Abstract
A novel label-free photoelectrochemical biosensing method for highly sensitive and specific detection of DNA hybridization using a CdS quantum dot (QD)–dendrimer nanocomposite is presented. A molecular beacon (MB) was assembled on a gold-nanoparticle-modified indium tin oxide electrode surface. Hybridization to a complementary target DNA disrupts the stem–loop structure of the MB, which was afterward labeled with the QD–dendrimer nanocomposite. The modified indium tin oxide electrode showed a stable anodic photocurrent response at 300 mV (vs Ag/AgCl) to light excitation at 410 nm in the presence of 0.1 M ascorbic acid as an electron donor. The protocol developed integrates the specificity of an MB for molecular recognition and the advantages of gold nanoparticles for increasing the loading capacity of the MB on the electrode surface and accelerating the electron transfer. Moreover, the photocurrent was greatly enhanced because of the high loading of QDs by the dendrimer, which eliminated the surface defects of CdS QDs and prevented recombination of their photogenerated electron–hole pairs. Under the optimal conditions, a linear relationship between the increase of photocurrent and target DNA concentration was obtained in the range from 1 fM to 0.1 nM, with a detection limit of 0.5 fM. The sequence-specificity experiment showed that one or three mismatches of DNA bases could be discriminated. This photoelectrochemical method is a prospective technique for DNA hybridization detection because of its great advantages: label-free, high sensitivity and specificity, low cost, and easy fabrication. This could create a new platform for the application of CdS QD–dendrimer nanocomposites in photoelectrochemical bioanalysis.
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References
Lazcka O, Del Campo FJ, Munoz FX. Pathogen detection: a perspective of traditional methods and biosensors. Biosens Bioelectron. 2007;22:1205–17.
Palchetti I, Mascini M. Nucleic acid biosensors for environmental pollution monitoring. Analyst. 2008;133:846–54.
Chang HX, Yuan Y, Shi NL, Guan YF. Electrochemical DNA biosensor based on conducting polyaniline nanotube array. Anal Chem. 2007;79:5111–5.
Gore MR, Szalai VA, Ropp PA, Yang IV, Silverman JS, Thorp HH. Detection of attomole quantities [correction of quantitites] of DNA targets on gold microelectrodes by electrocatalytic nucleobase oxidation. Anal Chem. 2003;75:6586–92.
Divsar F, Ju HX. Electrochemiluminescence detection of near single DNA molecules by using quantum dots–dendrimer nanocomposites for signal amplification. Chem Commun. 2011;47:9879–81.
Kim HY, Kane MD, Kim S, Dominguez W, Applegate BM, Savikhin S. A molecular beacon DNA microarray system for rapid detection of E. coli O157:H7 that eliminates the risk of a false negative signal. Biosens Bioelectron. 2007;22:1041–7.
Wu ZS, Jiang JH, Fu L, Shen GL, Yu RQ. Optical detection of DNA hybridization based on fluorescence quenching of tagged oligonucleotide probes by gold nanoparticles. Anal Biochem. 2006;353:22–9.
Wang HB, Ou LJ, Huang KJ, Wen XG, Wang LL, Liu YM. A sensitive biosensing strategy for DNA detection based on graphene oxide and T7 exonuclease assisted target recycling amplification. Can J Chem. 2013;91:1266–71.
Elghanian R, Storhoff JJ, Mucic RC, Letsinger RL, Mirkin CA. Selective colorimetric detection of polynucleotides based on the distance-dependent optical properties of gold nanoparticles. Science. 1997;277:1078–81.
Storhoff JJ, Elghanian R, Mucic RC, Mirkin CA, Letsinger RL. One-pot colorimetric differentiation of polynucleotides with single base imperfections using gold nanoparticle probes. J Am Chem Soc. 1998;120:1959–64.
Ananthanawat C, Vilaivan T, Mekboonsonglarp W, Hoven VP. Thiolated pyrrolidinyl peptide nucleic acids for the detection of DNA hybridization using surface plasmon resonance. Biosens Bioelectron. 2009;24:3544–9.
