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Biomedical subjects

Itamar Willner

Publications and source records attributed to Itamar Willner.

104 records · Page 6Linked to original sources
PubMed2002

Integration of polyaniline/poly(acrylic acid) films and redox enzymes on electrode supports: an in situ electrochemical/surface plasmon resonance study of the bioelectrocatalyzed oxidation of glucose or lactate in the integrated bioelectrocatalytic systems.

Electropolymerization of aniline in the presence of poly(acrylic acid) on Au electrodes yields a polyaniline/poly(acrylic acid) composite film, exhibiting reversible redox functions in aqueous solutions at pH = 7.0. In situ electrochemical-SPR measurements are used to identify the dynamics of swelling and shrinking of the polymer film upon the oxidation of the polyaniline (PAn) to its oxidized state (PAn(2+)) and the reduction of the oxidized polymer (PAn(2+)) back to its reduced state (PAn), respectively. Covalent attachment of N(6)-(2-aminoethyl)-flavin adenin dinucleotide (amino-FAD, 1) to the carboxylic groups of the composite polyaniline/poly(acrylic acid) film followed by the reconstitution of apoglucose oxidase on the functional polymer yields an electrically contacted glucose oxidase of unprecedented electrical communication efficiency with the electrode: electron-transfer turnover rate approximately 1000 s(-1) at 30 degrees C. In situ electrochemical-SPR analyses are used to characterize the bioelectrocatalytic functions of the biomaterial-polymer interface. The current responses of the bioelectrocatalytic system increase as the glucose concentrations are elevated. Similarly, the SPR spectra of the system are controlled by the concentration of glucose. The glucose concentration controls the steady-state concentration ratio of PAn/PAn(2+) in the film composition. Therefore, the SPR spectrum of the film measured upon its electrochemical oxidation is shifted from the spectrum typical for the oxidized PAn(2+) at low glucose concentration to the spectrum characteristic of the reduced PAn at high glucose concentration. Similarly, the polyaniline/poly(acrylic acid) film acts as an electrocatalyst for the oxidation of NADH. Accordingly, an integrated bioelectrocatalytic assembly was constructed on the electrode by the covalent attachment of N(6)-(2-aminoethyl)-beta-nicotinamide adenine dinucleotide (amino-NAD(+), 2) to the polymer film, and the two-dimensional cross-linking of an affinity complex formed between lactate dehydrogenase and the NAD(+)-cofactor units associated with the polymer using glutaric dialdehyde as a cross-linker. In situ electrochemical-SPR measurements are used to characterize the bioelectrocatalytic functions of the system. The amperometric responses of the system increase as the concentrations of lactate are elevated, and an electron-transfer turnover rate of 350 s(-1) between the biocatalyst and the electrode is estimated. As the PAn(2+) oxidizes the NADH units generated by the biocatalyzed oxidation of lactate, the PAn/PAn(2+) steady-state ratio in the film is controlled by the concentration of lactate. Accordingly, the SPR spectrum measured upon electrochemical oxidation of the film is similar to the spectrum of PAn(2+) at low lactate concentration, whereas the SPR spectrum resembles that of PAn at high concentrations of lactate.

Acrylic Resins↗
PubMed2002

Self-assembled, helically stacked anionic aggregates of 2,5,8,11-tetra-tert-butylcycloocta[1,2,3,4-def;5,6,7,8-d'e'f']bisbiphenylene, stabilized by electrostatic interactions.

Tetraanions of alkyl-substituted derivatives of cycloocta[1,2,3,4-def;5,6,7,8-d'e'f']bisbiphenylene (BPD) and their counter lithium cations self-assemble to form helically stacked assemblies, including a dimer, a trimer, and a tetramer. NMR self-diffusion measurements and unprecedented magnetic shielding effects for the sandwiched lithium cations support their aggregated nature. The D(2)-tetramer assembly is fully characterized by NMR spectroscopy, providing unequivocal evidence for a helix of four tetraanionic BPD layers with an estimated relative twist angle of about 45 degrees and interlayer spacing of ca. 4 A. The barrier for racemization through the in-plane inter-deck rotation is DeltaG(200)= 9.5 +/- 0.2 kcal mol(-1) in the dimer compared to >15 kcal mol(-1) in the tetramer.

Journal Article↗
PubMed2002

Redox-active nucleic-acid replica for the amplified bioelectrocatalytic detection of viral DNA.

