DNA nanostructure-decorated surfaces for enhanced aptamer-target binding and electrochemical cocaine sensors.

The sensitivity of aptamer-based electrochemical sensors is often limited by restricted target accessibility and surface-induced perturbation of the aptamer structure, which arise from imperfect packing of probes on the heterogeneous and locally crowded surface. In this study, we have developed an ultrasensitive and highly selective electrochemical aptamer-based cocaine sensor (EACS), based on a DNA nanotechnology-based sensing platform. We have found that the electrode surface decorated with an aptamer probe-pendant tetrahedral DNA nanostructure greatly facilitates cocaine-induced fusion of the split anticocaine aptamer. This novel design leads to a sensitive cocaine sensor with a remarkably low detection limit of 33 nM. It is also important that the tetrahedra-decorated surface is protein-resistant, which not only suits the enzyme-based signal amplification scheme employed in this work, but ensures high selectivity of this sensor when deployed in sera or other adulterated samples.

[1]  Yi Lu,et al.  Quantum dot encoding of aptamer-linked nanostructures for one-pot simultaneous detection of multiple analytes. , 2007, Analytical chemistry.

[2]  Kevin W Plaxco,et al.  High specificity, electrochemical sandwich assays based on single aptamer sequences and suitable for the direct detection of small-molecule targets in blood and other complex matrices. , 2009, Journal of the American Chemical Society.

[3]  Michael Famulok,et al.  Functional aptamers and aptazymes in biotechnology, diagnostics, and therapy. , 2007, Chemical reviews.

[4]  Xinrui Duan,et al.  An engineered riboswitch as a potential gene-regulatory platform for reducing antibacterial drug resistance. , 2011, Chemical communications.

[5]  Guo-Li Shen,et al.  Fluorescence aptameric sensor for strand displacement amplification detection of cocaine. , 2010, Analytical chemistry.

[6]  Chunhai Fan,et al.  Visual cocaine detection with gold nanoparticles and rationally engineered aptamer structures. , 2008, Small.

[7]  Itamar Willner,et al.  Spotlighting of cocaine by an autonomous aptamer-based machine. , 2007, Journal of the American Chemical Society.

[8]  A. Heeger,et al.  An electronic, aptamer-based small-molecule sensor for the rapid, label-free detection of cocaine in adulterated samples and biological fluids. , 2006, Journal of the American Chemical Society.

[9]  Yingfu Li,et al.  DNA aptamer folding on gold nanoparticles: from colloid chemistry to biosensors. , 2008, Journal of the American Chemical Society.

[10]  Milan N Stojanovic,et al.  Aptamer-based colorimetric probe for cocaine. , 2002, Journal of the American Chemical Society.

[11]  S. Satija,et al.  Using Self-Assembly To Control the Structure of DNA Monolayers on Gold: A Neutron Reflectivity Study , 1998 .

[12]  N. Seeman,et al.  Design and self-assembly of two-dimensional DNA crystals , 1998, Nature.

[13]  Russell P. Goodman,et al.  Rapid Chiral Assembly of Rigid DNA Building Blocks for Molecular Nanofabrication , 2005, Science.

[14]  J F Van Bocxlaer,et al.  Analysis of cocaine, benzoylecgonine, and cocaethylene in urine by HPLC with diode array detection. , 1996, Analytical chemistry.

[15]  Kevin W Plaxco,et al.  A reagentless signal-on architecture for electronic, aptamer-based sensors via target-induced strand displacement. , 2005, Journal of the American Chemical Society.

[16]  Kevin W Plaxco,et al.  Biosensors based on binding-modulated donor-acceptor distances. , 2005, Trends in biotechnology.

[17]  S. Clavijo,et al.  Analysis of cocaine and benzoylecgonine in urine by using multisyringe flow injection analysis-gas chromatography-mass spectrometry system. , 2010, Journal of separation science.

[18]  N K Mello,et al.  Management of cocaine abuse and dependence. , 1996, The New England journal of medicine.

[19]  Hao Yan,et al.  Nucleic Acid Nanotechnology , 2004, Science.

[20]  M. Stojanović,et al.  Aptamer-based folding fluorescent sensor for cocaine. , 2001, Journal of the American Chemical Society.

[21]  Chun-Yang Zhang,et al.  Single quantum-dot-based aptameric nanosensor for cocaine. , 2009, Analytical chemistry.

[22]  Chunhai Fan,et al.  Design of an oligonucleotide-incorporated nonfouling surface and its application in electrochemical DNA sensors for highly sensitive and sequence-specific detection of target DNA. , 2008, Analytical chemistry.

[23]  I. Buryakov,et al.  Express analysis of explosives, chemical warfare agents and drugs with multicapillary column gas chromatography and ion mobility increment spectrometry. , 2004, Journal of chromatography. B, Analytical technologies in the biomedical and life sciences.

[24]  Hao Yan,et al.  In vivo cloning of artificial DNA nanostructures , 2008, Proceedings of the National Academy of Sciences.

[25]  Arica A Lubin,et al.  Continuous, real-time monitoring of cocaine in undiluted blood serum via a microfluidic, electrochemical aptamer-based sensor. , 2009, Journal of the American Chemical Society.

[26]  P. Gong,et al.  DNA surface hybridization: comparison of theory and experiment. , 2010, The journal of physical chemistry. B.

[27]  R. Breaker DNA aptamers and DNA enzymes. , 1997, Current opinion in chemical biology.

