TY - JOUR A1 - Mennicken, Max A1 - Peter, Sophia K. A1 - Kaulen, Corinna A1 - Simon, Ulrich A1 - Karthäuser, Silvia T1 - Transport through Redox-Active Ru-Terpyridine Complexes Integrated in Single Nanoparticle Devices JF - The Journal of Physical Chemistry C N2 - Transition metal complexes are electrofunctional molecules due to their high conductivity and their intrinsic switching ability involving a metal-to-ligand charge transfer. Here, a method is presented to contact reliably a few to single redox-active Ru-terpyridine complexes in a CMOS compatible nanodevice and preserve their electrical functionality. Using hybrid materials from 14 nm gold nanoparticles (AuNP) and bis-{4′-[4-(mercaptophenyl)-2,2′:6′,2″-terpyridine]}-ruthenium(II) complexes a device size of 30² nm² inclusive nanoelectrodes is achieved. Moreover, this method bears the opportunity for further downscaling. The Ru-complex AuNP devices show symmetric and asymmetric current versus voltage curves with a hysteretic characteristic in two well separated conductance ranges. By theoretical approximations based on the single-channel Landauer model, the charge transport through the formed double-barrier tunnel junction is thoroughly analyzed and its sensibility to the molecule/metal contact is revealed. It can be verified that tunneling transport through the HOMO is the main transport mechanism while decoherent hopping transport is present to a minor extent. Y1 - 2020 U6 - http://dx.doi.org/10.1021/acs.jpcc.9b11716 SN - 1932-7455 VL - 124 IS - 8 SP - 4881 EP - 4889 PB - ACS Publications CY - Washington, DC ER - TY - JOUR A1 - Muschallik, Lukas A1 - Kipp, Carina Ronja A1 - Recker, Inga A1 - Bongaerts, Johannes A1 - Pohl, Martina A1 - Gelissen, Melanie A1 - Schöning, Michael Josef A1 - Selmer, Thorsten A1 - Siegert, Petra T1 - Synthesis of α-hydroxy ketones and vicinal diols with the Bacillus licheniformis DSM 13T butane-2, 3-diol dehydrogenase JF - Journal of Biotechnology N2 - The enantioselective synthesis of α-hydroxy ketones and vicinal diols is an intriguing field because of the broad applicability of these molecules. Although, butandiol dehydrogenases are known to play a key role in the production of 2,3-butandiol, their potential as biocatalysts is still not well studied. Here, we investigate the biocatalytic properties of the meso-butanediol dehydrogenase from Bacillus licheniformis DSM 13T (BlBDH). The encoding gene was cloned with an N-terminal StrepII-tag and recombinantly overexpressed in E. coli. BlBDH is highly active towards several non-physiological diketones and α-hydroxyketones with varying aliphatic chain lengths or even containing phenyl moieties. By adjusting the reaction parameters in biotransformations the formation of either the α-hydroxyketone intermediate or the diol can be controlled. Y1 - 2020 SN - 2590-1559 U6 - http://dx.doi.org/10.1016/j.jbiotec.2020.09.016 VL - 202 IS - Vol. 324 SP - 61 EP - 70 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Muschallik, Lukas A1 - Molinnus, Denise A1 - Jablonski, Melanie A1 - Kipp, Carina Ronja A1 - Bongaerts, Johannes A1 - Pohl, Martina A1 - Wagner, Torsten A1 - Schöning, Michael Josef A1 - Selmer, Thorsten A1 - Siegert, Petra T1 - Synthesis of α-hydroxy ketones and vicinal (R, R)-diols by Bacillus clausii DSM 8716ᵀ butanediol dehydrogenase JF - RSC Advances N2 - α-hydroxy ketones (HK) and 1,2-diols are important building blocks for fine chemical synthesis. Here, we describe the R-selective 2,3-butanediol dehydrogenase from B. clausii DSM 8716ᵀ (BcBDH) that belongs to the metal-dependent medium chain dehydrogenases/reductases family (MDR) and catalyzes the selective asymmetric reduction of prochiral 1,2-diketones to the corresponding HK and, in some cases, the reduction of the same to the corresponding 1,2-diols. Aliphatic diketones, like 2,3-pentanedione, 2,3-hexanedione, 5-methyl-2,3-hexanedione, 