes are transformed into compact polyelectrolyte complexes (coPECs) with controlled water contents and densities via baroplastic processing. Rotational shear tests demonstrate that coPECs containing sulfated GAGs (HEP or CS) have solid-like properties, whereas HA-based complexes form highly hydrated viscous-like networks. The adhesiveness of the generated coPECs (normalized lap shear strength) is tested in dry and wet states using polystyrene and rabbit skin, respectively. In dry state, the adhesives exhibit lap shear strengths in the order of hundreds of kPa, with coPLL/FIEP and coPLL/CS being about 1.5 times stronger than coPLL/HA. In wet state, all coPECs seal rabbit skin and recover over 60% of the elongation capacity of intact skin with coPLL/HA providing the sturdiest adhesion (-85% elongation recovery). We demonstrate that this is due to the higher water fraction that improves the bonding between the wet specimens, showcasing the potential superior mechanical recovery on injured tissues.Statement of SignificanceThe development of medical sealants with sufficient adhesive strength in the presence of water and moist remains a huge challenge. We present glycosaminoglycans (GAGs) as biomaterials for the assembly of baroplastics with strong adhesive strength to soft tissues at physiological conditions. Baroplastics with tacky properties were generated by a mild assembly process based on polyelectrolyte complexation and compaction. These materials behave as versatile sealants: their adhesiveness can be adjusted to either dry or wet specimens because of the different sulfation degree of GAGs. These sealants were noncytotoxic towards L929 cells and allowed the damaged skin to recover a great deal of its native elasticity: they preserved the J-shaped stress/strain mechanical response that is typical of biological soft tissues. (C) 2019 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.