含蛋白質類澱粉纖維混合材料之製備與性質探討

Synthesis and Characterization of Protein Fibril-Containing Hybrid Materials

鍾旻芝(Min-Chih Chung)

指導教授 ： 王勝仕

國立臺灣大學/工學院/化學工程學研究所/碩士(2017年)

https://doi.org/10.6342/NTU201701629

摘要

許多年來，類澱粉纖維(amyloid fibril)一直被視為導致類澱粉症的主要原因，但近年許多研究漸漸證明，類澱粉纖維僅是類澱粉症的副產物，又類澱粉纖維本身為一種變性蛋白質，擁有高穩定性和纖維狀結構，因此類澱粉纖維的應用逐漸被重視，另一方面，由於近年生醫領域的發展，材料研發講求高生物相容性和生物可降解性，類澱粉纖維本身即為蛋白質，又有一定機械強度和穩定性，很適合用於材料合成。
本文嘗試將母雞蛋白溶菌酶(Hen egg white lysozyme)形成之類澱粉纖維以不同比例加入氧化石墨烯(Graphene oxide)製備氧化石墨烯-類澱粉纖維複合材料，並對其型態、結合方式、熱穩定性和機械性質進行量測。
由本研究結果推測，在複合材料合成過程當中，類澱粉纖維和氧化石墨烯皆會可能先進行拆解，類澱粉纖維會還原成類澱粉纖維原絲；氧化石墨烯會剝離成更薄或較無規則的型態，接著類澱粉纖維原絲會以靜電作用力和氫鍵作用力平貼在氧化石墨烯表面，加入些微的類澱粉纖維即可造成氧化石墨烯結構很大的改變。
在比較加入不同量類澱粉纖維的複合材料方面，加入越多的類澱粉纖維有越高的熱穩定性，但關於其機械性質，加入微量的類澱粉纖維有助剛性提升，但加入更多的類澱粉纖維可能導致其分散相更趨明顯而使剛性延性皆降低。總結來說，加入類澱粉纖維後的氧化石墨烯複合材料預期會有更好的生物可降解性和生物相容性，和更低的生物毒性，且此材料擁有可調整性，可以依據加入類澱粉纖維量的不同有的熱穩定性和機械性質，在氧化石墨烯應用於如生醫材料或生物感測器上有很大的潛力。

關鍵字

類澱粉纖維 ； 氧化石墨烯 ； 混合材料

並列摘要

For many years, amyloid fibrils have been considered the cause of amyloidosis. However, recent evidence has proved that amyloid fibrils are only the side product formed during amyloidogenesis. Moreover, amyloid fibrils belong to one kind of denatured proteins that have high stability and fiber structure. Therefore, the applications of amyloid fibrils are now receiving an increasing attention. Given their excellent mechanical property and stability, amyloid fibrils are suitable for material applications.
In this research, attempts were made to first prepare the graphene oxide-amyloid fibril hybrid materials by adding hen lysozyme derived-amyloid fibrils into graphene oxide with different ratios, and then analyze their morphology, interaction, thermal and mechanical properties. The results show that during the synthesis, amyloid fibril and graphene oxide may both undergo disassembly: amyloid fibrils may disaggregate to form protofilaments, wherease graphene oxide may exfoliate. Furthermore, results suggest that the binding between protofilament and thinner graphene oxide may be governed by the electrostatic interaction and hydrogen bonding, which means the hybrid materials made of protofilament and thin graphene oxide exhibit lower energy. Comparison of the hydrid materials with different ratios indicates that the thermal stability could be enhanced upon adding more amyloid fibrils. However, as for the mechanical property, there exists a positive correlation between the rigidity and added amount of amyloid fibrils during the range of 1:0.016, followed by a decrease in the rigidity upon further increase in the amount of fibrillar species. We speculate that this may attributed to the formation of highly dispersed phase. In conclusion, the hybrid materials resulted from the addition of amyloid fibril to graphene oxide are expected to be more biodegradable and biocompatible with less toxicity. Also, the aforesaid hybrid materials exhibit adjustability. The thermal and mechanical properties could be controlled by the ratio between amyloid fibrils and graphene oxide. Therefore, these hybrid materials hold great potential for the applications in the fields of biomaterials and bio-sensoring.

並列關鍵字

Amyloid fibril ； Graphene oxide ； Hybrid material

參考文獻

[1] M.J. Buehler, Y.C. Yung, How protein materials balance strength, robustness, and adaptability, Hfsp J, 4 (2010) 26-40.

[2] Ting Yan, Huijie Zhang *, Dandi Huang, Shini Feng, M. Fujita, X.-D. Gao, Chitosan-Functionalized Graphene Oxide as a Potential Immunoadjuvant, Nanomaterials-Basel, 7 (2017).

[3] Z.U. Khan, A. Kausar, H. Ullah, A. Badshah, W.U. Khan, A review of graphene oxide, graphene buckypaper, and polymer/graphene composites: Properties and fabrication techniques, J Plast Film Sheet, 32 (2016) 336-379.

[4] D.C. Schafhaeutl, Ueber die Verbindungen des Kohlenstoffes mit Silicium, Eisen und anderen Metallen, welche die verschiedenen Gallungen von Roheisen, Stahl und Schmiedeeisen bilden, 21 (1840) 129-157.

[5] B. BC, On the atomic weight of graphite, Philos Trans R Soc London, (1859) 249-259.