3,4-hexanedione and 2,3-heptanedione are well transformed. In addition, surprisingly alkyl phenyl dicarbonyls, like 2-hydroxy-1-phenylpropan-1-one and phenylglyoxal are accepted, whereas their derivatives with two phenyl groups are not substrates. Supplementation of Mn²⁺ (1 mM) increases BcBDH's activity in biotransformations. Furthermore, the biocatalytic reduction of 5-methyl-2,3-hexanedione to mainly 5-methyl-3-hydroxy-2-hexanone with only small amounts of 5-methyl-2-hydroxy-3-hexanone within an enzyme membrane reactor is demonstrated. Y1 - 2020 U6 - http://dx.doi.org/10.1039/D0RA02066D SN - 2046-2069 VL - 10 SP - 12206 EP - 12216 PB - Royal Society of Chemistry (RSC) CY - Cambridge ER - TY - THES A1 - Achtsnicht, Stefan T1 - Multiplex-Magnetdetektion von superparamagnetischen Beads zur Identifizierung von Trinkwasserkontaminationen N2 - Die qualitative und quantitative Detektion von Zielsubstanzen innerhalb einer wässrigen Probe ist für viele Fragestellungen von Interesse, etwa bei der Detektion von Kontaminationen in Trinkwasser in Krisensituationen. Hierbei ist es nicht nur wichtig, dass Pathogene möglichst sensitiv detektiert werden können, sondern auch, dass die Analyse schnell erfolgt, um Betroffenen im Katastrophenfall zügig sicheres Trinkwasser zu Verfügung stellen zu können. Da bei einem solchen Szenario nicht von einer in der Nähe befindlichen funktionierenden Laborinfrastruktur ausgegangen werden kann, ist es wichtig, dass die Messung direkt vor Ort erfolgen kann. Im Rahmen dieser Arbeit wurde untersucht, ob eine derartige Schnellanalytik mithilfe von superparamagnetischen Beads (MBs) und der magnetischen Frequenzmischtechnik möglich ist. Dabei werden die MBs mit Hilfe von primären Antikörpern an die Zielsubstanz gebunden und mit sekundären Antikörpern an die Poren-Oberfläche eines Polyethylen-Filters fixiert (Sandwich-Immunoassay). So kann die Quantifizierung der Zielsubstanz auf eine magnetische Messung der immobilisierten MB-Marker zurückgeführt werden. Die magnetische Frequenzmischtechnik basiert auf der Anregung der Probe mit Magnetfeldern zweier verschiedener Frequenzen. Die durch die nichtlineare Magnetisierungsform der superparamagnetischen MBs entstehenden Mischfrequenzen werden typischerweise mithilfe einer zweistufigen Lock-in-Detektion analysiert (analoge Demodulation), die in einem Magnetreader als Handheldgerät realisiert wurde. Zusätzlich zu dieser Technik wurde das Prinzip der direkten Digitalisierung des gesamten Antwortsignals mit anschließender Fourier-Analyse der erzeugten Mischfrequenzen experimentell umgesetzt, um die Amplituden und Phasen mehrerer Mischfrequenzen simultan zu erfassen. Eine Möglichkeit zur Sensitivitätssteigerung ist die magnetische Aufkonzentration, indem vor der magnetischen Analyse eine Separation der MBs aus einem größeren Probenvolumen mittels magnetischem Feldgradienten durchgeführt wird. Zur Charakterisierung verschiedener kommerzieller MBs hinsichtlich ihrer magnetischen Separierbarkeit wurde ein Aufbau zur Messung ihrer magnetophoretischen Beweglichkeiten realisiert und ihre Geschwindigkeiten im Gradientenfeld mikroskopisch gemessen.Da eine Probe oftmals nicht nur auf eine einzige Zielsubstanz, sondern simultan auf mehrere verschiedene Pathogene hin untersucht werden soll, wurden verschiedene Ansätze entwickelt und getestet, die einen solchen multiparametrischen magnetischen Immunoassay ermöglichen. Einerseits wurde eine räumliche Separation der Bindungsbereiche für verschiedene Zielsubstanzen realisiert, die sequentiell ausgewertet werden können. Andererseits wurde die Unterscheidung von verschiedenen Zielsubstanzen anhand der Charakteristika der an sie gebundenen, verschieden funktionalisierten MB-Typen untersucht. Für eine solche Unterscheidung wurde zum einen die Anregefrequenz der magnetischen Frequenzmischtechnik während einer Messung variiert. Damit konnte gezeigt