College of Chemistry and Chemical Engineering, Key Laboratory of Shandong Provincial Universities for Functional Molecules and Materials, Qingdao University, Qingdao, 266000, PR China.
College of Chemistry and Chemical Engineering, Key Laboratory of Shandong Provincial Universities for Functional Molecules and Materials, Qingdao University, Qingdao, 266000, PR China.
Biosens Bioelectron. 2024 Oct 15;262:116553. doi: 10.1016/j.bios.2024.116553. Epub 2024 Jul 14.
A spatial-resolved and self-calibrated photoelectrochemical (PEC) biosensor has been fabricated by a multifunctional CeO/CdS heterostructure, achieving portable and sensitive detection of carcinoembryonic antigen (CEA) using a homemade 3D printing device. The CeO/CdS heterostructure with matched band structure is prepared to construct the dual-photoelectrodes to improve the PEC response of CeO. In particular, as the photoactive nanomaterial, the CeO also plays the role of peroxidase mimetic nanozymes. Therefore, the catalytic performance of CeO with different morphologies (e.g., nano-cubes, nano-rods and nano-octahedra) have been studied, and CeO nano-cubes (c-CeO) achieve the optimal catalytic activity. Upon introducing CEA, the sandwich-type immunocomplex is formed in the microplate using GOx-AuNPs-labeled second antibody as detection antibody. As a result, HO can be produced from the catalytic oxidization of glucose substrate by GOx, which is further catalyzed by CeO to form •OH, thus in situ etching CdS and decreasing the photocurrents. The self-calibration is achieved by the dual-channel photoelectrodes on the homemade 3D printing device to obtain the photocurrents ratio, thus effectively normalizing the fluctuations of external factors to enhance the accuracy. This integrated biosensor with a detection limit as low as 0.057 ng mL provides a promising way for ultrasensitive immunoassay in clinic application in complex environments.
一种空间分辨和自校准光电化学（PEC）生物传感器已通过多功能 CeO/CdS 异质结构制备，使用自制的 3D 打印设备实现了对癌胚抗原（CEA）的便携式和灵敏检测。具有匹配能带结构的 CeO/CdS 异质结构被制备以构建双光电极，以提高 CeO 的 PEC 响应。特别是，作为光活性纳米材料，CeO 还起到过氧化物酶模拟纳米酶的作用。因此，研究了不同形态的 CeO（例如纳米立方体、纳米棒和纳米八面体）的催化性能，CeO 纳米立方体（c-CeO）具有最佳的催化活性。引入 CEA 后，GOx-AuNPs 标记的第二抗体作为检测抗体在微孔板中形成夹心型免疫复合物。结果，GOx 可以从葡萄糖底物的催化氧化中产生 HO，HO 进一步被 CeO 催化形成•OH，从而原位蚀刻 CdS 并减少光电流。通过自制 3D 打印设备上的双通道光电极实现自校准，以获得光电流比，从而有效归一化外部因素的波动，提高准确性。这种具有低至 0.057ng/mL 检测限的集成生物传感器为在复杂环境中的临床应用中的超灵敏免疫分析提供了一种有前途的方法。
