A colorimetric nanobiosensor with enhanced sensitivity for detection of lead (II) in real-water samples via an adenine-cytosine mismatched DNAzyme
Jinchuan Liu, Hang Yang, Huanxing Li, Jiancheng Wang, Xiaohong Zhou
A colorimetric nanobiosensor with enhanced sensitivity for detection of lead (II) in real-water samples via an adenine-cytosine mismatched DNAzyme
● A colorimetric nanobiosensor with one-step was developed for Pb2+ detection.
● An A-C mismatched DNAzyme was designed to improve the sensitivity.
● The detection limit of 8.6 nmol/L was achieved for Pb2+.
● Satisfactory recoveries were achieved in various real water samples.
● An entire detection time was less than 30 min.
Facile and ultrasensitive detection of Pb2+ in water for remote or resource-limited environments remains challenging. DNAzyme-based colorimetric nanobiosensors have been extensively studied to regulate the assembly of functionalized gold nanoparticles (AuNPs). However, these nanobiosensors have been criticized for their low sensitivity owing to the difficulty of dissociating DNAzyme embedded in AuNP aggregates. To address this issue, we rationally designed a DNAzyme by introducing an adenine-cytosine (A-C) mismatch to strengthen the disassembly of DNAzyme-linked nanostructures. As proof of concept, a “turn on” colorimetric nanobiosensor integrated with mismatched DNAzyme and functionalized AuNPs was first developed for Pb2+ detection. Under the optimal detection conditions, the obtained typical calibration curve shows a detection limit of 8.6 nmol/L, with an approximately 11-fold sensitivity improvement in Pb2+ detection compared with unmismatched DNAzyme, and a linear response range from 10 to 300 nmol/L. This nanobiosensor demonstrated robust selectivity and satisfactory recovery rates between 86.5% and 106.4% for Pb2+ in spiked environmental water samples. Additionally, the detection process is user-friendly and can be completed within 30 min, requiring only a simple water sample addition step. Considering the extensive applications of DNAzyme in conjunction with nanoparticles, this study provides a valuable reference for designing other DNAzyme-powered nanoparticle assemblies in biosensing systems.
Trace lead(II) ions / Modified mismatched DNAzyme / Gold nanoparticles / Colorimetric nanobiosensor / Environmental water samples
[1] |
Allawi H T, SantaLucia J. (1998). Nearest-neighbor thermodynamics of internal A·C mismatches in DNA: sequence dependence and pH effects. Biochemistry, 37(26): 9435–9444
CrossRef
Google scholar
|
[2] |
Annadhasan M, Muthukumarasamyvel T, Sankar Babu V, Rajendiran N. (2014). Green synthesized silver and gold nanoparticles for colorimetric detection of Hg2+, Pb2+, and Mn2+ in aqueous medium. ACS Sustainable Chemistry & Engineering, 2(4): 887–896
CrossRef
Google scholar
|
[3] |
Breaker R R, Joyce G F. (1994). A DNA enzyme that cleaves RNA. Chemistry & Biology, 1(4): 223–229
CrossRef
Google scholar
|
[4] |
Brown A K, Li J, Pavot C M B, Lu Y. (2003). A lead-dependent DNAzyme with a two-step mechanism. Biochemistry, 42(23): 7152–7161
CrossRef
Google scholar
|
[5] |
Cairns M J, Hopkins T M, Witherington C, Sun L Q. (2000). The influence of arm length asymmetry and base substitution on the activity of the 10–23 DNA enzyme. Antisense & Nucleic Acid Drug Development, 10(5): 323–332
CrossRef
Google scholar
|
[6] |