werden, dass sich verschiedene MB-Sorten anhand der Phase ihrer Frequenzmischsignale voneinander unterscheiden lassen. Weiterhin wurde gezeigt, dass sich der Signalverlauf einer binären Mischung zweier verschiedener MB-Typen als gradueller Übergang der Verläufe der beiden reinen MB-Lösungen ergibt. Eine weitere Analysemethode für einen multiparametrischen Immunoassay besteht darin, ein zusätzliches einstellbares statisches magnetisches Offsetfeld zu verwenden. Hierfür wurden mehrere Aufbauten auf Basis von Permanent- und Elektromagneten simuliert, konstruiert und charakterisiert. Mithilfe von Simulationen konnte gezeigt werden, dass eine auf diesem Verfahren beruhende Unterscheidung für MBs mit unterschiedlichen magnetischen Partikelmomenten möglich ist. Als direkte Anwendung des hier entwickelten Magnetreaders in Zusammenspiel mit der digitalen Demodulation wurde ein magnetischer Assay gegen die B-Untereinheit des Choleratoxins in Trinkwasser mit einem niedrigen Detektionslimit von 0,2 ng/ml demonstriert. N2 - The qualitative and quantitative detection of target substances in an aqueous sample is of interest for many questions, for example in the detection of contaminations in drinking water in crisis situations. It is not only important that pathogens can be detected with highest possible sensitivity, but also that the analysis is carried out quickly so that safe drinking water can be provided in the event of a disaster. During such a scenario one cannot rely on a functioning laboratory infrastructure nearby. Therefore it is important that the measurement can be carried out directly on site. Within the scope of this work, it was investigated whether such a quick analysis can be performed using superparamagnetic beads (MBs) and the magnetic frequency mixing technique. The MBs are bound to the target substance with the aid of primary antibodies and fixed to the pore surfaces of a polyethylene filter with secondary antibodies (sandwich immunoassay). The quantification of the target substance can thus be traced back to a magnetic measurement of the immobilized MB markers. The magnetic frequency mixing technique is based on the excitation of the sample with magnetic fields of two different frequencies. The mixing frequencies generated due to the non-linear shape of the magnetization of the superparamagnetic MBs are typically analyzed using a two-stage Lock-in detection (analog demodulation), which was implemented in a magnetic reader as a handheld device. In addition to this technique, the principle of direct digitization of the entire response signal with subsequent Fourier analysis of the generated mixing frequencies was experimentally implemented in order to simultaneously record the amplitudes and phases of several mixing frequencies. One possibility for increasing the sensitivity is magnetic concentration. In that case, the MBs are separated from a larger sample volume by means of a magnetic field gradient before the magnetic analysis. To characterize various commercial MBs with regard to their magnetic separability, a setup for measuring their magnetophoretic mobility was implemented and their velocities in the gradient field were measured with an optical microscope.Often, a sample has to be examined not only for a single target substance, but for several different pathogens simultaneously. Various approaches have been developed and tested which enable such a multiparametric magnetic immunoassay. On the one hand, a spatial separation of the binding areas for different target substances was realized, which can be evaluated sequentially. On the other hand, a distinction among different target substances based on the magnetic characteristics of their attached different MB types was examined. For this discrimination, the excitation frequency of the magnetic frequency mixing technology was varied during measurement. It is shown that different