[28]  Y. Wan,et al.  An enzyme-based E-DNA sensor for sequence-specific detection of femtomolar DNA targets. , 2008, Journal of the American Chemical Society.

[29]  Weihong Tan,et al.  Aptamer-based microfluidic device for enrichment, sorting, and detection of multiple cancer cells. , 2009, Analytical chemistry.

[30]  Xiwen He,et al.  Tetrahedron-structured DNA and functional oligonucleotide for construction of an electrochemical DNA-based biosensor. , 2011, Chemical communications.

[31]  Juewen Liu,et al.  Fast colorimetric sensing of adenosine and cocaine based on a general sensor design involving aptamers and nanoparticles. , 2005, Angewandte Chemie.

[32]  Ming Zhou,et al.  Solid-state probe based electrochemical aptasensor for cocaine: a potentially convenient, sensitive, repeatable, and integrated sensing platform for drugs. , 2010, Analytical chemistry.

[33]  L. Cerchia,et al.  Targeting cancer cells with nucleic acid aptamers. , 2010, Trends in biotechnology.

[34]  Chunhai Fan,et al.  Electrochemical interrogation of conformational changes as a reagentless method for the sequence-specific detection of DNA , 2003, Proceedings of the National Academy of Sciences of the United States of America.

[35]  Ming Zhou,et al.  Microfluidic electrochemical aptameric assay integrated on-chip: a potentially convenient sensing platform for the amplified and multiplex analysis of small molecules. , 2011, Analytical chemistry.

[36]  N. Seeman DNA in a material world , 2003, Nature.

[37]  Xiaogang Qu,et al.  Sensitive, selective and label-free protein detection using a smart polymeric transducer and aptamer/ligand system. , 2009, Chemical communications.

[38]  Itamar Willner,et al.  Detection of single-base DNA mutations by enzyme-amplified electronic transduction , 2001, Nature Biotechnology.

[39]  T. G. Drummond,et al.  Electrochemical DNA sensors , 2003, Nature Biotechnology.

[40]  Itamar Willner,et al.  Supramolecular cocaine-aptamer complexes activate biocatalytic cascades. , 2009, Journal of the American Chemical Society.

[41]  J. Gooding,et al.  DNA recognition interfaces: the influence of interfacial design on the efficiency and kinetics of hybridization. , 2005, Langmuir : the ACS journal of surfaces and colloids.

[42]  C. Mao,et al.  Hierarchical self-assembly of DNA into symmetric supramolecular polyhedra , 2008, Nature.

[43]  Jian-hui Jiang,et al.  A new aptameric biosensor for cocaine based on surface-enhanced Raman scattering spectroscopy. , 2008, Chemistry.

[44]  J. Kjems,et al.  Self-assembly of a nanoscale DNA box with a controllable lid , 2009, Nature.

[45]  A DNA nanostructure for the functional assembly of chemical groups with tunable stoichiometry and defined nanoscale geometry. , 2009, Angewandte Chemie.

[46]  J. Szostak,et al.  In vitro selection of RNA molecules that bind specific ligands , 1990, Nature.

[47]  Hao Yan,et al.  A DNA Nanostructure‐based Biomolecular Probe Carrier Platform for Electrochemical Biosensing , 2010, Advanced materials.

[48]  Itamar Willner,et al.  Electrochemical, photoelectrochemical, and surface plasmon resonance detection of cocaine using supramolecular aptamer complexes and metallic or semiconductor nanoparticles. , 2009, Analytical chemistry.

[49]  Chunhai Fan,et al.  Regenerable electrochemical immunological sensing at DNA nanostructure-decorated gold surfaces. , 2011, Chemical communications.

[50]  P. Gong,et al.  DNA surface hybridization regimes , 2008, Proceedings of the National Academy of Sciences.

[51]  Hao Yan,et al.  Control of Self-Assembly of DNA Tubules Through Integration of Gold Nanoparticles , 2009, Science.

[52]  Yi Lu,et al.  Non-base pairing DNA provides a new dimension for controlling aptamer-linked nanoparticles and sensors. , 2007, Journal of the American Chemical Society.

[53]  Weihong Tan,et al.  DNA aptamer–micelle as an efficient detection/delivery vehicle toward cancer cells , 2009, Proceedings of the National Academy of Sciences.

[54]  Francesco Botrè,et al.  Rapid screening of drugs of abuse and their metabolites by gas chromatography/mass spectrometry: application to urinalysis. , 2005, Rapid communications in mass spectrometry : RCM.

[55]  M. Heller DNA microarray technology: devices, systems, and applications. , 2002, Annual review of biomedical engineering.

[56]  M. Estévez,et al.  Using aptamer-conjugated fluorescence resonance energy transfer nanoparticles for multiplexed cancer cell monitoring. , 2009, Analytical chemistry.

[57]  Hao Yan,et al.  Designer DNA nanoarchitectures. , 2009, Biochemistry.

[58]  Heloísa Maria Tristão,et al.  Voltammetric determination of cocaine in confiscated samples using a cobalt hexacyanoferrate film-modified electrode. , 2009, Forensic science international.

[59]  Xiaoling Zhang,et al.  An aptamer cross-linked hydrogel as a colorimetric platform for visual detection. , 2010, Angewandte Chemie.

[60]  Chunhai Fan,et al.  A gold nanoparticle-based chronocoulometric DNA sensor for amplified detection of DNA , 2007, Nature Protocols.

[61]  Siegfried Schneider,et al.  Combination of high-performance liquid chromatography and SERS detection applied to the analysis of drugs in human blood and urine , 2004 .