Abstract
Graphitic carbon nitride (g-C3N4) materials with a layered structure have unusual physicochemical properties. Herein it was shown that g-C3N4 quantum dots (QDs) obtained through a thermal-chemical etching route exhibited attractive upconversion and electrochemiluminescence (ECL) properties. After modification on nanoporous gold (NPG) with a sponge-like porous structure, g-C3N4 QDs were employed to fabricate an ECL sensor for the determination of Pb2+ using target - dependent DNAzyme as the recognition unit. Moreover, magnetic reduced graphene oxide nanosheets (rGO) attached with Fe3O4 nanoparticles (rGO-Fe3O4) were obtained via a one-pot in situ reduction approach, and used as carriers of DNAzyme. To make full use of the unique magnetic property the prepared rGO-Fe3O4, a flow injection ECL detecting cell was designed using indium tin oxide (ITO) glass as working electrode. Due to the unique separation and enrichment properties of magnetic Fe3O4-rGO materials as well as wire-like conductivity of NPG, high sensitivity and selectivity for the determination of Pb2+ in real water samples were achieved. This indicates that g-C3N4 has excellent anodic ECL performance in the presence of triethanolamine, and could be applied in real environmental samples analyses.
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References
Zang Y, Lei J, Hao Q, Ju H. “Signal-on” photoelectrochemical sensing strategy based on target dependent aptamer conformational conversion for selective detection of lead(II) ion. ACS Appl Mater Interfaces. 2014;6:15991–7.
Dong Y, Tian W, Ren S, Dai R, Chi Y, Chen G. Graphene quantum dots/l-cysteine coreactant electrochemiluminescence system and its application in sensing lead(II) ions. ACS Appl Mater Interfaces. 2014;6:1646–51.
Xu H, Xu P, Gao S, Zhang S, Zhao X, Fan C, et al. Highly sensitive recognition of Pb2+ using Pb2+ triggered exonuclease aided DNA recycling. Biosens Bioelectron. 2013;47:520–3.
Chen J, Zhou X, Zeng L. Enzyme-free strip biosensor for amplified detection of Pb2+ based on a catalytic DNA circuit. Chem Commun. 2013;49:984–6.
Un H, Huang C, Huang J, Huang C, Jia T, Xu L. A naphthalimide-based fluorescence “Turn-On” probe for the detection of Pb2+ in aqueous solution and living cells. Chem Asian J. 2014;9:3397–402.
Shi X, Gu W, Peng W, Li B, Chen N, Zhao K, et al. Sensitive Pb2+ probe based on the fluorescence quenching by graphene oxide and enhancement of the leaching of gold nanoparticles. ACS Appl Mater Interfaces. 2014;6:2568–75.
Xu H, Zhan S, Zhang D, Xia B, Zhan X, Wang L, et al. A label-free fluorescent sensor for the detection of Pb2+ and Hg2+. Anal Methods. 2015;7:6260–5.
Kuo SY, Li HH, Wu PJ, Chen CP, Huang YC, Chan YH. Dual colorimetric and fluorescent sensor based on semiconducting polymer dots for ratiometric detection of lead ions in living cells. Anal Chem. 2015;87:4765–71.
Zhu J, Yu Y, Li J, Zhao J. Colorimetric detection of lead (II) ions based on accelerating surface etching of gold nanorods to nanospheres: the effect of sodium thiosulfate. RSC Adv. 2016. doi:10.1039/C5RA26560F.
Pelossof G, Tel-Vered R, Willner I. Amplified surface plasmon resonance and electrochemical detection of Pb2+ ions using the Pb2+-dependent DNAzyme and hemin/G-quadruplex as a label. Anal Chem. 2012;84:3703–9.
Xia H, Li L, Yin Z, Hou X, Zhu JJ. Biobar-coded gold nanoparticles and DNAzyme-based dual signal amplification strategy for ultrasensitive detection of protein by electrochemiluminescence. ACS Appl Mater Interfaces. 2015;7:696–703.
Liu Z, Qi W, Xu G. Recent advances in electrochemiluminescence. Chem Soc Rev. 2015;44:3117–42.
