TY - JOUR A1 - Jildeh, Zaid B. A1 - Kirchner, Patrick A1 - Baltes, Klaus A1 - Wagner, Patrick H. A1 - Schöning, Michael Josef T1 - Development of an in-line evaporation unit for the production of gas mixtures containing hydrogen peroxide – numerical modeling and experimental results JF - International Journal of Heat and Mass Transfer N2 - Hydrogen peroxide (H2O2) is a typical surface sterilization agent for packaging materials used in the pharmaceutical, food and beverage industries. We use the finite-elements method to analyze the conceptual design of an in-line thermal evaporation unit to produce a heated gas mixture of air and evaporated H2O2 solution. For the numerical model, the required phase-transition variables of pure H2O2 solution and of the aerosol mixture are acquired from vapor-liquid equilibrium (VLE) diagrams derived from vapor-pressure formulations. This work combines homogeneous single-phase turbulent flow with heat-transfer physics to describe the operation of the evaporation unit. We introduce the apparent heat-capacity concept to approximate the non-isothermal phase-transition process of the H2O2-containing aerosol. Empirical and analytical functions are defined to represent the temperature- and pressure-dependent material properties of the aqueous H2O2 solution, the aerosol and the gas mixture. To validate the numerical model, the simulation results are compared to experimental data on the heating power required to produce the gas mixture. This shows good agreement with the deviations below 10%. Experimental observations on the formation of deposits due to the evaporation of stabilized H2O2 solution fits the prediction made from simulation results. Y1 - 2019 U6 - http://dx.doi.org/10.1016/j.ijheatmasstransfer.2019.118519 SN - 0017-9310 VL - 143 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Dantism, Shahriar A1 - Röhlen, Desiree A1 - Selmer, Thorsten A1 - Wagner, Torsten A1 - Wagner, Patrick A1 - Schöning, Michael Josef T1 - Quantitative differential monitoring of the metabolic activity of Corynebacterium glutamicum cultures utilizing a light-addressable potentiometric sensor system JF - Biosensors and Bioelectronics Y1 - 2019 U6 - http://dx.doi.org/10.1016/j.bios.2019.111332 VL - 139 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Iken, Heiko A1 - Bronder, Thomas A1 - Goretzki, Alexander A1 - Kriesel, Jana A1 - Ahlborn, Kristina A1 - Gerlach, Frank A1 - Vonau, Winfried A1 - Zander, Willi A1 - Schubert, Jürgen A1 - Schöning, Michael Josef T1 - Development of a Combined pH- and Redox-Sensitive Bi-Electrode Glass Thin-Film Sensor JF - physica status solidi a : applications and materials sciences Y1 - 2019 U6 - http://dx.doi.org/10.1002/pssa.201900114 SN - 1862-6319 VL - 216 IS - 12 SP - 1 EP - 8 PB - Wiley CY - Weinheim ER - TY - JOUR A1 - Özsoylu, Dua A1 - Kizildag, Sefa A1 - Schöning, Michael Josef A1 - Wagner, Torsten T1 - Effect of plasma treatment on the sensor properties of a light‐addressable potentiometric sensor (LAPS) JF - physica status solidi a : applications and materials sciences N2 - A light-addressable potentiometric sensor (LAPS) is a field-effect-based (bio-) chemical sensor, in which a desired sensing area on the sensor surface can be defined by illumination. Light addressability can be used to visualize the concentration and spatial distribution of the target molecules, e.g., H+ ions. This unique feature has great potential for the label-free imaging of the metabolic activity of living organisms. The cultivation of those organisms needs specially tailored surface properties of the sensor. O2 plasma treatment is an attractive and promising tool for rapid surface engineering. However, the potential impacts of the technique are carefully investigated for the sensors that suffer from plasma-induced damage. Herein, a LAPS with a Ta2O5 pH-sensitive surface is successfully patterned by plasma treatment, and its effects are investigated by contact angle and scanning LAPS measurements. The plasma duration of 30 s (30 W) is found to be the threshold value, where excessive wettability begins. Furthermore, this treatment approach causes moderate plasma-induced damage, which can be reduced by thermal annealing (10 min at 300 °C). These findings provide a useful guideline to support future studies, where the LAPS surface is desired to be more hydrophilic by O2 plasma treatment. Y1 - 2019 U6 - http://dx.doi.org/10.1002/pssa.201900259 SN - 1862-6319 N1 - Corresponding author: Torsten Wagner VL - 216 IS - 20 PB - Wiley CY - Weinheim ER - TY - JOUR A1 - Pilas, Johanna A1 - Selmer, Thorsten A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Screen-printed carbon electrodes modified with graphene oxide for the design of a reagent-free NAD+-dependent biosensor array JF - Analytical Chemistry Y1 - 2019 U6 - http://dx.doi.org/10.1021/acs.analchem.9b04481 VL - 91 IS - 23 SP - 15293 EP - 15299 PB - ACS Publications CY - Washington ER - TY - JOUR A1 - Figueroa-Miranda, Gabriela A1 - Feng, Lingyan A1 - Shiu, Simon Chi-Chin A1 - Dirkzwager, Roderick Marshall A1 - Cheung, Yee-Wai A1 - Tanner, Julian Alexander A1 - Schöning, Michael Josef A1 - Offenhäusser, Andreas A1 - Mayer, Dirk T1 - Aptamer-based electrochemical biosensor for highly sensitive and selective malaria detection with adjustable dynamic response range and reusability JF - Sensor and Actuators B: Chemical N2 - Malaria infection remains a significant risk for much of the population of tropical and subtropical areas, particularly in developing countries. Therefore, it is of high importance to develop sensitive, accurate and inexpensive malaria diagnosis tests. Here, we present a novel aptamer-based electrochemical biosensor (aptasensor) for malaria detection by impedance spectroscopy, through the specific recognition between a highly discriminatory DNA aptamer and its target Plasmodium falciparum lactate dehydrogenase (PfLDH). Interestingly, due to the isoelectric point (pI) of PfLDH, the aptasensor response showed an adjustable detection range based on the different protein net-charge at variable pH environments. The specific aptamer recognition allows sensitive protein detection with an expanded detection range and a low detection limit, as well as a high specificity for PfLDH compared to analogous proteins. The specific feasibility of the aptasensor is further demonstrated by detection of the target PfLDH in human serum. Furthermore, the aptasensor can be easily regenerated and thus applied for multiple usages. The robustness, sensitivity, and reusability of the presented aptasensor make it a promising candidate for point-of-care diagnostic systems. Y1 - 2018 U6 - http://dx.doi.org/10.1016/j.snb.2017.07.117 SN - 0925-4005 VL - 255 IS - P1 SP - 235 EP - 243 PB - Elsevier CY - Amsterdam 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 - Oberländer, Jan A1 - Mayer, Marlena A1 - Greeff, Anton A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Spore-based biosensor to monitor the microbicidal efficacy of gaseous hydrogen peroxide sterilization processes JF - Biosensors and Bioelectronics N2 - In this work, a spore-based biosensor is evaluated to monitor the microbicidal efficacy of sterilization processes applying gaseous hydrogen peroxide (H2O2). The sensor is based on interdigitated electrode structures (IDEs) that have been fabricated by means of thin-film technologies. Impedimetric measurements are applied to study the effect of sterilization process on spores of Bacillus atrophaeus. This resilient microorganism is commonly used in industry to proof the sterilization efficiency. The sensor measurements are accompanied by conventional microbiological challenge tests, as well as morphological characterizations with scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The sensor measurements are correlated with the microbiological test routines. In both methods, namely the sensor-based and microbiological one, a tailing effect has been observed. The results are evaluated and discussed in a three-dimensional calibration plot demonstrating the sensor's suitability to enable a rapid process decision in terms of a successfully performed sterilization. Y1 - 2018 U6 - http://dx.doi.org/10.1016/j.bios.2017.12.045 SN - 0956-5663 VL - 104 SP - 87 EP - 94 PB - Elsevier CY - Amsterdam 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 - Pilas, Johanna A1 - Yazici, Y. A1 - Selmer, Thorsten A1 - Keusgen, M. A1 - Schöning, Michael Josef T1 - Application of a portable multi-analyte biosensor for organic acid