以濾紙抽氣沾附及旋鍍改質法製備奈米碳材生物感測紙製程及性質研究

Study on the Fabrication and Characterization of Nanocarbon Paper Based Biosensor Prepared through Filter Paper Pumping Adhesion and Spin-coating Modification

湯竣翔(Chun-Hsiang Tang)

指導教授 ： 李國榮

義守大學/理工學院/材料科學與工程學系/碩士(2021年)

摘要

本研究分別利用不同比例之奈米碳管(CNT)、石墨烯(G)及氧化石墨烯(GO)混合分散劑(1-(3二甲基氨基丙基)-3-乙基碳二亞胺, EDC+ N-羥基丁二醯亞胺, NHS)，以濾紙抽氣沾附及旋鍍不同改質劑(單寧酸, TA、聚(4-苯乙烯磺酸鈉), PSS、十二烷基硫酸鈉, SDS)等方式製作各類奈米碳材生物感測紙，藉此改善奈米碳材容易團聚且不易分散之問題，並提升試紙的表面活性與親水性。此外，將各類自製奈米碳材生物感測紙添加不同濃度的牛血清白蛋白(Bovine Serum Albumin, BSA)，探討不同試片在旋鍍改質前後與蛋白質接合前後的電性、官能基、接觸角、顯微結構與EDS元素分析之變化，藉此找出導電性質良好，且片電阻變化率明顯的試片，實驗結果顯示：
在接觸角量測方面，未改質的各類(BP、C1G1、C1GO1)試片的接觸角皆大於100°，表示試片表面為疏水性，而各類試片分別旋鍍改質劑後，試片接觸角皆下降，其中又以旋鍍改質劑SDS的試片接觸角下降最為明顯，親水性最佳。
在電性量測方面，在未改質的試片中，以添加低電阻石墨烯的C1G1試片片電阻為最低，而在改質後的各類試片中，則以旋鍍改質劑TA的試片片電阻下降最多；而比較添加不同濃度BSA後的試片片電阻變化率，可發現不論旋鍍何種改質劑，皆以C1G1試片的平均片電阻變化率最高，其中又以旋鍍改質劑TA試片的平均片電阻變化率最高，且隨BSA濃度的變化C1G1-TA-BSA試片片電阻變化率也大致呈現規律變化趨勢，主要原因是TA具大量的π鍵，能與BSA的π鍵進行π-π堆疊，因此試片在添加BSA後呈現分布較均勻且範圍較廣的膜狀蛋白質顯微組織，而此絕緣性的BSA會讓不同濃度的試片片電阻產生較明顯的變化，片電阻變化率也就較能隨著BSA添加的濃度上升呈現規律的提高。

關鍵字

奈米碳管 ； 石墨烯 ； 氧化石墨烯 ； 奈米碳材生物感測紙 ； 旋鍍 ； 改質劑 ； 牛血清白蛋白

並列摘要

This study adopts different proportions of carbon nanotubes (CNT), graphene (G) and graphene oxide (GO) with dispersant (1-ethyl-3-(3-dimethylaminopropyl)-carbodiimide (EDC) + N-hydroxysuccinimide (NHS)), pumping attached on filter paper and spin-coated with different modifying agent (Tannic acid (TA), Poly(Sodium 4-Styrenesulfonate (PSS) and Sodium Dodecyl Sulfate (SDS)) to fabricate nanocarbon paper based biosensors. Thus, the disadvantages of easy agglomeration and difficult dispersion of nano carbon materials are improved, and surface activity and hydrophilicity of specimens are also improved. The main purpose of this study is to investigate electrical properties, functional groups, contact angle, microstructure and EDS element analysis of different specimens before and after modification and protein bonding, so as to find out the specimen with good electric conductivity and obvious sheet resistance change rate for application in biosensors.
The experimental results show that in terms of contact angle measurement, the contact angles of all unmodified specimens are greater than 100 °, and surfaces of these specimens are hydrophobic, while the hydrophilic properties of all specimens after spin coating modification are improved. The specimen modified with SDS the best hydrophilic performance. In terms of electrical property measurement, among the unmodified specimens, the resistance of C1G1 specimen with low resistance graphene is the lowest. Among the modified specimens, the resistance of those specimens with TA agent decreased obviously.
Furthermore, comparing the resistance change rate of specimens after adding different concentrations of BSA, it can be found that no matter what kind of modifying agent is spin coated, the average resistance change rate of C1G1 specimen is the highest, and the average resistance change rate of specimens with TA agent is the highest.
Comparing the sheet resistance of various specimens before and after adding different concentrations of protein, it is found that the C1G1-TA-BSA specimen showed the most obvious change rate of sheet resistance with change of protein concentration. The main reason is that TA agent has a large number of π bonds, which can be further π - π stacked with the π bonds of BSA. Therefore, after adding BSA, a film-like protein will be formed on the specimen. This wide, uniform distributed and insulated BSA will cause a significant change in the resistance of specimens with different concentrations.

並列關鍵字

carbon nanotubes ； graphene ； graphene oxide ； nanocarbon paper based biosensors ； spin-coating ； modified agent ； bovine serum albumin

參考文獻

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