A new concept for the amplified electrochemical detection of the 7229-base viral DNA of M13phi is developed. A thiolated 27-base nucleic acid (1) is assembled on an Au-electrode. Hybridization between the sensing interface and the M13phi DNA is followed by the polymerase-induced replication of the analyte DNA in the presence of dCTP, dGTP, dATP, and ferrocene-tethered-dUTP (2). The generated redox-active replica mediates electron transfer between the enzyme glucose oxidase (GOx) and the electrode and activates the bioelectrocatalyzed oxidation of glucose. The bioelectrocatalyzed oxidation of glucose provides a biocatalytic amplification path for the formation of the redox-active replica. The electrochemical techniques to follow the replication and the bioelectrocatalytic amplification are differential pulse voltammetry and cyclic voltammetry. The electrical responses from the system relate to the bulk concentration of the M13phi DNA, thus enabling the quantitative analysis of the viral gene.

Catalysis↗
PubMed2002

Imprinting of nucleotide and monosaccharide recognition sites in acrylamidephenylboronic acid-acrylamide copolymer membranes associated with electronic transducers.

Molecular recognition sites for the nucleotides adenosine 5'-monophosphate (1), guanosine 5'-monophosphate (2), cytosine 5'-monophosphate (3), and uridine 5'-monophosphate (4) are imprinted in an acrylamide-acrylamidephenylboronic acid copolymer (5) membrane. The imprinted membranes are assembled on piezoelectric Au quartz crystals or Au electrodes via electropolymerization or on the gate surface of an ISFET device by radical polymerization. The imprinted membranes reveal selectivity toward the imprinted nucleotide, and the association of the respective nucleotides with the recognition sites is transduced by the following: (i) microgravimetric, quartz crystal microbalance (QCM) measurements; (ii) Faradaic impedance analyses, and (iii) potentiometric responses of the ISFET devices. While the microgravimetric QCM measurements reflect the swelling of the polymers upon the association of the nucleotides with the recognition sites, the ISFET response is due to the charging of the polymer membrane as a result of the formation of the nucleotide-boronate complex. The selective detection of the nucleotides may lead to new DNA/RNA sequencing methods. Also, specific recognition sites for beta-D(+)-glucose (6), D(+)-galactose (7), and beta-D(-)-fructose (8) were imprinted in an acrylamide-acrylamidephenylboronic acid copolymer (5) membrane associated with an ISFET device. Selective sensing of the respective monosaccharides is accomplished in the presence of the imprinted membrane-functionalized ISFET devices.

Acrylic Resins↗
PubMed2002

Functional biosensor systems via surface-nanoengineering of electronic elements.

Bioelectronics is a progressing interdisciplinary research field that involves the integration of biomaterials with electronic transducers such as electrodes, field-effect transistors or piezoelectric crystals. Surface engineering of biomaterials such as enzymes, antigen-antibodies or DNA on the electronic supports controls the electrical properties of the biomaterial/transducer interface and enables the electronic transduction of biorecognition events, or biocatalyzed transformation, on the transducers. The development of biosensor systems of tailored sensitivities and specificities represents a major advance in bioelectronics.

Antigen-Antibody Reactions↗
PubMed2002

Selective sensing of triazine herbicides in imprinted membranes using ion-sensitive field-effect transistors and microgravimetric quartz crystal microbalance measurements.

A series of triazine herbicides consisting of the chlorotriazine atranex (atrazine), (1), prozinex, (2), tyllanex, (3), simanex, (4) and the methylthiolated triazines ametrex, (5), prometrex, (6) and terbutex, (7), were imprinted in an acrylamide-methacrylate copolymer. The polymer was deposited on the gate surface of ion-sensitive field-effect transistors (ISFETs) and piezoelectric Au-quartz crystals. Selective sensing of the imprinted substrates was accomplished by the imprinted polymer membrane associated with the ISFETs and Au-quartz crystals. Binding of the substrates onto the imprinted polymer associated with the gate of the ISFET alters the electrical charge and potential of the gate interface, thus allowing the potentiometric transduction of the binding events. The association of the substrates with the imprinted membrane linked to the Au-quartz crystal results in the membrane swelling, thus enabling the microgravimetric quartz crystal microbalance assay of the substrate binding events. The specificity of the imprinted recognition sites is attributed to complementary H-bond and electrostatic interactions between the substrates and the acrylamide-methacrylic acid copolymer.

Electrochemistry↗
PubMed2001

Electronic Transduction of Polymerase or Reverse Transcriptase Induced Replication Processes on Surfaces: Highly Sensitive and Specific Detection of Viral Genomes Parts of this research are supported by the Israel Ministry of Science as an Infrastructure Project in Biomicroelectronics and as an Israel-Japan cooperation. M.K. acknowledges the support of the American Foundation for Aids Research, AmfAR (grant No. 02730-28-RG).

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Journal Article↗