García-Hernández Celia, García-Cabezón Cristina, Martín-Pedrosa Fernando, De Saja José Antonio, Rodríguez-Méndez María Luz
Grupo Uvasens, Escuela de Ingenierías Industriales, Universidad de Valladolid, Paseo del Cauce 59, 47011 Valladolid, Spain.
Beilstein J Nanotechnol. 2016 Dec 8;7:1948-1959. doi: 10.3762/bjnano.7.186. eCollection 2016.
The sensing properties of electrodes chemically modified with PEDOT/PSS towards catechol and hydroquinone sensing have been successfully improved by combining layers of PEDOT/PSS with layers of a secondary electrocatalytic material such as gold nanoparticles (PEDOT/PSS/AuNPs), copper phthalocyanine (PEDOT/PSS/CuPc) or lutetium bisphthalocyanine (PEDOT/PSS/LuPc). Layered composites exhibit synergistic effects that strongly enhance the electrocatalytic activity as indicated by the increase in intensity and the shift of the redox peaks to lower potentials. A remarkable improvement has been achieved using PEDOT/PSS/LuPc, which exhibits excellent electrocatalytic activity towards the oxidation of catechol. The kinetic studies demonstrated diffusion-controlled processes at the electrode surfaces. The kinetic parameters such as Tafel slopes and charge transfer coefficient (α) confirm the improved electrocatalytic activity of the layered electron mediators. The peak currents increased linearly with concentration of catechol and hydroquinone over the range of 1.5 × 10 to 4.0 × 10 mol·L with a limit of detection on the scale of μmol·L. The layered composite hybrid systems were also found to be excellent electron mediators in biosensors containing tyrosinase and laccase, and they combine the recognition and biocatalytic properties of biomolecules with the unique catalytic features of composite materials. The observed increase in the intensity of the responses allowed detection limits of 1 × 10 mol·L to be attained.
通过将聚(3,4-乙撑二氧噻吩)/聚苯乙烯磺酸盐(PEDOT/PSS)层与诸如金纳米颗粒(PEDOT/PSS/AuNPs)、铜酞菁(PEDOT/PSS/CuPc)或镥双酞菁(PEDOT/PSS/LuPc)等二次电催化材料层相结合,已成功改善了用PEDOT/PSS化学修饰的电极对儿茶酚和对苯二酚的传感特性。层状复合材料表现出协同效应,如强度增加和氧化还原峰向更低电位的移动所示,这强烈增强了电催化活性。使用PEDOT/PSS/LuPc已取得了显著改善,其对儿茶酚的氧化表现出优异的电催化活性。动力学研究表明电极表面存在扩散控制过程。诸如塔菲尔斜率和电荷转移系数(α)等动力学参数证实了层状电子媒介体的电催化活性得到了改善。在1.5×10至4.0×10 mol·L的范围内,峰电流随儿茶酚和对苯二酚浓度呈线性增加,检测限在μmol·L级别。还发现层状复合杂化系统在含有酪氨酸酶和漆酶的生物传感器中是优异的电子媒介体,并且它们将生物分子的识别和生物催化特性与复合材料的独特催化特征相结合。观察到的响应强度增加使得检测限达到1×10 mol·L。