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调控基于 Zr 的混合配体金属-有机骨架的高光电流活性以实现对α-葡萄糖苷酶的灵敏电致化学发光传感。

Regulating highly photoelectrochemical activity of Zr-based mixed-linker metal-organic frameworks toward sensitive electrogenerated chemiluminescence sensing of α-glucosidase.

机构信息

Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University, Tianjin 300072, China.

Institute of Photoelectronic Thin Film Devices and Technology, Solar Energy Conversion Center, Key Laboratory of Photoelectronic Thin Film Devices and Technology of Tianjin, Engineering Research Center of Thin Film Photoelectronic Technology of Ministry of Education, Nankai University, Tianjin, 300350, China.

出版信息

Biosens Bioelectron. 2023 Oct 1;237:115530. doi: 10.1016/j.bios.2023.115530. Epub 2023 Jul 16.

Abstract

The conductivity and emission efficiency of metal-organic frameworks (MOFs) remain challenging factors that limit their electrogenerated chemiluminescence (ECL) sensing applications. Herein, we report a facile approach to address these challenges by integrating an electroactive linker (H-TCPP) with an ECL active electrogenerated chemiluminescence linker (H-TBAPy) to construct a highly photoelectrochemical active mixed-linker MOFs (ML-MOFs). ECL results revealed a remarkable 15.4-fold enhancement for the top-performing ML-MOFs (M6-MOFs), surpassing the single linker MOFs. In addition, M6-MOFs also exhibit a remarkable 73-fold enhancement in ECL efficiency compared to commercial Ru (bpy). This improvement should be attributed to the synergistic effects resulting from the combination of two linkers. Furthermore, M6-MOFs are found to be served as a model ECLphore for sensitive and selective detection of α-glucosidase for the first time with good potential practicability in human serum samples. This work represents a promising direction to guide for designing good conductivity and high ECL efficiency MOFs in terms of linker functionalization and thus bandgap modulation for advancing their ECL sensing applications.

摘要

金属-有机骨架(MOFs)的电导率和发射效率仍然是限制其电致化学发光(ECL)传感应用的挑战性因素。在本文中,我们报告了一种通过将电活性连接体(H-TCPP)与 ECL 活性电致化学发光连接体(H-TBAPy)集成来构建高光电化学活性混合配体 MOFs(ML-MOFs)来解决这些挑战的简便方法。ECL 结果表明,性能最佳的 ML-MOFs(M6-MOFs)的增强幅度达到了惊人的 15.4 倍,超过了单配体 MOFs。此外,与商业 Ru(bpy)相比,M6-MOFs 的 ECL 效率也提高了 73 倍。这种改进应该归因于两种配体结合产生的协同效应。此外,M6-MOFs 首次被用作模型 ECLphore,用于灵敏和选择性检测α-葡萄糖苷酶,在人血清样本中具有良好的实际应用潜力。这项工作为通过配体功能化和能带隙调制来设计具有良好导电性和高 ECL 效率的 MOFs 提供了有希望的指导方向,从而推进了它们在 ECL 传感应用中的发展。

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