School of Electrical Engineering and Computer Science, The Pennsylvania State University, University Park, PA 16802, USA.
Materials Research Institute, The Pennsylvania State University, University Park, PA 16802, USA.
Biosensors (Basel). 2021 Oct 21;11(11):409. doi: 10.3390/bios11110409.
Transition metals have been explored extensively for non-enzymatic electrochemical detection of glucose. However, to enable glucose oxidation, the majority of reports require highly alkaline electrolytes which can be damaging to the sensors and hazardous to handle. In this work, we developed a non-enzymatic sensor for detection of glucose in near-neutral solution based on copper-nickel electrodes which are electrochemically modified in phosphate-buffered saline (PBS). Nickel and copper were deposited using chronopotentiometry, followed by a two-step annealing process in air (Step 1: at room temperature and Step 2: at 150 °C) and electrochemical stabilization in PBS. Morphology and chemical composition of the electrodes were characterized using scanning electron microscopy and energy-dispersive X-ray spectroscopy. Cyclic voltammetry was used to measure oxidation reaction of glucose in sodium sulfate (100 mM, pH 6.4). The PBS-Cu-Ni working electrodes enabled detection of glucose with a limit of detection (LOD) of 4.2 nM, a dynamic response from 5 nM to 20 mM, and sensitivity of 5.47 ± 0.45 μA cm-2/log10(mole.L-1) at an applied potential of 0.2 V. In addition to the ultralow LOD, the sensors are selective toward glucose in the presence of physiologically relevant concentrations of ascorbic acid and uric acid spiked in artificial saliva. The optimized PBS-Cu-Ni electrodes demonstrate better stability after seven days storage in ambient compared to the Cu-Ni electrodes without PBS treatment.
过渡金属已被广泛探索用于非酶电化学检测葡萄糖。然而,为了实现葡萄糖氧化,大多数报道都需要高碱性电解质,这可能对传感器造成损害,而且处理起来也具有危险性。在这项工作中,我们基于电化学修饰在磷酸盐缓冲盐水 (PBS) 中的铜镍电极,开发了一种用于近中性溶液中葡萄糖检测的非酶传感器。镍和铜使用恒电流计时法沉积,然后在空气中进行两步退火处理(步骤 1:室温,步骤 2:150°C),并在 PBS 中进行电化学稳定化。使用扫描电子显微镜和能量色散 X 射线光谱法对电极的形貌和化学组成进行了表征。使用循环伏安法测量了在硫酸钠(100 mM,pH 6.4)中葡萄糖的氧化反应。PBS-Cu-Ni 工作电极能够检测葡萄糖,其检测限 (LOD) 为 4.2 nM,动态响应范围从 5 nM 到 20 mM,在 0.2 V 的应用电位下灵敏度为 5.47 ± 0.45 μA·cm-2/log10(mole·L-1)。除了超低的 LOD 之外,这些传感器在添加了人工唾液中生理相关浓度的抗坏血酸和尿酸的情况下,对葡萄糖具有选择性。与未经 PBS 处理的 Cu-Ni 电极相比,优化后的 PBS-Cu-Ni 电极在七天的环境储存后具有更好的稳定性。