Integrated differential enzyme sensors using hydrogen and fluoride ion sensitive multigate FETs

doi:10.1016/0956-5663(90)85005-W

Biosensors and Bioelectronics

Volume 5, Issue 4, 1990, Pages 327-334

https://doi.org/10.1016/0956-5663(90)85005-W Get rights and content

Abstract

Enzyme field effect transistors (ENFETs) were assembled by immobilizing enzymes to a multigate proton and fluoride ion sensitive field effect transistor. All the six gates and two thin film noble metal electrodes (TFME) at the chip have been covered by crosslinked polyurethane entrapping the enzymes. Two variations of difference mode measurements of glucose have been realized. The difference of the output voltages of a pH-ENFET and a pF-reference FET (REFET) or the difference output voltages of a pF-ENFET based on a glucose oxidase/peroxidase-catalyzed reaction liberating fluoride ions and a pH-REFET are measured using the integrated TFME as pseudo-reference. Besides the convenient handling of the devices, the homogeneous coverage of the active area of the chip simplifies the construction and production of ENFETs.

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Simultaneous monitoring of glucose and lactate by an interference and cross-talk free dual electrode amperometric biosensor based on electropolymerized thin films
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An interference and cross-talk free dual electrode amperometric biosensor integrated with a microdialysis sampling system is described, for simultaneous monitoring of glucose and lactate by flow injection analysis. The biosensor is based on a conventional thin layer flow-through cell equipped with a Pt dual electrode (parallel configuration). Each Pt disk was modified by a composite bilayer consisting of an electrosynthesised overoxidized polypyrrole (PPYox) anti-interference membrane covered by an enzyme entrapping gel, obtained by glutaraldehyde co-crosslinking of glucose oxidase or lactate oxidase with bovine serum albumin. The advantages of covalent immobilization techniques were coupled with the excellent interference-rejection capabilities of PPYox. Ascorbate, cysteine, urate and paracetamol produced lactate or glucose bias in the low micromolar range; their responses were, however, completely suppressed when the sample was injected through the microdialysis unit. Under these operational conditions the flow injection responses for glucose and lactate were linear up to 100 and 20 mM with typical sensitivities of 9.9 (±0.1) and 7.2 (±0.1) nA/mM, respectively. The shelf-lifetime of the biosensor was at least 2 months. The potential of the described biosensor was demonstrated by the simultaneous determination of lactate and glucose in untreated tomato juice samples; results were in good agreement with those of a reference method.
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A gate surface of an ion-selective field-effect transistor was modified with a monolayer enzyme array that stimulates biocatalytic reactions that control the gate potential. Stepwise assemblage of the biocatalytic layer included primary silanization of the Al₂O₃-gate with 3-aminopropyltriethoxysilane, subsequent activation of the amino groups with glutaric dialdehyde and the covalent attachment of the enzyme to the functionalized gate surface. Urease, glucose oxidase, acetylcholine esterase and α-chymotrypsin were used to organize the biocatalytic matrices onto the chip gate. The resulting enzyme-based field-effect transistors, ENFETs, demonstrated capability to sense urea, glucose, acetylcholine and N-acetyl-l-tyrosine ethyl ester, respectively. The mechanism of the biosensing involves the alteration of the pH in the sensing layer by the biocatalytic reactions and the detection of the pH change by the ENFET. The major advantage of the enzyme-thin-layered FET devices as biosensors is the fast response-time (several tens of seconds) of these bioelectronic devices. This advantage over traditional thick-polymer-based ENFETs results from the low diffusion barrier for the substrate penetration to the biocatalytic active sites and minute isolation of the pH-sensitive gate surface from the bulk solution.
Chemical cross-talk in flow-type integrated enzyme sensors
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In flow-type integrated enzyme sensors, hydrogen peroxide produced at an upstream electrode is transported to downstream electrodes, and causes non-specific responses which are called as “chemical cross talks (CCTs)”. In this study, the relationship between CCTs and enzyme immobilization methods, namely an electrochemical pyrrole polymerization, a gelatin–glutaraldehyde crosslinking, and a photocrosslinkable prepolymer (PVA-SbQ) method, was investigated. The flow rate dependency and the substrate concentration dependency of CCTs were dependent on the enzyme immobilization methods. Therefore, the effects of the membrane permeability and enzyme density of bioselective layers on upstream and downstream electrodes, on CCT were investigated by using a gelatin–glutaraldehyde crosslinking method as an enzyme immobilization method. The CCTs correspond to the membrane permeability and enzyme density of a bioselective layer on an upstream electrode. Based on these results, an elimination method for CCT was proposed.
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The construction and electrochemical response characteristics of poly(vinyl chloride) matrix membrane sensors for fluorouracil are described. The membranes incorporate ion association complexes of fluorouracil anion with bathophenanthroline–nickel(II) [sensor 1], bathophenanthroline–iron(II) [sensor 2] and phenanthroline–iron(II) [sensor 3] as electroactive materials. These sensors show linear response for fluorouracil over the range 1.3–130 μg ml⁻¹, with anionic slopes of 29.0, 27.9 and 34.3 mV per concentration decade with sensors 1, 2 and 3, respectively. These sensors exhibit fast response time (1.0–1.5 min), low determination limit (1×10⁻⁵ M), good stability (4–8 weeks) and reasonable selectivity. The sensors were used for direct potentiometry and potentiometric titration of fluorouracil in some pharmaceutical preparations. Results with mean accuracy of 98.6±0.9% of nominal were obtained which compare well with data obtained using the British Pharmacopoeial method. The sensors were also used to follow the stability of the drug in the presence of its degradates, namely formaldehyde, fluoroacetate and urea. In the presence of glycine, these products have no effect on the responses of the sensors.
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Short communicationIntegrated differential enzyme sensors using hydrogen and fluoride ion sensitive multigate FETs

Abstract

Sens. Actuat.

Anal. Chim. Acta

Field effect transistor sensitive to penicillin

Anal. Chem.

Biosensors for glucose and lactate using fluoride ion sensitive field effect transistors

Anal. Lett.

Short communication
Integrated differential enzyme sensors using hydrogen and fluoride ion sensitive multigate FETs