Chen J, Zhang Y, Cheng M, Mergny J L, Lin Q, Zhou J, Ju H. (2019). Highly active G-quadruplex/hemin DNAzyme for sensitive colorimetric determination of lead (II). Microchimica Acta, 186(12): 786–794
CrossRef
Google scholar
|
[7] |
Chen J, Zhao J, Feng R, Ma H, Wang H, Ren X, Wei Q, Ju H. (2023). Competitive photoelectrochemical aptamer sensor based on a Z-scheme Fe2O3/g-C3N4 heterojunction for sensitive detection of lead ions. Journal of Hazardous Materials, 459: 132122
CrossRef
Google scholar
|
[8] |
Chen Y, Wu H, Qian S, Yu X, Chen H, Wu J. (2022). Applying CRISPR/Cas system as a signal enhancer for DNAzyme-based lead ion detection. Analytica Chimica Acta, 1192: 339356
CrossRef
Google scholar
|
[9] |
Cheng Z, Wei J, Gu L, Zou L, Wang T, Chen L, Li Y, Yang Y, Li P. (2022). DNAzyme-based biosensors for mercury (II) detection: Rational construction, advances and perspectives. Journal of Hazardous Materials, 431: 128606
CrossRef
Google scholar
|
[10] |
Cho H H, Jung D H, Heo J H, Lee C Y, Jeong S Y, Lee J H. (2023). Gold nanoparticles as exquisite colorimetric transducers for water pollutant detection. ACS Applied Materials & Interfaces, 15(16): 19785–19806
CrossRef
Google scholar
|
[11] |
Diao W, Wang G, Wang L, Zhang L, Ding S, Takarada T, Maeda M, Liang X. (2020). Opposite effects of flexible single-stranded DNA regions and rigid loops in DNAzyme on colloidal nanoparticle stability for “turn-on” plasmonic detection of lead ions. ACS Applied Bio Materials, 3(10): 7003–7010
CrossRef
Google scholar
|
[12] |
Dong Y, Lee A, Ban D K, Wang K, Bandaru P. (2023). Femtomolar level-specific detection of lead ions in aqueous environments, using aptamer-derivatized graphene field-effect transistors. ACS Applied Nano Materials, 6(3): 2228–2235
CrossRef
Google scholar
|
[13] |
Duan N, Li C, Song M, Wang Z, Zhu C, Wu S. (2022). Signal amplification of SiO2 nanoparticle loaded horseradish peroxidase for colorimetric detection of lead ions in water. Spectrochimica Acta. Part A: Molecular and Biomolecular Spectroscopy, 265: 120342
CrossRef
Google scholar
|
[14] |
Düzgün A, Maroto A, Mairal T, O’Sullivan C, Rius F X. (2010). Solid-contact potentiometric aptasensor based on aptamer functionalized carbon nanotubes for the direct determination of proteins. Analyst, 135(5): 1037–1041
CrossRef
Google scholar
|
[15] |
Ebrahimi-Najafabadi H, Pasdaran A, Rezaei Bezenjani R, Bozorgzadeh E. (2019). Determination of toxic heavy metals in rice samples using ultrasound assisted emulsification microextraction combined with inductively coupled plasma optical emission spectroscopy. Food Chemistry, 289: 26–32
CrossRef
Google scholar
|
[16] |
Hai X, Li Y, Zhu C, Song W, Cao J, Bi S. (2020). DNA-based label-free electrochemical biosensors: from principles to applications. Trends in Analytical Chemistry, 133: 116098
CrossRef
Google scholar
|
[17] |
HasanM N, Rijiravanich P, SurareungchaiW (2023). Label-free GR5 DNAzyme-based colorimetric sensing for lead ions (Pb2+) detection. AIP Conference Proceedings, Yogyakarta, AIP Publishing, 2720(1): 1–15
|
[18] |
Hu L, Fu X, Kong G, Yin Y, Meng H M, Ke G, Zhang X B. (2020). DNAzyme-gold nanoparticle-based probes for biosensing and bioimaging. Journal of Materials Chemistry. B, Materials for Biology and Medicine, 8(41): 9449–9465
CrossRef
Google scholar
|
[19] |
