Zhou Yifan, Ding Zhenyao, Sun Qinghao, Chen Liping, Wang Dandan, Bao Xiaoguang, Feng Xinjian
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China.
Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou 215123, China.
J Am Chem Soc. 2024 Jun 6. doi: 10.1021/jacs.4c03341.
Bioassay systems that can selectively detect biomarkers at both high and low levels are of great importance for clinical diagnosis. In this work, we report an enzyme electrode with an oxygen reduction reaction (ORR)-tolerant HO reduction property and an air-liquid-solid triphase interface microenvironment by regulating the surface defects and wettability of nanoporous tin oxide (SnO). The enzyme electrode allows the oxygen that is required for the oxidase catalytic reaction to be transported from the air phase to the reaction zone, which greatly enhances the enzymatic kinetics and increases the linear detection upper limit. Meanwhile, the ORR-tolerant HO reduction property of SnO catalysts achieved via oxygen vacancy engineering greatly reduces the interferent signals caused by oxygen and various easily oxidizable endogenous/exogenous species, which enables the selective detection of biomarkers at trace levels. The synergistic effect between these two novel qualities features a bioassay system with a wide dynamic linear range and high selectivity for the accurate detection of a wide range of biomarkers, such as glucose, lactic acid, uric acid, and galactose, offering the potential for reliable clinical diagnosis applications.
能够选择性地检测高、低水平生物标志物的生物测定系统对于临床诊断至关重要。在这项工作中,我们通过调节纳米多孔氧化锡(SnO)的表面缺陷和润湿性,报道了一种具有耐氧还原反应(ORR)的HO还原特性和气-液-固三相界面微环境的酶电极。该酶电极使氧化酶催化反应所需的氧气从气相传输到反应区,极大地增强了酶促动力学并提高了线性检测上限。同时,通过氧空位工程实现的SnO催化剂的耐ORR的HO还原特性大大降低了由氧气和各种易氧化的内源性/外源性物质引起的干扰信号,从而能够选择性地检测痕量水平的生物标志物。这两种新特性之间的协同效应形成了一种生物测定系统,该系统具有宽动态线性范围和高选择性,可准确检测多种生物标志物,如葡萄糖、乳酸、尿酸和半乳糖,为可靠的临床诊断应用提供了潜力。