Department of Chemistry, School of Science, Xi'an Jiaotong-Liverpool University, No. 111 Ren'ai Road, Suzhou Industrial Park, Dushu Lake Higher Education and Innovation Park, Suzhou 215123, Jiangsu Province, People's Republic of China.
Department of General Surgery, First Affiliated Hospital of Soochow University, No. 188 Shizi Street, Suzhou 215006, Jiangsu Province, People's Republic of China.
Langmuir. 2024 Oct 1;40(39):20797-20810. doi: 10.1021/acs.langmuir.4c02999. Epub 2024 Sep 17.
This study has focused on adjusting sensing environment from basic to neutral pH and improve sensing performance by doping electrodeposited gold (Au) with metal oxide for nonenzymatic glucose measurements in forming a Schottky interface for superior glucose sensing with detailed analysis for the sensing mechanism. The prepared sensor also holds the ability to measure pH with the identical electrospun metal oxide-electrodeposited Au, which composed a dual sensor (glucose and pH sensor) through applying chronoamperometry and open circuit potential methods. The rhodium oxide nanocoral structure was fabricated with an electrospinning precursor solution, followed by a calcination process, and it was mixed with electrodeposited nanocoral gold to form the Schottky interface by constructing a p-n type heterogeneous junction for improved sensitivity in glucose detection. The prepared materials were characterized by X-ray powder diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray photoelectron spectrometry (XPS), etc. The prepared materials were used for both pH responsive testing and amperometric glucose measurements. The rhodium oxide nanocoral doped gold demonstrated a sensitivity of 3.52 μA mM cm and limit of detection of 20 μM with linear range up to 3 mM glucose concentration compared to solely electrodeposited gold for a sensitivity of 0.46 μA mM cm and a limit of detection of 450 μM. The Mott-Schottky method was used for the analysis of an electron transfer process from noble metal to metal oxide to electrolyte in demonstrating the improved sensitivity at neutral pH for glucose measurements due to the Schottky barrier adjustment mechanism at an applied flat band potential of 0.3 V. This work opens a new venue in illustrating the metal oxide/metal materials in the glucose neutral response mechanism. In the end, human serum samples were tested against current commercial glucose meter to certify the accuracy of the proposed sensor.
本研究专注于调整从基本到中性 pH 的传感环境，并通过掺杂金属氧化物来提高电沉积金（Au）的传感性能，用于非酶葡萄糖测量，形成肖特基界面，以进行具有详细分析的葡萄糖感测。该制备的传感器还具有通过计时安培法和开路电位法测量 pH 的能力，相同的电纺金属氧化物-电沉积金组成了双传感器（葡萄糖和 pH 传感器）。氧化铑纳米珊瑚结构通过电纺前体溶液制备，然后经过煅烧过程，并与电沉积纳米珊瑚金混合，通过构建 p-n 型异质结形成肖特基界面，从而提高葡萄糖检测的灵敏度。所制备的材料通过 X 射线粉末衍射（XRD）、扫描电子显微镜（SEM）、透射电子显微镜（TEM）和 X 射线光电子能谱（XPS）等进行了表征。所制备的材料用于 pH 响应测试和安培葡萄糖测量。与仅电沉积金相比，氧化铑纳米珊瑚掺杂金具有 3.52 μA mM cm 的灵敏度和 20 μM 的检测限，线性范围高达 3 mM 葡萄糖浓度，而仅电沉积金的灵敏度为 0.46 μA mM cm，检测限为 450 μM。Mott-Schottky 方法用于分析从贵金属到金属氧化物到电解质的电子转移过程，以证明在中性 pH 下测量葡萄糖的灵敏度提高，这是由于在施加的平带电位为 0.3 V 时肖特基势垒调节机制。这项工作为阐明金属氧化物/金属材料在葡萄糖中性响应机制方面开辟了新途径。最后，用人血清样本对当前的商业葡萄糖计进行测试，以证明所提出的传感器的准确性。
