Fully integrated graphene electronic biosensor for label-free detection of lead (II) ion based on G-quadruplex structure-switching.

This work presents a fully integrated graphene field-effect transistor (GFET) biosensor for the label-free detection of lead ions (Pb2+) in aqueous-media, which first implements the G-quadruplex structure-switching biosensing principle in graphene nanoelectronics. We experimentally illustrate the biomolecular interplay that G-rich DNA single-strands with one-end confined on graphene surface can specifically interact with Pb2+ ions and switch into G-quadruplex structures. Since the structure-switching of electrically charged DNA strands can disrupt the charge distribution in the vicinity of graphene surface, the carrier equilibrium in graphene sheet might be altered, and manifested by the conductivity variation of GFET. The experimental data and theoretical analysis show that our devices are capable of the label-free and specific quantification of Pb2+ with a detection limit down to 163.7ng/L. These results first verify the signaling principle competency of G-quadruplex structure-switching in graphene electronic biosensors. Combining with the advantages of the compact device structure and convenient electrical signal, a label-free GFET biosensor for Pb2+ monitoring is enabled with promising application potential.

[1]  Mitchell B. Lerner,et al.  Detecting Lyme disease using antibody-functionalized single-walled carbon nanotube transistors. , 2013, Biosensors & bioelectronics.

[2]  Yunfeng Shi,et al.  Wetting transparency of graphene. , 2012, Nature materials.

[3]  Michael Kumpf,et al.  Total internal reflectance fluorescence (TIRF) biosensor for environmental monitoring of testosterone with commercially available immunochemistry: antibody characterization, assay development and real sample measurements. , 2006, Talanta.

[4]  Wei Yang,et al.  Peroxidase activity-structure relationship of the intermolecular four-stranded G-quadruplex-hemin complexes and their application in Hg2+ ion detection. , 2009, Talanta.

[5]  V. Kanický,et al.  Diode laser thermal vaporization ICP MS with a simple tubular cell for determination of lead and cadmium in whole blood , 2014 .

[6]  B. Welz,et al.  Determination of lead in biomass and products of the pyrolysis process by direct solid or liquid sample analysis using HR-CS GF AAS. , 2016, Talanta.

[7]  Colin Nuckolls,et al.  Debye screening in single-molecule carbon nanotube field-effect sensors. , 2011, Nano letters.

[8]  Lain-Jong Li,et al.  Label-free detection of DNA hybridization using transistors based on CVD grown graphene. , 2013, Biosensors & bioelectronics.

[9]  Kexin Xu,et al.  A graphene-based affinity nanosensor for detection of low-charge and low-molecular-weight molecules. , 2016, Nanoscale.

[10]  Tao Li,et al.  Potassium-lead-switched G-quadruplexes: a new class of DNA logic gates. , 2009, Journal of the American Chemical Society.

[11]  Judit Zsuga,et al.  The Hill equation and the origin of quantitative pharmacology , 2012 .

[12]  Y. Ohno,et al.  Chemical and biological sensing applications based on graphene field-effect transistors. , 2010, Biosensors & bioelectronics.

[13]  Xiaohong Zhou,et al.  Triple functional DNA-protein conjugates: Signal probes for Pb(2+) using evanescent wave-induced emission. , 2015, Biosensors & bioelectronics.

[14]  Feng Yan,et al.  Solution‐Gated Graphene Transistors for Chemical and Biological Sensors , 2014, Advanced healthcare materials.

[15]  Guojun Zhang,et al.  Gold nanoparticles-decorated graphene field-effect transistor biosensor for femtomolar MicroRNA detection. , 2015, Biosensors & bioelectronics.

[16]  A mesofluidic platform integrating restricted access-like sorptive microextraction as a front end to ICP-AES for the determination of trace level concentrations of lead and cadmium as contaminants in honey , 2016 .

[17]  Matthew R. Leyden,et al.  Scalable graphene field-effect sensors for specific protein detection , 2013, Nanotechnology.

[18]  Itamar Willner,et al.  DNA-based machines. , 2006, Organic & biomolecular chemistry.

[19]  Guonan Chen,et al.  A G-quadruplex based label-free fluorescent biosensor for lead ion. , 2012, Biosensors & bioelectronics.

[20]  M. Hepel,et al.  Effect of buried potential barrier in label-less electrochemical immunodetection of glutathione and glutathione-capped gold nanoparticles. , 2011, Biosensors & bioelectronics.

