Chen Junhao, Chen Siyu, Lou Yafei, Nilghaz Azadeh, Tian Junfei
State Key Laboratory of Pulp and Paper Engineering, School of Light Industry and Engineering, South China University of Technology, Guangzhou 510630, China.
Drug Delivery, Disposition, and Dynamics, Monash Institute of Pharmaceutical Sciences, Monash University, Parkville, Victoria 3052, Australia.
Anal Chem. 2025 Jun 24;97(24):12699-12707. doi: 10.1021/acs.analchem.5c01393. Epub 2025 Jun 10.
Currently, biosensor antifouling and biorecognition layer designs are considered apart. The antifouling layer unavoidably impairs the electrochemical link between the biorecognition layer and base electrodes, resulting in a double-edged antifouling strategy. Here, we propose an approach guided by the concept of the multiplicative sensor, which transforms the biorecognition layer into an antifouling coating. For example, we fabricate a multiplicative sensor integrated with antifouling, hydrogen peroxide detection, and tetramethylbenzidine (TMB) detection in a 2 mm working electrode. The antifouling function was obtained by controlling the crosslinking time of bovine serum albumin (BSA) and glucose oxidase (GOx) and remained effective for a week, even in simulations of contamination with plasma and 1 wt % BSA. By leveraging the capacity of the Prussian blue-containing working electrode to detect hydrogen peroxide and TMB and the numerous active functional groups (e.g., -NH, -COOH) on BSA@GOx, we have successfully constructed both a glucose biosensor and a human chorionic gonadotropin (HCG) immunosensor using the BSA@GOx layer. The multiplicative sensor exhibited detection limits of glucose, and HCG assays were measured as 0.036 mM and 0.341 ng mL with dynamic ranges of 0-0.8 mM and 0.1-100 ng mL (1.24-124 mIU mL), respectively. Integrating enzymatic glucose detection into the immunosensor detection process enhances its sensitivity, thereby facilitating the detection of low-concentration enzymatic substrates. We anticipate that this methodology can be easily applied in special electrochemical biosensors featuring simplicity, cost-effectiveness, and high sensitivity.
目前，生物传感器的防污层和生物识别层设计是分开考虑的。防污层不可避免地会削弱生物识别层与基底电极之间的电化学连接，从而导致一种双刃剑式的防污策略。在此，我们提出一种以乘法传感器概念为指导的方法，该方法将生物识别层转化为防污涂层。例如，我们在一个2毫米的工作电极中制造了一种集成了防污、过氧化氢检测和四甲基联苯胺（TMB）检测功能的乘法传感器。通过控制牛血清白蛋白（BSA）和葡萄糖氧化酶（GOx）的交联时间获得了防污功能，即使在血浆和1 wt% BSA污染模拟中，该功能也能保持一周有效。通过利用含普鲁士蓝的工作电极检测过氧化氢和TMB的能力以及BSA@GOx上众多的活性官能团（如-NH、-COOH），我们成功地使用BSA@GOx层构建了葡萄糖生物传感器和人绒毛膜促性腺激素（HCG）免疫传感器。该乘法传感器对葡萄糖的检测限为0.036 mM，对HCG检测的测量值为0.341 ng/mL，动态范围分别为0 - 0.8 mM和0.1 - 100 ng/mL（1.24 - 124 mIU/mL）。将酶促葡萄糖检测整合到免疫传感器检测过程中可提高其灵敏度，从而便于检测低浓度的酶底物。我们预计这种方法可以很容易地应用于具有简单性、成本效益和高灵敏度的特殊电化学生物传感器中。
