Reusable fluorescence nanoprobe based on DNA-functionalized metal-organic framework for ratiometric detection of mercury (II) ions.
Shenghua Li, Jianhui Pi, Yingjie Huang, Yong Li, Hongliang Tan
Author Information
Shenghua Li: Key Laboratory of Research and Utilization of Ethnomedicinal Plant Resources of Hunan Province, College of Biological and Food Engineering, Huaihua University, Huaihua, 418008, P. R. China.
Jianhui Pi: Key Laboratory of Research and Utilization of Ethnomedicinal Plant Resources of Hunan Province, College of Biological and Food Engineering, Huaihua University, Huaihua, 418008, P. R. China. pijh817@126.com.
Yingjie Huang: Jiangxi Provincial Key Laboratory of Natural and Biomimetic Drugs Research, College of Chemistry and Materials, Jiangxi Normal University, Nanchang, 330022, P. R. China.
Yong Li: Jiangxi Provincial Key Laboratory of Natural and Biomimetic Drugs Research, College of Chemistry and Materials, Jiangxi Normal University, Nanchang, 330022, P. R. China.
Hongliang Tan: Key Laboratory of Research and Utilization of Ethnomedicinal Plant Resources of Hunan Province, College of Biological and Food Engineering, Huaihua University, Huaihua, 418008, P. R. China. hltan@jxnu.edu.cn.
A reusable fluorescent nanoprobe was developed using DNA-functionalized metal-organic framework (MOF) for ratiometric detection of Hg. We utilized a zirconium-based MOF (UiO-66) to encapsulate tris(bipyridine) ruthenium(II) chloride (Ru(bpy)), resulting in Ru(bpy)@UiO-66 (RU) with red fluorescence. The unsaturated metal sites in UiO-66 facilitate the attachment of thymine-rich single-strand DNA (T-ssDNA) through Zr-O-P bond, producing T-ssDNA-functionalized RU complex (RUT). The T-ssDNA selectively binds to Hg, forming stable T-Hg-T base pairs and folding into double-stranded DNA, which permits the intercalation of SYBR Green I (SGI) and activates its green fluorescence. In the presence of Hg, SGI fluorescence increases in a dose-dependent manner, while Ru(bpy) fluorescence remains constant. This fluorescence contrast enables RUT to serve as an effective ratiometric nanoprobe for Hg detection, with a detection limit of 3.37 nM. Additionally, RUT demonstrates exceptional reusability due to the ability of cysteine to remove Hg, given its stronger affinity for thiol groups. The RUT was successfully applied to detect Hg in real water samples. This work advances the development of ratiometric fluorescence nanoprobe based on DNA-functionalized MOFs.
Jiménez-Moreno M, Barre JPG, Perrot V, Bérail S, Rodríguez Martín-Doimeadios RC, Amouroux D (2016) Sources and fate of mercury pollution in Almadén mining district (Spain): evidences from mercury isotopic compositions in sediments and lichens. Chemosphere 147:430–438
[PMID: 26774309]
Campbell L, Dixon DG, Hecky RE (2003) Review of mercury in lake wictoria, east africa: implications for human and ecosystem health. J Toxicol Environ Health, Part B 6:325–356
Zalups RK (2000) Molecular interactions with mercury in the kidney. Pharmacol Rev 52:113–144
[PMID: 10699157]
Nolan EM, Lippard SJ (2008) Tools and tactics for the optical detection of mercuric ion. Chem Rev 108:3443–3480
[PMID: 18652512]
Louie H, Wong C, Huang YJ, Fredrickson S (2012) A study of techniques for the preservation of mercury and other trace elements in water for analysis by inductively coupled plasma mass spectrometry (ICP-MS). Anal Methods 4:522–529
Ghaedi M, Reza Fathi M, Shokrollahi A, Shajarat F (2006) Highly selective and sensitive preconcentration of mercury ion and determination by cold vapor atomic absorption spectroscopy. Anal Lett 39:1171–1185
Huang YL, Gao ZF, Jia J, Luo HQ, Li NB (2016) A label-free electrochemical sensor for detection of mercury(II) ions based on the direct growth of guanine nanowire. J Hazard Mater 308:173–178
[PMID: 26835893]
Li T, Dong S, Wang E (2009) Label-free colorimetric detection of aqueous mercury ion (Hg) using Hg-modulated G-quadruplex-based DNAzymes. Anal Chem 81:2144–2149
[PMID: 19227981]
