多孔網印碳漿電極用於肌酐酸感測

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姓名

陳柏任(Po-jen Chen) 查詢紙本館藏

畢業系所

電機工程學系

論文名稱

多孔網印碳漿電極用於肌酐酸感測
(Porous carbon paste electrode for creatinine detection)

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摘要(中)

肌酐酸是人類體內肌肉運動後代謝產生的最終產物，人體中每日的肌酐酸產量皆由腎臟過濾後經由尿液排出。所以在人體血液中的肌酐酸濃度是一個診斷腎小球過濾功能的一個重要指標。一般的肌酐酸感測電極是由鉑或金製作而成，這些金屬非常的昂貴，而且難以製造。本研究利用網版印刷技術搭配表面粗糙化技術，建構出一種多孔指叉碳電極，並用於肌酐酸感測。透過在網印碳漿中均勻混合碳酸鈣(CaCO3)粉末，並且以鹽酸溶解這些粉末，在電極表面製作出許多細微孔洞，增加電極的檢測表面積，並增強其量測電流響應。
本研究利用計時伏安法，量測電極的電化學響應。根據實驗結果顯示，電極在純系統溶液的肌酐酸量測中，有著廣大的線性量測區間，為0 ~ 550 μM(約0 ~ 6.2 mg/dL)，R2=0.99309。涵蓋了傳統的肌酐酸網印碳電極無法檢測到的低濃度區間。電極也有3.46 μA/mM的優良靈敏度。透過表面粗糙化的方法，也使電極在純系統量測下無論在靈敏度和線性區間上，相較於傳統網印碳電極，皆有所提升。在模擬人體樣本的人類血清中，電極也在88 ~ 438 μM(1.0 ~ 4.9 mg/dL)的線性區間(R2=0.98584)，靈敏度為2.78μA/mM。顯示經過表面粗糙化的電極，在血清的檢測環境下也能提升電極的檢測效能，使其線性檢測範圍能媲美先前文獻的肌酐酸鉑電極。電極同時在含有人類血液中各種干擾物質的樣本接受測試，實驗結果也顯示以計時伏安法量測的電極，受到干擾物影響造成的量測偏差皆小於5%。最後在實際的人體樣本檢驗中，和臨床的檢驗方法也有著良好的相關性，量測電流變異皆在95%的信賴區間內。中、高濃度的檢測濃度值誤差皆小於10%。透過這種電極，提高了網印碳電極在肌酐酸的感測效能，也為肌酐酸診斷提供了一個更加便宜方便的選擇。

摘要(英)

Creatinine is a product of muscle metabolism. The daily produce of creatinine is filtered by kidney and excreted by urine. Creatinine level in human blood is an important indication of renal corpuscle status. Conventional creatinine sensors are made up with noble metals, such as platinum or gold, and are hard to fabricate. In this study, we develop a porous carbon-paste interdigitated electrode by screen printing technology for the measurement of creatinine. Made of carbon paste doped with CaCO3 powder and subsequently dissolved with HCl, the electrodes possessed increased surface area and enhanced current response.
In this study, we use chronoamperometry to measure the current response. By the surface roughing procedure, the linear range and sensitivity of the electrode is enhanced to be better than conventional screen-printing creatinine electrode. The creatinine sensor has a wide linear range from 0 to 550 μM (06.2 mg/dL) with R2 = 0.99309 in deionized water. It covers a lower concentration range than conventional screen printed creatinine sensors. The sensitivity is enhanced to 3.46 μA/mM.. In normal human serum sample, the creatinine sensor has wide linear range from 88 to 438 μM (1.0¬ 4.9 mg/dL) with R2 = 0.98584 and a sensitivity of 2.78 μA/mM. With the surface roughing procedure, the performance of electrode is also enhanced in normal human serum, like in DI water. This makes the linear detection range of the screen-printing carbon electrode becomes close to conventional platinum electrode. The creatinine sensor was also tested in creatinine sample with three interferences. The resultant interference current was less than 5%. In real human blood sample, the performance of the proposed creatinine sensor is highly similar to that of the Jaffe method. The difference between the measurement results of the homemade electrode and Jaffe method in middle and high concentrations are within 10%. This porous creatinine sensor outperformed conventional screen printed carbon electrodes. It provides a better choice for creatinine diagnosis.

