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This paper reports a first microbial biosensor for rapid and cost-effective determination of organophosphorus pesticides fenitrothion and EPN. The biosensor consisted of recombinant PNP-degrading/oxidizing bacteria Pseudomonas putida JS444 anchoring and displaying organophosphorus hydrolase (OPH) on its cell surface as biological sensing element and a dissolved oxygen electrode as the transducer. Surfaceexpressed OPH catalyzed the hydrolysis of fenitrothion and EPN to release 3-methyl-4-nitrophenol and p-nitrophenol, respectively, which were oxidized by the enzymatic machinery of Pseudomonas putida JS444 to carbon dioxide while consuming oxygen, which was measured and correlated to the concentration of organophosphates. Under the optimum operating conditions, the biosensor was able to measure as low as 277 ppb of fenitrothion and 1.6 ppm of EPN without interference from phenolic compounds and other commonly used pesticides such as carbamate pesticides, triazine herbicides and organophosphate pesticides without nitrophenyl substituent. The applicability of the biosensor to lake water was also demonstrated.
This paper presents a two-dimensional-in-space mathematical model of biosensors based on an array of enzyme microreactors immobilised on a single electrode. The modeling system acts under amperometric conditions. The microreactors were modeled by particles and by strips. The model is based on the diffusion equations containing a nonlinear term related to the Michaelis-Menten kinetics of the enzymatic reaction. The model involves three regions: an array of enzyme microreactors where enzyme reaction as well as mass transport by diffusion takes place, a diffusion limiting region where only the diffusion takes place, and a convective region, where the analyte concentration is maintained constant. Using computer simulation, the influence of the geometry of the microreactors and of the diffusion region on the biosensor response was investigated. The digital simulation was carried out using the finite difference technique.
The applicability of differential pulse voltammetry (DPV) and adsorptive stripping voltammetry (AdSV) at a non-toxic meniscus-modified silver solid amalgam electrode (m-AgSAE) for the determination of trace amounts of genotoxic substances was demonstrated on the determination of micromolar and submicromolar concentrations of 3-nitrofluoranthene using methanol - 0.01 mol L-1 NaOH (9:1) mixture as a base electrolyte and of Ostazine Orange using 0.01 mol L-1 NaOH as a base electrolyte.
Novel organic membrane-based thin-film microsensors for the determination of heavy metal cations
(2006)
A first step towards the fabrication and electrochemical evaluation of thin-film microsensors based on organic PVC membranes for the determination of Hg(II), Cd(II), Pb(II) and Cu(II) ions in solutions has been realised. The membrane-coating mixture used in the preparation of this new type of microsensors is incorporating PVC as supporting matrix, o-nitrophenyloctylether (o-NPOE) as solvent mediator and a recently synthesized Hg[dimethylglyoxime(phene)]2+ and Bis-(4-hydroxyacetophenone)-ethylenediamine as electroactive materials for Hg(II) and Cd(II), respectively. A set of three commercialised ionophores for Cd(II), Pb(II) and Cu(II) has been also used for comparison. Thin-film microsensors based on these membranes showed a Nernstian response of slope (26-30 mV/dec.) for the respective tested cations. The potentiometric response characteristics (linear range, pH range, detection limit and response time) are comparable with those obtained by conventional membranes as well as coated wire electrodes prepared from the same membrane. The realisation of the new organic membrane-based thin-film microsensors overcomes the problem of an insufficient selectivity of solid-state-based thinfilm sensors.
In this paper, methods of sample preparation for potentiometric measurement of phenylalanine are presented. Basing on the spectrophotometric measurements of phenylalanine, the concentrations of reagents of the enzymatic reaction (10 mM L-Phe, 0,4 mM NAD+, 2U L-PheDH) were determined. Then, the absorption spectrum of the reaction product, NADH, was monitored (maximum peak at 340 nm). The results obtained by the spectrophotometric method were compared with the results obtained by the colourimetry, using pH indicators. The above-mentioned two methods will be used as references for potentiometric measurements of phenylalanine concentration.
Hydrophobic magnetic nanoparticles (NPs) consisting of undecanoate-capped magnetite (Fe3O4, average diameter ca. 5 nm) are used to control quantized electron transfer to surface-confined redox units and metal NPs. A two-phase system consisting of an aqueous electrolyte solution and a toluene phase that includes the suspended undecanoatecapped magnetic NPs is used to control the interfacial properties of the electrode surface. The attracted magnetic NPs form a hydrophobic layer on the electrode surface resulting in the change of the mechanisms of the surface-confined electrochemical processes. A quinone-monolayer modified Au electrode demonstrates an aqueous-type of the electrochemical process (2e-+2H+ redox mechanism) for the quinone units in the absence of the hydrophobic magnetic NPs, while the attraction of the magnetic NPs to the surface results in the stepwise single-electron transfer mechanism characteristic of a dry nonaqueous medium. Also, the attraction of the hydrophobic magnetic NPs to the Au electrode surface modified with Au NPs (ca. 1.4 nm) yields a microenvironment with a low dielectric constant that results in the single-electron quantum charging of the Au NPs.