Liu S, Li C, Cheng J, Zhou Y. Selective photoelectrochemical detection of DNA with high-affinity metallointercalator and tin oxide nanoparticle electrode. Anal Chem. 2006;78:4722–6.
Wang GL, Yu PP, Xu JJ, Chen HY. A label-free photoelectrochemical immunosensor based on water-soluble Cds quantum dots. J Phys Chem C. 2009;113:11142–8.
Ikeda A, Nakasu M, Ogasawara S, Nakanishi H, Nakamura M, Kikuchi JI. Photoelectrochemical sensor with porphyrin-deposited electrodes for determination of nucleotides in water. Org Lett. 2009;11:1163–6.
Lu W, Wang G, Jin Y, Yao X, Hu JQ, Li JH. Label-free photoelectrochemical strategy for hairpin DNA hybridization detection on titanium dioxide electrode. Appl Phys Lett. 2006;89:263902.
Lu W, Jin Y, Wang G, Chen D, Li JH. Enhanced photoelectrochemical method for linear DNA hybridization detection using Au-nanopaticle labeled DNA as probe onto titanium dioxide electrode. Biosens Bioelectron. 2008;23:1534–9.
Tokudome H, Yamada Y, Sonezaki S, Ishikawa H, Bekki M, Kanehira K, et al. Photoelectrochemical deoxyribonucleic acid sensing on a nanostructured TiO2 electrode. Appl Phys Lett. 2005;87:213901.
Willner I, Patolsky F, Wasserman J. Photoelectrochemistry with controlled DNA-cross-linked CdS nanoparticle arrays. Angew Chem. 2001;113:1913–6.
Wang GL, Xu JJ, Chen HY. Progress in the studies of photoelectrochemical sensors. Sci China Ser B. 2009;52:1789–800.
Wang B, Dong YX, Wang YL, Cao JT, Ma SH, Liu YM. Quenching effect of exciton energy transfer from CdS:Mn to Au nanoparticles: a highly efficient photoelectrochemical strategy for microRNA-21 detection. Sensors Actuators B Chem. 2018;254:159–65.
Fan GC, Zhu H, Du D, Zhang J, Zhu JJ, Lin Y. Enhanced photoelectrochemical immunosensing platform based on CdSeTe@CdS:Mn core-shell quantum dots sensitized TiO2 amplified by CuS nanocrystals conjugated signal antibodies. Anal Chem. 2016;88:3392–9.
Dong YX, Cao JT, Wang B, Ma SH, Liu YM. Exciton−plasmon interactions between CdS@g-C3N4 heterojunction and Au@Ag nanoparticles coupled with DNAase-triggered signal amplification: Toward highly sensitive photoelectrochemical bioanalysis of microRNA. ACS Sustain Chem Eng. 2017;5:10840–8.
Dastan D, Panahi SL, Chaure NB. Characterization of titania thin films grown by dip-coating technique. J Mater Sci Mater Electron. 2016;27:12291–6.
Dastan D, Panahi SL, Yengntiwar AP, Banpurkar AG. Morphological and electrical studies of titania powder and films grown by aqueous solution method. Adv Sci Lett. 2016;22:950–3.
Panahi SL, Dastan D, Chaure NB. Characterization of zirconia nanoparticles grown by sol-gel method. Adv Sci Lett. 2016;22:941–4.
Nasr C, Hotchandani S, Kim WY, Schmehl RH, Kamat PV. Photoelectrochemistry of composite semiconductor thin films. Photosensitization of SnO2/CdS coupled nanocrystallites with a ruthenium polypyridyl complex. J Phys Chem B. 1997;101:7480–7.
Shen Q, Ayuzawa Y, Katayama K, Sawada T, Toyoda T. Separation of ultrafast photoexcited electron and hole dynamics in CdSe quantum dots adsorbed onto nanostructured TiO2 films. Appl Phys Lett. 2010;97:263113.
Zhao WW, Yu PP, Xu JJ, Chen HY. Ultrasensitive photoelectrochemical biosensing based on biocatalytic deposition. Electrochem Commun. 2011;13:495–7.
Sheeney-Haj-Ichia L, Pogorelova S, Gofer Y, Willner I. Enhanced photoelectrochemistry in CdS/Au nanoparticle bilayers. Adv Funct Mater. 2004;14:416–24.
