TY - JOUR A1 - Molinnus, Denise A1 - Poghossian, Arshak A1 - Keusgen, Michael A1 - Katz, Evgeny A1 - Schöning, Michael Josef T1 - Coupling of Biomolecular Logic Gates with Electronic Transducers: From Single Enzyme Logic Gates to Sense/Act/Treat Chips JF - Electroanalysis N2 - The integration of biomolecular logic principles with electronic transducers allows designing novel digital biosensors with direct electrical output, logically triggered drug-release, and closed-loop sense/act/treat systems. This opens new opportunities for advanced personalized medicine in the context of theranostics. In the present work, we will discuss selected examples of recent developments in the field of interfacing enzyme logic gates with electrodes and semiconductor field-effect devices. Special attention is given to an enzyme OR/Reset logic gate based on a capacitive field-effect electrolyte-insulator-semiconductor sensor modified with a multi-enzyme membrane. Further examples are a digital adrenaline biosensor based on an AND logic gate with binary YES/NO output and an integrated closed-loop sense/act/treat system comprising an amperometric glucose sensor, a hydrogel actuator, and an insulin (drug) sensor. Y1 - 2017 U6 - http://dx.doi.org/10.1002/elan.201700208 SN - 1521-4109 VL - 29 IS - 8 SP - 1840 EP - 1849 PB - Wiley CY - Weinheim ER - TY - JOUR A1 - Molinnus, Denise A1 - Muschallik, Lukas A1 - Gonzalez, Laura Osorio A1 - Bongaerts, Johannes A1 - Wagner, Torsten A1 - Selmer, Thorsten A1 - Siegert, Petra A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Development and characterization of a field-effect biosensor for the detection of acetoin JF - Biosensors and Bioelectronics N2 - A capacitive electrolyte-insulator-semiconductor (EIS) field-effect biosensor for acetoin detection has been presented for the first time. The EIS sensor consists of a layer structure of Al/p-Si/SiO₂/Ta₂O₅/enzyme acetoin reductase. The enzyme, also referred to as butane-2,3-diol dehydrogenase from B. clausii DSM 8716T, has been recently characterized. The enzyme catalyzes the (R)-specific reduction of racemic acetoin to (R,R)- and meso-butane-2,3-diol, respectively. Two different enzyme immobilization strategies (cross-linking by using glutaraldehyde and adsorption) have been studied. Typical biosensor parameters such as optimal pH working range, sensitivity, hysteresis, linear concentration range and long-term stability have been examined by means of constant-capacitance (ConCap) mode measurements. Furthermore, preliminary experiments have been successfully carried out for the detection of acetoin in diluted white wine samples. Y1 - 2018 U6 - http://dx.doi.org/10.1016/j.bios.2018.05.023 VL - 115 SP - 1 EP - 6 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Molinnus, Denise A1 - Janus, Kevin Alexander A1 - Fang, Anyelina C. A1 - Drinic, Aleksander A1 - Achtsnicht, Stefan A1 - Köpf, Marius A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Thick-film carbon electrode deposited onto a biodegradable fibroin substrate for biosensing applications JF - Physica status solidi (a) N2 - This study addresses a proof-of-concept experiment with a biocompatible screen-printed carbon electrode deposited onto a biocompatible and biodegradable substrate, which is made of fibroin, a protein derived from silk of the Bombyx mori silkworm. To demonstrate the sensor performance, the carbon electrode is functionalized as a glucose biosensor with the enzyme glucose oxidase and encapsulated with a silicone rubber to ensure biocompatibility of the contact wires. The carbon electrode is fabricated by means of thick-film technology including a curing step to solidify the carbon paste. The influence of the curing temperature and curing time on the electrode morphology is analyzed via scanning electron microscopy. The electrochemical characterization of the glucose biosensor is performed by amperometric/voltammetric measurements of different glucose concentrations in phosphate buffer. Herein, systematic studies at applied potentials from 500 to 1200 mV to the carbon working electrode (vs the Ag/AgCl reference electrode) allow to determine the optimal working potential. Additionally, the influence of the curing parameters on the glucose sensitivity is examined over a time period of up to 361 days. The sensor shows a negligible cross-sensitivity toward ascorbic acid, noradrenaline, and adrenaline. The developed biocompatible biosensor is highly promising for future in vivo and epidermal applications. KW - biocompatible materials KW - biodegradable electronic devices KW - biosensors KW - carbon electrodes KW - glucose Y1 - 2022 U6 - http://dx.doi.org/10.1002/pssa.202200100 SN - 1862-6319 N1 - Corresponding author: Michael J. Schöning VL - 219 IS - 23 SP - 1 EP - 9 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Molinnus, Denise A1 - Hardt, Gabriel A1 - Siegert, Petra A1 - Willenberg, Holger S. A1 - Poghossian, Arshak A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Detection