determination in silage JF - Sensors N2 - Multi-analyte biosensors may offer the opportunity to perform cost-effective and rapid analysis with reduced sample volume, as compared to electrochemical biosensing of each analyte individually. This work describes the development of an enzyme-based biosensor system for multi-parametric determination of four different organic acids. The biosensor array comprises five working electrodes for simultaneous sensing of ethanol, formate, d-lactate, and l-lactate, and an integrated counter electrode. Storage stability of the biosensor was evaluated under different conditions (stored at +4 °C in buffer solution and dry at −21 °C, +4 °C, and room temperature) over a period of 140 days. After repeated and regular application, the individual sensing electrodes exhibited the best stability when stored at −21 °C. Furthermore, measurements in silage samples (maize and sugarcane silage) were conducted with the portable biosensor system. Comparison with a conventional photometric technique demonstrated successful employment for rapid monitoring of complex media. Y1 - 2018 U6 - http://dx.doi.org/10.3390/s18051470 SN - 1424-8220 VL - 18 IS - 5 PB - MDPI CY - Basel ER - TY - JOUR A1 - Dantism, Shahriar A1 - Röhlen, Desiree A1 - Wagner, Torsten A1 - Wagner, Patrick A1 - Schöning, Michael Josef T1 - Optimization of Cell-Based Multi-Chamber LAPS Measurements Utilizing FPGA-Controlled Laser-Diode Modules JF - physica status solidi a : applications and materials sciences N2 - A light-addressable potentiometric sensor (LAPS) is a field-effect-based potentiometric device, which detects concentration changes of an analyte solution on the sensor surface in a spatially resolved way. It uses a light source to generate electron–hole pairs inside the semiconductor, which are separated in the depletion region due to an applied bias voltage across the sensor structure and hence, a surface-potential-dependent photocurrent can be read out. However, depending on the beam angle of the light source, scattering effects can occur, which influence the recorded signal in LAPS-based differential measurements. To solve this problem, a novel illumination unit based on a field programmable gate array (FPGA) consisting of 16 small-sized tunable infrared laser-diode modules (LDMs) is developed. Due to the improved focus of the LDMs with a beam angle of only 2 mrad, undesirable scattering effects are minimized. Escherichia coli (E. coli) K12 bacteria are used as a test microorganism to study the extracellular acidification on the sensor surface. Furthermore, a salt bridge chamber is built up and integrated with the LAPS system enabling multi-chamber differential measurements with a single Ag/AgCl reference electrode. Y1 - 2018 U6 - http://dx.doi.org/10.1002/pssa.201800058 SN - 1862-6319 VL - 215 IS - 15 SP - Article number 1800058 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 - Welden, Rene A1 - Scheja, Sabrina A1 - Schöning, Michael Josef A1 - Wagner, Patrick A1 - Wagner, Torsten T1 - Electrochemical Evaluation of Light‐Addressable Electrodes Based on TiO2 for the Integration in Lab‐on‐Chip Systems JF - physica status solidi a : applications and materials sciences N2 - In lab-on-chip systems, electrodes are important for the manipulation (e.g., cell stimulation, electrolysis) within such systems. An alternative to commonly used electrode structures can be a light-addressable electrode. Here, due to the photoelectric effect, the conducting area can be adjusted by modification of the illumination area which enables a flexible control of the electrode. In this work, titanium dioxide based light-addressable electrodes are fabricated by a sol–gel technique and a spin-coating process, to deposit a thin film on a fluorine-doped tin oxide glass. To characterize the fabricated electrodes, the thickness, and morphological structure are measured by a profilometer and a scanning electron microscope. For the electrochemical behavior, the dark current and the photocurrent are determined for various film thicknesses. For the spatial resolution behavior, the dependency of the photocurrent while changing the area of the illuminated area is studied. Furthermore, the addressing of single fluid compartments in a three-chamber system, which is added to the electrode, is demonstrated. Y1 - 2018 U6 - http://dx.doi.org/10.1002/pssa.201800150 SN - 1862-6319 VL - 215 IS - 15 SP - Article number 1800150 PB - Wiley-VCH CY - Weinheim ER - TY - CHAP A1 - Koch, Claudia A1 - Poghossian, Arshak A1 - Wege, Christina A1 - Schöning, Michael Josef ED - Wege, Christina T1 - TMV-Based Adapter Templates for Enhanced Enzyme Loading in Biosensor Applications T2 - Virus-Derived Nanoparticles for Advanced Technologies N2 - Nanotubular tobacco mosaic virus (TMV) particles and RNA-free lower-order coat protein (CP) aggregates have been employed as enzyme carriers in different diagnostic layouts and compared for their influence on biosensor performance. In the following, we describe a label-free electrochemical biosensor for improved glucose detection by use of TMV adapters and the enzyme glucose oxidase (GOD). A specific and efficient immobilization of streptavidin-conjugated GOD ([SA]-GOD) complexes on biotinylated TMV nanotubes or CP aggregates was achieved via bioaffinity binding. Glucose sensors with adsorptively immobilized [SA]-GOD, and with [SA]-GOD cross-linked with glutardialdehyde, respectively, were tested in parallel on the same sensor chip. Comparison of these sensors revealed that TMV adapters enhanced the amperometric glucose detection remarkably, conveying highest sensitivity, an extended linear detection range and fastest response times. These results underline a great potential of an integration of virus/biomolecule hybrids with electronic transducers for applications in biosensorics and biochips. Here, we describe the fabrication and use of amperometric sensor chips combining an array of circular Pt electrodes, their loading with GOD-modified TMV nanotubes (and other GOD immobilization methods), and the subsequent investigations of the sensor performance. KW - Tobacco mosaic virus (TMV) KW - Coat protein KW - Enzyme nanocarrier KW - Glucose biosensor KW - Glucose oxidase Y1 - 2018 SN - 978-1-4939-7808-3 U6 - http://dx.doi.org/10.1007/978-1-4939-7808-3 N1 - Methods in Molecular Biology, vol 1776 SP - 553 EP - 568 PB - Humana Press CY - New York, NY ER - TY - JOUR A1 - Bronder, Thomas A1 - Jessing, Max P. A1 - Poghossian, Arshak A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Detection of PCR-Amplified Tuberculosis DNA Fragments with Polyelectrolyte-Modified Field-Effect Sensors JF - Analytical Chemistry N2 - Field-effect-based electrolyte-insulator-semiconductor (EIS) sensors were modified with a bilayer of positively charged weak polyelectrolyte (poly(allylamine hydrochloride) (PAH)) and probe single-stranded DNA (ssDNA) and are used for the detection of complementary single-stranded target DNA (cDNA) in different test solutions. The sensing mechanism is based on the detection of the intrinsic molecular charge of target cDNA molecules after the hybridization event between cDNA and immobilized probe ssDNA. The test solutions contain synthetic cDNA oligonucleotides (with a sequence of tuberculosis mycobacteria genome) or PCR-amplified DNA (which origins from a template DNA strand that has been extracted from Mycobacterium avium paratuberculosis-spiked human sputum samples), respectively. Sensor responses up to 41 mV have been measured for the test solutions with DNA, while only small signals of ∼5 mV were detected for solutions without DNA. The lower detection limit of the EIS sensors was ∼0.3 nM, and the sensitivity was ∼7.2 mV/decade. Fluorescence experiments using SybrGreen I fluorescence dye support the electrochemical results. Y1 - 2018 U6 - http://dx.doi.org/10.1021/acs.analchem.8b01807 SN - 0003-2700 VL - 90 IS - 12 SP - 7747 EP - 7753 PB - ACS Publications CY - Washington, DC ER - TY - JOUR A1 - Jildeh, Zaid B. A1 - Oberländer, Jan A1 - Kirchner, Patrick A1 - Keusgen, Michael A1 - Wagner, Patrick H. A1 - Schöning, Michael Josef T1 - Experimental and Numerical Analyzes of a Sensor Based on Interdigitated Electrodes for Studying Microbiological Alterations JF - physica status solidi (a): applications and materials science N2 - In this work, a cell-based biosensor to evaluate the sterilization efficacy of hydrogen peroxide vapor sterilization processes is characterized. The transducer of the biosensor is based on