Department of General Surgery, State Key Laboratory of Complex Severe and Rare Diseases, Peking Union Medical College Hospital, Chinese Academy of Medical Science and Peking Union Medical College, Beijing, 100730, PR China.
College of Biological Science and Engineering, Fuzhou University, Fuzhou, 350108, PR China.
Anal Chim Acta. 2023 Jul 18;1265:341362. doi: 10.1016/j.aca.2023.341362. Epub 2023 May 12.
This work presents an integrated photoelectrochemical, impedance and colorimetric biosensing platform for flexible detection of cancer markers based on the targeted response by combining liposome amplification strategies and target-induced non-in situ formation of electronic barriers as the signal transduction modality on carbon-modified CdS photoanodes. Inspired by game theory, the carbon layer modified CdS hyperbranched structure with low impedance and high photocurrent response was firstly obtained by surface modification of CdS nanomaterials. Through a liposome-mediated enzymatic reaction amplification strategy, a large number of organic electron barriers were formed by a biocatalytic precipitation (BCP) reaction triggered by horseradish peroxidase released from cleaved liposomes after the introduction of the target molecule, thereby increasing the impedance characteristics of the photoanode as well as attenuating the photocurrent. The BCP reaction in the microplate was accompanied by a significant color change, which opened up a new window for point-of-care testing. Taking carcinoembryonic antigen (CEA) as a proof of concept, the multi-signal output sensing platform showed a satisfactory sensitive response to CEA with an optimal linear range of 20 pg mL-100 ng mL. The detection limit was as low as 8.4 pg mL. Meanwhile, with the assistance of a portable smartphone and a miniature electrochemical workstation, the electrical signal obtained was synchronized with the colorimetric signal to correct the actual target concentration in the sample, further reducing the occurrence of false reports. Importantly, this protocol provides a new idea for the sensitive detection of cancer markers and the construction of a multi-signal output platform.
本工作提出了一种基于脂质体放大策略和目标诱导的非原位形成电子势垒的靶向响应的光电化学、阻抗和比色生物传感平台，用于基于结合的碳修饰 CdS 光电阳极的信号转导模式对癌症标志物进行灵活检测。受博弈论的启发，首先通过 CdS 纳米材料的表面修饰，获得了具有低阻抗和高光电流响应的碳层修饰 CdS 超支化结构。通过脂质体介导的酶反应放大策略，通过从被切割的脂质体中释放的辣根过氧化物酶触发的生物催化沉淀 (BCP) 反应，在引入目标分子后形成大量的有机电子势垒，从而增加光电阳极的阻抗特性并衰减光电流。微孔板中的 BCP 反应伴随着明显的颜色变化，为即时检测开辟了新的窗口。以癌胚抗原 (CEA) 为概念验证，多信号输出传感平台对 CEA 表现出令人满意的灵敏响应，最佳线性范围为 20 pg mL-100 ng mL。检测限低至 8.4 pg mL。同时，借助便携式智能手机和微型电化学工作站，将获得的电信号与比色信号同步，以校正样品中实际目标浓度，进一步降低误报的发生。重要的是，该方案为癌症标志物的灵敏检测和多信号输出平台的构建提供了新的思路。