Ji R, Niu W, Chen S, Xu W, Ji X, Yuan L, Zhao H, Geng M, Qiu J, Li C. (2019). Target-inspired Pb2+-dependent DNAzyme for ultrasensitive electrochemical sensor based on MoS2-AuPt nanocomposites and hemin/G-quadruplex DNAzyme as signal amplifier. Biosensors & Bioelectronics, 144: 111560
CrossRef
Google scholar
|
[20] |
Kataria R, Sethuraman K, Vashisht D, Vashisht A, Mehta S K, Gupta A. (2019). Colorimetric detection of mercury ions based on anti-aggregation of gold nanoparticles using 3,5-dimethyl-1-thiocarboxamidepyrazole. Microchemical Journal, 148: 299–305
CrossRef
Google scholar
|
[21] |
Khan S, Burciu B, Filipe C D, Li Y, Dellinger K, Didar T F. (2021). DNAzyme-based biosensors: immobilization strategies, applications, and future prospective. ACS Nano, 15(9): 13943–13969
CrossRef
Google scholar
|
[22] |
Lan T, Furuya K, Lu Y. (2010). A highly selective lead sensor based on a classic lead DNAzyme. Chemical Communications, 46(22): 3896–3898
CrossRef
Google scholar
|
[23] |
Lee J H, Wang Z, Liu J, Lu Y. (2008). Highly sensitive and selective colorimetric sensors for uranyl (UO22+): Development and comparison of labeled and label-free DNAzyme-gold nanoparticle systems. Journal of the American Chemical Society, 130(43): 14217–14226
CrossRef
Google scholar
|
[24] |
Li L, Li B, Qi Y, Jin Y. (2009). Label-free aptamer-based colorimetric detection of mercury ions in aqueous media using unmodified gold nanoparticles as colorimetric probe. Analytical and Bioanalytical Chemistry, 393(8): 2051–2057
CrossRef
Google scholar
|
[25] |
Li X Y, Zhang M M, Zhou X D, Hu J M. (2021). A functional peptide-mediated colorimetric assay for mercury ion based on dual-modified gold nanoparticles. Analytical Biochemistry, 631: 114369
CrossRef
Google scholar
|
[26] |
Li Y, Sen D. (1997). Toward an efficient DNAzyme. Biochemistry, 36(18): 5589–5599
CrossRef
Google scholar
|
[27] |
Liu C, Chen Y, Zhao J, Wang Y, Shao Y, Gu Z, Li L, Zhao Y. (2021). Self-assembly of copper-DNAzyme nanohybrids for dual-catalytic tumor therapy. Angewandte Chemie, 133(26): 14445–14449
CrossRef
Google scholar
|
[28] |
Liu J, Lu Y. (2003). A colorimetric lead biosensor using DNAzyme-directed assembly of gold nanoparticles. Journal of the American Chemical Society, 125(22): 6642–6643
CrossRef
Google scholar
|
[29] |
Liu J, Lu Y. (2005). Stimuli-responsive disassembly of nanoparticle aggregates for light-up colorimetric sensing. Journal of the American Chemical Society, 127(36): 12677–12683
CrossRef
Google scholar
|
[30] |
Marguí E, Queralt I, De Almeida E. (2022). X-ray fluorescence spectrometry for environmental analysis: basic principles, instrumentation, applications and recent trends. Chemosphere, 303: 135006
CrossRef
Google scholar
|
[31] |
Memon A G, Xing Y, Zhou X, Wang R, Liu L, Zeng S, He M, Ma M. (2020). Ultrasensitive colorimetric aptasensor for Hg2+ detection using Exo-III assisted target recycling amplification and unmodified AuNPs as indicators. Journal of Hazardous Materials, 384: 120948
CrossRef
Google scholar
|
[32] |
Memon A G, Zhou X, Xing Y, Wang R, Liu L, Khan M, He M. (2019). Label-free colorimetric nanosensor with improved sensitivity for Pb2+ in water by using a truncated 8–17 DNAzyme. Frontiers of Environmental Science & Engineering, 13(1): 12
CrossRef
Google scholar
|
[33] |
Nagraj N, Liu J, Sterling S, Wu J, Lu Y. (2009). DNAzyme catalytic beacon sensors that resist temperature-dependent variations. Chemical Communications, 27: 4103–4105
CrossRef
Google scholar
|
[34] |