He Y, Huang G, Jiang J, Zhang Q, Cui H. Preparation and electrochemiluminescent and photoluminescent properties of a graphene oxide colloid. Carbon. 2013;56:201–7.
Zhang Y, Dai W, Liu F, Li L, Li M, Ge S, et al. Ultrasensitive electrochemiluminescent immunosensor based on dual signal amplification strategy of gold nanoparticles-dotted graphene composites and CdTe quantum dots coated silica nanoparticles. Anal Bioanal Chem. 2013;405:4921–9.
Zhang Y, Liu W, Ge S, Yan M, Wang S, Yu J, et al. Multiplexed sandwich immunoassays using flow-injection electrochemiluminescence with designed substrate spatial-resolved technique for detection of tumor markers. Biosens Bioelectron. 2013;41:684–90.
Zhou M, Roovers J, Robertson GP, Grover CP. Multilabeling biomolecules at a single site. 1. Synthesis and characterization of a dendritic label for electrochemiluminescence assays. Anal Chem. 2003;75:6708–17.
Derfus AM, Chan WCW, Bhatia SN. Probing the cytotoxicity of semiconductor quantum dots. Nano Lett. 2004;4:11–8.
Chen L, Zeng X, Si P, Chen Y, Chi Y, Kim DH, et al. Gold nanoparticle-graphite-like C3N4 nanosheet nanohybrids used for electrochemiluminescent immunosensor. Anal Chem. 2014;86:4188–95.
Cheng C, Huang Y, Wang J, Zheng B, Yuan H, Xiao D. Anodic electrogenerated chemiluminescence behavior of graphite-like carbon nitride and its sensing for rutin. Anal Chem. 2013;85:2601–5.
Wang YZ, Hao N, Feng QM, Shi HW, Xu JJ, Chen HY. A ratiometric electrochemiluminescence detection for cancer cells using g-C3N4 nanosheets and Ag–PAMAM–luminol nanocomposites. Biosens Bioelectron. 2016;77:76–82.
Lu Q, Zhang J, Liu X, Wu Y, Yuan R, Chen S. Enhanced electrochemiluminescence sensor for detecting dopamine based on gold nanoflower@graphitic carbon nitride polymer nanosheet-polyaniline hybrids. Analyst. 2014;139:6556–62.
Shen B, Zhai W, Tao M, Ling J, Zheng W. Lightweight, multifunctional polyetherimide/graphene@Fe3O4 composite foams for shielding of electromagnetic pollution. ACS Appl Mater Interfaces. 2013;5:11383–91.
Tang J, Tang D, Niessner R, Chen G, Knopp D. Magneto-controlled graphene immunosensing platform for simultaneous multiplexed electrochemical immunoassay using distinguishable signal tags. Anal Chem. 2011;83:5407–14.
Li YR, Liu Q, Hong Z, Wang HF. Magnetic separation-assistant fluorescence resonance energy transfer inhibition for highly sensitive probing of nucleolin. Anal Chem. 2015;87:12183–9.
Liu W, Zhang Y, Ge S, Song X, Huang J, Yan M, et al. Core-shell Fe3O4-Au magnetic nanoparticles based nonenzymatic ultrasensitive electrochemiluminescence immunosensor using quantum dots functionalized graphene sheet as labels. Anal Chim Acta. 2013;770:132–9.
Gu W, Deng X, Gu X, Jia X, Lou B, Zhang X, et al. Stabilized, superparamagnetic functionalized graphene/Fe3O4@Au nanocomposites for a magnetically-controlled solid-state electrochemiluminescence biosensing application. Anal Chem. 2015;87:1876–81.
Han F, Jiang H, Fang D, Jiang D. Potential-resolved electrochemiluminescence for determination of two antigens at the cell surface. Anal Chem. 2014;86:6896–902.
Duan H, Xu C. Low-temperature CO oxidation over unsupported nanoporous gold catalysts with active or inert oxide residues. J Catal. 2015;332:31–7.
Xu C, Wang L, Mu X, Ding Y. Nanoporous PtRu alloys for electrocatalysis. Langmuir. 2010;26:7437–43.
