Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, PR China.
Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, PR China.
Talanta. 2018 Aug 15;186:238-247. doi: 10.1016/j.talanta.2018.04.068. Epub 2018 Apr 23.
In this work, a highly selective and sensitive chemiluminescence (CL) biosensor was prepared for adenosine (AD) detection based on carbon quantum dots (CQDs) catalyzing the CL system of luminol-HO under alkaline environment and CQDs was released from the surface of AD aptamers functionalized graphene @ magnetic β-cyclodextrin polymers (GO@FeO@β-CD@A-Apt). Firstly, GO@FeO@β-CD and CQDs were prepared and characterized by transmission electron microscopy (TEM), scanning electron microscope (SEM), UV-Vis absorption spectra (UV), fluorescence spectra (FL), fourier transform infrared (FTIR) and X-ray powder diffraction (XRD). For GO@FeO@β-CD, FeO was easy to separate, GO had good biocompatibility and large specific surface area, and β-CD further increased the specific surface area of the adenosine polymers (A-Apt) to provided larger binding sites to A-Apt. Then, A-Apt was modified on the surface of GO@FeO@β-CD while CQDs was modified by ssDNA (a single stranded DNA partially complementary to A-Apt). The immobilization property (GO@FeO@β-CD to A-Apt) and the adsorption property (GO@FeO@β-CD@A-Apt to CQDs-ssDNA) were sequentially researched. The base-supported chain-like polymers - GO@FeO@β-CD@A-Apt/CQDs-ssDNA was successfully obtained. When AD existed, CQDs-ssDNA was released from the surface of GO@FeO@β-CD@A-Apt and catalyzed CL. After that, under optimized CL conditions, AD could be measured with the linear concentration range of 5.0 × 10-5.0 × 10 mol/L and the detection limit of 2.1 × 10 mol/L (3δ) while the relative standard deviation (RSD) was 1.4%. Finally, the GO@FeO@β-CD@A-Apt/CQDs-ssDNA-CL biosensor was used for the determination of AD in urine samples and recoveries ranged from 98.6% to 101.0%. Those satisfactory results illustrated the proposed CL biosensor could achieve highly selective, sensitive and reliable detection of AD and revealed potential application for AD detection in monitoring and diagnosis of human cancers.
在这项工作中，基于碳量子点（CQDs）在碱性环境下催化鲁米诺-HO 的 CL 体系，制备了一种用于检测腺苷（AD）的高选择性和高灵敏度的化学发光（CL）生物传感器，并且 CQDs 从 AD 适体功能化石墨烯@磁性β-环糊精聚合物（GO@FeO@β-CD@A-Apt）的表面释放。首先，通过透射电子显微镜（TEM）、扫描电子显微镜（SEM）、紫外-可见吸收光谱（UV）、荧光光谱（FL）、傅里叶变换红外光谱（FTIR）和 X 射线粉末衍射（XRD）对 GO@FeO@β-CD 和 CQDs 进行了制备和表征。对于 GO@FeO@β-CD，FeO 易于分离，GO 具有良好的生物相容性和大的比表面积，β-CD 进一步增加了适体聚合物（A-Apt）的比表面积，为 A-Apt 提供了更大的结合位点。然后，将 A-Apt 修饰在 GO@FeO@β-CD 的表面，而 CQDs 则通过 ssDNA（与 A-Apt 部分互补的单链 DNA）进行修饰。GO@FeO@β-CD 与 A-Apt 的固定化性质（GO@FeO@β-CD 对 A-Apt）和 GO@FeO@β-CD@A-Apt 对 CQDs-ssDNA 的吸附性质（GO@FeO@β-CD@A-Apt 对 CQDs-ssDNA）依次进行了研究。成功获得了基于碱基支撑链状聚合物的 GO@FeO@β-CD@A-Apt/CQDs-ssDNA。当存在 AD 时，CQDs-ssDNA 从 GO@FeO@β-CD@A-Apt 的表面释放出来并催化 CL。在优化后的 CL 条件下，AD 可以在 5.0×10-5.0×10 mol/L 的线性浓度范围内进行测量，检测限为 2.1×10 mol/L（3δ），相对标准偏差（RSD）为 1.4%。最后，将 GO@FeO@β-CD@A-Apt/CQDs-ssDNA-CL 生物传感器用于尿液样品中 AD 的测定，回收率范围为 98.6%至 101.0%。这些令人满意的结果表明，所提出的 CL 生物传感器可以实现对 AD 的高选择性、高灵敏度和可靠检测，并显示出在监测和诊断人类癌症方面检测 AD 的潜在应用。