[21]  Tao Li,et al.  A lead(II)-driven DNA molecular device for turn-on fluorescence detection of lead(II) ion with high selectivity and sensitivity. , 2010, Journal of the American Chemical Society.

[22]  C. Nuckolls,et al.  A solid dielectric gated graphene nanosensor in electrolyte solutions. , 2015, Applied physics letters.

[23]  M. Hepel,et al.  Ligand exchange effects in gold nanoparticle assembly induced by oxidative stress biomarkers: homocysteine and cysteine. , 2010, Biophysical chemistry.

[24]  D. Yoon,et al.  Flexible glucose sensor using CVD-grown graphene-based field effect transistor. , 2012, Biosensors & bioelectronics.

[25]  M. Hepel.  Functional Gold Nanoparticles for Biointerfaces , 2012 .

[26]  Y. Ohno,et al.  Label-free biosensors based on aptamer-modified graphene field-effect transistors. , 2010, Journal of the American Chemical Society.

[27]  M. Hepel,et al.  Assembly of Gold Nanoparticles Induced by Metal Ions , 2012 .

[28]  J. Herrera,et al.  Role of Pb(II) defects in the mechanism of dissolution of plattnerite (β-PbO2) in water under depleting chlorine conditions. , 2014, Environmental science & technology.

[29]  Jing Hong,et al.  Statistical method for determining and comparing limits of detection of bioassays. , 2015, Analytical chemistry.

[30]  Guohua Liu,et al.  An aptameric graphene nanosensor for label-free detection of small-molecule biomarkers. , 2015, Biosensors & bioelectronics.

[31]  Zhiyong Zhang,et al.  Ultrasensitive label-free detection of PNA-DNA hybridization by reduced graphene oxide field-effect transistor biosensor. , 2014, ACS nano.

[32]  Qiyuan He,et al.  Real-time DNA detection using Pt nanoparticle-decorated reduced graphene oxide field-effect transistors. , 2012, Nanoscale.

[33]  E. Williams,et al.  Charged Impurity Scattering in Graphene , 2007, 0708.2408.

[34]  Stephan Gekle,et al.  Dielectric profile of interfacial water and its effect on double-layer capacitance. , 2011, Physical review letters.

[35]  Miao He,et al.  Practical, highly sensitive, and regenerable evanescent-wave biosensor for detection of Hg(2+) and Pb(2+) in water. , 2016, Biosensors & bioelectronics.

[36]  J. Homola.  Surface plasmon resonance sensors for detection of chemical and biological species. , 2008, Chemical reviews.

[37]  James N. Weiss.  The Hill equation revisited: uses and misuses , 1997, FASEB journal : official publication of the Federation of American Societies for Experimental Biology.

[38]  John E. Snawder,et al.  Comparison of a Multiplexed Fluorescent Covalent Microsphere Immunoassay and an Enzyme-Linked Immunosorbent Assay for Measurement of Human Immunoglobulin G Antibodies to Anthrax Toxins , 2004, Clinical Diagnostic Laboratory Immunology.

[39]  S. Neidle,et al.  G‐quadruplexes as therapeutic targets , 2000, Biopolymers.

[40]  A. Geim,et al.  Two-dimensional gas of massless Dirac fermions in graphene , 2005, Nature.

[41]  A. Wilson,et al.  DIFFICULTIES WITH DETERMINING THE DETECTION LIMIT WITH NONLINEAR CALIBRATION CURVES IN SPECTROMETRY , 1976 .

[42]  Stephen Neidle,et al.  Crystal structure of parallel quadruplexes from human telomeric DNA , 2002, Nature.

[43]  K. Novoselov,et al.  Effect of a high-kappa environment on charge carrier mobility in graphene. , 2008, Physical review letters.

[44]  Zhenzhen Lin,et al.  Pb2+ induced DNA conformational switch from hairpin to G-quadruplex: electrochemical detection of Pb2+. , 2011, The Analyst.

[45]  M. He,et al.  High‐κ Solid‐Gate Transistor Configured Graphene Biosensor with Fully Integrated Structure and Enhanced Sensitivity , 2016 .

[46]  Juewen Liu,et al.  Functional nucleic acid sensors. , 2009, Chemical reviews.

[47]  G. Stotzky.  Persistence and Biological Activity in Soil of Insecticidal Proteins from Bacillus thuringiensis and of Bacterial DNA Bound on Clays and Humic Acids , 2000 .