interdigitated gold electrodes fabricated on an inert glass substrate. Impedance spectroscopy is applied to evaluate the sensor behavior and the alteration of test microorganisms due to the sterilization process. These alterations are related to changes in relative permittivity and electrical conductivity of the bacterial spores. Sensor measurements are conducted with and without bacterial spores (Bacillus atrophaeus), as well as after an industrial sterilization protocol. Equivalent two-dimensional numerical models based on finite element method of the periodic finger structures of the interdigitated gold electrodes are designed and validated using COMSOL® Multiphysics software by the application of known dielectric properties. The validated models are used to compute the electrical properties at different sensor states (blank, loaded with spores, and after sterilization). As a final result, we will derive and tabulate the frequency-dependent electrical parameters of the spore layer using a novel model that combines experimental data with numerical optimization techniques. Y1 - 2018 U6 - http://dx.doi.org/10.1002/pssa.201700920 SN - 1862-6319 VL - 215 IS - 15 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Jildeh, Zaid B. A1 - Oberländer, Jan A1 - Kirchner, Patrick A1 - Wagner, Patrick H. A1 - Schöning, Michael Josef T1 - Thermocatalytic Behavior of Manganese (IV) Oxide as Nanoporous Material on the Dissociation of a Gas Mixture Containing Hydrogen Peroxide JF - Nanomaterials N2 - In this article, we present an overview on the thermocatalytic reaction of hydrogen peroxide (H₂O₂) gas on a manganese (IV) oxide (MnO₂) catalytic structure. The principle of operation and manufacturing techniques are introduced for a calorimetric H₂O₂ gas sensor based on porous MnO₂. Results from surface analyses by X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM) of the catalytic material provide indication of the H₂O₂ dissociation reaction schemes. The correlation between theory and the experiments is documented in numerical models of the catalytic reaction. The aim of the numerical models is to provide further information on the reaction kinetics and performance enhancement of the porous MnO₂ catalyst. Y1 - 2018 U6 - http://dx.doi.org/10.3390/nano8040262 SN - 2079-4991 VL - 8 IS - 4 PB - MDPI CY - Basel ER - TY - JOUR A1 - Koch, Claudia A1 - Poghossian, Arshak A1 - Schöning, Michael Josef A1 - Wege, Christian T1 - Penicillin Detection by Tobacco Mosaic Virus-Assisted Colorimetric Biosensors JF - Nanotheranostics N2 - The presentation of enzymes on viral scaffolds has beneficial effects such as an increased enzyme loading and a prolonged reusability in comparison to conventional immobilization platforms. Here, we used modified tobacco mosaic virus (TMV) nanorods as enzyme carriers in penicillin G detection for the first time. Penicillinase enzymes were conjugated with streptavidin and coupled to TMV rods by use of a bifunctional biotin-linker. Penicillinase-decorated TMV particles were characterized extensively in halochromic dye-based biosensing. Acidometric analyte detection was performed with bromcresol purple as pH indicator and spectrophotometry. The TMV-assisted sensors exhibited increased enzyme loading and strongly improved reusability, and higher analysis rates compared to layouts without viral adapters. They extended the half-life of the sensors from 4 - 6 days to 5 weeks and thus allowed an at least 8-fold longer use of the sensors. Using a commercial budget-priced penicillinase preparation, a detection limit of 100 µM penicillin was obtained. Initial experiments also indicate that the system may be transferred to label-free detection layouts. Y1 - 2018 U6 - http://dx.doi.org/10.7150/ntno.22114 SN - 2206-7418 VL - 2 IS - 2 SP - 184 EP - 196 PB - Ivyspring CY - Sydney ER - TY - JOUR A1 - Vahidpour, Farnoosh A1 - Oberländer, Jan A1 - Schöning, Michael Josef T1 - Flexible Calorimetric Gas Sensors for Detection of a Broad Concentration Range of Gaseous Hydrogen Peroxide: A Step Forward to Online Monitoring of Food-Package Sterilization Processes JF - Phys. Status Solidi A N2 - In this study, flexible calorimetric gas sensors are developed for specificdetection of gaseous hydrogen peroxide (H₂O₂) over a wide concentrationrange, which is used in sterilization processes for aseptic packaging industry.The flexibility of these sensors is an advantage for identifying the chemical components of the sterilant on the corners of the food boxes, so-called “coldspots”, as critical locations in aseptic packaging, which are of great importance. These sensors are fabricated on flexible polyimide films by means of thin-film technique. Thin layers of titanium and platinum have been deposited on polyimide to define the conductive structures of the sensors. To detect the high-temperature evaporated H₂O₂, a differential temperature set-up is proposed. The sensors are evaluated in a laboratory-scaled sterilizationsystem to simulate the sterilization process. The concentration range of the evaporated H₂O₂ from 0 to 7.7% v/v was defined and the sensors have successfully detected high as well as low H₂O₂ concentrations with a sensitivity of 5.04 °C/% v/v. The characterizations of the sensors confirm their precise fabrication, high sensitivity and the novelty of low H₂O₂ concentration detections for future inline monitoring of food-package sterilization. Y1 - 2018 U6 - http://dx.doi.org/10.1002/pssa.201800044 VL - 215 IS - 15 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Poghossian, Arshak A1 - Jablonski, Melanie A1 - Koch, Claudia A1 - Bronder, Thomas A1 - Rolka, David A1 - Wege, Christina A1 - Schöning, Michael Josef T1 - Field-effect biosensor using virus particles as scaffolds for enzyme immobilization JF - Biosensors and Bioelectronics N2 - A field-effect biosensor employing tobacco mosaic virus (TMV) particles as scaffolds for enzyme immobilization is presented. Nanotubular TMV scaffolds allow a dense immobilization of precisely positioned enzymes with retained activity. To demonstrate feasibility of this new strategy, a penicillin sensor has been developed by coupling a penicillinase with virus particles as a model system. The developed field-effect penicillin biosensor consists of an Al-p-Si-SiO₂-Ta₂O₅-TMV structure and has been electrochemically characterized in buffer solutions containing different concentrations of penicillin G. In addition, the morphology of the biosensor surface with virus particles was characterized by scanning electron microscopy and atomic force microscopy methods. The sensors possessed a high penicillin sensitivity of ~ 92 mV/dec in a nearly-linear range from 0.1 mM to 10 mM, and a low detection limit of about 50 µM. The long-term stability of the penicillin biosensor was periodically tested over a time period of about one year without any significant loss of sensitivity. The biosensor has also been successfully applied for penicillin detection in bovine milk samples. Y1 - 2018 U6 - http://dx.doi.org/10.1016/j.bios.2018.03.036 SN - 0956-5663 VL - 110 SP - 168 EP - 174 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Miyamoto, Koichiro A1 - Seki, Kosuke A1 - Suto, Takeyuki A1 - Werner, Frederik A1 - Wagner, Torsten A1 - Schöning, Michael Josef A1 - Yoshinobu, Tatsuo T1 - Improved spatial resolution of the chemical imaging sensor with a hybrid illumination that suppresses lateral diffusion of photocarriers JF - Sensor and Actuators B: Chemical N2 - The chemical imaging sensor is a semiconductor-based chemical sensor capable of visualizing pH and ion distributions. The spatial resolution depends on the lateral diffusion of photocarriers generated by illumination of the semiconductor substrate. In this study, two types of optical setups, one based on a bundle of optical fibers and the other based on a binocular tube head, were developed to project a hybrid illumination of a modulated light beam and a ring-shaped constant illumination onto the sensor plate. An improved spatial resolution was realized by the ring-shaped constant illumination, which suppressed lateral diffusion of photocarriers by enhanced recombination due to the increased carrier concentration. Y1 - 2018 U6 - http://dx.doi.org/10.1016/j.snb.2018.07.016 SN - 0925-4005 VL - 273 SP - 1328 EP - 1333 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Röhlen, Desiree A1 - Pilas, Johanna A1 - Dahmen, Markus A1 - Keusgen, Michael A1 - Selmer, Thorsten A1 - Schöning, Michael Josef T1 - Toward a Hybrid Biosensor System for