新型电化学传感器的研究
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摘要
电化学传感器是分析化学领域的一个研究热点,本论文基于电沉积到DNA网络膜上的银纳米颗粒、电沉积到Ⅰ型胶原蛋白质网络膜上的银纳米颗粒和聚二茂铁硅烷/DNA网络膜修饰电极开展了相关的电化学传感器研究工作。具体工作分为以下三个方面:
1.第一部分利用DNA形成的网路结构控制电沉积银纳米粒子制备新型过氧化氢(H2O2)传感器。首先,将DNA直接滴到空白玻碳电极上形成DNA网络膜;然后,在DNA网络修饰的玻碳电极上电沉积制备银纳米粒子形成H2O2传感器。此方法制备的传感器对H2O2有很好的催化行为,其归结于DNA形成的网络结构控制了银纳米粒子的生长从而得到了大小和分布均一的银纳米粒子。
2.第二部分考察了在Ⅰ-型胶原蛋白质修饰的玻碳电极上电沉积制备银纳米粒子及其作为H2O2传感器。原子力显微镜实验结果发现,构筑在Ⅰ-型胶原蛋白质修饰的玻碳电极上的银纳米粒子小且分布均一。Ⅰ-型胶原蛋白网络膜可以控制Ag纳米粒子的生长,并使Ag纳米粒子分布均匀。电化学实验证明,制备的银纳米粒子对H2O2有很好的催化还原能力,可以作为一个很好的H2O2传感器。此催化活性归因于Ⅰ-型胶原蛋白质控制生成了大小和分布均一的银纳米粒子,因此相应的催化活性与Ⅰ-型胶原蛋白质的浓度和沉积时间有关。
3.第三部分研究了包埋在DNA膜中的聚二茂铁甲硅烷(PFS)修饰电极的电化学行为及对抗坏血酸(AA)的电催化。实验发现对AA起催化氧化作用的为PFS的电活性中心(二茂铁单元)。同时研究了FPS/DNA/GCE电化学行为,实验发现PFS/DNA/GCE存在两个可逆的峰,说明了电活性单元分步进行氧化,其与PFS/GCE相比,ΔEp值更小,ip值更大。PFS/DNA/GCE的电化学行为受很多因素影响,如DNA、PFS和PBS的浓度,以及温度等。其中DNA起到了吸附固定PFS和促进电子传输的作用。
Electrochemical sensors are active and promising in the analytical chemistry fields. In the theses, we focused our studies on silver nanoparticles (Ag NPs) electrodeposited on type-Ⅰcollagen-modified electrode, Ag NPs electrodeposited on DNA modified electrode and PFS/DNA-modified electrode and developed the corresponding electrochemical sensors. This work mainly covered the following areas.
1. The first part was about a novel hydrogen peroxide (H2O2) sensor based on Ag NPs electrodeposited on DNA-networks modified glassy carbon electrode (GCE). In this part, we have exploited Ag NPs electrodeposited on three-dimensional DNA networks that were directly dropped on the surface of glassy carbon electrode as an electrocatalyst to fabricate a H2O2 sensor. The Ag NPs electrodeposited on three-dimensional DNA networks showed very good catalytic ability for the reduction of H2O2. The well catalytic activity of the electrode was ascribed to the DNA networks that caused the formation of small Ag NPs and the homogenous distribution of Ag NPs.
2. The second part was concentrated on electrodeposition of Ag NPs on type ? collagen modified GCE and their applications as a H2O2 sensor. Atomic force microscopy (AFM) images showed that many small Ag NPs formed and uniformly distributed on type ? collagen/GCE. We found that the type ? collagen network film could control the growth of Ag NPs and the Ag NPs were well-distributed. Meanwhile, the electrochemical experiments proved that the Ag NPs had an excellent catalytic ability to reduction of H2O2, suggesting that they could be used as a sensor to determinate H2O2. The catalytic activity of Ag NPs was ascribed to type ? collagen that resulted in the homogenous distribution of many small Ag NPs and accordingly depended on the type ? collagen concentration and electrodeposition time.
3. The third part focused on studying electrochemical behaviors of poly (ferrocenylsilane)/DNA (PFS/DNA) modified GCE and as an ascorbic acid (AA) sensor. The embedded PFS in DNA film had a good electrocatalytic activity for AA. This behavior suggested that the electro-oxidation of AA could be catalyzed by FC/FC+ couple of PFS as a mediator. The PFS/DNA/GCE showed two reversible waves, which had a lower oxidation potential, smallerΔEp value, and larger ip values as compared with PFS/GCE. The concentration of DNA, PFS and PBS, and temperature influenced the electrochemical behaviors of PFS/DNA/GCE. DNA played an important role as an intermediate for the absorption of PFS and electron transfer.
1.第一部分利用DNA形成的网路结构控制电沉积银纳米粒子制备新型过氧化氢(H2O2)传感器。首先,将DNA直接滴到空白玻碳电极上形成DNA网络膜;然后,在DNA网络修饰的玻碳电极上电沉积制备银纳米粒子形成H2O2传感器。此方法制备的传感器对H2O2有很好的催化行为,其归结于DNA形成的网络结构控制了银纳米粒子的生长从而得到了大小和分布均一的银纳米粒子。
2.第二部分考察了在Ⅰ-型胶原蛋白质修饰的玻碳电极上电沉积制备银纳米粒子及其作为H2O2传感器。原子力显微镜实验结果发现,构筑在Ⅰ-型胶原蛋白质修饰的玻碳电极上的银纳米粒子小且分布均一。Ⅰ-型胶原蛋白网络膜可以控制Ag纳米粒子的生长,并使Ag纳米粒子分布均匀。电化学实验证明,制备的银纳米粒子对H2O2有很好的催化还原能力,可以作为一个很好的H2O2传感器。此催化活性归因于Ⅰ-型胶原蛋白质控制生成了大小和分布均一的银纳米粒子,因此相应的催化活性与Ⅰ-型胶原蛋白质的浓度和沉积时间有关。
3.第三部分研究了包埋在DNA膜中的聚二茂铁甲硅烷(PFS)修饰电极的电化学行为及对抗坏血酸(AA)的电催化。实验发现对AA起催化氧化作用的为PFS的电活性中心(二茂铁单元)。同时研究了FPS/DNA/GCE电化学行为,实验发现PFS/DNA/GCE存在两个可逆的峰,说明了电活性单元分步进行氧化,其与PFS/GCE相比,ΔEp值更小,ip值更大。PFS/DNA/GCE的电化学行为受很多因素影响,如DNA、PFS和PBS的浓度,以及温度等。其中DNA起到了吸附固定PFS和促进电子传输的作用。
Electrochemical sensors are active and promising in the analytical chemistry fields. In the theses, we focused our studies on silver nanoparticles (Ag NPs) electrodeposited on type-Ⅰcollagen-modified electrode, Ag NPs electrodeposited on DNA modified electrode and PFS/DNA-modified electrode and developed the corresponding electrochemical sensors. This work mainly covered the following areas.
1. The first part was about a novel hydrogen peroxide (H2O2) sensor based on Ag NPs electrodeposited on DNA-networks modified glassy carbon electrode (GCE). In this part, we have exploited Ag NPs electrodeposited on three-dimensional DNA networks that were directly dropped on the surface of glassy carbon electrode as an electrocatalyst to fabricate a H2O2 sensor. The Ag NPs electrodeposited on three-dimensional DNA networks showed very good catalytic ability for the reduction of H2O2. The well catalytic activity of the electrode was ascribed to the DNA networks that caused the formation of small Ag NPs and the homogenous distribution of Ag NPs.
2. The second part was concentrated on electrodeposition of Ag NPs on type ? collagen modified GCE and their applications as a H2O2 sensor. Atomic force microscopy (AFM) images showed that many small Ag NPs formed and uniformly distributed on type ? collagen/GCE. We found that the type ? collagen network film could control the growth of Ag NPs and the Ag NPs were well-distributed. Meanwhile, the electrochemical experiments proved that the Ag NPs had an excellent catalytic ability to reduction of H2O2, suggesting that they could be used as a sensor to determinate H2O2. The catalytic activity of Ag NPs was ascribed to type ? collagen that resulted in the homogenous distribution of many small Ag NPs and accordingly depended on the type ? collagen concentration and electrodeposition time.
3. The third part focused on studying electrochemical behaviors of poly (ferrocenylsilane)/DNA (PFS/DNA) modified GCE and as an ascorbic acid (AA) sensor. The embedded PFS in DNA film had a good electrocatalytic activity for AA. This behavior suggested that the electro-oxidation of AA could be catalyzed by FC/FC+ couple of PFS as a mediator. The PFS/DNA/GCE showed two reversible waves, which had a lower oxidation potential, smallerΔEp value, and larger ip values as compared with PFS/GCE. The concentration of DNA, PFS and PBS, and temperature influenced the electrochemical behaviors of PFS/DNA/GCE. DNA played an important role as an intermediate for the absorption of PFS and electron transfer.
引文
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