MB types can be distinguished from one another based on the phase of their frequency mixing signals. The signal curve of a binary mixture of two different MB types is obtained as a gradual transition of the curves of the two pure MB solutions. Another method of analysis for a multiparametric immunoassay is based on an additional adjustable static magnetic offset field. For this purpose, several setups based on permanent magnets and electromagnets were simulated, designed and characterized. The simulations show that a distinction based on this method is possible for MBs with different magnetic particle moments. As a direct application of the developed magnetic reader in conjunction with digital demodulation, a magnetic assay against the B subunit of cholera toxin in drinking water was demonstrated, and a low detection limit of 0.2 ng/ml was achieved. KW - Choleratoxin B KW - Trinkwassersicherheit KW - cholera toxin B KW - drinking water safety KW - magnetic frequency mixing technique Y1 - 2020 U6 - http://dx.doi.org/10.18154/RWTH-2020-12052 N1 - Dissertation, RWTH Aachen University, 2020 ER - TY - BOOK A1 - Yoshinobu, Tatsuo A1 - Schöning, Michael Josef ED - Yoshinobu, Tatsuo ED - Schöning, Michael Josef T1 - Light-addressing and chemical imaging technologies for electrochemical sensing Y1 - 2020 SN - 978-3-03943-029-1 U6 - http://dx.doi.org/10.3390/books978-3-03943-029-1 N1 - This book is a printed edition of the Special Issue Light-Addressing and Chemical Imaging Technologies for Electrochemical Sensing that was published in Sensors PB - MDPI CY - Basel ER - TY - JOUR A1 - Welden, Rene A1 - Schöning, Michael Josef A1 - Wagner, Patrick H. A1 - Wagner, Torsten T1 - Light-Addressable Electrodes for Dynamic and Flexible Addressing of Biological Systems and Electrochemical Reactions JF - Sensors N2 - In this review article, we are going to present an overview on possible applications of light-addressable electrodes (LAE) as actuator/manipulation devices besides classical electrode structures. For LAEs, the electrode material consists of a semiconductor. Illumination with a light source with the appropiate wavelength leads to the generation of electron-hole pairs which can be utilized for further photoelectrochemical reaction. Due to recent progress in light-projection technologies, highly dynamic and flexible illumination patterns can be generated, opening new possibilities for light-addressable electrodes. A short introduction on semiconductor–electrolyte interfaces with light stimulation is given together with electrode-design approaches. Towards applications, the stimulation of cells with different electrode materials and fabrication designs is explained, followed by analyte-manipulation strategies and spatially resolved photoelectrochemical deposition of different material types. Y1 - 2020 U6 - http://dx.doi.org/10.3390/s20061680 SN - 1424-8220 VL - 20 IS - 6 PB - MDPI CY - Basel ER - TY - JOUR A1 - Dantism, Shahriar A1 - Röhlen, Desiree A1 - Dahmen, Markus A1 - Wagner, Torsten A1 - Wagner, Patrick A1 - Schöning, Michael Josef T1 - LAPS-based monitoring of metabolic responses of bacterial cultures in a paper fermentation broth JF - Sensors and Actuators B: Chemical N2 - As an alternative renewable energy source, methane production in biogas plants is gaining more and more attention. Biomass in a bioreactor contains different types of microorganisms, which should be considered in terms of process-stability control. Metabolically inactive microorganisms within the fermentation process can lead to undesirable, time-consuming and cost-intensive interventions. Hence, monitoring of the cellular metabolism of bacterial populations in a fermentation broth is crucial to improve the biogas production, operation efficiency, and sustainability. In this work, the extracellular acidification of bacteria in a paper-fermentation broth is monitored