Analysis of Organic and Volatile Fatty Acids in Fermentation Processes JF - Frontiers in Chemistry N2 - Monitoring of organic acids (OA) and volatile fatty acids (VFA) is crucial for the control of anaerobic digestion. In case of unstable process conditions, an accumulation of these intermediates occurs. In the present work, two different enzyme-based biosensor arrays are combined and presented for facile electrochemical determination of several process-relevant analytes. Each biosensor utilizes a platinum sensor chip (14 × 14 mm²) with five individual working electrodes. The OA biosensor enables simultaneous measurement of ethanol, formate, d- and l-lactate, based on a bi-enzymatic detection principle. The second VFA biosensor provides an amperometric platform for quantification of acetate and propionate, mediated by oxidation of hydrogen peroxide. The cross-sensitivity of both biosensors toward potential interferents, typically present in fermentation samples, was investigated. The potential for practical application in complex media was successfully demonstrated in spiked sludge samples collected from three different biogas plants. Thereby, the results obtained by both of the biosensors were in good agreement to the applied reference measurements by photometry and gas chromatography, respectively. The proposed hybrid biosensor system was also used for long-term monitoring of a lab-scale biogas reactor (0.01 m³) for a period of 2 months. In combination with typically monitored parameters, such as gas quality, pH and FOS/TAC (volatile organic acids/total anorganic carbonate), the amperometric measurements of OA and VFA concentration could enhance the understanding of ongoing fermentation processes. Y1 - 2018 U6 - http://dx.doi.org/10.3389/fchem.2018.00284 IS - 6 PB - Frontiers CY - Lausanne ER - TY - JOUR A1 - Rodrigues, Raul T. A1 - Morais, Paulo V. A1 - Nordi, Cristina S. F. A1 - Schöning, Michael Josef A1 - Siqueira Jr., José R. A1 - Caseli, Luciano T1 - Carbon Nanotubes and Algal Polysaccharides To Enhance the Enzymatic Properties of Urease in Lipid Langmuir-Blodgett Films JF - Langmuir N2 - Algal polysaccharides (extracellular polysaccharides) and carbon nanotubes (CNTs) were adsorbed on dioctadecyldimethylammonium bromide Langmuir monolayers to serve as a matrix for the incorporation of urease. The physicochemical properties of the supramolecular system as a monolayer at the air–water interface were investigated by surface pressure–area isotherms, surface potential–area isotherms, interfacial shear rheology, vibrational spectroscopy, and Brewster angle microscopy. The floating monolayers were transferred to hydrophilic solid supports, quartz, mica, or capacitive electrolyte–insulator–semiconductor (EIS) devices, through the Langmuir–Blodgett (LB) technique, forming mixed films, which were investigated by quartz crystal microbalance, fluorescence spectroscopy, and field emission gun scanning electron microscopy. The enzyme activity was studied with UV–vis spectroscopy, and the feasibility of the thin film as a urea sensor was essayed in an EIS sensor device. The presence of CNT in the enzyme–lipid LB film not only tuned the catalytic activity of urease but also helped to conserve its enzyme activity. Viability as a urease sensor was demonstrated with capacitance–voltage and constant capacitance measurements, exhibiting regular and distinctive output signals over all concentrations used in this work. These results are related to the synergism between the compounds on the active layer, leading to a surface morphology that allowed fast analyte diffusion owing to an adequate molecular accommodation, which also preserved the urease activity. This work demonstrates the feasibility of employing LB films composed of lipids, CNT, algal polysaccharides, and enzymes as EIS devices for biosensing applications. Y1 - 2018 U6 - http://dx.doi.org/10.1021/acs.langmuir.7b04317 SN - 1520-5827 VL - 34 IS - 9 SP - 3082 EP - 3093 PB - ACS Publications CY - Washington, DC ER - TY - BOOK A1 - Schöning, Michael Josef A1 - Poghossian, Arshak T1 - Label-free biosensing: advanced materials, devices and applications Y1 - 2018 SN - 978-3-319-75219-8 PB - Springer CY - Cham ER - TY - CHAP A1 - Yoshinobu, Tatsuo A1 - Krause, Steffi A1 - Miyamoto, Ko-ichiro A1 - Werner, Frederik A1 - Poghossian, Arshak A1 - Wagner, Torsten A1 - Schöning, Michael Josef T1 - (Bio-)chemical Sensing and Imaging by LAPS and SPIM T2 - Label-free biosensing: advanced materials, devices and applications N2 - The light-addressable potentiometric sensor (LAPS) and scanning photo-induced impedance microscopy (SPIM) are two closely related methods to visualise the distributions of chemical species and impedance, respectively, at the interface between the sensing surface and the sample solution. They both have the same field-effect structure based on a semiconductor, which allows spatially resolved and label-free measurement of chemical species and impedance in the form of a photocurrent signal generated by a scanning light beam. In this article, the principles and various operation modes of LAPS and SPIM, functionalisation of the sensing surface for measuring various species, LAPS-based chemical imaging and high-resolution sensors based on silicon-on-sapphire substrates are described and discussed, focusing on their technical details and prospective applications. KW - Chemical imaging KW - Field-effect device KW - Light-addressable potentiometric sensor KW - Potentiometry Y1 - 2018 SN - 978-3-319-75219-8 SP - 103 EP - 132 PB - Springer CY - Cham ER - TY - CHAP A1 - Schöning, Michael Josef A1 - Wagner, Torsten A1 - Poghossian, Arshak A1 - Miyamoto, K.I. A1 - Werner, C.F. A1 - Krause, S. A1 - Yoshinobu, T. T1 - Light-addressable potentiometric sensors for (bio-)chemical sensing and imaging T2 - Encyclopedia of Interfacial Chemistry: Surface Science and Electrochemistry. Vol. 7 Y1 - 2018 SN - 9780128097397 SP - 295 EP - 308 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Bäcker, Matthias A1 - Koch, Claudia A1 - Eiben, Sabine A1 - Geiger, Fania A1 - Eber, Fabian A1 - Gliemann, Hartmut A1 - Poghossian, Arshak A1 - Wege, Christina A1 - Schöning, Michael Josef T1 - Tobacco mosaic virus as enzyme nanocarrier for electrochemical biosensors JF - Sensors and Actuators B: Chemical N2 - The conjunction of (bio-)chemical recognition elements with nanoscale biological building blocks such as virus particles is considered as a very promising strategy for the creation of biohybrids opening novel opportunities for label-free biosensing. This work presents a new approach for the development of biosensors using tobacco mosaic virus (TMV) nanotubes or coat proteins (CPs) as enzyme nanocarriers. Sensor chips combining an array of Pt electrodes loaded with glucose oxidase (GOD)-modified TMV nanotubes or CP aggregates were used for amperometric detection of glucose as a model system for the first time. The presence of TMV nanotubes or CPs on the sensor surface allows binding of a high amount of precisely positioned enzymes without substantial loss of their activity, and may also ensure accessibility of their active centers for analyte molecules. Specific and efficient immobilization of streptavidin-conjugated GOD ([SA]-GOD) complexes on biotinylated TMV nanotubes or CPs was achieved via bioaffinity binding. These layouts were tested in parallel with glucose sensors with adsorptively immobilized [SA]-GOD, as well as [SA]-GOD crosslinked with glutardialdehyde, and came out to exhibit superior sensor performance. The achieved results underline a great potential of an integration of virus/biomolecule hybrids with electronic transducers for future applications in biosensorics and biochips. Y1 - 2017 U6 - http://dx.doi.org/10.1016/j.snb.2016.07.096 SN - 0925-4005 VL - 238 SP - 716 EP - 722 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Poghossian, Arshak A1 - Werner, Frederik A1 - Buniatyan, V. V. A1 - Wagner, Torsten A1 - Miamoto, K. A1 - Yoshinobu, T. A1 - Schöning, Michael Josef T1 - Towards addressability of light-addressable potentiometric sensors: Shunting effect of non-illuminated region and cross-talk JF - Sensor and Actuators B: Chemical N2 - The LAPS (light-addressable potentiometric sensor) platform is one of the most attractive approaches for chemical and biological sensing with many applications ranging from pH and ion/analyte concentration measurements up to cell metabolism detection and chemical imaging. However, although it is generally accepted that LAPS