Mo Guangquan, Zheng Xinru, Ye Naobei, Ruan Zhixiong
Key Laboratory of Molecular Target & Clinical Pharmacology and the State Key Laboratory of Respiratory Disease, School of Pharmaceutical Sciences & the Fifth Affiliated Hospital of Guangzhou Medical University, Guangzhou, 511436, PR China.
Key Laboratory of Molecular Target & Clinical Pharmacology and the State Key Laboratory of Respiratory Disease, School of Pharmaceutical Sciences & the Fifth Affiliated Hospital of Guangzhou Medical University, Guangzhou, 511436, PR China.
Talanta. 2021 Apr 1;225:121954. doi: 10.1016/j.talanta.2020.121954. Epub 2020 Dec 28.
Developing high-performance sensors for glucose detection is extremely desirable for clinical diagnostics and life sciences. Particularly, it is greatly attractive to exploit composite materials with large surface area, doped heterojunction and non-precious metal as highly active electro-catalysts for nonenzymatic glucose sensing. Herein, we reported a N-doped carbon dodecahedron embedded with Co nanoparticles (Co@NCD) for the direct electro-oxidation of glucose and efficient nonenzymatic glucose detection. Co@NCD was synthesized by the pyrolysis of zeolitic imidazolate framework (ZIF). Field emission scanning electron microscope, high-resolution transmission electron microscope, powder X-ray diffraction, X-ray photoelectron spectroscopy and nitrogen adsorption-desorption experiments were performed to investigate Co@NCD. A well-defined dodecahedron morphology with uniform size and shape was observed. Besides, the original framework was carbonized after pyrolysis leading to a hollow and porous graphite dodecahedron containing N-doped carbon heterojunction. Moreover, Co nanoparticles were evenly distributed into the dodecahedron. With porous structure, N-doped carbon and embedded Co nanoparticles, Co@NCD displayed a notable electro-catalysis towards the direct oxidation of glucose (onset potential: 0.20 V). By using Co@NCD as electro-catalyst, an efficient nonenzymatic glucose sensor was obtained with a rapid amperometric response (within 1 s), low detection limit (0.11 μM) and broad detection range (0.2 μM-12.0 mM). In addition, remarkable selectivity, repeatability, reproducibility and long-term stability were also observed. Finally, Co@NCD prepared sensor was also successfully applied to the detection of glucose in human serum. Our results suggested that ZIF templated method could be an innovative solution for active composite catalysts in biomolecular electro-catalysis and Co@NCD prepared sensor could be a substantial preferable sensing platform for the nonenzymatic glucose detection.
开发用于葡萄糖检测的高性能传感器对于临床诊断和生命科学极为重要。特别是,利用具有大表面积、掺杂异质结和非贵金属的复合材料作为用于非酶葡萄糖传感的高活性电催化剂极具吸引力。在此,我们报道了一种嵌入钴纳米颗粒的氮掺杂碳十二面体(Co@NCD)用于葡萄糖的直接电氧化和高效的非酶葡萄糖检测。Co@NCD 通过沸石咪唑酯骨架(ZIF)的热解合成。进行了场发射扫描电子显微镜、高分辨率透射电子显微镜、粉末 X 射线衍射、X 射线光电子能谱和氮吸附-脱附实验来研究 Co@NCD。观察到具有均匀尺寸和形状的明确十二面体形态。此外,原始骨架在热解后碳化,形成了一个包含氮掺杂碳异质结的中空多孔石墨十二面体。而且,钴纳米颗粒均匀分布在十二面体中。凭借多孔结构、氮掺杂碳和嵌入的钴纳米颗粒,Co@NCD 对葡萄糖的直接氧化表现出显著的电催化作用(起始电位:0.20 V)。通过使用 Co@NCD 作为电催化剂,获得了一种高效的非酶葡萄糖传感器,具有快速的安培响应(在 1 秒内)、低检测限(0.11 μM)和宽检测范围(0.2 μM - 12.0 mM)。此外,还观察到了出色的选择性、重复性、再现性和长期稳定性。最后,Co@NCD 制备的传感器也成功应用于人体血清中葡萄糖的检测。我们的结果表明,ZIF 模板法可能是生物分子电催化中活性复合催化剂的一种创新解决方案,并且 Co@NCD 制备的传感器可能是用于非酶葡萄糖检测的一个非常理想的传感平台。