Near-Infrared Light-Initiated Photoelectrochemical Biosensor Based on Upconversion Nanorods for Immobilization-Free miRNA Detection with Double Signal Amplification
Near-Infrared Light-Initiated Photoelectrochemical Biosensor Based on Upconversion Nanorods for Immobilization-Free miRNA Detection with Double Signal Amplification
复制标题
DOI：
10.1021/acs.analchem.1c02160
复制
发表时间：
2021-08-09
影响因子：
7.4
通讯作者：
Yan, Mei
中科院分区：
文献类型：
--
作者：
Hao, Mengjiao;Miao, Pei;Yan, Mei
光电化学（PEC）传感器是一种检测灵敏度高、成本低的新型传感平台。然而，目前的PEC生物传感器依赖于紫外线或可见光作为激发源，对生物样品和系统造成损伤，限制了其在复杂基质中的应用。本文设计了一种基于NaYF4:Yb，Tm@NaYF4@TiO2的近红外光引发的PEC生物传感器。@CdS （csUCNRs@TiO2 @CdS）的构建是为了灵敏地检测急性心肌梗死（AMI）相关的miRNA-133a，采用无固定的形式，结合杂交链反应和氧化还原环信号放大策略。利用NaYF4:Yb，Tm@NaYF4上转换纳米棒，将低能量980 nm近红外入射激光转换成300-480 nm光，激发相邻TiO2@CdS光敏壳层产生光电流。同时，利用磁珠对靶miRNA-133a进行均匀检测，降低了识别的位阻，提高了检测灵敏度。当miRNA-133a出现后，抗坏血酸作为能量供体消耗csUCNRs@TiO2@CdS表面产生的光声孔，光电流响应与抗坏血酸水平正相关。利用nir光驱动和无固定化策略，构建的生物传感器对miRNA-133a具有线性敏感性和选择性，检测限为36.12 aM。更重要的是，该方法提供了近红外光驱动的PEC传感策略的新概念，以检测具有明显灵敏度，光稳定性和低光损伤的多种生物标志物。
Photoelectrochemical (PEC) sensors are relatively new sensing platforms with high detection sensitivity and low cost. However, the current PEC biosensors dependent on ultraviolet or visible light as the exciting resource cause injuries to biological samples and systems, which restrains the applications in complicated matrixes. Herein, a near-infrared light (NIR)-initiated PEC biosensor based on NaYF4:Yb,Tm@NaYF4@TiO2. @CdS (csUCNRs@TiO2 @CdS) was constructed for sensitive detection of acute myocardial infarction (AMI)-related miRNA-133a in an immobilization-free format coupled with a hybridization chain reaction and a redox circle signal amplification strategy. A low-energy 980 nm NIR incident laser was converted to 300-480 nm light to excite the adjacent TiO2@CdS photosensitive shell to generate photocurrent by NaYF4:Yb,Tm@NaYF4 upconversion nanorods. Also, magnetic beads were employed for the homogeneous determination of target miRNA-133a to reduce the recognition steric hindrance and improve the detection sensitivity. The photocurrent response was positively correlated with the level of ascorbic acid as the energy donor to consume photoacoustic holes produced on the surface of csUCNRs@TiO2@CdS, which was generated by alkaline phosphatase catalyzation and regenerated by tris(2-carboxyethyl) phosphine reduction upon the appearance of miRNA-133a. Exerting a NIR-light-driven and immobilization-free strategy, the as-constructed biosensor displayed linearly sensitive and selective determination of miRNA-133a with a detection limit of 36.12 aM. More significantly, the assay method provided a new concept of the PEC sensing strategy driven by NIR light to detect diverse biomarkers with pronounced sensitivity, light stability, and low photodamage.