金属有机框架材料荧光检测抗生素的研究进展

doi:10.16553/j.cnki.issn1000-985x.2025.0122

摘要/Abstract

摘要： 抗生素在医疗、农业及工业领域至关重要，但对人类健康及自然界的生态平衡构成了潜在的威胁。传统检测技术虽有效，但成本高且操作复杂。因此，开发高效灵敏的检测技术迫在眉睫。金属有机框架材料（MOFs）因多孔结构、可调节化学组成和荧光性能，在抗生素荧光检测中潜力巨大。本文以MOFs荧光检测抗生素中的光致电子转移（PET）、荧光共振能量转移（FRET）、内滤效应（IFE）等机制为切入点，通过荧光猝灭、荧光增强及比率荧光这三种检测策略，系统梳理了近年来基于MOFs的荧光传感器在抗生素检测领域的最新研究进展。具体探讨了MOFs及其主客体复合材料在检测β-内酰胺类、大环内酯类、四环素类、氨基糖苷类、喹诺酮类、磺胺类、酰胺醇类，以及磷酸化多糖类等多种抗生素的表现。此外，通过对现有研究成果的总结和分析，为该领域后续研究指明了方向，包括进一步优化MOFs的结构和性能、结合现代分析技术等，从而为推动MOFs荧光传感器在抗生素检测领域的实际应用提供了坚实基础。

关键词: 金属有机框架; 荧光检测; 荧光传感器; 抗生素; 环境和食品污染

Abstract: Antibiotics， as essential antimicrobial agents， are extensively used in medicine， agriculture， and various industrial sectors. However， their overuse and improper disposal have led to environmental contamination and the accumulation of antibiotic residues in water bodies， posing significant risks to human health and ecological balance. Conventional detection techniques—such as gas chromatography （GC）， liquid chromatography （LC）， gas chromatography-mass spectrometry （GC-MS）， and liquid chromatography-mass spectrometry （LC-MS）—though highly accurate， are often impeded by high costs， operational complexity， and time-intensive procedures， rendering them unsuitable for on-site and large-scale monitoring. Thus， there is a pressing need to develop efficient and sensitive detection technologies for quantifying antibiotic levels in food and environmental samples. Metal-organic frameworks （MOFs）， characterized by their unique porous structures， tunable chemical compositions， and exceptional fluorescence properties， have shown great promise for the fluorescent detection of antibiotics. Employing a literature review approach， this paper explores the fundamental mechanisms underlying MOF-based fluorescence sensing， including photoinduced electron transfer （PET）， Förster resonance energy transfer （FRET）， and the inner filter effect （IFE）. It systematically summarizes recent advances in fluorescent sensors constructed from MOFs and their host-guest composites for antibiotic detection， leveraging three primary signal transduction strategies： fluorescence quenching， fluorescence enhancement， and ratiometric fluorescence. This review bridges the conventional divides between chemical materials science， biomedicine， and environmental science， and investigates the innovative potential of MOFs in antibiotic monitoring across medical， agricultural， and industrial contexts. Specifically， it outlines the performance of MOF-based sensors in detecting major antibiotic classes， such as β-lactams， macrolides， tetracyclines， aminoglycosides， quinolones， sulfonamides， amphenicols， and phosphoglycolipids. Through strategies such as fluorescence quenching， enhancement， and ratiometric sensing， the reviewed MOF-based sensors demonstrate excellent performance. The quenching strategy exploits interactions between antibiotics and MOFs to markedly suppress fluorescence intensity， enabling highly sensitive detection. Conversely， the enhancement strategy capitalizes on the ability of certain antibiotics to augment MOF fluorescence under specific conditions， significantly amplifying weak signals and reducing interference. Ratiometric sensing employs the ratio of fluorescence intensities at two different wavelengths as a detection parameter， thereby improving accuracy and anti-interference capacity. This approach may involve one signal increasing while the other decreases， simultaneous changes in both signals， or change in one signal with the other remaining constant. These fluorescent sensors are characterized by straightforward operation， fast response， and relatively low cost， presenting promising alternatives for addressing challenges in antibiotic residue detection. Moreover， they exhibit distinct performance characteristics across different antibiotic classes， offering versatile and effective technical pathways for antibiotic analysis. In summary， fluorescent sensors based on MOFs and their host-guest composites demonstrate broad application prospects in antibiotic detection. By synthesizing and critically evaluating existing research， this review also outlines future directions for the field， including further optimization of MOF structures and properties， refinement of synthesis methods， and the integration of advanced machine learning techniques for data processing and analysis. This work provides a foundation for promoting the practical deployment of MOF-based fluorescent sensors， thereby supporting efforts to mitigate antibiotic pollution and protect human health and environmental safety.

Key words: metal-organic framework; fluorescence detection; fluorescence sensor; antibiotic; environmental and food pollution

中图分类号:

O657.3

李柯华, 伊魁宇, 史洪微, 康晓琦. 金属有机框架材料荧光检测抗生素的研究进展[J]. 人工晶体学报, 2025, 54(11): 1881-1892.

LI Kehua, YI Kuiyu, SHI Hongwei, KANG Xiaoqi. Research Progress on Fluorescence Detection of Antibiotics by Metal-Organic Frameworks[J]. Journal of Synthetic Crystals, 2025, 54(11): 1881-1892.