measurements are spatially resolved, the light-addressability feature of LAPS devices has not been discussed in detail so far. In this work, an extended electrical equivalent-circuit model of the LAPS has been presented, which takes into account possible cross-talk effects due to the capacitive coupling of the non-illuminated region. A shunting effect of the non-illuminated area on the measured photocurrent and addressability of LAPS devices has been studied. It has been shown, that the measured photocurrent will be determined not only by the local interfacial potential in the illuminated region but also by possible interfacial potential changes in the non-illuminated region, yielding cross-talk effects. These findings were supported by the experimental investigations of a penicillin-sensitive multi-spot LAPS and a metal-insulator-semiconductor LAPS as model systems. Y1 - 2017 U6 - http://dx.doi.org/10.1016/j.snb.2017.01.047 SN - 0925-4005 IS - 244 SP - 1071 EP - 1079 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Katz, Evgeny A1 - Poghossian, Arshak A1 - Schöning, Michael Josef T1 - Enzyme-based logic gates and circuits - analytical applications and interfacing with electronics JF - Analytical and Bioanalytical Chemistry N2 - The paper is an overview of enzyme-based logic gates and their short circuits, with specific examples of Boolean AND and OR gates, and concatenated logic gates composed of multi-step enzyme-biocatalyzed reactions. Noise formation in the biocatalytic reactions and its decrease by adding a “filter” system, converting convex to sigmoid response function, are discussed. Despite the fact that the enzyme-based logic gates are primarily considered as components of future biomolecular computing systems, their biosensing applications are promising for immediate practical use. Analytical use of the enzyme logic systems in biomedical and forensic applications is discussed and exemplified with the logic analysis of biomarkers of various injuries, e.g., liver injury, and with analysis of biomarkers characteristic of different ethnicity found in blood samples on a crime scene. Interfacing of enzyme logic systems with modified electrodes and semiconductor devices is discussed, giving particular attention to the interfaces functionalized with signal-responsive materials. Future perspectives in the design of the biomolecular logic systems and their applications are discussed in the conclusion. Y1 - 2017 U6 - http://dx.doi.org/10.1007/s00216-016-0079-7 SN - 1618-2650 VL - 409 SP - 81 EP - 94 PB - Springer CY - Berlin ER - TY - JOUR A1 - Honarvarfard, Elham A1 - Gamella, Maria A1 - Channaveerappa, Devika A1 - Darie, Costel C. A1 - Poghossian, Arshak A1 - Schöning, Michael Josef A1 - Katz, Evgeny T1 - Electrochemically Stimulated Insulin Release from a Modified Graphene–functionalized Carbon Fiber Electrode JF - Electroanalysis N2 - A graphene-functionalized carbon fiber electrode was modified with adsorbed polyethylenimine to introduce amino functionalities and then with trigonelline and 4-carboxyphenylboronic acid covalently bound to the amino groups. The trigonelline species containing quarterized pyridine groups produced positive charge on the electrode surface regardless of the pH value, while the phenylboronic acid species were neutral below pH 8 and negatively charged above pH 9 (note that their pKa=8.4). The total charge on the monolayer-modified electrode was positive at the neutral pH and negative at pH > 9. Note that 4-carboxyphenylboronic acid was attached to the electrode surface in molar excess to trigonelline, thus allowing the negative charge to dominate on the electrode surface at basic pH. Negatively charged fluorescent dye-labeled insulin (insulin-FITC) was loaded on the modified electrode surface at pH 7.0 due to its electrostatic attraction to the positively charged interface. The local pH in close vicinity to the electrode surface was increased to ca. 9–10 due to consumption of H+ ions upon electrochemical reduction of oxygen proceeding at the potential of −1.0 V (vs. Ag/AgCl) applied on the modified electrode. The process resulted in recharging of the electrode surface to the negative value due to the formation of the negative charge on the phenylboronic acid groups, thus resulting in the electrostatic repulsion of insulin-FITC and stimulating its release from the electrode surface. The insulin release was characterized by fluorescence spectroscopy (using the FITC-labeled insulin), by electrochemical measurements on an iridium oxide, IrOx, electrode and by mass spectrometry. The graphene-functionalized carbon fiber electrode demonstrated significant advantages in the signal-stimulated insulin release comparing with the carbon fiber electrode without the graphene species. Y1 - 2017 U6 - http://dx.doi.org/10.1002/elan.201700095 SN - 1521-4109 VL - 29 IS - 6 SP - 1543 EP - 1553 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Gamella, Maria A1 - Zakharchenko, Andrey A1 - Guz, Nataliia A1 - Masi, Madeline A1 - Minko, Sergiy A1 - Kolpashchikov, Dmitry M. A1 - Iken, Heiko A1 - Poghossian, Arshak A1 - Schöning, Michael Josef A1 - Katz, Evgeny T1 - DNA computing system activated by electrochemically triggered DNA realease from a polymer-brush-modified electrode array JF - Electroanalysis N2 - An array of four independently wired indium tin oxide (ITO) electrodes was used for electrochemically stimulated DNA release and activation of DNA-based Identity, AND and XOR logic gates. Single-stranded DNA molecules were loaded on the mixed poly(N,N-dimethylaminoethyl methacrylate) (PDMAEMA)/poly(methacrylic acid) (PMAA) brush covalently attached to the ITO electrodes. The DNA deposition was performed at pH 5.0 when the polymer brush is positively charged due to protonation of tertiary amino groups in PDMAEMA, thus resulting in electrostatic attraction of the negatively charged DNA. By applying electrolysis at −1.0 V(vs. Ag/AgCl reference) electrochemical oxygen reduction resulted in the consumption of hydrogen ions and local pH increase near the electrode surface. The process resulted in recharging the polymer brush to the negative state due to dissociation of carboxylic groups of PMAA, thus repulsing the negatively charged DNA and releasing it from the electrode surface. The DNA release was performed in various combinations from different electrodes in the array assembly. The released DNA operated as input signals for activation of the Boolean logic gates. The developed system represents a step forward in DNA computing, combining for the first time DNA chemical processes with electronic input signals. Y1 - 2017 U6 - http://dx.doi.org/10.1002/elan.201600389 SN - 1521-4109 VL - 29 IS - 2 SP - 398 EP - 408 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Sousa, Marcos A. M. A1 - Siqueira, Jose R. Jr. A1 - Vercik, Andres A1 - Schöning, Michael Josef A1 - Oliveira, Osvaldo N. Jr. T1 - Determining the optimized layer-by-layer film architecture with dendrimer/carbon nanotubes for field-effect sensors JF - IEEE Sensors Journal N2 - The capacitive electrolyte–insulator–semiconductor (EIS) structure is a typical device based on a field-effect sensor platform. With a simple silicon-based structure, EIS have been useful for several sensing applications, especially with incorporation of nanostructured films to modulate the ionic transport and the flat-band potential. In this paper, we report on ion transport and changes in flat-band potential in EIS sensors made with layer-by-layer films containing poly(amidoamine) (PAMAM) dendrimer and single-walled carbon nanotubes (SWNTs) adsorbed on p-Si/SiO 2 /Ta 2 O 5 chips with an Al ohmic contact. The impedance spectra were fitted using an equivalent circuit model, from which we could determine parameters such as the double-layer capacitance. This capacitance decreased with the number of bilayers owing to space charge accumulated at the electrolyte–insulator interface, up to three PAMAM/SWNTs bilayers, after which it stabilized. The charge-transfer resistance was also minimum for three bilayers, thus indicating that this is the ideal architecture for an optimized EIS performance. The understanding of the influence of nanostructures and the fine control of operation parameters pave the way for optimizing the design and performance of new EIS sensors. Y1 - 2017 U6 - http://dx.doi.org/10.1109/JSEN.2017.2653238 SN - 1558-1748 VL - 17 IS - 6 SP - 1735 EP - 1740 PB - IEEE CY - New York ER - TY - JOUR A1 - Yoshinobu, Tatsuo A1 - Miyamoto, Ko-ichiro A1 - Werner, Frederik A1 - Poghossian, Arshak A1 - Wagner, Torsten A1 - Schöning, Michael Josef T1 - Light-addressable potentiometric sensors for quantitative spatial imaging of chemical species JF - Annual Review of Analytical Chemistry N2 - A light-addressable potentiometric sensor (LAPS) is a semiconductor-based chemical sensor, in which a measurement site on the sensing surface is defined by illumination. This light addressability can be applied to visualize the spatial distribution of pH or the concentration of a specific chemical species, with potential applications in the fields of chemistry, materials science, biology, and medicine. In this review, the features of this chemical imaging sensor technology are compared with those of other technologies. Instrumentation, principles of operation, and various measurement modes of chemical imaging sensor systems are described. The review discusses and summarizes state-of-the-art technologies, especially with regard to the spatial resolution and measurement speed; for example, a high spatial resolution in a submicron range and a readout speed in the range of several tens of thousands of pixels per second have been achieved with the LAPS. The possibility of combining this technology with microfluidic devices and other potential future developments are discussed. Y1 - 2017 U6 - http://dx.doi.org/10.1146/annurev-anchem-061516-045158 SN - 1936-1327 VL - 10 SP - 225 EP - 246 PB - Annual Reviews CY - Palo Alto, Calif. ER - TY - JOUR A1 - Arreola, Julio A1 - Oberländer, Jan A1 - Mätzkow, M. A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Surface functionalization for spore-based biosensors with organosilanes JF - Electrochimica Acta N2 - In the present work, surface functionalization of different sensor materials was studied. Organosilanes are well known to serve as coupling agent for biomolecules or cells on inorganic materials. 3-aminopropyltriethoxysilane (APTES) was used to attach microbiological spores time to an interdigitated sensor surface. The functionality and physical properties of APTES were studied on isolated sensor materials, namely silicon dioxide (SiO2) and platinum (Pt) as well as the combined material on sensor level. A predominant immobilization of spores could be demonstrated on SiO2 surfaces. Additionally, the impedance signal of APTES-functionalized biosensor chips has been investigated. Y1 - 2017 U6 - http://dx.doi.org/10.1016/j.electacta.2017.04.157 SN - 0013-4686 VL - 241 SP - 237 EP - 243 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Bronder, Thomas A1 - Poghossian, Arshak A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Label-free detection of double-stranded DNA molecules with polyelectrolyte-modified capacitive field-effect sensors T1 - Markierungsfreie Detektion doppelsträngiger DNA Moleküle mit Hilfe von Polyelektrolyt-modifizierten kapazitiven Feldeffekt-Sensoren JF - tm - Technisches Messen N2 - In this study, polyelectrolyte-modified field-effect-based electrolyte-insulator-semiconductor (EIS) devices have been used for the label-free electrical detection of double-stranded deoxyribonucleic acid (dsDNA)molecules. The sensor-chip functionalization with a positively charged polyelectrolyte layer provides the possibility of direct adsorptive binding of negatively charged target DNA oligonucleotides onto theSiO2-chip surface.EIS sensors can be utilized as a tool to detect surface-charge changes; the electrostatic adsorption of oligonucleotides onto the polyelectrolyte layer leads to a measureable surface-potential change. Signals of 39mV have been recorded after the incubation with the oligonucleotide solution. Besides the electrochemical experiments, the successful adsorption of dsDNA onto the polyelectrolyte layer has been verified via fluorescence microscopy. The presented results demonstrate that the signal recording of EISchips, which are modified with a polyelectrolyte layer, canbe used as a favorable approach for a fast, cheap and simple detection method for dsDNA. Y1 - 2017 U6 - http://dx.doi.org/10.1515/teme-2017-0015 VL - 84 IS - 10 SP - 628 EP - 634 PB - De Gruyter CY - Oldenbourg ER - TY - CHAP A1 - Oberländer, Jan A1 - Arreola, Julio A1 - Hansen, Christina A1 - Greeff, Anton A1 - Mayer, Marlena A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Impedimetric Biosensor to Enable Fast Evaluation of Gaseous Sterilization Processes T2 - MDPI Proceedings Y1 - 2017 U6 - http://dx.doi.org/10.3390/proceedings1040435 N1 - Eurosensors 2017 Conference, Paris, France, 3–6 September 2017 VL - 1 IS - 4 ER - TY - CHAP A1 - Molinnus, Denise A1 - Hardt, Gabriel A1 - Käver, Larissa A1 - Willenberg, Holger S. A1 - Poghossian, Arshak A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Detection of Adrenaline Based on Bioelectrocatalytical System to Support Tumor Diagnostic Technology T2 - MDPI Proceedings Y1 - 2017 U6 - http://dx.doi.org/10.3390/proceedings1040506 ER - TY - JOUR A1 - Muschallik, Lukas A1 - Molinnus, Denise A1 - Bongaerts, Johannes A1 - Pohl, Martina A1 - Wagner, Torsten A1 - Schöning, Michael Josef A1 - Siegert, Petra A1 - Selmer, Thorsten T1 - (R,R)-Butane-2,3-diol Dehydrogenase from Bacillus clausii DSM 8716T: Cloning and Expression of the bdhA-Gene, and Initial Characterization of Enzyme JF - Journal of Biotechnology N2 - The gene encoding a putative (R,R)-butane-2,3-diol dehydrogenase (bdhA) from Bacillus clausii DSM 8716T was isolated, sequenced and expressed in Escherichia coli. The amino acid sequence of the encoded protein is only distantly related to previously studied enzymes (identity 33–43%) and exhibited some uncharted peculiarities. An N-terminally StrepII-tagged enzyme variant was purified and initially characterized. The isolated enzyme catalyzed the (R)-specific oxidation of (R,R)- and meso-butane-2,3-diol to (R)- and (S)-acetoin with specific activities of 12 U/mg and 23 U/mg, respectively. Likewise, racemic acetoin was reduced with a specific activity of up to 115 U/mg yielding a mixture of (R,R)- and meso-butane-2,3-diol, while the enzyme reduced butane-2,3-dione (Vmax 74 U/mg) solely to (R,R)-butane-2,3-diol via (R)-acetoin. For these reactions only activity with the co-substrates NADH/NAD+ was observed. The enzyme accepted a selection of vicinal diketones, α-hydroxy ketones and vicinal diols as alternative substrates. Although the physiological function of the enzyme in B. clausii remains elusive, the data presented herein clearly demonstrates that the encoded enzyme is a genuine (R,R)-butane-2,3-diol dehydrogenase with potential for applications in biocatalysis and sensor development. Y1 - 2017 U6 - http://dx.doi.org/10.1016/j.jbiotec.2017.07.020 SN - 0168-1656 VL - 258 SP - 41 EP - 50 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Morais, Paulo V. A1 - Gomes, Vanderley F., Jr. A1 - Silva, Anielle C. A. A1 - Dantas, Noelio O. A1 - Schöning, Michael Josef A1 - Siqueira, José R., Jr. T1 - Nanofilm of ZnO nanocrystals/carbon nanotubes as biocompatible layer for enzymatic biosensors in capacitive field-effect devices JF - Journal of Materials Science N2 - The incorporation of nanomaterials that are biocompatible with different types of biological compounds has allowed the development of a new generation of biosensors applied especially in the biomedical field. In particular, the integration of film-based nanomaterials employed in field-effect devices can be interesting to develop biosensors with enhanced properties. In this paper, we studied the fabrication of sensitive nanofilms combining ZnO nanocrystals and carbon nanotubes (CNTs), prepared by means of the layer-by-layer (LbL) technique, in a capacitive electrolyte-insulator-semiconductor (EIS) structure for detecting glucose and urea. The ZnO nanocrystals were incorporated in a polymeric matrix of poly(allylamine) hydrochloride (PAH), and arranged with multi-walled CNTs in a LbL PAH-ZnO/CNTs film architecture onto EIS chips. The electrochemical characterizations were performed by capacitance–voltage and constant capacitance measurements, while the morphology of the films was characterized by atomic force microscopy. The enzymes glucose oxidase and urease were immobilized on film’s surface for detection of glucose and urea, respectively. In order to obtain glucose and urea biosensors with optimized amount of sensitive films, we investigated the ideal number of bilayers for each detection system. The glucose biosensor showed better sensitivity and output signal for an LbL PAH-ZnO/CNTs nanofilm with 10 bilayers. On the