Meng Zongwu, Zhang Tao, Zhang Zerun, Qu Xiaolong, Wang Bin, Qiu Yuzhe, Wu Pian, Ding Ping
Xiangya School of Public Health, Central South University, Changsha, Hunan, 410078, PR China; Hunan Provincial Key Laboratory of Clinical Epidemiology, Changsha, Hunan, 410078, PR China.
Xiangya School of Public Health, Central South University, Changsha, Hunan, 410078, PR China.
Biosens Bioelectron. 2025 Mar 1;271:117012. doi: 10.1016/j.bios.2024.117012. Epub 2024 Dec 5.
The widespread presence of antibiotic residues in the environment and food represents a significant threat to human health. In this study, a novel MOF-on-MOF (FCZE) gel with excellent peroxidase activity and strong fluorescence properties successfully synthesized by using Polyvinyl pyrrolidone (PVP) as a cross-linker and H₄BTEC as a ligand. Based on the energy transfer from the FCZE ligand to Eu luminescence, an ultrasensitive fluorescence method was developed for the detection of chlortetracycline (CTC), achieving a limit of detection (LOD) as low as 0.43 nM. Furthermore, the combination of FCZE with the 3,3',5,5'-tetramethylbenzidine (TMB)-hydrogen peroxide (HO) system enabled sensitive colorimetric detection of D-penicillamine (D-PA) with an LOD of 8.66 nM. Theoretical calculations reveal that the fluorescence quenching of FCZE by CTC is attributed to the inner filter effect of CTC and its suppression of the HBTEC excited-state return to the ground state. Furthermore, Fukui function was employed for the first time to clarify the role of D-PA in scavenging free radicals and reducing oxidized TMB (oxTMB), providing a comprehensive understanding of the colorimetric detection mechanism. Additionally, a smartphone-assisted visual detection platform based on FCZE was developed for the detection of CTC and D-PA, with LODs of 0.71 μM and 0.13 μM, respectively. This study highlights the potential of nanomaterials for the simultaneous detection of multiple antibiotics, offering a novel strategy for the rapid and efficient monitoring of antibiotic residues in environmental samples.
环境和食品中广泛存在的抗生素残留对人类健康构成重大威胁。在本研究中，以聚乙烯吡咯烷酮（PVP）为交联剂、H₄BTEC为配体，成功合成了一种具有优异过氧化物酶活性和强荧光性能的新型MOF-on-MOF（FCZE）凝胶。基于从FCZE配体到铕发光的能量转移，开发了一种超灵敏荧光法用于检测金霉素（CTC），检测限（LOD）低至0.43 nM。此外，FCZE与3,3',5,5'-四甲基联苯胺（TMB）-过氧化氢（HO）体系相结合，实现了对D-青霉胺（D-PA）的灵敏比色检测，LOD为8.66 nM。理论计算表明，CTC对FCZE的荧光猝灭归因于CTC的内滤效应及其对HBTEC激发态返回基态的抑制。此外，首次采用福井函数来阐明D-PA在清除自由基和还原氧化TMB（oxTMB）中的作用，从而全面理解比色检测机制。此外，还开发了一种基于FCZE的智能手机辅助视觉检测平台，用于检测CTC和D-PA，LOD分别为0.71 μM和0.13 μM。本研究突出了纳米材料在同时检测多种抗生素方面的潜力，为快速高效监测环境样品中的抗生素残留提供了一种新策略。
