Crucial Impact of Residue Chirality on the Gelation Process and Biodegradability of Thermoresponsive Polypeptide Hydrogels,Biomacromolecules

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Crucial Impact of Residue Chirality on the Gelation Process and Biodegradability of Thermoresponsive Polypeptide Hydrogels
Biomacromolecules ( IF 5.5 ) Pub Date : 2021-08-17 , DOI: 10.1021/acs.biomac.1c00785
Dong Li _{1,

2} , Dan Zhao _{1,

2} , Chaoliang He _{1,

2} , Xuesi Chen _{1,

2}

Affiliation

Thermosensitive polypeptide hydrogels have gained considerable attention in potential biomedical applications, of which the polymer structure may be tuned by residue chirality. In this study, polypeptide-based block copolymers with different chiralities were synthesized by ring-opening polymerization of γ-ethyl-l-glutamate N-carboxyanhydride and/or γ-ethyl-d-glutamate N-carboxyanhydride using amino-terminated monomethoxy poly(ethylene glycol) as a macroinitiator. All mPEG-polypeptide copolymers underwent sol–gel transition with an increase in temperature. The block copolymers with mixed enantiomeric residues of γ-ethyl-l-glutamate (ELG) and γ-ethyl-d-glutamate (EDG) in the polypeptide blocks exhibited lower critical gelation concentrations and lower critical gelation temperatures compared with those composed of pure ELG or EDG residues. We established that the difference in gelation properties between the copolymers was derived from the distinction of the secondary structures. We further demonstrated the influence of polypeptide chirality on the degradability and biocompatibility of hydrogels in vivo. Our findings provide insights into the design of hydrogels having tailored secondary conformation, gelation property, and biodegradability.

中文翻译：

残留手性对热响应性多肽水凝胶的凝胶化过程和生物降解性的重要影响

热敏多肽水凝胶在潜在的生物医学应用中获得了相当大的关注，其聚合物结构可以通过残基手性进行调节。在这项研究中，用不同的手性基于多肽的嵌段共聚物是由γ乙基的开环聚合而合成升-谷氨酸Ñ -carboxyanhydride和/或γ乙基- d -谷氨酸Ñ使用氨基封端的单甲氧基聚-carboxyanhydride（乙二醇）作为大分子引发剂。随着温度的升高，所有 mPEG-多肽共聚物都经历了溶胶-凝胶转变。具有混合对映体残基的 γ-乙基-l-谷氨酸 (ELG) 和 γ-乙基-d的嵌段共聚物与由纯 ELG 或 EDG 残基组成的那些相比，多肽块中的 -谷氨酸 (EDG) 表现出较低的临界胶凝浓度和较低的临界胶凝温度。我们确定共聚物之间凝胶性能的差异源自二级结构的差异。我们进一步证明了多肽手性对水凝胶体内降解性和生物相容性的影响。我们的发现为设计具有定制二级构象、凝胶特性和生物降解性的水凝胶提供了见解。

更新日期：2021-09-13

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