藉由調整噴墨參數提升葡萄糖感測器靈敏度

Sensitivity Enhancement of Glucose Biosensors via Printing Parameter Adjustment

黃姵瑀(Pei-Yu Huang)

指導教授 ： 廖英志

國立臺灣大學/工學院/化學工程學研究所/碩士(2013年)

https://doi.org/10.6342/NTU.2013.00805

摘要

本研究利用多樣化印刷方式，採逐層堆積(Layer-by-layer)的方式，製成生物感測器工作電極，利用網刷技術製作碳膠導電層，接著利用點膠機沉積普魯士藍中介層，隨後在電極表面利用噴墨技術噴塗葡萄糖氧化酶酵素層，最後再利用浸製塗佈在電極表面修飾石蠟層，以便固定葡萄糖氧化酶。應用噴墨技術噴塗各式圖樣便利性，將此技術發展至生物感測器的製造用途上。

研究證實噴墨製程應用在生物感測器的可行性，探討系統最佳的電化學環境，發現若將操作電位越往負電位移動，可得到越大的電流訊號，然而操作電位的設定不僅要考慮電流訊號大小，仍要考慮操作電位過大會驅動其他干擾物質反應；探討電解質酸鹼值pH值6.53與7.4對電流訊號的影響，發現其兩者對於感測器的訊號大小影響不大；最後確認干擾測試中，系統是否能避開干擾物質的反應雜訊。

進一步探討改變噴墨參數、沉積不同葡萄糖氧化酶圖樣與靈敏度的關係，發現噴塗速度需與液滴、表面性質及乾燥情況配合，藉由調整溫度，以便得到完整、均勻沉積的表面；藉由噴墨技術在電極表面沉積快速，且可噴塗多種圖樣修飾的優勢，探討葡萄糖氧化酶圖樣是否會影響工作電極電流訊號，發現在使用同樣量的葡萄糖氧化酶時，若葡萄糖氧化酶與普魯士藍層接觸點越多，則訊號越高。除了改變葡萄糖氧化酶圖樣，增加接觸點外，本研究也藉由改變普魯士藍層的粗糙度，嘗試增加葡萄糖氧化酶與普魯士藍接觸點，以便增加反應生成的過氧化氫與普魯士藍接觸的機會，發現藉由碳紙吸附普魯士藍，增加其粗糙度，可確實增強過氧化氫感測訊號，然而增強葡萄糖感測訊號，則需均勻混合葡萄糖氧化酶與普魯士藍墨水，使其沉積在電極表面時，兩者界面均勻接觸，以期能增強訊號。

關鍵字

噴墨製程 ； 葡萄糖氧化酶靈敏度提升 ； 噴墨參數 ； 普魯士藍

並列摘要

By using versatile printing technique and layer-by-layer depositing method, the working electrode of biosensors are manufactured in this research. The manufacturing process is as following: screen-printing carbon paste conductive layer, depositing Prussian blue (PB) mediator layer by fluid dispenser, inkjet printing glucose oxidase (GOx) enzyme layer, and dip coating paraffin wax for enzyme immobilization. This research applies the inkjet printing method on biosensors fabrication for the convenience of printing patterns.

The feasibility of fabricating biosensors by inkjet printing process has been proved. Discussing the best electrochemical environment in this system, the result was found that the more negative applied voltage, the bigger response current. However, the setting of proper applied voltage has to take many factors into consideration not only the bigger amount of current signals but also the less interference reaction that the bigger applied voltage would trigger the interference substance reacts. The results from different pH values of electrolyte at pH 6.53 and pH 7.4 have no difference on current response signals. Furthermore, by the interference test, the research needs to make sure the selectivity of this system.

Then, this study discusses the relationship between the printing parameters, the printing patterns of glucose oxidase on the biosensor surface, and sensitivity. The printing velocity is adjusted by droplet and surface properties, and printing temperature is controlled to print uniform deposited surface. Due to the advantage of inkjet printing technique to print various patterns flexibly and fast, this study shows that the glucose oxidase patterns could effect on current signals, and the result shows that in the same amount of glucose oxidase, the more contacting points between PB and GOx are, the bigger electrochemical signals are. Besides, by changing the glucose oxidase patterns, this study also shows increasing the roughness of PB layer could increase the contacting points between GOx and PB, and the reacting area between PB and hydrogen peroxide which is produced by glucose and GOx. The results show that the biosensor electrochemical performance of hydrogen peroxide detection gets better by depositing PB adsorbed on carbon paper, which increases the roughness of PB surface. Then, it is expected to increase the glucose detection signals by mixing glucose oxidase and Prussian blue ink in order to make the homogeneous connecting surface while depositing on the electrode surface.

並列關鍵字

inkjet printing process ； glucose oxidase ； sensitivity improvement ； printing parameters ； Prussian blue

參考文獻

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