Analytical and Bioanalytical Chemistry ( IF 3.8 ) Pub Date : 2021-08-31 , DOI: 10.1007/s00216-021-03616-w Negin Jahani 1 , Mandana Amiri 1 , Mina Ghiasi 2 , Hamideh Imanzadeh 1 , Rabah Boukherroub 3 , Sabine Szunerits 3 , Frank Marken 4 , Neil B McKeown 5
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Advances in materials science have accelerated the development of diagnostic tools with the last decade witnessing the development of enzyme-free sensors, owing to the improved stability, low cost and simple fabrication of component materials. However, the specificity of non-enzymatic sensors for certain analytes still represents a challenging task, for example the determination of cholesterol level in blood is vital due to its medical relevance. In this work, a reagent displacement assay for cholesterol sensing in serum samples was developed. It is based on coating of a glassy carbon electrode with a polymer of intrinsic microporosity (PIM) that forms a host-guest complex with methylene blue (MB). In the presence of cholesterol, the MB electroactive probe was displaced due to the stronger association of cholesterol guest to the PIM host. The decrease in the oxidative current was proportional to the cholesterol concentration achieving a detection limit of approximately 0.1 nM. Moreover, to further assist the experimental studies, comprehensive theoretical calculations are also performed by using density functional theory (DFT) calculations.
Graphical abstract
中文翻译：
基于与固有微孔 (PIM) 聚合物的强主客相互作用和 DFT 研究的非酶电化学胆固醇传感器
材料科学的进步加速了诊断工具的发展，过去十年见证了无酶传感器的发展，这是由于组件材料的稳定性提高、成本低和制造简单。然而，非酶传感器对某些分析物的特异性仍然是一项具有挑战性的任务，例如，由于其医学相关性，血液中胆固醇水平的测定至关重要。在这项工作中，开发了一种用于检测血清样品中胆固醇的试剂置换分析。它基于用固有微孔 (PIM) 聚合物涂覆玻璃碳电极，该聚合物与亚甲蓝 (MB) 形成主客体复合物。在胆固醇存在的情况下，由于胆固醇客体与 PIM 主体的结合更强，MB 电活性探针被取代。氧化电流的降低与胆固醇浓度成正比，达到约 0.1 nM 的检测限。此外，为了进一步协助实验研究，还使用密度泛函理论 (DFT) 计算进行了全面的理论计算。
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