Niu X, Zhong Y, Chen R, Wang F, Liu Y, Luo D. (2018). A “turn-on” fluorescence sensor for Pb2+ detection based on graphene quantum dots and gold nanoparticles. Sensors and Actuators. B, Chemical, 255: 1577–1581
CrossRef
Google scholar
|
[35] |
Rajaji P, Panneerselvam P. (2020). A novel polydopamine grafted 3D MOF nanocubes mediated GR-5/GC DNAzyme complex with enhanced fluorescence emission response toward spontaneous detection of Pb(II) and Ag(I) ions. ACS Omega, 5(39): 25188–25198
CrossRef
Google scholar
|
[36] |
Ravikumar A, Panneerselvam P, Radhakrishnan K, Morad N, Anuradha C, Sivanesan S. (2017). DNAzyme based amplified biosensor on ultrasensitive fluorescence detection of Pb (II) ions from aqueous system. Journal of Fluorescence, 27(6): 2101–2109
CrossRef
Google scholar
|
[37] |
Saran R, Liu J. (2016). A comparison of two classic Pb2+-dependent RNA-cleaving DNAzymes. Inorganic Chemistry Frontiers, 3(4): 494–501
CrossRef
Google scholar
|
[38] |
Schubert S, GuÈl D C, Grunert H P, Zeichhardt H, Erdmann V A, Kurreck J. (2003). RNA cleaving ‘10–23’ DNAzymes with enhanced stability and activity. Nucleic Acids Research, 31(20): 5982–5992
CrossRef
Google scholar
|
[39] |
Song Y, Guo F, Zeng P, Liu J, Wang Y, Cheng H. (2022). Simultaneous measurements of Cr, Cd, Hg and Pb species in ng L-1 levels by interfacing high performance liquid chromatography and inductively coupled plasma mass spectrometry. Analytica Chimica Acta, 1212: 339935
CrossRef
Google scholar
|
[40] |
Suo L, Dong X, Gao X, Xu J, Huang Z, Ye J, Lu X, Zhao L. (2019). Silica-coated magnetic graphene oxide nanocomposite based magnetic solid phase extraction of trace amounts of heavy metals in water samples prior to determination by inductively coupled plasma mass spectrometry. Microchemical Journal, 149: 104039
CrossRef
Google scholar
|
[41] |
Tan Y, Qiu J, Cui M, Wei X, Zhao M, Qiu B, Chen G. (2016). An immobilization free DNAzyme based electrochemical biosensor for lead determination. Analyst, 141(3): 1121–1126
CrossRef
Google scholar
|
[42] |
Truong P L, Yin Y, Lee D, Ko S H. (2023). Advancement in COVID-19 detection using nanomaterial-based biosensors. Exploration, 3(1): 20210232
CrossRef
Google scholar
|
[43] |
Wang F, Dai J, Shi H, Luo X, Xiao L, Zhou C, Guo Y, Xiao D. (2020). A rapid and colorimetric biosensor based on GR-5 DNAzyme and self-replicating catalyzed hairpin assembly for lead detection. Analytical Methods, 12(17): 2215–2220
CrossRef
Google scholar
|
[44] |
Wang F, Zhang Y, Lu M, Du Y, Chen M, Meng S, Ji W, Sun C, Peng W. (2021a). Near-infrared band Gold nanoparticles-Au film “hot spot” model based label-free ultratrace lead (II) ions detection via fiber SPR DNAzyme biosensor. Sensors and Actuators. B, Chemical, 337: 129816
CrossRef
Google scholar
|
[45] |
Wang H, Liang A, Wen G, Jiang Z. (2021b). A simple SPR absorption method for ultratrace Pb2+ based on DNAzyme-COFPd nanocatalysis of Ni–P alloy reaction. Sensors and Actuators. B, Chemical, 330: 129381
CrossRef
Google scholar
|
[46] |
Wang Q, Wang Z, He Y, Xiong B, Li Y, Wang F. (2022). Chemical and structural modification of RNA-cleaving DNAzymes for efficient biosensing and biomedical applications. Trends in Analytical Chemistry, 159: 116910
|
[47] |
Wei H, Li B, Li J, Dong S, Wang E. (2008). DNAzyme-based colorimetric sensing of lead (Pb2+) using unmodified gold nanoparticle probes. Nanotechnology, 19(9): 095501
CrossRef
Google scholar
|
[48] |