Yang Y-K, Yook K-J, Tae J (2005) A rhodamine-based fluorescent and colorimetric chemodosimeter for the rapid detection of Hg ions in aqueous media. J Am Chem Soc 127:16760–16761
[PMID: 16316202]
Wu Y, Jiang T, Wu Z, Yu R (2018) Novel ratiometric surface-enhanced raman spectroscopy aptasensor for sensitive and reproducible sensing of Hg. Biosens Bioelectron 99:646–652
[PMID: 28843197]
Huang X, Song J, Yung BC, Huang X, Xiong Y, Chen X (2018) Ratiometric optical nanoprobes enable accurate molecular detection and imaging. Chem Soc Rev 47:2873–2920
[PMID: 29568836]
Li T, Tuo Y, Hao Y, Pang J, Tian M, Rokhum SL, Zhang F, Chai F (2024) Carbon dot-based ratiometric fluorescent probe platform for visual quantitative determination of Hg. ACS Appl Nano Mater 7:1509–1518
Xie H, Dong J, Duan J, Waterhouse GIN, Hou J, Ai S (2018) Visual and ratiometric fluorescence detection of Hg2+ based on a dual-emission carbon dots-gold nanoclusters nanohybrid. Sens Actuators B-Chem 259:1082–1089
Yang C, Li Y, Wu N, Zhang Y, Feng W, Yu M, Li Z (2021) Ratiometric upconversion luminescence nanoprobes for quick sensing of Hg and cells imaging. Sens Actuators B-Chem 326:128841
Simon-Yarza T, Mielcarek A, Couvreur P, Serre C (2018) Nanoparticles of metal-organic frameworks: on the road to in vivo efficacy in biomedicine. Adv Mater 30:1707365
Fan W, Zhang X, Kang Z, Liu X, Sun D (2021) Isoreticular chemistry within metal-organic frameworks for gas storage and separation. Coord Chem Rev 443:213968
Wang Q, Astruc D (2020) State of the art and prospects in metal-organic framework (MOF)-based and MOF-derived nanocatalysis. Chem Rev 120:1438–1511
[PMID: 31246430]
Ma W, Jiang Q, Yu P, Yang L, Mao L (2013) Zeolitic imidazolate framework-based electrochemical biosensor for in vivo electrochemical measurements. Anal Chem 85:7550–7557
[PMID: 23815314]
Mallakpour S, Nikkhoo E, Hussain CM (2022) Application of MOF materials as drug delivery systems for cancer therapy and dermal treatment. Coord Chem Rev 451:214262
Lyu F, Zhang Y, Zare RN, Ge J, Liu Z (2014) One-pot synthesis of protein-embedded metal-organic frameworks with enhanced biological activities. Nano Lett 14:5761–5765
[PMID: 25211437]
Luo F, Lin Y, Zheng L, Lin X, Chi Y (2015) Encapsulation of hemin in meta-organic frameworks for catalyzing the chemiluminescence reaction of the HO-luminol system and detecting glucose in the neutral condition. ACS Appl Mater Interfaces 7:11322–11329
[PMID: 25928385]
Fang C, Deng Z, Cao G, Chu Q, Wu Y, Li X, Peng X, Han G (2020) Co-ferrocene MOF/glucose oxidase as cascade nanozyme for effective tumor therapy. Adv Funct Mater 30:1910085
Gao J, Wang C, Tan H (2017) Dual-emissive polystyrene@zeolitic imidazolate framework-8 composite for ratiometric detection of singlet oxygen. J Mater Chem B 5:9175–9182
[PMID: 32264599]
Lin X, Gao G, Zheng L, Chi Y, Chen G (2014) Encapsulation of strongly fluorescent carbon quantum dots in metal-organic frameworks for enhancing chemical sensing. Anal Chem 86:1223–1228
[PMID: 24328057]
Zhang X, Zeng Y, Zheng A, Cai Z, Huang A, Zeng J, Liu X, Liu J (2017) A fluorescence based immunoassay for galectin-4 using gold nanoclusters and a composite consisting of glucose oxidase and a metal-organic framework. Microchim Acta 184:1933–1940
Yan S, Deng D, Zhang L, Lv Y (2019) Fluorescence nano metal organic frameworks modulated by encapsulation for construction of versatile biosensor. Talanta 201:96–103
[PMID: 31122467]
Wei X, Zheng L, Luo F, Lin Z, Guo L, Qiu B, Chen G (2013) Fluorescence biosensor for the H5N1 antibody based on a metal-organic framework platform. J Mater Chem B 1:1812–1817
[PMID: 32261146]
Wu L-L, Wang Z, Zhao S-N, Meng X, Song X-Z, Feng J, Song S-Y, Zhang H-J (2016) A metal-organic framework/DNA hybrid system as a novel fluorescent biosensor for mercury(II) ion detection. Chem Eur J 22:477–480
[PMID: 26555340]
Huang N-H, Li R-T, Fan C, Wu K-Y, Zhang Z, Chen J-X (2019) Rapid sequential detection of Hg and biothiols by a probe DNA-MOF hybrid sensory system. J Inorg Biochem 197:110690
[PMID: 31075721]
Liu S, Huo Y, Fan L, Ning B, Sun T, Gao Z (2022) Rapid and ultrasensitive detection of DNA and microRNA-21 using a zirconium porphyrin metal-organic framework-based switch fluorescence biosensor. Anal Chim Acta 1192:339340