Zhang X, Du B, Wu D, Ma H, Zhang Y, Li H, et al. Signal amplification strategy of triple-layered core–shell Au@Pd@Pt nanoparticles for ultrasensitive immunoassay detection of squamous cell carcinoma antigen. J Biomed Nanotechnol. 2015;11:245–52.
He H, Gao C. Supraparamagnetic, conductive, and processable multifunctional graphene nanosheets coated with high-density Fe3O4 nanoparticles. ACS Appl Mater Interfaces. 2010;2:3201–10.
Zhang Y, Su M, Ge L, Ge S, Yu J, Song X. Synthesis and characterization of graphene nanosheets attached to spiky MnO2 nanospheres and its application in ultrasensitive immunoassay. Carbon. 2013;57:22–33.
Zhang S, Li J, Zeng M, Zhao G, Xu J, Hu W, et al. In situ synthesis of water-soluble magnetic graphitic carbon nitride photocatalyst and its synergistic catalytic performance. ACS Appl Mater Interfaces. 2013;5:12735–43.
Wang W, Yu JC, Shen Z, Chan DKL, Gu T. g-C3N4 quantum dots: direct synthesis, up-conversion properties, and photocatalytic application. Chem Commun. 2014;50:10148–50.
Shen J, Zhu Y, Chen C, Yang X, Li C. Facile preparation and up-conversion luminescence of graphene quantum dots. Chem Commun. 2011;47:2580–2.
Wang X, Maeda K, Thomas A, Takanabe K, Xin G, Carlsson JM, et al. A metal-free polymeric photocatalyst for hydrogen production from water under visible light. Nat Mater. 2009;8:76–80.
Yin XB, Sha BB, Zhang XH, He XW, Xie H. The factors affecting the electrochemiluminescence of tris(2,2′-bipyridyl) ruthenium (II)/tertiary amines. Electroanalysis. 2008;20:1085–91.
Bruce D, Richter MM. Green electrochemiluminescence from ortho-metalated tris(2-phenylpyridine)iridium(III). Anal Chem. 2002;74:1340–2.
Tang S, Lu W, Gu F, Tong P, Yan Z, Zhang L. A novel electrochemical sensor for lead ion based on cascade DNA and quantum dots amplification. Electrochim Acta. 2014;134:1–7.
Zhang B, Lu L, Hu Q, Huang F, Lin Z. ZnO nan flower-based photoelectrochemical DNAzyme sensor for the detection of Pb2+. Biosens Bioelectron. 2014;56:243–9.
Wang HB, Wang L, Huang KJ, Xu SP, Wang HQ, Wanga LL, et al. A highly sensitive and selective biosensing strategy for the detection of Pb2+ ions based on GR-5 DNAzyme functionalized AuNPs. New J Chem. 2013;37:2557–63.
Ma F, Sun B, Qi H, Zhang H, Gao Q, Zhang C. A signal-on electrogenerated chemiluminescent biosensor for lead ion based on DNAzyme. Anal Chim Acta. 2011;683:234–41.
Hai H, Yang F, Li J. Electrochemiluminescence sensor using quantum dots based on a G-quadruplex aptamer for the detection of Pb2+. RSC Adv. 2013;3:13144–8.
Wang H, Chen Q, Tan Z, Yin X, Wang L. Electrochemiluminescence of CdTe quantum dots capped with glutathione and thioglycolic acid and its sensing of Pb2+. Electrochim Acta. 2012;72:28–31.
Acknowledgments
This work was financially supported by the Special Fund for Shandong Independent Innovation and Achievements Transformation (2014ZZCX02703), National High-tech R&D Program (863 Program) (SQ2015AAJY1562), and National Natural Science Foundation of China (21575051).
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Published in the topical collection Analytical Electrochemiluminescence with guest editors Hua Cui, Francesco Paolucci, Neso Sojic, and Guobao Xu.
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Zhang, Y., Zhang, L., Kong, Q. et al. Electrochemiluminescence of graphitic carbon nitride and its application in ultrasensitive detection of lead(II) ions. Anal Bioanal Chem 408, 7181–7191 (2016). https://doi.org/10.1007/s00216-016-9718-2
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DOI: https://doi.org/10.1007/s00216-016-9718-2