Micromachined thermal heater platforms offer low electrical power consumption and high modulation speed, i.e. properties which are advantageous for realizing nondispersive infrared (NDIR) gas- and liquid monitoring systems. In this paper, we report on investigations on silicon-on-insulator (SOI) based infrared (IR) emitter devices heated by employing different kinds of metallic and semiconductor heater materials. Our results clearly reveal the superior high-temperature performance of semiconductor over metallic heater materials. Long-term stable emitter operation in the vicinity of 1300 K could be attained using heavily antimony-doped tin dioxide (SnO2:Sb) heater elements.
Various planar technologies are employed for developing solid-state sensors having low cost, small size and high reproducibility; thin- and thick-film technologies are most suitable for such productions. Screen-printing is especially suitable due to its simplicity, low-cost, high reproducibility and efficiency in large-scale production. This technology enables the deposition of a thick layer and allows precise pattern control. Moreover, this is a highly economic technology, saving large amounts of the used inks. In the course of repetitions of the film-deposition procedure there is no waste of material due to additivity of this thick-film technology. Finally, the thick films can be easily and quickly deposited on inexpensive substrates. In this contribution, thick-film ion-selective electrodes based on ionophores as well as crystalline ion-selective materials dedicated for potentiometric measurements are demonstrated. Analytical parameters of these sensors are comparable with those reported for conventional potentiometric electrodes. All mentioned thick-film strip electrodes have been totally fabricated in only one, fully automated thickfilm technology, without any additional manual, chemical or electrochemical steps. In all cases simple, inexpensive, commercially available materials, i.e. flexible, plastic substrates and easily cured polymer-based pastes were used.
Multi-interface level sensors and new development in monitoring and control of oil separators
(2006)
In the oil industry, huge saving may be made if suitable multi-interface level measurement systems are employed for effectively monitoring crude oil separators and efficient control of their operation. A number of techniques, e.g. externally mounted displacers, differential pressure transmitters and capacitance rod devices, have been developed to measure the separation process with gas, oil, water and other components. Because of the unavailability of suitable multi-interface level measurement systems, oil separators are currently operated by the trial-and-error approach. In this paper some conventional techniques, which have been used for level measurement in industry, and new development are discussed.
In this paper, methods of surface modification of different supports, i.e. glass and polymeric beads for enzyme immobilisation are described. The developed method of enzyme immobilisation is based on Schiff’s base formation between the amino groups on the enzyme surface and the aldehyde groups on the chemically modified surface of the supports. The surface of silicon modified by APTS and GOPS with immobilised enzyme was characterised by atomic force microscopy (AFM), time-of-flight secondary ion mass spectroscopy (ToF-SIMS) and infrared spectroscopy (FTIR). The supports with immobilised enzyme (urease) were also tested in combination with microreactors fabricated in silicon and Perspex, operating in a flow-through system. For microreactors filled with urease immobilised on glass beads (Sigma) and on polymeric beads (PAN), a very high and stable signal (pH change) was obtained. The developed method of urease immobilisation can be stated to be very effective.
A new and simple method for nanostructuring using conventional photolithography and layer expansion or pattern-size reduction technique is presented, which can further be applied for the fabrication of different nanostructures and nano-devices. The method is based on the conversion of a photolithographically patterned metal layer to a metal-oxide mask with improved pattern-size resolution using thermal oxidation. With this technique, the pattern size can be scaled down to several nanometer dimensions. The proposed method is experimentally demonstrated by preparing nanostructures with different configurations and layouts, like circles, rectangles, trapezoids, “fluidic-channel”-, “cantilever”- and meander-type structures.
GaAs-based Gunn diodes with graded AlGaAs hot electron injector heterostructures have been developed under the special needs in automotive applications. The fabrication of the Gunn diode chips was based on total substrate removal and processing of integrated Au heat sinks. Especially, the thermal and RF behavior of the diodes have been analyzed by DC, impedance and S-parameter measurements. The electrical investigations have revealed the functionality of the hot electron injector. An optimized layer structure could fulfill the requirements in adaptive cruise control (ACC) systems at 77 GHz with typical output power between 50 and 90 mW.
A concept for a sensitive micro total analysis system for high throughput fluorescence imaging
(2006)
This paper discusses possible methods for on-chip fluorescent imaging for integrated bio-sensors. The integration of optical and electro-optical accessories, according to suggested methods, can improve the performance of fluorescence imaging. It can boost the signal to background ratio by a few orders of magnitudes in comparison to conventional discrete setups. The methods that are present in this paper are oriented towards building reproducible arrays for high-throughput micro total analysis systems (µTAS). The first method relates to side illumination of the fluorescent material placed into microcompartments of the lab-on-chip. Its significance is in high utilization of excitation energy for low concentration of fluorescent material. The utilization of a transparent µLED chip, for the second method, allows the placement of the excitation light sources on the same optical axis with emission detector, such that the excitation and emission rays are directed controversly. The third method presents a spatial filtering of the excitation background.
