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標題: Electroanalysis of Clay Modified Copper-Plated Screen Printed Carbon Electrode
作者: Yao, Kai-Yuan
關鍵字: Clay modified copper-plated screen printed electrode;黏粒修飾鍍銅電極;Clay mineral;黏土礦物
出版社: 土壤環境科學系所
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黏粒修飾電極過去已經應用在電化學分析、光催化性與生化感測器等各方面,也有研究探討合成具催化性的金屬離子於黏粒膜層後再修飾於電極表面以達到催化與分析等用途,但過去鮮少有文獻報導結合金黏土礦物與金屬電極的研究。本試驗研究以不同黏土礦物修飾於鍍銅電極上(Copper screen-printed carbon electrode, CuSPE)探討其電化學行為,試驗結果指出不同黏土礦物種類修飾於鍍銅電極上於銅的氧化還原行為有著顯著的影響,四種黏土礦物修飾鍍銅電極在pH 7磷酸緩衝溶液環境下對銅的氧化還原訊號上都有促進的作用,其中多鐵蒙特石與綠脫石在八面體層中含多量同構代換的三價鐵,對銅氧化還原波峰電流量上的增大作用較大於鈉蒙特石與高嶺石,多鐵蒙特石與綠脫石修飾鍍銅電極在還原波峰處發現兩價銅的還原訊號消失而一價銅的還原訊號則不變,且其具有相當大的氧化波峰。礦物晶格的三價鐵在銅的氧化還原行為扮演了電子傳遞者的角色,並能穩定Cu2IO於修飾電極表面。多鐵蒙特石修飾鍍銅網版印刷電極所量測到的氧化還原訊號隨著pH值增加而急遽下降,銅離子於鹼性環境下吸附在礦物晶格邊緣並形成錯合物後電化學活性降低導致電流值變小;在光電化學的應用方面我們利用多鐵蒙特石能吸附並透過電子傳遞作用將銅離子轉換成一價銅的特性,碘離子直接與一價銅反應生成具有光電半導體特性的CuI。在pH7、0.1M磷酸緩衝溶液與KI濃度5mM條件下,當施予光照強度20flux到300flux光還原電流隨著光照強度增加電流訊號呈現穩定與線性關係。
在生化物質的微量分析方面我們發現多鐵蒙特石修飾電極在多巴胺氧化訊號上具有電催化作用,且其用於多巴胺偵測的氧化波峰電流量不會隨循環圈數的增加而衰減,其搭配流動注入系統對0.5–10μM多巴胺的偵測具有良好的線性關係(R2 = 0.9995),顯示有良好的偵測結果。多鐵蒙特石修飾鍍銅網版印刷電極在鹼性環性下銅離子吸附在礦物晶格邊緣形成錯合物並失去電活性,添加入NH3與吸附的銅錯合物形成具有電活性的銅銨複合物,在pH10的磷酸溶液中隨著NH3濃度的增加銅銨複合物的氧化還原電流值也隨之增加。搭配i-t法將電位定在-0.4V對於200μM到4000μM的NH3偵測也具有良好的線性關係。未來期望能結合超微電極技術提升靈敏度與開發成氣體感測器等目標。

Clay-modified electrode was applied in electroanalysis, photocatalysis biosensor, and catalysis and analysis of synthesis catalytic metal in clay structure. We studied electroanalysis of copper screen-printed carbon electrode (CuSPE) modified by different clay minerals. The experimental results indicated four clay minerals amplified copper redox currents in
0.1M pH7 phorsphate buffer. Furthermore, Ferruginous smectite (SWa-1) and nontronite (NG-1) with octahedral Fe(III) had larger redox currents than Na-montmorillonite (SWy-1) and Kaolinite (KG-1). We observed decreasing reductive peak current of CuII in SWa-1 and NG-1 modified copper-plated electrode, and peak current of CuI was same. That implied octahedral Fe(III) of clay mineral play important role on electron transfer between clay mineral and copper on electrode. Reductive and oxidative currents of SWa-1CuSPE decreased apparently with increasing pH due to formation of electroinactive copper complex on clay mineral edges in alkaline solution. SWa-1CuSPE could be transferred to a photoelectric and semiconductive CuI in in pH7 0.1M phorsphate buffer with 5mM KI. That had stable and linear relationships between photoelectric currents and light intensity from 20 to 300flux.
As biosensor, Electrocatalysis of dopamine can be observed at the ferruginous smectite modified copper-plated electrode with a linear range of 0.5 μM - 10 μM (R2 = 0.9995) by flow injection analysis. Complexed copper of SWa-1 modified copper-plated electrode could be transferred to electroactive copper-ammonia complex in alkaline solution. Reductive currents of copper-ammonia complex increased with increasing ammonia concentration in pH10 phosphate buffer solution. We could obtained a good linear relationship from 200-4000μM NH3 using i-t method. We respect combine screen-printed edge band ultramicroelectrode (SPUME) and application of ammonia gas sensor in future.
其他識別: U0005-2007200913193800
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