other hand, the urea biosensor presented enhanced properties even for the first bilayer, exhibiting high sensitivity and output signal. The presence of the LbL PAH-ZnO/CNTs films led to biosensors with better sensitivity and enhanced response signal, demonstrating that the adequate use of nanostructured films is feasible for proof-of-concept biosensors with improved properties that may be employed for biomedical applications. Y1 - 2017 U6 - http://dx.doi.org/10.1007/s10853-017-1369-y SN - 1573-4803 VL - 52 IS - 20 SP - 12314 EP - 12325 PB - Springer CY - Berlin ER - TY - JOUR A1 - Dantism, Shahriar A1 - Takenaga, Shoko A1 - Wagner, Torsten A1 - Wagner, Patrick A1 - Schöning, Michael Josef T1 - Differential imaging of the metabolism of bacteria and eukaryotic cells based on light-addressable potentiometric sensors JF - Electrochimica Acta N2 - A light-addressable potentiometric sensor (LAPS) is a field-effect-based potentiometric sensor with an electrolyte/insulator/semiconductor (EIS) structure, which is able to monitor analyte concentrations of (bio-)chemical species in aqueous solutions in a spatially resolved way. Therefore, it is also an appropriate tool to record 2D-chemical images of concentration variations on the sensor surface. In the present work, two differential, LAPS-based measurement principles are introduced to determine the metabolic activity of Escherichia coli (E. coli) K12 and Chinese hamster ovary (CHO) cells as test microorganisms. Hereby, we focus on i) the determination of the extracellular acidification rate (ΔpH/min) after adding glucose solutions to the cell suspensions; and ii) recording the amplitude increase of the photocurrent (Iph) related to the produced acids from E. coli K12 bacteria and CHO cells on the sensor surface by 2D-chemical imaging. For this purpose, 3D-printed multi-chamber structures were developed and mounted on the planar sensor-chip surface to define four independent compartments, enabling differential measurements with varying cell concentrations. The differential concept allows eliminating unwanted drift effects and, with the four-chamber structures, measurements on the different cell concentrations were performed simultaneously, thus reducing also the overall measuring time. Y1 - 2017 U6 - http://dx.doi.org/10.1016/j.electacta.2017.05.196 SN - 0013-4686 VL - 246 SP - 234 EP - 241 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Jildeh, Zaid B. A1 - Kirchner, Patrick A1 - Oberländer, Jan A1 - Kremers, Alexander A1 - Wagner, Torsten A1 - Wagner, Patrick H. A1 - Schöning, Michael Josef T1 - FEM-based modeling of a calorimetric gas sensor for hydrogen peroxide monitoring JF - physica status solidi a : applications and materials sciences N2 - A physically coupled finite element method (FEM) model is developed to study the response behavior of a calorimetric gas sensor. The modeled sensor serves as a monitoring device of the concentration of gaseous hydrogen peroxide (H2 O2) in a high temperature mixture stream in aseptic sterilization processes. The principle of operation of a calorimetric H2 O2 sensor is analyzed and the results of the numerical model have been validated by using previously published sensor experiments. The deviation in the results between the FEM model and experimental data are presented and discussed. Y1 - 2017 U6 - http://dx.doi.org/10.1002/pssa.201600912 SN - 1862-6319 IS - Early View PB - Wiley-VCH CY - Weinheim ER - 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 - CHAP A1 - Poghossian, Arshak A1 - Schöning, Michael Josef T1 - Nanomaterial-Modified Capacitive Field-Effect Biosensors T2 - Springer Series on Chemical Sensors and Biosensors (Methods and Applications) N2 - The coupling of charged molecules, nanoparticles, and more generally, inorganic/organic nanohybrids with semiconductor field-effect devices based on an electrolyte–insulator–semiconductor (EIS) system represents a very promising strategy for the active tuning of electrochemical properties of these devices and, thus, opening new opportunities for label-free biosensing by the intrinsic charge of molecules. The simplest field-effect sensor is a capacitive EIS sensor, which represents a (bio-)chemically sensitive capacitor. In this chapter, selected examples of recent developments in the field of label-free biosensing using nanomaterial-modified capacitive EIS sensors are summarized. In the first part, we present applications of EIS sensors modified with negatively charged gold nanoparticles for the label-free electrostatic detection of positively charged small proteins and macromolecules, for monitoring the layer-by-layer formation of oppositely charged polyelectrolyte (PE) multilayers as well as for the development of an enzyme-based biomolecular logic gate. In the second part, examples of a label-free detection by means of EIS sensors modified with a positively charged weak PE layer are demonstrated. These include electrical detection of on-chip and in-solution hybridized DNA (deoxyribonucleic acid) as well as an EIS sensor with pH-responsive weak PE/enzyme multilayers for enhanced field-effect biosensing. KW - Biomolecular logic gate KW - DNA KW - Enzyme biosensor KW - Field-effect sensor KW - Gold nanoparticle Y1 - 2017 U6 - http://dx.doi.org/10.1007/5346_2017_2 SP - 1 EP - 25 PB - Springer CY - Berlin, Heidelberg ER - TY - JOUR A1 - Arreola, Julio A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Effect of O2 plasma on properties of electrolyte-insulator-semiconductor structures JF - physica status solidi a : applications and materials sciences N2 - Prior to immobilization of biomolecules or cells onto biosensor surfaces, the surface must be physically or chemically activated for further functionalization. Organosilanes are a versatile option as they facilitate the immobilization through their terminal groups and also display self-assembly. Incorporating hydroxyl groups is one of the important methods for primary immobilization. This can be done, for example, with oxygen plasma treatment. However, this treatment can affect the performance of the biosensors and this effect is not quite well understood for surface functionalization. In this work, the effect of O2 plasma treatment on EIS sensors was investigated by means of electrochemical characterizations: capacitance–voltage (C–V) and constant capacitance (ConCap) measurements. After O2 plasma treatment, the potential of the EIS sensor dramatically shifts to a more negative value. This was successfully reset by using an annealing process. KW - surface functionalization KW - O2 plasma KW - hydroxylation KW - electrolyte-insulator semiconductor sensor (EIS) KW - annealing Y1 - 2017 U6 - http://dx.doi.org/10.1002/pssa.201700025 SN - 1862-6319 VL - 214 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Miyamoto, Ko-ichiro A1 - Hayashi, Kosuke A1 - Sakamoto, Azuma A1 - Werner, Frederik A1 - Wagner, Torsten A1 - Schöning, Michael Josef A1 - Yoshinobu, Tatsuo T1 - A high-Q resonance-mode measurement of EIS capacitive sensor by elimination of series resistance JF - Sensor and Actuators B: Chemical N2 - An EIS capacitive sensor is a semiconductor-based potentiometric sensor, which is sensitive to the ion concentration or pH value of the solution in contact with the sensing surface. To detect a small change in the ion concentration or pH, a small capacitance change must be detected. Recently, a resonance-mode measurement was proposed, in which an inductor was connected to the EIS capacitive sensor and the resonant frequency was correlated with the pH value. In this study, the Q factor of the resonant circuit was enhanced by canceling the internal resistance of the reference electrode and the internal resistance of the inductor coil with the help of a bypass capacitor and a negative impedance converter, respectively. 