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Die Detektion von Schadstoffen repräsentiert in der Umweltanalytik eine wichtige Aufgabenstellung. Gerade die Abwasser- bzw. Brauchwasseranalytik sowie die Prozesskontrolle haben einen hohen Stellenwert. Siliziumbasierte Dünnschichtsensoren bieten eine kostengünstige Möglichkeit, „online“-Messungen bzw. Vor-Ort-Messungen zeitnah durchzuführen. In dieser Arbeit wird ein potentiometrisches Sensorarray auf der Basis von Chalkogenidgläsern zur Detektion von Schwermetallen in wässrigen Medien vorgestellt.
A multi-spot (16 spots) light-addressable potentiometric sensor (MLAPS) consisting of an Al–p-Si–SiO2 structure modified with a weak polyelectrolyte layer of PAH (poly(allylamine hydrochloride)) was applied for the label-free electrical detection of DNA (deoxyribonucleic acid) immobilization and hybridization by the intrinsic molecular charge for the first time. To achieve a preferentially flat orientation of DNA strands and thus, to reduce the distance between the DNA charge and MLAPS surface, the negatively charged probe single-stranded DNAs (ssDNA) were electrostatically adsorbed onto the positively charged PAH layer using a simple layer-by-layer (LbL) technique. In this way, more DNA charge can be positioned within the Debye length, yielding a higher sensor signal. The surface potential changes in each spot induced due to the surface modification steps (PAH adsorption, probe ssDNA immobilization, hybridization with complementary target DNA (cDNA), non-specific adsorption of mismatched ssDNA) were determined from the shifts of photocurrent–voltage curves along the voltage axis. A high sensor signal of 83 mV was registered after immobilization of probe ssDNA onto the PAH layer. The hybridization signal increases from 5 mV to 32 mV with increasing the concentration of cDNA from 0.1 nM to 5 μM. In contrast, a small signal of 5 mV was recorded in the case of non-specific adsorption of fully mismatched ssDNA (5 μM). The obtained results demonstrate the potential of the MLAPS in combination with the simple and rapid LbL immobilization technique as a promising platform for the future development of multi-spot light-addressable label-free DNA chips with direct electrical readout.
Capacitive field-effect sensors modified with a multi-enzyme membrane have been applied for an electronic transduction of biochemical signals processed by enzyme-based AND-Reset and OR-Reset logic gates. The local pH change at the sensor surface induced by the enzymatic reaction was used for the activation of the Reset function for the first time.
Sterilisation processes are compulsory in medicine, pharmacy, and food industries to prevent infections of consumers and microbiological contaminations of products. Monitoring the sterilisation by conventional microbiological methods is time- and lab-consuming. To overcome this problem, in this work a novel biosensor has been proposed. The sensor enables a fast method to evaluate sterilisation processes. By means of thin-film technology the sensor's transducer structures in form of IDEs (interdigitated electrodes) have been fabricated on a silicon substrate. Physical characterisation of the developed sensor was done by AFM, SEM, and profilometry. Impedance analyses were conducted for the electrical characterisation. As microbiological layer spores of B. atrophaeus have been immobilised on the sensing structure; spores of this type are a well-known sterilisation test organism. Impedance measurements at a fixed frequency over time were performed to monitor the immobilisation process. A sterilisation process according to aseptic filling machines was applied to demonstrate the sensor functionality. After both, immobilisation and sterilisation, a change in impedance could successfully be detected.
High-k perovskite oxide of barium strontium titanate (BST) represents a very attractive multi-functional transducer material for the development of (bio-)chemical sensors. In this work, a Si-based sensor chip containing Pt interdigitated electrodes covered with a thin BST layer (485 nm) has been developed for multi-parameter chemical sensing. The chip has been applied for the contactless measurement of the electrolyte conductivity, the detection of adsorbed charged macromolecules (positively charged polyelectrolytes of polyethylenimine) and the concentration of hydrogen peroxide (H2O2) vapor. The experimental results of functional testing of individual sensors are presented. The mechanism of the BST sensitivity to charged polyelectrolytes and H2O2 vapor has been proposed and discussed.
Simulating the electromagnetic‐thermal treatment of thin aluminium layers for adhesion improvement
(2015)
A composite layer material used in packaging industry is made from joining layers of different materials using an adhesive. An important processing step in the production of aluminium-containing composites is the surface treatment and consequent coating of adhesive material on the aluminium surface. To increase adhesion strength between aluminium layer and the adhesive material, the foil is heat treated. For efficient heating, induction heating was considered as state-of-the-art treatment process. Due to the complexity of the heating process and the unpredictable nature of the heating source, the control of the process is not yet optimised. In this work, a finite element analysis of the process was established and various process parameters were studied. The process was simplified and modelled in 3D. The numerical model contains an air domain, an aluminium layer and a copper coil fitted with a magnetic field concentrating material. The effect of changing the speed of the aluminium foil (or rolling speed) was studied with the change of the coil current. Statistical analysis was used for generating a general control equation of coil current with changing rolling speed.
An enzyme-based multi-parameter biosensor is developed for monitoring the concentration of formate, d-lactate, and l-lactate in biological samples. The sensor is based on the specific dehydrogenation by an oxidized β-nicotinamide adenine dinucleotide (NAD+)-dependent dehydrogenase (formate dehydrogenase, d-lactic dehydrogenase, and l-lactic dehydrogenase, respectively) in combination with a diaphorase from Clostridium kluyveri (EC 1.8.1.4). The enzymes are immobilized on a platinum working electrode by cross-linking with glutaraldehyde (GA). The principle of the determination scheme in case of l-lactate is as follows: l-lactic dehydrogenase (l-LDH) converts l-lactate into pyruvate by reaction with NAD+. In the presence of hexacyanoferrate(III), the resulting reduced β-nicotinamide adenine dinucleotide (NADH) is then regenerated enzymatically by diaphorase. The electrochemical detection is based on the current generated by oxidation of hexacyanoferrate(II) at an applied potential of +0.3 V vs. an Ag/AgCl reference electrode. The biosensor will be electrochemically characterized in terms of linear working range and sensitivity. Additionally, the successful practical application of the sensor is demonstrated in an extract from maize silage.
Poly(N-isopropylacrylamide) (PNIPAAm) hydrogel films with incorporated graphene oxide (GO) were developed and tested as light-stimulated actuators. GO dispersions were synthesized via Hummers method and characterized toward their optical properties and photothermal energy conversion. The hydrogels were prepared by means of photopolymerization. In addition, the influence of GO within the hydrogel network on the lower critical solution temperature (LCST) was investigated by differential scanning calorimetry (DSC). The optical absorbance and the response to illumination were determined as a function of GO concentration for thin hydrogel films. A proof of principle for the stimulation with light was performed.
LAPS are field-effect-based potentiometric sensors which are able to monitor analyte concentrations in a spatially resolved manner. Hence, a LAPS sensor system is a powerful device to record chemical imaging of the concentration of chemical species in an aqueous solution, chemical reactions, or the growth of cell colonies on the sensor surface, to record chemical images. In this work, multi-chamber 3D-printed structures made out of polymer (PP-ABS) were combined with LAPS chips to analyse differentially and simultaneously the metabolic activity of Escherichia coli K12 and Chinese hamster ovary (CHO) cells, and the responds of those cells to the addition of glucose solution.
An amperometric enzyme biosensor has been applied for the detection of adrenaline. The adrenaline biosensor has been prepared by modification of an oxygen electrode with the enzyme laccase that operates at a broad pH range between pH 3.5 to pH 8. The enzyme molecules were immobilized via cross-linking with glutaraldehyde. The sensitivity of the developed adrenaline biosensor in different pH buffer solutions has been studied.
A sensor system for investigating (bio)degradationprocesses of polymers is presented. The system utilizes semiconductor field-effect sensors and is capable of monitoring the degradation process in-situ and in real-time. The degradation of the polymer poly(d,l-lactic acid) is exemplarily monitored in solutions with different pH value, pH-buffer solution containing the model enzyme lipase from Rhizomucormiehei and cell-culture medium containing supernatants from stimulated and non-stimulated THP-1-derived macrophages mimicking activation of the immune system.
The chemical imaging sensor is a field-effect sensor which is able to visualize both the distribution of ions (in LAPS mode) and the distribution of impedance (in SPIM mode) inthe sample. In this study, a novel wound-healing assay is proposed, in which the chemical imaging sensor operated in SPIM mode is applied to monitor the defect of a cell layer brought into proximity of the sensing surface.A reduced impedance inside the defect, which was artificially formed ina cell layer, was successfully visualized in a photocurrent image.
Capacitive field-effect electrolyte-insulator-semiconductor sensors consisting of an Al-p-Si-SiO2 structure have been used for the electrical detection of unlabelled single- and double-stranded DNA (dsDNA) molecules by their intrinsic charge. A simple functionalization protocol based on the layer-by-layer (LbL) technique was used to prepare a weak polyelectrolyte/probe-DNA bilayer, followed by the hybridization with complementary target DNA molecules. Due to the flat orientation of the LbL-adsorbed DNA molecules, a high sensor signal has been achieved. In addition, direct label-free detection of in-solution hybridized dsDNA molecules has been studied.