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使用镧系离子作为离液剂对再生丝素蛋白进行拉曼、广角X射线散射和固态核磁共振表征

Raman, WAXS, and Solid-State NMR Characterizations of Regenerated Silk Fibroin Using Lanthanide Ions as Chaotropic Agents.

作者信息

Rizzo Giorgio, Petrelli Valentina, Sibillano Teresa, De Caro Liberato, Giangregorio Maria Michela, Lo Presti Marco, Omenetto Fiorenzo G, Giannini Cinzia, Mastrorilli Piero, Farinola Gianluca M

机构信息

Dipartimento di Chimica, Università degli Studi di Bari Aldo Moro, via Orabona 4, 70125 Bari, Italy.

DICATECh, Politecnico di Bari, via Orabona 4, 70125 Bari, Italy.

出版信息

ACS Omega. 2023 Jun 28;8(27):24165-24175. doi: 10.1021/acsomega.2c07149. eCollection 2023 Jul 11.

DOI:10.1021/acsomega.2c07149
PMID:37457447
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10339335/
Abstract

silk fibroin (SF) has been reported as a convenient natural material for regenerative medicine, optoelectronics, and many other technological applications. SF owes its unique features to the hierarchical organization of the fibers. Many efforts have been made to set up protocols for dissolution since many applications of SF are based on regenerated solutions and fibers, but chaotropic conditions required to disassemble the packing of the polymer afford solutions with poor crystalline behavior. Our previous research has disclosed a dissolution and regeneration process of highly crystalline fibers involving lanthanide ions as chaotropic agents, demonstrating that each lanthanide has its own unique interaction with SF. Herein, we report elucidation of the structure of Ln-SF fibers by the combined use of Raman spectroscopy, wide-angle X-ray scattering (WAXS), and solid-state NMR techniques. Raman spectra confirmed the coordination of metal ions to SF, WAXS results highlighted the crystalline content of fibers, and solid-state NMR enabled the assessment of different ratios of secondary structures in the protein.

摘要

丝素蛋白（SF）已被报道为一种适用于再生医学、光电子学及许多其他技术应用的便捷天然材料。SF的独特特性归因于其纤维的分级结构。由于SF的许多应用都基于再生溶液和纤维，因此人们为建立溶解方案付出了诸多努力，但聚合物堆积解体所需的离液条件会产生结晶行为不佳的溶液。我们之前的研究揭示了一种涉及镧系离子作为离液剂的高结晶纤维的溶解和再生过程，表明每种镧系元素与SF都有其独特的相互作用。在此，我们报告通过联合使用拉曼光谱、广角X射线散射（WAXS）和固态核磁共振技术对Ln-SF纤维结构的阐明。拉曼光谱证实了金属离子与SF的配位，WAXS结果突出了纤维的结晶含量，固态核磁共振能够评估蛋白质中不同二级结构的比例。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8eed/10339335/2c677a659cca/ao2c07149_0011.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8eed/10339335/2c677a659cca/ao2c07149_0011.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8eed/10339335/6ec6c0bee6ff/ao2c07149_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8eed/10339335/32e176c491ad/ao2c07149_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8eed/10339335/1f79630675a4/ao2c07149_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8eed/10339335/9b66b68ef667/ao2c07149_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8eed/10339335/b8781bcb9a37/ao2c07149_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8eed/10339335/59204ee1c3bb/ao2c07149_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8eed/10339335/d25592917915/ao2c07149_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8eed/10339335/8c4ab8000922/ao2c07149_0009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8eed/10339335/3789b06a4843/ao2c07149_0010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8eed/10339335/2c677a659cca/ao2c07149_0011.jpg

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Lamellar Structure in Alanine-Glycine Copolypeptides Studied by Solid-State NMR Spectroscopy: A Model for the Crystalline Domain of Silk Fibroin in Silk II Form.通过固态核磁共振光谱研究丙氨酸-甘氨酸共聚物中的层状结构：丝素蛋白II型结晶域的模型。
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