of Adrenaline in Blood Plasma as Biomarker for Adrenal Venous Sampling JF - Electroanalysis N2 - An amperometric bi-enzyme biosensor based on substrate recycling principle for the amplification of the sensor signal has been developed for the detection of adrenaline in blood. Adrenaline can be used as biomarker verifying successful adrenal venous sampling procedure. The adrenaline biosensor has been realized via modification of a galvanic oxygen sensor with a bi-enzyme membrane combining a genetically modified laccase and a pyrroloquinoline quinone-dependent glucose dehydrogenase. The measurement conditions such as pH value and temperature were optimized to enhance the sensor performance. A high sensitivity and a low detection limit of about 0.5–1 nM adrenaline have been achieved in phosphate buffer at pH 7.4, relevant for measurements in blood samples. The sensitivity of the biosensor to other catecholamines such as noradrenaline, dopamine and dobutamine has been studied. Finally, the sensor has been successfully applied for the detection of adrenaline in human blood plasma. Y1 - 2018 U6 - http://dx.doi.org/10.1002/elan.201800026 SN - 1521-4109 VL - 30 IS - 5 SP - 937 EP - 942 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Molinnus, Denise A1 - Hardt, G. A1 - Käver, L. A1 - Willenberg, H.S. A1 - Kröger, J.-C. A1 - Poghossian, Arshak A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Chip-based biosensor for the detection of low adrenaline concentrations to support adrenal venous sampling JF - Sensor and Actuators B: Chemical N2 - A chip-based amperometric biosensor referring on using the bioelectrocatalytical amplification principle for the detection of low adrenaline concentrations is presented. The adrenaline biosensor has been prepared by modification of a platinum thin-film electrode with an enzyme membrane containing the pyrroloquinoline quinone-dependent glucose dehydrogenase and glutaraldehyde. Measuring conditions such as temperature, pH value, and glucose concentration have been optimized to achieve a high sensitivity and a low detection limit of about 1 nM adrenaline measured in phosphate buffer at neutral pH value. The response of the biosensor to different catecholamines has also been proven. Long-term stability of the adrenaline biosensor has been studied over 10 days. In addition, the biosensor has been successfully applied for adrenaline detection in human blood plasma for future biomedical applications. Furthermore, preliminary experiments have been carried to detect the adrenaline-concentration difference measured in peripheral blood and adrenal venous blood, representing the adrenal vein sampling procedure of a physician. Y1 - 2018 U6 - http://dx.doi.org/10.1016/j.snb.2018.05.136 SN - 0925-4005 VL - 272 SP - 21 EP - 27 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Molinnus, Denise A1 - Bäcker, Matthias A1 - Iken, Heiko A1 - Poghossian, Arshak A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Concept for a biomolecular logic chip with an integrated sensor and actuator function JF - Physica status solidi (a) N2 - A concept for a new generation of an integrated multi-functional biosensor/actuator system is developed, which is based on biomolecular logic principles. Such a system is expected to be able to detect multiple biochemical input signals simultaneously and in real-time and convert them into electrical output signals with logical operations such as OR, AND, etc. The system can be designed as a closed-loop drug release device triggered by an enzyme logic gate, while the release of the drug induced by the actuator at the required dosage and timing will be controlled by an additional drug sensor. Thus, the system could help to make an accurate and specific diagnosis. The presented concept is exemplarily demonstrated by using an enzyme logic gate based on a glucose/glucose oxidase system, a temperature-responsive hydrogel mimicking the actuator function and an insulin (drug) sensor. In this work, the results of functional testing of individual amperometric glucose and insulin sensors as well as an impedimetric sensor for the detection of the hydrogel swelling/shrinking are presented. Y1 - 2015 U6 - http://dx.doi.org/10.1002/pssa.201431913 SN - 1862-6319 VL - 212 IS - 6 SP - 1382 EP - 1388 PB - Wiley CY - Weinheim ER - TY - JOUR A1 - Kirchner, Patrick A1 - Reisert, Steffen A1 - Pütz, Patrick A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Characterisation of polymeric materials as passivation layer for calorimetric H2O2 gas sensors JF - Physica Status Solidi (a) N2 - Calorimetric gas sensors for monitoring the H₂O₂ concentration at elevated temperatures in industrial sterilisation processes have been presented in previous works. These sensors are built up in form of a differential set-up of a catalytically active and passive temperature-sensitive structure. Although, various types of catalytically active dispersions have been studied, the passivation layer has to be established