An array of 50 MHz quartz microbalances (QMBs) coated with a dendronized polymer was used to detect small amounts of volatile organic compounds (VOCs) in the gas phase. The results were compared to those obtained with the commonly used 10 MHz QMBs. The 50 MHz QMBs proved to be a powerful tool for the detection of VOCs in the gas phase; therefore, they represent a promising alternative to the much more delicate surface acoustic wave devices (SAWs).
Quartz crystal nanobalance (QCN) sensors are considered as powerful masssensitive sensors to determine materials in the sub-nanogram level. In this study, a single piezoelectric quartz crystal nanobalance modified with polystyrene was employed to detect benzene, toluene, ethylbenzene and xylene (BTEX compounds). The frequency shift of the QCN sensor was found to be linear against the BTEX compound concentrations in the range about 1-45 mg l-1. The correlation coefficients for benzene, toluene, ethylbenzene, and xylene were 0.991, 0.9977, 0.9946 and 0.9971, respectively. The principal component analysis was also utilized to process the frequency response data of the single piezoelectric crystal at different times, considering to the different adsorption-desorption dynamics of BTEX compounds. Using principal component analysis, it was found that over 90% of the data variance could still be explained by use of two principal components (PC1 and PC2). Subsequently, the successful identification of benzene and toluene was possible through the principal component analysis of the transient responses of the polystyrene modified QCN sensor. The results showed that the polystyrene-modified QCN had favorable identification and quantification performances for the BTEX compounds.
We report on the synthesis and CO gas-sensing properties of mesoporous tin(IV) oxides (SnO2). For the synthesis cetyltrimethylammonium bromide (CTABr) was used as a structure-directing agent; the resulting SnO2 powders were applied as films to commercially available sensor substrates by drop coating. Nitrogen physisorption shows specific surface areas up to 160 m2·g-1 and mean pore diameters of about 4 nm, as verified by TEM. The film conductance was measured in dependence on the CO concentration in humid synthetic air at a constant temperature of 300 °C. The sensors show a high sensitivity at low CO concentrations and turn out to be largely insensitive towards changes in the relative humidity. We compare the materials with commercially available SnO2-based sensors.
An H2O2 sensor for the application in industrial sterilisation processes has been developed. Therefore, automated sterilisation equipment at laboratory scale has been constructed using parts from industrial sterilisation facilities. In addition, a software tool has been developed for the control of the sterilisation equipment at laboratory scale. First measurements with the developed sensor set-up as part of the sterilisation equipment have been performed and the sensor has been physically characterised by optical microscopy and SEM.
The workflow of a high throughput screening setup for the rapid identification of new and improved sensor materials is presented. The polyol method was applied to prepare nanoparticular metal oxides as base materials, which were functionalised by surface doping. Using multi-electrode substrates and high throughput impedance spectroscopy (HT-IS) a wide range of materials could be screened in a short time. Applying HT-IS in search of new selective gas sensing materials a NO2-tolerant NO sensing material with reduced sensitivities towards other test gases was identified based on iridium doped zinc oxide. Analogous behaviour was observed for iridium doped indium oxide.
A solid-state amperometric hydrogen sensor based on a protonated Nafion membrane and catalytic active electrode operating at room temperature was fabricated and tested. Ionic conducting polymer-metal electrode interfaces were prepared chemically by using the impregnation-reduction method. The polymer membrane was impregnated with tetra-ammine platinum chloride hydrate and the metal ions were subsequently reduced by using either sodium tetrahydroborate or potassium tetrahydroborate. The hydrogen sensing characteristics with air as reference gas is reported. The sensors were capable of detecting hydrogen concentrations from 10 ppm to 10% in nitrogen. The response time was in the range of 10-30 s and a stable linear current output was observed. The thin Pt films were characterized by XRD, Infrared Spectroscopy, Optical Microscopy, Atomic Force Microscopy, Scanning Electron Microscopy and EDAX.
A multi-sensor system is a chemical sensor system which quantitatively and qualitatively records gases with a combination of cross-sensitive gas sensor arrays and pattern recognition software. This paper addresses the issue of data analysis for identification of gases in a gas sensor array. We introduce a software tool for gas sensor array configuration and simulation. It concerns thereby about a modular software package for the acquisition of data of different sensors. A signal evaluation algorithm referred to as matrix method was used specifically for the software tool. This matrix method computes the gas concentrations from the signals of a sensor array. The software tool was used for the simulation of an array of five sensors to determine gas concentration of CH4, NH3, H2, CO and C2H5OH. The results of the present simulated sensor array indicate that the software tool is capable of the following: (a) identify a gas independently of its concentration; (b) estimate the concentration of the gas, even if the system was not previously exposed to this concentration; (c) tell when a gas concentration exceeds a certain value. A gas sensor data base was build for the configuration of the software. With the data base one can create, generate and manage scenarios and source files for the simulation. With the gas sensor data base and the simulation software an on-line Web-based version was developed, with which the user can configure and simulate sensor arrays on-line.