College of Chemistry and Chemical Engineering, Fujian Normal University, Fuzhou 350108, PR China.
College of Chemistry and Chemical Engineering, Fujian Normal University, Fuzhou 350108, PR China.
Biosens Bioelectron. 2017 Jun 15;92:687-694. doi: 10.1016/j.bios.2016.10.028. Epub 2016 Oct 15.
Herein, a delicate photoelectrochemical biosensor for quantitative detection of trypsin was successfully established by virtue of polyethylenimine-sensitized TiO mesocrystal as the photoactive matrix integrated with Boron-doped carbon quantum dots labeled peptide as the signal amplification tags. Specifically, polyethylenimine with fine photo-stability was introduced here as the electron transporting layer to reduce the energy barrier of TiO mesocrystal, thereby facilitating the carriers transfer and improving the photocurrent response. Moreover, the Boron-doped carbon dots-peptide bioconjugates could noticeably decrease the photocurrent due to the competitively light harvesting by Boron-doped carbon dots and the steric hindrance of peptide chains, leading to less light energy arriving at the TiO mesocrystal and hindering the electrons transfer between the electrolyte and electrode. The anchored conjugates synergistically promoted the decline of photocurrent signal, evidently enhancing the sensitivity of this detection protocol. When trypsin was incubated, the photoelectric signal was obviously re-promoting because arginine-containing peptide chains could be specifically cleaved by trypsin and the Boron-doped carbon quantum dots was affranchised from the electrode, making the most of the previous suppression effects released. Therefore, the intensity of photocurrent signal was proportional to the trypsin concentration in a wide linger range from 1×10mg/mL to 1.0mg/mL. This practical and elegant "on-off-on" biosensor with high sensitivity offered a promising scheme to monitor various proteases and the inhibitors screening for early diagnoses of different diseases.
本文成功构建了一种基于聚乙二胺敏化的 TiO 介孔晶体的光电化学生物传感器,用于定量检测胰蛋白酶。具体来说,聚乙二胺具有良好的光稳定性,被引入作为电子传输层,以降低 TiO 介孔晶体的能量势垒,从而促进载流子转移并提高光电流响应。此外,硼掺杂碳点-肽生物缀合物由于硼掺杂碳点的竞争性光捕获和肽链的空间位阻,会显著降低光电流,导致到达 TiO 介孔晶体的光能减少,并阻碍电解质和电极之间的电子转移。固定的缀合物协同促进光电流信号的下降,显著提高了该检测方案的灵敏度。当孵育胰蛋白酶时,由于含精氨酸的肽链可以被胰蛋白酶特异性切割,硼掺杂碳量子点从电极上释放出来,从而充分释放先前的抑制作用,因此光电信号明显得到恢复。因此,光电流信号的强度与 1×10mg/mL 至 1.0mg/mL 宽范围内的胰蛋白酶浓度呈正比。这种实用且优雅的“开-关-开”高灵敏度生物传感器为监测各种蛋白酶和抑制剂筛选提供了一种有前途的方案,用于不同疾病的早期诊断。