and therefore, chemically as well as physically characterised. In the present work, fluorinated ethylene propylene (FEP), perfluoralkoxy (PFA) and epoxy-based SU-8 photoresist as temperature-stable polymeric materials have been investigated for sensor passivation in terms of their chemical inertness against H₂O₂, their hygroscopic properties as well as their morphology. The polymeric materials were deposited via spin-coating on the temperature-sensitive structure, wherein spin-coated FEP and PFA show slight agglomerates. However, they possess a low absorption of humidity due to their hydrophobic surface, whereas the SU-8 layer has a closed surface but shows a slightly higher absorption of water. All of them were inert against gaseous H₂O₂ during the characterisation in H₂O₂ atmosphere that demonstrates their suitability as passivation layer for calorimetric H₂O₂ gas sensors. Y1 - 2012 U6 - http://dx.doi.org/10.1002/pssa.201100773 SN - 1862-6319 VL - 209 IS - 5 SP - 859 EP - 863 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Kirchner, Patrick A1 - Oberländer, Jan A1 - Suso, Henri-Pierre A1 - Rysstad, Gunnar A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Towards a wireless sensor system for real-time H2O2 monitoring in aseptic food processes JF - Physica status solidi (a) N2 - A wireless sensor system based on the industrial ZigBee standard for low-rate wireless networking was developed that enables real-time monitoring of gaseous H2O2 during the package sterilization in aseptic food processes. The sensor system consists of a remote unit connected to a calorimetric gas sensor, which was already established in former works, and an external base unit connected to a laptop computer. The remote unit was built up by an XBee radio frequency (RF) module for data communication and a programmable system-on-chip controller to read out the sensor signal and process the sensor data, whereas the base unit is a second XBee RF module. For the rapid H2O2 detection on various locations inside the package that has to be sterilized, a novel read-out strategy of the calorimetric gas sensor was established, wherein the sensor response is measured within the short sterilization time and correlated with the present H2O2 concentration. In an exemplary measurement application in an aseptic filling machinery, the suitability of the new, wireless sensor system was demonstrated, wherein the influence of the gas velocity on the H2O2 distribution inside a package was determined and verified with microbiological tests. KW - calorimetric gas sensor;hydrogen peroxide;wireless sensor system Y1 - 2013 U6 - http://dx.doi.org/10.1002/pssa.201200920 SN - 1862-6319 VL - 210 IS - 5 SP - 877 EP - 883 PB - Wiley CY - Weinheim ER - TY - JOUR A1 - Kirchner, Patrick A1 - Oberländer, Jan A1 - Friedrich, Peter A1 - Berger, Jörg A1 - Suso, Henri-Pierre A1 - Kupyna, Andriy A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Optimisation and fabrication of a calorimetric gas sensor built up on a polyimide substrate for H2O2 monitoring JF - Physica status solidi (a) : applications and material science. 208 (2011), H. 6 Y1 - 2011 SN - 1862-6319 SP - 1235 EP - 1240 PB - Wiley CY - Weinheim ER - TY - JOUR A1 - Kirchner, Patrick A1 - Oberländer, Jan A1 - Friedrich, Peter A1 - Berger, Jörg A1 - Rysstad, Gunnar A1 - Schöning, Michael Josef A1 - Keusgen, Michael T1 - Realisation of a calorimetric gas sensor on polyimide foil for applications in aseptic food industry JF - Sensors and Actuators B: Chemical N2 - A calorimetric gas sensor is presented for the monitoring of vapour-phase H2O2 at elevated temperature during sterilisation processes in aseptic food industry. The sensor was built up on a flexible polyimide foil (thickness: 25 μm) that has been chosen due to its thermal stability and low thermal conductivity. The sensor set-up consists of two temperature-sensitive platinum thin-film resistances passivated by a layer of SU-8 photo resist and catalytically activated by manganese(IV) oxide. Instead of an active heating structure, the calorimetric sensor utilises the elevated temperature of the evaporated H2O2 aerosol. In an experimental test rig, the sensor has shown a sensitivity of 4.78 °C/(%, v/v) in a H2O2 concentration range of 0%, v/v to 8%, v/v. Furthermore, the sensor possesses the same, unchanged sensor signal even at varied medium temperatures between 210 °C and 270 °C of the gas stream. At flow rates of the gas stream from 8 m3/h to 12 m3/h, the sensor has shown only a slightly reduced sensitivity at a low flow rate of 8 m3/h. The sensor characterisation demonstrates the suitability of the calorimetric gas sensor for monitoring the efficiency of industrial sterilisation processes. KW - Sterilisation process KW - Hydrogen peroxide KW - Polyimide KW - Calorimetric gas sensor Y1 - 2012 U6 - http://dx.doi.org/10.1016/j.snb.2011.01.032 SN - 0925-4005 N1 - Part of special issue "Eurosensors XXIV, 2010" VL - 170 SP - 60 EP - 66 PB - Elsevier CY - Amsterdam ER -