以抽氣過濾及旋鍍改質法製備紙質奈米碳材應用於電化學生物感測器研究

Fabrication and Modification of Nanocarbon Paper Prepared through Pumping Filtration and Spin-coating for Electrochemical Biosensor Applications

李銘軒(Ming-Husan Lee)

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

本實驗主要分為兩部分進行，第一部分會先以採用不同種類之奈米碳管(C)、石墨烯(G)以及氧化石墨烯(GO)製作紙質奈米碳材感測器試片，過程中會分別針對奈米碳管進行羧化(Caboxylation)進行改質，並添加固定濃度(100000 ng/mL)之牛血清白蛋白(Bovine Serum Albumin，BSA)，篩選出對於添加牛血清白蛋白有較為明顯變化之試片。第二部分則以篩選出的試片添加不同改質劑(聚(4-苯乙烯磺酸鈉) PSS、十二烷基硫酸鈉 SDS、(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、單寧酸 TA)等進行表面改質，最後再將各類經改質過後的紙質奈米碳材感測器試片添加不同濃度(10、100、1000、10000、100000 ng/mL)之牛血清白蛋白(BSA)製備與蛋白質接合之試片，藉此探討不同試片在添加不同濃度的蛋白質前後的電化學、電性、以及顯微結構之變化，其實驗結果顯示：
在所製備的 BP、S-BP、C1GO1、S-C1GO1、C1G1、S-C1G1 六種紙質奈米碳材感測器試片中，以羧化碳管所組成的 S-BP 試片所表現的電化學性質最佳。而在添加牛血清白蛋白後，對於含有羧化碳管的 S-BP、S-C1G1 及 S-C1GO1 試片，有較為明顯的蛋白質偵測效果，而這三種試片中又以完全由羧化碳管所製成的 S-BP 試片在添加蛋白質後的偵測效果最為明顯，所以篩選出 S-BP 試片作為後續檢測實驗。而比較各類經表面改質過後的 S-BP 系列試片，經過添加不同濃度之牛血清白蛋白前後發現，以 EDC/NHS 為改質劑的 S-BP-EDC/NHS 試片其在添加不同濃度的牛血清白蛋白前後的電化學性質有較為明顯的變化，且變化量與添加蛋白質濃度呈現良好的線性關係。
在顯微結構分析方面，可明顯在羧化後的奈米碳管表面觀察到較明顯的顆粒狀蛋白質與試片表面接合之現象，而對應試片的電化學性質、片電阻量測發現，若能在試片表面觀察到蛋白質與試片表面接合的現象，所對應之試片在添加蛋白質後的電化學、電性變化也會較為明顯。

關鍵字

奈米碳管 ； 石墨烯 ； 氧化石墨烯 ； 紙質奈米碳材 ； 羧化 ； 改質劑 ； 牛血清白蛋白 ； 電化學量測

並列摘要

This study is to fabricate the nanocarbon paper prepared through pumping filtration and spin-coating. Firstly, we use carbon nanotubes (C), graphene (G) and graphene oxide (GO) to make different nanocarbon papers, and further modify the specimen's surface by different agent (1-(3dimethylaminopropyl)ethylcarbodiimide (EDC)+ N-hydroxysuccinimide (NHS), Tannic acid (TA), Poly(Sodium 4-Styrenesulfonate (PSS), Sodium Dodecyl Sulfate, (SDS)). The main purpose is to investigate the electrochemical, electrical, and microstructure performance of various specimens before and after adding different concentrations of bovine serum albumin (BSA).
The experimental results show that among the six unmodified specimens, the S-BP specimen composed of carboxylation carbon nanotubes exhibits the best electrochemical properties. In the meantime, the S-BP specimen also has the most obvious effect on the detection of protein addition.
Comparing various S-BP series specimens after surface modification, it is found that the electrochemical properties of S-BP-EDC/NHS specimens change most obviously before and after adding different concentrations of bovine serum albumin, and there was a good linear relationship between the change amount and the concentration of protein.
Through the observation of microstructure, it is obvious that some granular protein are bonded to the surface of the specimen with carboxylated carbon nanotubes. In addition, if the bonded protein can be observed on the specimen, the corresponding specimen will also change significantly in the measurement of electrochemical properties and sheet resistance.

並列關鍵字

carbon nanotubes ； graphene ； graphite oxide ； nanocarbon paper ； carboxylation ； modified agent ； bovine serum albumin ； electrochemical measurement

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