用于增强自组装能力和控制药物释放的酶促交联肽水凝胶,New Journal of Chemistry

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用于增强自组装能力和控制药物释放的酶促交联肽水凝胶
New Journal of Chemistry ( IF 2.7 ) Pub Date : 2023-04-18 , DOI: 10.1039/d2nj06256a
Xiujie Wang ₁ , Guoru Dai ₁ , Bianli Cheng ₁ , Jing Xu ₁ , Keming Xu _{1,

2} , Wenying Zhong _{1,

2,

3}

Affiliation

自组装肽水凝胶是一类具有固有生物相容性和良好生物活性的多功能材料；然而，它们往往表现出较弱的机械性能和不令人满意的药物释放曲线。为了解决这些问题，我们提出了一种酶促方法，在酪氨酸 (Tyr) 的相互交联的基础上合成酶促交联的肽水凝胶 (Fmoc-Gly-Phe-Tyr-Tyr，或 Fmoc-GFYY)辣根过氧化物酶 (HRP) 和过氧化氢 (H ₂ O ₂ )的作用。_{与不含 HRP 或 H 2} O ₂的 Fmoc-GFYY 相比, Fmoc-GFYY/酶交联水凝胶表现出更密集的交联网络、更有序的二级结构和更高的机械强度。_{使用 HPLC、UV、荧光和 LC-MS 的进一步表征证实，在 HRP 和 H 2} O ₂的作用下，Fmoc-GFYY 的酪氨酸相互交联形成二聚体酪氨酸。以多柔比星 (DOX) 和罗丹明 B (RhB) 为模型药物，Fmoc-GFYY/酶促交联水凝胶在体外表现出缓慢的 DOX 释放和在体内较长的 RhB 保留时间. 细胞实验表明，与单独的 DOX 溶液相比，载有 DOX 的酶促交联水凝胶制剂具有更高的抗癌功效。本研究中酶促交联的应用代表了一种肽水凝胶结构优化的新方法，在各种治疗药物的控释方面具有广阔的前景。

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Enzymatically cross-linked peptide hydrogels for enhanced self-assembling capability and controlled drug release

Self-assembled peptide hydrogels are a class of versatile materials with inherent biocompatibility and sound biological activities; however, they tend to exhibit weak mechanical properties and unsatisfactory release profiles of drugs. To address these problems, we propose an enzymatic approach to synthesize an enzymatically cross-linked peptide hydrogel (Fmoc-Gly-Phe-Tyr-Tyr, or Fmoc-GFYY) on the basis of inter-cross-linking of tyrosines (Tyr) under the action of horseradish peroxidase (HRP) and hydrogen peroxide (H₂O₂). Compared to Fmoc-GFYY without HRP or H₂O₂, the Fmoc-GFYY/enzymatically cross-linked hydrogels exhibited denser cross-linking networks, a more orderly secondary structure, and greater mechanical strength. Further characterizations using HPLC, UV, fluorescence, and LC-MS confirmed that the tyrosines of Fmoc-GFYY were inter-cross-linked to give dimeric tyrosines under the action of HRP and H₂O₂. By taking doxorubicin (DOX) and rhodamine B (RhB) as model drugs, the Fmoc-GFYY/enzymatically cross-linked hydrogel displayed slow release of DOX in vitro and a long retention time of RhB in vivo. Cell experiments revealed that the DOX-loaded enzymatically cross-linked hydrogel formulation exhibited higher anticancer efficacy compared to DOX solution alone. The utility of enzymatic cross-linking in this study represents a new approach for the structural optimization of peptide hydrogels, which could have broad prospects in the controlled release of various therapeutics.

更新日期：2023-04-18

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