關鍵字(中)

★ 肌酐酸
★ 生物感測器

關鍵字(英)

論文目次

中文摘要 VIII
Abstract X
致謝 XII
目錄 XIII
圖目錄 XVIII
表目錄 XXIV
第一章緒論 1
1-1肌酐酸簡介 1
1-2腎臟簡介 2
1-2-1結構與功能 3
1-2-2慢性腎臟病 5
1-2-3肌酐酸濃度指標在腎臟病的重要性 8
1-3現今肌酐酸的臨床檢測方法 10
1-4生物感測器簡介 13
第二章文獻回顧 17
2-1肌酐酸生物感測器 17
2-1-1光學型肌酐酸生物感測器 17
2-1-2免疫型肌酐酸生物感測器 18
2-1-3電化學型肌酐酸生物感測器 20
2-1-4其他肌酐酸生物感測器 23
2-2網版印刷生物感測器 27
2-3表面粗糙化 34
2-3-1熱分解法 34
2-3-2模板輔助合成 36
2-3-3電漿蝕刻法 37
2-3-4侵蝕法 39
2-4分子固定化 41
2-4-1物理性吸附 42
2-4-2膠體包埋法 44
2-4-3共價鍵結合 46
2-4-4交聯劑連結 48
2-5電化學感測器量測方法 49
2-5-1交流阻抗法 50
2-5-2循環伏安法 52
2-5-3計時伏安法 58
第三章研究動機與目標 60
3-1 研究動機 60
2-2 研究目標 61
第四章材料與方法 62
4-1電極的製備 62
4-1-1電極製備的材料 62
4-1-2實驗使用儀器 62
4-1-3電極印製步驟 66
4-1-4電極檢驗步驟 69
4-2酵素的固定 70
4-2-1酵素固定的材料與儀器 70
4-2-2 PEG固定濃度最佳化 72
4-2-3固定環境溫度最佳化 74
4-2-4固定環境酸鹼值最佳化 76
4-2-5酵素的熱穩定性 78
4-3純溶液系統下的檢測 80
4-3-1純溶液系統下的肌酐酸檢測 81
4-3-2純溶液系統下的干擾物檢測 83
4-3-3純溶液系統下的計時伏安法 85
4-4人類血清下的檢測 88
4-4-1人類血清下的肌酐酸檢測 88
4-4-2人類血清下的干擾物檢測 90
4-5實際樣本的肌酐酸檢測 92
第五章結果與討論 95
5-1電極的特性分析 95
5-1-1自製電極的電學特性分析 95
5-1-2碳漿混合攪拌時間最佳化分析 99
5-1-3電極混合碳酸鈣粉末比例最佳化分析 111
5-2酵素的固定 121
5-2-1 PEG固定濃度最佳化分析 121
5-2-2固定環境溫度最佳化分析 124
5-2-3固定環境酸鹼值最佳化分析 130
5-2-4酵素的熱穩定性分析 134
5-3純溶液系統下的檢測結果分析 137
5-3-1純溶液系統下的肌酐酸檢測結果分析 137
5-3-2純溶液系統下的干擾物檢測結果分析 139
5-3-3純溶液系統下的計時伏安法量測分析 148
5-4人類血清下的檢測結果分析 162
5-4-1人類血清下的肌酐酸檢測結果分析 162
5-4-2人類血清下的干擾物檢測結果分析 164
5-5人體樣本量測結果分析 170
第六章結論 176
第七章未來展望 177
第八章參考文獻 178

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指導教授

蔡章仁(Jang-zern Tsai)

審核日期

2014-4-1

推文