after glucose uptake, utilizing a differential light-addressable potentiometric sensor (LAPS) system. The LAPS system is loaded with three different model microorganisms (Escherichia coli, Corynebacterium glutamicum, and Lactobacillus brevis) and the effect of the fermentation broth at different process stages on the metabolism of these bacteria is studied. In this way, different signal patterns related to the metabolic response of microorganisms can be identified. By means of calibration curves after glucose uptake, the overall extracellular acidification of bacterial populations within the fermentation process can be evaluated. Y1 - 2020 U6 - http://dx.doi.org/10.1016/j.snb.2020.128232 SN - 0925-4005 VL - 320 IS - Art. 128232 PB - Elsevier CY - Amsterdam ER - TY - THES A1 - Bronder, Thomas T1 - Label-free detection of tuberculosis DNA with capacitive field-effect biosensors Y1 - 2020 U6 - http://dx.doi.org/10.17192/z2021.0056 N1 - Dissertation, Universität, Marburg 2020 PB - Philipps-Universität Marburg CY - Marburg ER - TY - JOUR A1 - Poghossian, Arshak A1 - Jablonski, Melanie A1 - Molinnus, Denise A1 - Wege, Christina A1 - Schöning, Michael Josef T1 - Field-Effect Sensors for Virus Detection: From Ebola to SARS-CoV-2 and Plant Viral Enhancers JF - Frontiers in Plant Science N2 - Coronavirus disease 2019 (COVID-19) is a novel human infectious disease provoked by severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). Currently, no specific vaccines or drugs against COVID-19 are available. Therefore, early diagnosis and treatment are essential in order to slow the virus spread and to contain the disease outbreak. Hence, new diagnostic tests and devices for virus detection in clinical samples that are faster, more accurate and reliable, easier and cost-efficient than existing ones are needed. Due to the small sizes, fast response time, label-free operation without the need for expensive and time-consuming labeling steps, the possibility of real-time and multiplexed measurements, robustness and portability (point-of-care and on-site testing), biosensors based on semiconductor field-effect devices (FEDs) are one of the most attractive platforms for an electrical detection of charged biomolecules and bioparticles by their intrinsic charge. In this review, recent advances and key developments in the field of label-free detection of viruses (including plant viruses) with various types of FEDs are presented. In recent years, however, certain plant viruses have also attracted additional interest for biosensor layouts: Their repetitive protein subunits arranged at nanometric spacing can be employed for coupling functional molecules. If used as adapters on sensor chip surfaces, they allow an efficient immobilization of analyte-specific recognition and detector elements such as antibodies and enzymes at highest surface densities. The display on plant viral bionanoparticles may also lead to long-time stabilization of sensor molecules upon repeated uses and has the potential to increase sensor performance substantially, compared to conventional layouts. This has been demonstrated in different proof-of-concept biosensor devices. Therefore, richly available plant viral particles, non-pathogenic for animals or humans, might gain novel importance if applied in receptor layers of FEDs. These perspectives are explained and discussed with regard to future detection strategies for COVID-19 and related viral diseases. Y1 - 2020 U6 - http://dx.doi.org/10.3389/fpls.2020.598103 VL - 11 IS - Article 598103 SP - 1 EP - 14 PB - Frontiers CY - Lausanne ER - TY - JOUR A1 - Özsoylu, Dua A1 - Kizildag, Sefa A1 - Schöning, Michael Josef A1 - Wagner, Torsten T1 - Differential chemical imaging of extracellular acidification within microfluidic channels using a plasma-functionalized light-addressable potentiometric sensor (LAPS) JF - Physics in Medicine N2 - