Improvement of Selectivity and Stability of Amperometric Detection of Hydrogen Peroxide Using Prussian Blue‐PAMAM Supramolecular Complex Membrane as a Catalytic Layer

Improvement of Selectivity and Stability of Amperometric Detection of Hydrogen Peroxide Using Prussian Blue‐PAMAM Supramolecular Complex Membrane as a Catalytic Layer
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DOI:
10.1002/elan.200603780
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发表时间:
2007-03
期刊:
影响因子:
3
通讯作者:
Shouguo Wu;Taoling Wang;Changqin Wang;Z. Gao;Chuanqing Wang
Shouguo Wu;Taoling Wang;Changqin Wang;Z. Gao;Chuanqing Wang
中科院分区:
化学4区
文献类型:
--
作者:
Shouguo Wu;Taoling Wang;Changqin Wang;Z. Gao;Chuanqing Wang

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利用吸附在多晶金电极上的3-巯基丙酸(3-MPA)亚单层,进一步与聚酰胺胺(PAMAM)树枝状分子(4.0代)反应,获得膜,随后在膜上与普鲁士蓝(PB)配位,形成混合且稳定的H2 O2还原电催化层,从而制备了一种新型过氧化氢(H2 O2)传感器。电化学行为、原子力显微镜(AFM)和X射线光电子能谱(XPS)的研究表明,PB分子位于PAMAM树枝状大分子的树枝状结构中。结果表明,PB/PAMAM/3-MPA/Au修饰电极对H2 O2具有良好的电催化还原活性。考察了电位和溶液pH值对修饰电极响应的影响,以获得最佳的分析性能。即使在溶解氧的存在下,该传感器表现出高灵敏度和快速响应H2 O2。在空气饱和的0.1 mol L-1磷酸盐缓冲溶液(PBS,pH 6.50)中,在-0.20 V(vs. SCE)下,该修饰电极的稳态阴极电流响应与H2 O2浓度在1.2×10 - 6 mol L-1 ~ 6.5×10 - 4 mol L-1范围内呈线性关系,检出限为3.1×10 - 7 mol L-1。电极的性能进行了评价与尊重可能的干扰,如抗坏血酸和尿酸等的选择性,稳定性和重现性的修饰电极是令人满意的。
A novel hydrogen peroxide (H2O2) sensor was fabricated by using a submonolayer of 3-mercaptopropionic acid (3-MPA) adsorbed on a polycrystalline gold electrode further reacted with poly(amidoamine) (PAMAM) dendrimer (generation 4.0) to obtain a film on which Prussian Blue (PB) was later coordinated to afford a mixed and stable electrocatalytic layer for H2O2 reduction. On the basis of the electrochemical behaviors, atomic force microscopy (AFM) and X-ray photoelectron spectra (XPS), it is suggested that the PB molecules are located within the dendritic structure of the surface attached PAMAM dendrimers. It was found that the PB/PAMAM/3-MPA/Au modified electrode showed an excellent electrocatalytic activity for H2O2 reduction. The effects of applied potential and pH of solution upon the response of the modified electrode were investigated for an optimum analytical performance. Even in the presence of dissolved oxygen, the sensor exhibited highly sensitive and rapid response to H2O2. The steady-state cathodic current responses of the modified electrode obtained at −0.20 V (vs. SCE) in air-saturated 0.1 mol L−1 phosphate buffer solution (PBS, pH 6.50) showed a linear relationship to H2O2 concentration ranging from 1.2×10−6 mol L−1 to 6.5×10−4 mol L−1 with a detection limit of 3.1×10−7 mol L−1. Performance of the electrode was evaluated with respected to possible interferences such as ascorbic acid and uric acid etc. The selectivity, stability, and reproducibility of the modified electrode were satisfactory.