Abstract
An innovative synthesis of boron and nitrogen co-doped ceria-based nanoparticles (B/N-CeFNPs) with bright blue fluorescence emission is reported using the hydrothermal method. Based on the aggregation-induced emission enhancement (AIEE) effect between B/N-CeFNPs and chlortetracycline (CTC), a rapid detection method for CTC through fluorescence enhancement was developed. In addition, through the electron transfer process (ET), fluorescence resonance energy transfer (FRET) effect and static quenching between B/N-CeFNPs and oxytetracycline (OTC), a ratio fluorescence strategy for detecting OTC was generated. The fluorescence of B/N-CeFNPs at 410 nm can be effectively quenched by OTC, and new fluorescence emission appears at a wavelength of 500 nm. B/N-CeFNPs showed good linear responses with CTC and OTC in the range 0.1-1 µM and 1-40 µM, respectively. This system was used to simultaneously detect the CTC and OTC in milk and honey, realizing multi-residues detection of TCs in actual samples by using the same ceria-based fluorescence nanomaterial.
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References
Chopra I (2002) New developments in tetracycline antibiotics: glycylcyclines and tetracycline efflux pump inhibitors. Drug Resist Updat 5:119–125. https://doi.org/10.1016/s1368-7646(02)00051-1
Rodríguez Beltrán J, Rodríguez Rojas A, Yubero E, Blázquez J (2013) The animal food supplement sepiolite promotes a direct horizontal transfer of antibiotic resistance plasmids between bacterial species. Antimicrob Agents Ch 57:2651–2653. https://doi.org/10.1128/AAC.02363-12
Leverstein-van HM, Box AT, Blok HE, Paauw A, Fluit AC, Verhoef J (2002) Evidence of extensive interspecies transfer of integron-mediated antimicrobial resistance genes among multidrug-resistant Enterobacteriaceae in a clinical setting. J Infect Dis 186:49–56. https://doi.org/10.1086/341078
Daghrir R, Drogui P (2013) Tetracycline antibiotics in the environment: a review. Environ Chem Lett 11:209–227. https://doi.org/10.1007/s10311-013-0404-8
Li ZH, Hu XJ, Lu YF, Xie LN, Zhu Y (2023) Determination of sixteen antibiotics and four β-agonists in human urine samples using ultra-performance liquid chromatography-tandem mass spectrometry based on high-throughput automatic solid-phase extraction. Chin J Chromatogr 41:397–408. https://doi.org/10.3724/SP.J.1123.2022.08025
Baghani A, Mesdaghinia A, Rafieiyan M, Soltan DM, Douraghi M (2019) Tetracycline and ciprofloxacin multiresidues in beef and chicken meat samples using indirect competitive ELISA. J Immunoass Immunochem 40:328–342. https://doi.org/10.1080/15321819.2019.1597735
Wang C, Hu FX, Feng X, Zou XC, Zhao X, Ren YR (2023) A novel micron europium cluster coordination polymer as a strong electrochemiluminescent emitter for accurate and sensitive detection of tetracycline. Food Chem 419:135887. https://doi.org/10.1016/j.foodchem.2023.135887
Liu BX, Zhu HJ, Liu JJ, Wang MZ, Pan JM, Feng RL, Hu PW, Niu XH (2023) Alkali-etched imprinted Mn-Based prussian Blue analogues with superior oxidase-mimetic activity and precise recognition for tetracycline colorimetric sensing. Acs Appl Mater Inter 15:24736–24746. https://doi.org/10.1021/acsami.3c02207
Tang JM, Zheng XL, Jiang S, Cao MD, Wang SX, Zhou ZY, Nie XQ, Fang Y, Le T (2022) Dual fluorescent aptasensor for simultanous and quantitative detection of sulfadimethoxine and oxytetracycin residues in animal-derived foods tissues based on mesoporous silica. Front Nutr 9:1077893. https://doi.org/10.3389/fnut.2022.1077893
Yang WK, Zheng XY, Gao F, Li HH, Fu B, Guo DY, Wang FX, Pan QH (2022) CdTe QDs@ZIF-8 composite-based recyclable ratiometric fluorescent sensor for rapid and sensitive detection of chlortetracycline. Spectrochim Acta Mol Biomol Spectrosc 270:120785. https://doi.org/10.1016/j.saa.2021.120785
