[[alternative]]Novel Electrochemical Sensing Scheme Base on Nano Porous Metal Oxide Modified Electrode

計畫編號：NSC100-2113-M032-001-MY3 研究期間：20110801~20120731 研究經費：1,160,000[[abstract]]本三年計畫將利用金屬氧化物修飾電極開發三系列新穎電化學分析方式，包括第一年錯合型電化學分析技術，利用分析物做為配位基，在溶液與金屬電極表面氧化物產生錯合物而溶出，在控制的氧化條件下利用電極表面再氧化所得到響應電流訊號將正比於錯合反應之配位分析物的濃度。此電化學偵測方法將可擴充至以往不具電化學活性以及氧化會毒化電極之分析物，故在本研究將針對含氮官能團的藥物以及環境重要分子如糖尿病藥物Metformin、尿素聚合物物質二縮脲以及除草劑農藥硫化物類分子進行間接型電化學偵測方法的開發。第二年金屬氧化物將作為固態氧化劑提供固定的氧化電位，將嘗試合成金屬奈米氧化物，並利用金屬氧化態的氧化力，局部氧化苯胺(aniline)使之形成低分子量但仍具電化學可逆性之聚苯胺，並利用電極施加還原電位進行偵測分析，以其解決以往利用氧化方式進行偵測時，電極遭受毒化之缺點。 第三年將利用第二年合成之奈米氧化物發展輔酶－NADH的催化偵側技術，利用金屬氧化物的價態做為電子傳遞媒介，期許降低偵測分析電位以其避開易氧化物質的干擾，並結合各式去氫酶酵素延伸於相關生化指標如膽固醇、三酸甘油酯等生化感測技術的開發，最後將結合網版印刷技術製作成拋棄式感測試片，更研究探討是否能開發出具商業應用之潛力。[[abstract]]The aims of this proposal include three series of novel mechanism studies for novel electrochemical sensing studies by using various metal oxide modified electrode. In the first year, a new strategy for determination the non-electrochemical active species by using analyte complexation－surface oxide regeneration mode are purposed. In this unique electroanalytical method, a suitable potential is utilized to regenerate the oxide layer, which is independent of the oxidation potential of the analyte. Several amine base non-electrochemical active species such as metformin, biuret will be investigated in this mechanism. Besides, thionic based pesticide may be also studied since they are known to forming a fouling layer on the electrode surface. In the second year, various metal oxides will be evaluated to establish a sequence of oxidative strength by potentiometric method. These metal oxides may serve as an upstream-oxidarive electrode to provide a stable potential to oxidize the analyte, and nano scale metal oxides with high surface area will be synthesis to enhance the kinetic rate of oxidation of the analyte. In this project, an environmental unfriendly aniline might be a candidate, because of the oxidized product, polyaniline, is a famous redox polymer. Here we will use the flow injection system modified with the metal oxide at the upstream to oxidize the aniline into low molecular weight polyaniline, and subsequently determinates the aniline via polyaniline reduction at downstream electrode. NADH is the most critical coenzyme in biochemistry. In the final year, nano scale metal oxide could be test as a catalyst to determinate the NADH. Our strategy is using various valance state of the metal oxides to mediate the electron of the NADH. This unique strategy of metal oxide modified electrodes will integrated with several dehydrogenase enzymes and screen printing method to fabrication of a disposable biosensor.[[sponsorship]]行政院國家科學委員