Key Laboratory of Luminescence Analysis and Molecular Sensing (Southwest University), Ministry of Education, College of Chemistry and Chemical Engineering, Southwest University, Chongqing 400715, P. R. China.
Key Laboratory of Luminescent and Real-Time Analytical System (Southwest University), Chongqing Science and Technology Bureau, College of Pharmaceutical Sciences, Southwest University, Chongqing 400715, P. R. China.
Anal Chem. 2023 May 2;95(17):7030-7035. doi: 10.1021/acs.analchem.3c00687. Epub 2023 Apr 19.
In this work, a novel aluminum metal-organic framework (Al-MOF)/-2-hydroxyethylpiperazine-'-ethane-sulfonic acid (HEPES) system with an excellent electrochemiluminescence (ECL) property was developed. First, Al-MOF was successfully synthesized through a one-pot solvothermal method by using 9,10-di(-carboxyphenyl)anthracene (DPA) as the organic luminescence ligand and Al as the metal node. Compared with DPA, Al-MOF showed high ECL intensity and excellent stability without an additional coreactant in the HEPES buffer. The corresponding ECL mechanism was studied in detail, verifying HEPES was not only the buffer in the system but also the coreactant of Al-MOF. In particular, the system of Al-MOF/HEPES showed a high ECL efficiency of 30.0%, taking the Ru(bpy) system as the standard. In addition, the ECL signal of Al-MOF was effectively quenched by dopamine (DA). The biosensor for HBV DNA detection was constructed through the ECL signal on-off-on mode of DNA specific recognition integrated with the DNA walker signal amplification strategy. The ultrasensitive detection for HBV DNA was achieved with a linear range of 100 aM to 10 pM and a limit of detection (LOD) of 62.1 aM. This work proposed a high-efficiency Al-MOF/HEPES system, providing a new viewpoint for a coreactant-free system in the field of ECL.
在这项工作中，开发了一种新型的铝金属有机骨架（Al-MOF）/-2-羟乙基哌嗪-N'-2-乙磺酸（HEPES）体系，具有优异的电致化学发光（ECL）性能。首先，通过一锅溶剂热法成功合成了 Al-MOF，该方法使用 9,10-二（-羧基苯基）蒽（DPA）作为有机发光配体，Al 作为金属节点。与 DPA 相比，Al-MOF 在 HEPES 缓冲液中无需额外的共反应物即可表现出高 ECL 强度和优异的稳定性。详细研究了相应的 ECL 机制，验证了 HEPES 不仅是体系中的缓冲剂，也是 Al-MOF 的共反应物。特别是，Al-MOF/HEPES 体系的 ECL 效率高达 30.0%，以 Ru（bpy）体系为标准。此外，DA 有效猝灭了 Al-MOF 的 ECL 信号。通过将 DNA 特异性识别与 DNA 行走者信号放大策略相结合，构建了用于 HBV DNA 检测的生物传感器。通过 DNA 特异性识别的 ECL 信号开-关-开模式实现了对 HBV DNA 的超灵敏检测，线性范围为 100 aM 至 10 pM，检测限（LOD）为 62.1 aM。这项工作提出了一种高效的 Al-MOF/HEPES 体系，为 ECL 领域无共反应物体系提供了新的视角。