1% variation of the signal in the developed system corresponded to a pH change of 3.93 mpH, which was about 1/12 of the conventional method, suggesting a better performance in detection of a small pH change. KW - Negative impedance convertor KW - Resonance-mode measurement KW - Chemical sensor KW - EIS capacitive sensor Y1 - 2017 U6 - http://dx.doi.org/10.1016/j.snb.2017.03.002 SN - 0925-4005 VL - 248 SP - 1006 EP - 1010 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Werner, Frederik A1 - Miyamoto, Ko-ichiro A1 - Wagner, Torsten A1 - Schöning, Michael Josef A1 - Yoshinobu, Tatsuo T1 - Lateral resolution enhancement of pulse-driven light-addressable potentiometric sensor JF - Sensor and Actuators B: Chemical N2 - To study chemical and biological processes, spatially resolved determination of the concentrations of one or more analyte species is of distinct interest. With a light-addressable potentiometric sensor (LAPS), chemical images can be created, which visualize the concentration distribution above the sensor plate. One important challenge is to achieve a good lateral resolution in order to detect events that take place in a small and limited region. LAPS utilizes a focused light spot to address the measurement region. By moving this light spot along the semiconductor sensor plate, the concentration distribution can be observed. In this study, we show that utilizing a pulse as light excitation instead of a traditionally used continuously modulated light excitation, the lateral resolution can be improved by a factor of 6 or more. KW - Chemical images KW - LAPS KW - Light-addressable potentiometric sensor Y1 - 2017 U6 - http://dx.doi.org/10.1016/j.snb.2017.02.057 SN - 0925-4005 VL - 248 SP - 961 EP - 965 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Scholl, Fabio A1 - Morais, Paulo A1 - Gabriel, Rayla A1 - Schöning, Michael Josef A1 - Siqueira, Jose Roberto, Jr. A1 - Caseli, Luciano T1 - Carbon nanotubes arranged as smart interfaces in lipid Langmuir-Blodgett films enhancing the enzymatic properties of penicillinase for biosensing applications JF - Applied Materials & Interfaces N2 - In this paper, carbon nanotubes (CNTs) were incorporated in penicillinase-phospholipid Langmuir and Langmuir–Blodgett (LB) films to enhance the enzyme catalytic properties. Adsorption of the penicillinase and CNTs at dimyristoylphosphatidic acid (DMPA) monolayers at the air–water interface was investigated by surface pressure–area isotherms, vibrational spectroscopy, and Brewster angle microscopy. The floating monolayers were transferred to solid supports through the LB technique, forming mixed DMPA-CNTs-PEN films, which were investigated by quartz crystal microbalance, vibrational spectroscopy, and atomic force microscopy. Enzyme activity was studied with UV–vis spectroscopy and the feasibility of the supramolecular device nanostructured as ultrathin films were essayed in a capacitive electrolyte–insulator–semiconductor (EIS) sensor device. The presence of CNTs in the enzyme–lipid LB film not only tuned the catalytic activity of penicillinase but also helped conserve its enzyme activity after weeks, showing increased values of activity. Viability as penicillin sensor was demonstrated with capacitance/voltage and constant capacitance measurements, exhibiting regular and distinctive output signals over all concentrations used in this work. These results may be related not only to the nanostructured system provided by the film, but also to the synergism between the compounds on the active layer, leading to a surface morphology that allowed a fast analyte diffusion because of an adequate molecular accommodation, which also preserved the penicillinase activity. This work therefore demonstrates the feasibility of employing LB films composed of lipids, CNTs, and enzymes as EIS devices for biosensing applications. Y1 - 2017 U6 - http://dx.doi.org/10.1021/acsami.7b08095 SN - 1944-8252 VL - 9 IS - 36 SP - 31054 EP - 31066 PB - ACS CY - Washington ER - TY - JOUR A1 - Honarvarfard, Elham A1 - Gamella, Maria A1 - Poghossian, Arshak A1 - Schöning, Michael Josef A1 - Katz, Evgeny T1 - An enzyme-based reversible Controlled NOT (CNOT) logic gate operating on a semiconductor transducer JF - Applied Materials Today N2 - An enzyme-based biocatalytic system mimicking operation of a logically reversible Controlled NOT (CNOT) gate has been interfaced with semiconductor electronic transducers. Electrolyte–insulator–semiconductor (EIS) structures have been used to transduce chemical changes produced by the enzyme system to an electronically readable capacitive output signal using field-effect features of the EIS device. Two enzymes, urease and esterase, were immobilized on the insulating interface of EIS structure producing local pH changes performing XOR logic operation controlled by various combinations of the input signals represented by urea and ethyl butyrate. Another EIS transducer was functionalized with esterase only, thus performing Identity (ID) logic operation for the ethyl butyrate input. Both semiconductor devices assembled in parallel operated as a logically reversible CNOT gate. The present system, despite its simplicity, demonstrated for the first time logically reversible function of the enzyme system transduced electronically with the semiconductor devices. The biomolecular realization of a CNOT gate interfaced with semiconductors is promising for integration into complex biomolecular networks and future biosensor/biomedical applications. KW - Electrolyte–insulator–semiconductor KW - Capacitive field-effect KW - CNOT KW - XOR KW - Enzyme logic gate Y1 - 2017 U6 - http://dx.doi.org/10.1016/j.apmt.2017.08.003 SN - 2352-9407 VL - 9 SP - 266 EP - 270 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Röhlen, Desiree A1 - Pilas, Johanna A1 - Schöning, Michael Josef A1 - Selmer, Thorsten T1 - Development of an amperometric biosensor platform for the combined determination of l-Malic, Fumaric, and l-Aspartic acid JF - Applied Biochemistry and Biotechnology N2 - Three amperometric biosensors have been developed for the detection of L-malic acid, fumaric acid, and L -aspartic acid, all based on the combination of a malate-specific dehydrogenase (MDH, EC 1.1.1.37) and diaphorase (DIA, EC 1.8.1.4). The stepwise expansion of the malate platform with the enzymes fumarate hydratase (FH, EC 4.2.1.2) and aspartate ammonia-lyase (ASPA, EC 4.3.1.1) resulted in multi-enzyme reaction cascades and, thus, augmentation of the substrate spectrum of the sensors. Electrochemical measurements were carried out in presence of the cofactor β-nicotinamide adenine dinucleotide (NAD+) and the redox mediator hexacyanoferrate (III) (HCFIII). The amperometric detection is mediated by oxidation of hexacyanoferrate (II) (HCFII) at an applied potential of + 0.3 V vs. Ag/AgCl. For each biosensor, optimum working conditions were defined by adjustment of cofactor concentrations, buffer pH, and immobilization procedure. Under these improved conditions, amperometric responses were linear up to 3.0 mM for L-malate and fumarate, respectively, with a corresponding sensitivity of 0.7 μA mM−1 (L-malate biosensor) and 0.4 μA mM−1 (fumarate biosensor). The L-aspartate detection system displayed a linear range of 1.0–10.0 mM with a sensitivity of 0.09 μA mM−1. The sensor characteristics suggest that the developed platform provides a promising method for the detection and differentiation of the three substrates. Y1 - 2017 U6 - http://dx.doi.org/10.1007/s12010-017-2578-1 SN - 1559-0291 VL - 183 SP - 566 EP - 581 PB - Springer CY - Berlin ER - TY - JOUR A1 - Pilas, Johanna A1 - Yazici, Yasemen A1 - Selmer, Thorsten A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Optimization of an amperometric biosensor array for simultaneous measurement of ethanol, formate, d- and l-lactate JF - Electrochimica Acta N2 - The immobilization of NAD+-dependent dehydrogenases, in combination with a diaphorase, enables the facile development of multiparametric sensing devices. In this work, an amperometric biosensor array for simultaneous determination of ethanol, formate, d- and l-lactate is presented. Enzyme immobilization on platinum thin-film electrodes was realized by chemical cross-linking with glutaraldehyde. The optimization of the sensor performance was investigated with regard to enzyme loading, glutaraldehyde concentration, pH, cofactor concentration and temperature. Under optimal working conditions (potassium phosphate buffer with pH 7.5, 2.5 mmol L-1 NAD+, 2.0 mmol L-1 ferricyanide, 25 °C and 0.4% glutaraldehyde) the linear working range and sensitivity of the four sensor elements was improved. Simultaneous and cross-talk free measurements of four different metabolic parameters were performed successfully. The reliable analytical performance of the biosensor array was demonstrated by application in a clarified sample of inoculum sludge. Thereby, a promising approach for on-site monitoring of fermentation processes is provided. KW - Simultaneous determination KW - Enzymatic biosensor KW - Diaphorase KW - Dehydrogenase Y1 - 2017 U6 - http://dx.doi.org/10.1016/j.electacta.2017.07.119 SN - 0013-4686 VL - 251 SP - 256 EP - 262 PB - Elsevier CY - Amsterdam ER -