Sheeney-Haj-Ichia L, Basnar B, Willner I. Efficient generation of photocurrents by using CdS/carbon nanotube assemblies on electrodes. Angew Chem Int Ed. 2005;44:78–83.
Zhang X, Li S, Jin X, Zhang S. A new photoelectrochemical aptasensor for the detection of thrombin based on functionalized graphene and CdSe nanoparticles multilayers. Chem Commun. 2011;47:4929–31.
Kongkanand A, Domínguez RM, Kamat PV. Single wall carbon nanotube scaffolds for photoelectrochemical solar cells. Capture and transport of photogenerated electrons. Nano Lett. 2007;7:676–80.
Gill R, Zayats M, Willner I. Semiconductor quantum dots for bioanalysis. Angew Chem Int Ed. 2008;47:7602–25.
Tu WW, Dong Y, Lei JP, Ju HX. Low-potential photoelectrochemical biosensing using porphyrin-functionalized TiO2 nanoparticles. Anal Chem. 2010;82:8711–6.
Dastan D, Chaure N, Kartha M. Surfactants assisted solvothermal derived titania nanoparticles: synthesis and simulation. J Mater Sci Mater Electron. 2017;28:7784–96.
Dastan D. Effect of preparation methods on the properties of titania nanoparticles: solvothermal versus sol-gel. Appl Phys A Mater Sci Process. 2017;123:1–13.
Dastan D, Banpurkar A. Solution processable sol-gel derived titania gate dielectric for organic field effect transistors. J Mater Sci Mater Electron. 2016;28:3851–9.
Qian Z, Bai HJ, Wang GL, Xu JJ, Chen HY. A photoelectrochemical sensor based on CdS-polyamidoamine nanocomposite film for cell capture and detection. Biosens Bioelectron. 2010;25:2045–50.
Grabar KC, Freeman RG, Hommer MB, Natan MJ. Preparation and characterization of Au colloid monolayers. Anal Chem. 1995;67:735–43.
Priyam A, Chatterjee A, Das SK, Saha A. Synthesis and spectral studies of cysteine-capped CdS nanoparticles. Res Chem Intermed. 2005;31:691–702.
Jin YJ, Luo YJ, Li GP, Li J, Wang YF, Yang RQ, et al. Application of photoluminescent CdS/PAMAM nanocomposites in fingerprint detection. Forensic Sci Int. 2008;179:34–8.
Murray CB, Norris DJ, Bawendi MG. Synthesis and characterization of nearly monodisperse CdE (E = sulfur, selenium, tellurium) semiconductor nanocrystallites. J Am Chem Soc. 1993;115:8706–15.
Yu WW, Qu LH, Guo WZ, Peng XG. Experimental determination of the extinction coefficient of CdTe, CdSe, and CdS nanocrystals. Chem Mater. 2003;15:2854–60.
Zhang CX, O’Brien S, Balogh L. Comparison and stability of CdSe nanocrystals covered with amphiphilic poly(amidoamine) dendrimers. J Phys Chem B. 2002;106:10316–21.
Qingwen L, Guoan L, Jun F, Dawen C, Qi O. Photoelectrochemistry as a novel strategy for DNA hybridization detection. Analyst. 2000;125:1908–10.
Street RA, Qi P, Lujan R, Wong WS. Reflectivity of disordered silicon nanowires. Appl Phys Lett. 2008;93:163109.
Gao Z, Tansil NC. An ultrasensitive photoelectrochemical nucleic acid biosensor. Nucleic Acids Res. 2005;33:e123.
Zhang X, Zhao Y, Zhou H, Qu B. A new strategy for photoelectrochemical DNA biosensor using chemiluminescence reaction as light source. Biosens Bioelectron. 2011;26:2737–41.
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Divsar, F. A label-free photoelectrochemical DNA biosensor using a quantum dot–dendrimer nanocomposite. Anal Bioanal Chem 411, 6867–6875 (2019). https://doi.org/10.1007/s00216-019-02058-9
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DOI: https://doi.org/10.1007/s00216-019-02058-9