图/表 12

图1 MOFs荧光检测抗生素

Fig.1 MOFs fluorescently detect antibiotics

图2 Eu3+@MIL-53（Al）合成路线示意图及MG的识别原理［31］

Fig.2 Schematic illustration of synthetic route with Eu3+@MIL-53（Al） and the recognition principle for MG［31］

图3 基于IFE的主要传感方法［33］

Fig.3 Primary IFE-based sensing method［33］

表1 金属有机框架基合成材料对不同目标物荧光猝灭型的检测性能参数

Table 1 Detection performance parameter of fluorescence quenching type of metal-organic framework-based synthetic materials for different target substances

Synthetic substance	MOF type	Objective	Linear range	LOD	Sample	Reference
Tb-MOF	Pure MOF	CEF	0~40 µmol/L	0.179 µmol/L	Water	［36］
FCZE	Composite MOF	CTC	0.5~200 nmol/L	0.43 nmol/L	—	［38］
［Eu（L）_1/2H₂O］ _n	Pure MOF	GM	0~140 µmol/L	0.009 1 nmol/L	—	［39］
｛Zn（bib）·（SO₄）·（H₂O）｝ _n	Pure MOF	NOR	0~10 µmol/L	7.04 µmol/L	Water	［41］
［Cd₄（MTPTC）₂（DMF）₄］·5DMF·2H₂O	Pure MOF	SDZ	0~40 µmol/L	0.070 µmol/L	—	［42］
Eu-MOF	Pure MOF	CHL	5~150 µmol/L	3.16 µmol/L	Milk	［43］

图4 Zn-MOF与OTC@Zn-MOF的合成及检测OTC的机理［46］

Fig.4 Synthesis of Zn-MOF and OTC@Zn-MOF and the mechanism for detecting OTC［46］

图5 智能手机辅助Zn-TCPE试纸在不同TOB浓度下的荧光特征分析［47］。（a）一部装载了颜色识别应用的智能手机；（b）TOB检测的校准曲线。插图展示了Zn-TCPE制成的试纸在365 nm紫外灯照射下，随着TOB浓度增加（从左至右：5、10、20、30及40 μmol/L）所呈现的荧光彩色照片

Fig.5 Analysis of fluorescence characteristics of Zn-TCPE test strips assisted by smart phones under different TOB concentrations［47］. （a） A smartphone with a color recognition App loaded；（b） a calibration curve for TOB detection. The illustration shows fluorescence color photographs of test papers made by Zn-TCPE with increasing TOB concentrations under 365 nm UV lamp light （from left to right： 5， 10， 20， 30， and 40 μmol/L）

图6 Cu-MOF实现鸡肉中氟苯尼考选择性荧光检测的示意图［50］

Fig.6 A schematic diagram of the Cu-MOF achieving selective fluorescence detection of florfenicol in chicken［50］

表2 金属有机框架基合成材料对不同目标物荧光增强型的检测性能参数

Table 2 Performance parameter of fluorescence enhancement detection of metal-organic framework-based synthetic materials for different target substances

Synthetic substance	MOF type	Objective	Linear range	LOD	Sample	Reference
Cd-MOF［Cd（L）_0.5（1，2-bimb）］	Pure MOF	AMB	0~200 µmol/L	2.39 µmol/L	—	［45］
Zn-MOF	Composite MOF	OTC	0.02~13 µmol/L	0.017 nmol/L	Water	［46］
Zn-TCPE	Composite MOF	TOB	79.3~10 000 nmol/L	23.8 nmol/L	River water	［47］
Cd-MOF	Pure MOF	ENR	0~45 µmol/L	0.025 µmol/L	Water	［48］
［Ln₂（tcptp）（btca）（H₂O） _m ］ _n， Ln=Tb³⁺	Pure MOF	LVX	0~20 µmol/L	0.256 mg/kg	—	［49］
Cu-MOF	Pure MOF	FFC	1~50 µmol/L	2.93 µmol/L	Chicken	［50］

图7 ERY检测原理［53］

Fig.7 Principle of ERY detection［53］

图8 基于CDs@HZIF-8的比率荧光探针制备及应用示意图，用于四环素类抗生素检测［54］

Fig.8 Schematic diagram of the preparation and application of ratiometric fuorescent probe based on CDs@HZIF-8 for the detection of tetracycline antibiotics［54］

图9 使用Eu-MOF负载纸张进行AP检测的示意图［59］

Fig.9 Schematic diagram of AP detection using Eu-MOF loaded paper［59］

表3 金属有机框架基合成材料对不同目标物比率荧光型的检测性能参数

Table 3 Detection performance parameters of metal-organic framework-based synthetic materials for different target substance ratio fluorescence types

Synthetic substance	MOF type	Objective	Linear range	LOD	Sample	Reference
QDs@Al-MOF	Composite MOF	ERY	液态24.83~242.6 nmol/L；水凝胶膜26~728 pmol/L	液态2.16 nmol/L；水凝胶膜2.42 pmol/L	—	［53］
CDs@HZIF-8	Composite MOF	TC； OTC； DOX	0.5~50 µmol/L； 0.5~40 µmol/L； 0.5~40 µmol/L	6.56 nmol/L； 29.46 nmol/L； 30.58 nmol/L	Milk	［54］
FS@UIO66	Composite MOF	LEV	79.3~10 000 nmol/L	0.280 8 µmol/L	Water	［55］
Tb_0.6Eu_0.4-MOF	Pure MOF	SMZ	2~140 µmol/L	0.1 µmol/L	Fish	［56］
TCPP@UiO-66-NDC	Composite MOF	AMX	10~1 000 nmol/L； 1~100 µmol/L	27 nmol/L	Capsules； Milk	［57］
Eu-BDC	Composite MOF	TCH	0.38~75 µmol/L	0.115 µmol/L	Carp； Clam	［58］
Eu-MOF	Composite MOF	AP； AMK； KAN	0.001~100 µmol/L	0.33 nmol/L； 0.32 nmol/L； 0.30 nmol/L	Milk； Honey	［59］
NH₂-MIL-101（Eu）@Fe-MOF	Composite MOF	FLA	6~8 µmol/L	4.8 nmol/L	—	［60］

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