Wu H, Wang S, Li S F Y, Bao Q, Xu Q. (2020). A label-free lead (II) ion sensor based on surface plasmon resonance and DNAzyme-gold nanoparticle conjugates. Analytical and Bioanalytical Chemistry, 412(27): 7525–7533
CrossRef
Google scholar
|
[49] |
Wu J, Wei S, Lu Y, Ren N, Bian X, Zhang J. (2018). Ultrasensitive DNAzyme-based electrochemical biosensor for Pb2+ based on FcHT-mediated biocatalytic amplification. International Journal of Electrochemical Science, 13(10): 9630–9641
CrossRef
Google scholar
|
[50] |
Xing Y, Xue B, Lin Y, Wu X, Fang F, Qi P, Guo J, Zhou X. (2022). A cellphone-based colorimetric multi-channel sensor for water environmental monitoring. Frontiers of Environmental Science & Engineering, 16(12): 155
|
[51] |
Xu J, Liu M, Zhao W, Wang S, Gui M, Li H, Yu R. (2022). DNAzyme-based cascade signal amplification strategy for highly sensitive detection of lead ions in the environment. Journal of Hazardous Materials, 429: 128347
CrossRef
Google scholar
|
[52] |
Yan W, Zhong Z, Ma J, Rujiralai T. (2021). Highly sensitive colorimetric sensing of copper(II) ions based on “CLICK-17” DNAzyme-catalyzed azide modified gold nanoparticles and alkyne capped dsDNA cycloaddition. RSC Advances, 11(39): 24196–24205
CrossRef
Google scholar
|
[53] |
Yang Y, Li W, Liu J. (2021). Review of recent progress on DNA-based biosensors for Pb2+ detection. Analytica Chimica Acta, 1147: 124–143
CrossRef
Google scholar
|
[54] |
Yim T J, Liu J, Lu Y, Kane R S, Dordick J S. (2005). Highly active and stable DNAzyme-carbon nanotube hybrids. Journal of the American Chemical Society, 127(35): 12200–12201
CrossRef
Google scholar
|
[55] |
Yu Y, Hong Y, Gao P, Nazeeruddin M K. (2016). Glutathione modified gold nanoparticles for sensitive colorimetric detection of Pb2+ ions in rainwater polluted by leaking perovskite solar cells. Analytical Chemistry, 88(24): 12316–12322
CrossRef
Google scholar
|
[56] |
Yu Z, Li N, Hu X, Dong Y, Lin Y, Cai H, Xie Z, Qu D, Li X. (2019). Highly efficient electrochemical detection of lead ion using metal-organic framework and graphene as platform based on DNAzyme. Synthetic Metals, 254: 164–171
CrossRef
Google scholar
|
[57] |
Zhang D, Yu X, Wu L, Jin H, Wei M. (2021). Ultrasensitive electrochemical detection of Pb2+ based on DNAzyme coupling with exonuclease III-assisted target recycling. Journal of Electroanalytical Chemistry, 882: 114960
CrossRef
Google scholar
|
[58] |
Zhang L, Huang D, Zhao P, Yue G, Yang L, Dan W. (2022). Colorimetric detection for uranyl ions in water using vinylphosphonic acid functionalized gold nanoparticles based on smartphone. Spectrochimica Acta. Part A: Molecular and Biomolecular Spectroscopy, 269: 120748
CrossRef
Google scholar
|
[59] |
Zhao Y, Yavari K, Wang Y, Pi K, Van Cappellen P, Liu J. (2022). Deployment of functional DNA-based biosensors for environmental water analysis. Trends in Analytical Chemistry, 153: 116639
CrossRef
Google scholar
|
[60] |
Zhou R, Hu C, Jin Y, Zhang J, Du H, Yang P, Chen J, Hou X, Cheng N. (2020). Spatially constrained DNA nanomachines to accelerate kinetics in response to external input: design and bioanalysis. Analytical Chemistry, 92(13): 8909–8916
CrossRef
Google scholar
|
[61] |
Zhu D, Pei H, Chao J, Su S, Aldalbahi A, Rahaman M, Wang L, Wang L, Huang W, Fan C.
CrossRef
Google scholar
|
[62] |
Zhu D, Song P, Shen J, Su S, Chao J, Aldalbahi A, Zhou Z, Song S, Fan C, Zuo X.
CrossRef
Google scholar
|
/
〈 | 〉 |