[PMID: 35057960]
Xu J, Cui X, Wang L, Chen G, Ji S, Zhao S, Wang H, Luo Z, Zeng A, Fu Q (2024) DNA-functionalized MOF fluorescent probes for the enzyme-free and pretreatment-free detection of MicroRNA in serum. Talanta 275:126083
[PMID: 38636442]
Jia S-M, Liu X-F, Li P, Kong D-M, Shen H-X (2011) G-quadruplex DNAzyme-based Hg and cysteine sensors utilizing Hg2+-mediated oligonucleotide switching. Biosens Bioelectron 27:148–152
[PMID: 21775125]
Yang S, Guo Y, Fan J, Yang Y, Zuo C, Bai S, Sheng S, Li J, Xie G (2020) A fluorometric assay for rapid enrichment and determination of bacteria by using zirconium-metal organic frameworks as both capture surface and signal amplification tag. Microchim Acta 187:188
Han Q, Zhang D, Zhang R, Tang J, Xu K, Shao M, Li Y, Du P, Zhang R, Yang D, Zhang L, Lu X (2022) DNA-functionalized metal-organic framework ratiometric nanoprobe for MicroRNA detection and imaging in live cells. Sens Actuators B-Chem 361:131676
Zucchiatti P, Mitri E, Kenig S, Billè F, Kourousias G, Bedolla DE, Vaccari L (2016) Contribution of ribonucleic acid (RNA) to the Fourier transform infrared (FTIR) spectrum of eukaryotic cells. Anal Chem 88:12090–12098
[PMID: 28193045]
Momeni F, Khoshfetrat SM, Zarei K (2023) Electrochemical sandwich-type aptasensor based on the multifunctional catechol-loaded Au/MIL-53(Fe) for detection of cardiac troponin I. ACS Appl Nano Mater 6:19239–19248
Vitzthum F, Geiger G, Bisswanger H, Brunner H, Bernhagen J (1999) A quantitative fluorescence-based microplate assay for the determination of double-stranded DNA using SYBR Green I and a standard ultraviolet transilluminator gel imaging system. Anal Biochem 276:59–64
[PMID: 10585744]
Zipper H, Brunner H, Bernhagen J, Vitzthum F (2004) Investigations on DNA intercalation and surface binding by SYBR Green I, its structure determination and methodological implications. Nucleic Acids Res 32:e103–e103
[PMID: 15249599]
Cosa G, Focsaneanu K-S, McLean JRN, McNamee JP, Scaiano JC (2001) Photophysical properties of fluorescent DNA-dyes bound to single- and double-stranded DNA in aqueous buffered solution. Photochem Photobiol 73:585–599
[PMID: 11421063]
Tan H, Zhang Y, Chen Y (2011) Detection of mercury ions (Hg) in urine using a terbium chelate fluorescent probe. Sens Actuators B-Chem 156:120–125
Xu X-Y, Yan B (2016) Fabrication and application of a ratiometric and colorimetric fluorescent probe for Hg based on dual-emissive metal–organic framework hybrids with carbon dots and Eu. J Mater Chem C 4:1543–1549
Zhang Z, Wu Y, He S, Xu Y, Li G, Ye B (2018) Ratiometric fluorescence sensing of mercuric ion based on dye-doped lanthanide coordination polymer particles. Anal Chim Acta 1014:85–90
[PMID: 29523256]
Zhang X, Li Y, Su H, Zhang S (2010) Highly sensitive and selective detection of Hg using mismatched DNA and a molecular light switch complex in aqueous solution. Biosens Bioelectron 25:1338–1343
[PMID: 19926467]
Ye B-C, Yin B-C (2008) Highly sensitive detection of mercury(II) ions by fluorescence polarization enhanced by gold nanoparticles. Angew Chem Int Ed 47:8386–8389
Tan H, Chen Y (2012) Detection of biothiols in cells by a terbium chelate-Hg (II) system. J Biomed Opt 17:017001–017008
[PMID: 22352667]
Wang Y-W, Tang S, Yang H-H, Song H (2016) A novel colorimetric assay for rapid detection of cysteine and Hg based on gold clusters. Talanta 146:71–74
[PMID: 26695236]
Khoshfetrat SM, Fasihi K, Moradnia F, Kamil Zaidan H, Sanchooli E (2023) A label-free multicolor colorimetric and fluorescence dual mode biosensing of HIV-1 DNA based on the bifunctional NiFeO@UiO-66 nanozyme. Anal Chim Acta 1252:341073
[PMID: 36935160]
Grants
22064011/National Natural Science Foundation of China
22064011/National Natural Science Foundation of China
22064011/National Natural Science Foundation of China
22064011/National Natural Science Foundation of China
22064011/National Natural Science Foundation of China
20202ACB205003/Natural Science Foundation of Jiangxi Province