Wang BY, Gu CX, Jiao Y, Gao YF, Liu XN, Guo JM, Qian TW (2023) Novel preparation of red fluorescent carbon dots for tetracycline sensing and its application in trace determination. Talanta 253:123975. https://doi.org/10.1016/j.talanta.2022.123975
Ma YY, Tian ZM, Zhai WF, Qu Y (2022) Insights on catalytic mechanism of CeO2 as multiple nanozymes. Nano Res 15:10328–10342. https://doi.org/10.1007/s12274-022-4666-y
He C, Ke ZY, Liu K, Peng JS, Yang QH, Wang LX, Feng GF, Fang J (2023) Nanozyme-based dual-signal sensing system for colorimetric and photothermal detection of AChE activity in the blood of liver-injured mice. Anal Bioanal Chem 415:2655–2664. https://doi.org/10.1007/s00216-023-04663-1
Kim S, Han J, Chung H, Choi YK, Hashkavayi AB, Zhou Y, Park KS (2021) Pyrophosphate-enhanced oxidase activity of Cerium Oxide nanoparticles for Colorimetric detection of nucleic acids. Sensors-Basel. https://doi.org/10.3390/s21227567
Shen Y, Wei Y, Gao X, Nie C, Wang J, Wu Y (2023) Engineering an enzymatic cascade catalytic smartphone-based sensor for onsite visual ratiometric fluorescence-colorimetric dual-mode detection of methyl mercaptan. Environ Sci Technol 57:1680–1691. https://doi.org/10.1021/acs.est.2c07899
Pan L, Li XZ, Zhang QP, Xu SH, Yang L, Yang F, Jiang CL (2022) A boric acid functional multi-emission metal organic frameworks-based fluorescence sensing platform for visualization of gallic acid. Chem Eng J 450:138283. https://doi.org/10.1016/j.cej.2022.138283
Yang ZY, Luo SL, Zeng YP, Shi CM, Li R (2017) Albumin-mediated biomineralization of shape-controllable and biocompatible Ceria nanomaterials. Acs Appl Mater Inter 9:6839–6848. https://doi.org/10.1021/acsami.6b15442
Ding L, Zhao Y, Li H, Zhang Q, Yang W, Fu B, Pan Q (2021) A highly selective ratiometric fluorescent probe for doxycycline based on the sensitization effect of bovine serum albumin. J Hazard Mater 416:125759. https://doi.org/10.1016/j.jhazmat.2021.125759
Liang YQ, Wu XY, Zeng JY, Wu YN, Lai JP, Sun H (2022) A novel fluorescence ratio probe based on dual-emission carbon dots for highly selective and sensitive detection of chlortetracycline and cell imaging. Anal Bioanal Chem 414:3043–3055. https://doi.org/10.1007/s00216-022-03908-9
Lin BX, Zhang TY, Xin XL, Wu D, Huang Y, Liu YW, Cao YJ, Guo ML, Yu Y (2019) Europium(III) modified silicone nanoparticles for ultrasensitive visual determination of tetracyclines by employing a fluorescence color switch. Microchim Acta 186:442. https://doi.org/10.1007/s00604-019-3557-8
Ps PJ, Tharayil NJ (2020) Crystal plane effect on antioxidant efficacy of nanoceria synthesized with assistance of DNA. J Phys Chem Solids 141:109421. https://doi.org/10.1016/j.jpcs.2020.109421
Zhang YL, Mehedi Hassan M, Rong YW, Liu R, Li HH, Ouyang Q, Chen QS (2022) An upconversion nanosensor for rapid and sensitive detection of tetracycline in food based on magnetic-field-assisted separation. Food Chem 373:131497. https://doi.org/10.1016/j.foodchem.2021.131497
Mousavizadegan M, Hosseini M, Sheikholeslami MN, Hamidipanah Y, Reza Ganjali M (2023) Smartphone image analysis-based fluorescence detection of tetracycline using machine learning. Food Chem 403:134364. https://doi.org/10.1016/j.foodchem.2022.134364
Zhang HF, Zhou Q, Han X, Li M, Yuan J, Wei R, Zhang XF, Wu MY, Zhao W (2021) Nitrogen-doped carbon dots derived from hawthorn for the rapid determination of chlortetracycline in pork samples. Spectrochim Acta Mol Biomol Spectrosc 255:119736. https://doi.org/10.1016/j.saa.2021.119736
Bhattacharjee S, Chakraborty T, Bhaumik A (2022) A Ce-MOF as an alkaline phosphatase mimic: Ce-OH2 sites in catalytic dephosphorylation. Inorg Chem Front 9:5735–5744. https://doi.org/10.1039/D2QI01443B
Qi HJ, Teng M, Liu M, Liu SX, Li J, Yu HP, Teng CB, Huang ZH, Hu L, Qian S, Ahmad U, Tao D, Qiang G, Hu GZ (2019) Biomass-derived nitrogen-doped carbon quantum dots: highly selective fluorescent probe for detecting Fe (3+) ions and tetracyclines. J Colloid Interf Sci 539:332–341. https://doi.org/10.1016/j.jcis.2018.12.047
