Department of Biological Systems Engineering, University of Wisconsin-Madison, 460 Henry Mall, Madison, WI 53706, USA.
Biosens Bioelectron. 2013 Sep 15;47:530-8. doi: 10.1016/j.bios.2013.03.051. Epub 2013 Apr 3.
A facile one-step strategy is reported to synthesize nanocomposites of chitosan-reduced graphene oxide-nickel nanoparticles (CS-RGO-NiNPs) onto a screen-printed electrode (SPE). The synthesis is initiated by electrostatic and hydrophobic interactions and formation of self-assembled nanocomposite precursors of negatively charged graphene oxide (GO) and positively charged CS and nickel cations (Ni(2+)). The intrinsic mechanism of co-depositions from the nanocomposite precursor solution under cathodic potentials is based on simultaneous depositions of CS at high localized pH and in situ reduced hydrophobic RGO from GO as well as cathodically reduced metal precursors into nanoparticles. There is no need for any pre- or post-reduction of GO due to the in situ electrochemical reduction and the removal of oxygenated functionalities, which lead to an increase in hydrophobicity of RGO and successive deposition on the electrode surface. The as-prepared CS-RGO-NiNPs-modified SPE sensor exhibited outstanding performance for enzymeless glucose (Glc) sensing in alkaline media with high sensitivity (318.4µAmM(-1)cm(-2)), wide linear range (up to 9mM), low detection limit (4.1µM), acceptable selectivity against common interferents in physiological fluids, and excellent stability. A microfluidic device was fabricated incorporating the SPE sensor for real-time Glc detection in human urine samples; the results obtained were comparable to those obtained using a high-performance liquid chromatography (HPLC) coupled with an electrochemical detector. The excellent sensing performance, operational characteristics, ease of fabrication, and low cost bode well for this electrochemical microfluidic device to be developed as a point-of-care healthcare monitoring unit.
报道了一种简便的一步法策略,用于在丝网印刷电极(SPE)上合成壳聚糖还原氧化石墨烯-镍纳米粒子(CS-RGO-NiNPs)纳米复合材料。该合成是通过静电和疏水相互作用以及带负电荷的氧化石墨烯(GO)和带正电荷的 CS 和镍阳离子(Ni(2+))的自组装纳米复合材料前体的形成引发的。纳米复合材料前体溶液在阴极电势下共沉积的内在机制基于 CS 在高局部 pH 值下的同时沉积以及 GO 原位还原为疏水性 RGO 以及阴极还原的金属前体成纳米颗粒。由于原位电化学还原和含氧官能团的去除,无需对 GO 进行任何预还原或后还原,这导致 RGO 的疏水性增加,并在电极表面上连续沉积。制备的 CS-RGO-NiNPs 修饰的 SPE 传感器在碱性介质中具有出色的无酶葡萄糖(Glc)传感性能,具有高灵敏度(318.4µAmM(-1)cm(-2))、宽线性范围(高达 9mM)、低检测限(4.1µM)、对生理流体中常见干扰物的可接受选择性和出色的稳定性。制造了一种微流控装置,其中包含 SPE 传感器,用于实时检测人尿液样品中的 Glc;得到的结果与使用与电化学检测器耦合的高效液相色谱(HPLC)得到的结果相当。这种电化学微流控装置具有出色的传感性能、操作特性、易于制造和低成本,有望开发为即时医疗保健监测单元。