Zhang M, Yu HM, Tang XD, Zhu XH, Deng SP, Chen W (2022) Multifunctional Carbon dots-based fluorescence detection for Sudan I, Sudan IV and Tetracycline Hydrochloride in Foods. Nanomaterials-Basel 12:4166. https://doi.org/10.3390/nano12234166
Fan YJ, Wang ZG, Su M, Liu XT, Shen SG, Dong JX (2023) A dual-signal fluorescent colorimetric tetracyclines sensor based on multicolor carbon dots as probes and smartphone-assisted visual assay. Anal Chim Acta 1247:340843. https://doi.org/10.1016/j.aca.2023.340843
Fan Y, Qiao WJ, Long WJ, Chen HY, Fu HY, Zhou CS, She YB (2022) Detection of tetracycline antibiotics using fluorescent turn-off sensor based on S, N-doped carbon quantum dots. Spectrochim Acta Mol Biomol Spectrosc 274:121033. https://doi.org/10.1016/j.saa.2022.121033
Zhang LX, Zhong H, Zhang H, Ding CF (2021) A multifunctional nano system based on DNA and CeO2 for intracellular imaging of miRNA and enhancing photodynamic therapy. Talanta 221:121554. https://doi.org/10.1016/j.talanta.2020.121554
Liu Y, Liu BW, Huang PC, Wu FY, Ma LH (2021) Concentration-dependent photoluminescence carbon dots for visual recognition and detection of three tetracyclines. Anal Bioanal Chem 413:2565–2575. https://doi.org/10.1007/s00216-021-03221-x
Che HC, Nie YL, Tian XK, Li Y (2023) New method for morphological identification and simultaneous quantification of multiple tetracyclines by a white fluorescent probe. J Hazard Mater 441:129956. https://doi.org/10.1016/j.jhazmat.2022.129956
Jia YC, Cheng Z, Wang GH, Shuang SM, Zhou YH, Dong C, Du FF (2023) Nitrogen doped biomass derived carbon dots as a fluorescence dual-mode sensing platform for detection of tetracyclines in biological and food samples. Food Chem 402:134245. https://doi.org/10.1016/j.foodchem.2022.134245
Wang CY, Huang GL, Luo XL, Tang WZ, Yue TL, Li ZH (2022) Construction of ratiometric fluorescence sensor and test strip with smartphone based on dual-emission carbon dots for the specific detection of chlortetracycline. Anal Bioanal Chem 414:8143–8154. https://doi.org/10.1007/s00216-022-04349-0
Liu J, Wang TF, Wang ZL, Zou X, Wang WJ, Zhang SL, Gong ZJ (2021) Ratiometric fluorescent probe for tetracycline detection based on waste printing paper. Luminescence 36:1553–1560. https://doi.org/10.1002/bio.4100
Fu Q, Long CC, Qin LF, Jiang ZX, Qing TP, Zhang P, Feng B (2021) Fluorescent and colorimetric dual-mode detection of tetracycline in wastewater based on heteroatoms-doped reduced state carbon dots. Environ Pollut 283:117109. https://doi.org/10.1016/j.envpol.2021.117109
Liu L, Chen Q, Lv J, Li YP, Wang KC, Li JR (2022) Stable metal–Organic frameworks for fluorescent detection of Tetracycline Antibiotics. Inorg Chem 61:8015–8021. https://doi.org/10.1021/acs.inorgchem.2c00754
Funding
This research was supported by the National Natural Science Foundation of China (No. 82173571), and Postgraduate Research & Practice Innovation Program of Jiangsu Province (JX10314198).
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Qianji Li: Data curation, Formal analysis, Investigation, Methodology, Validation, Visualization, Writing-original draft. Pengfei Fan: Data curation, Formal analysis, Methodology, Validation. Zejia Hao: Visualization, Formal analysis. Shanhong Ni: Formal analysis. Qian Wu: Formal analysis. Lei Li: Conceptualization, Funding acquisition, Resources, Supervision, Project administration, Writing-review & editing.
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Li, Q., Fan, P., Hao, Z. et al. Fluorimetric determination of tetracycline antibiotics in animal derived foods using boron and nitrogen co-doped ceria-based nanoparticles. Microchim Acta 191, 147 (2024). https://doi.org/10.1007/s00604-024-06214-6
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DOI: https://doi.org/10.1007/s00604-024-06214-6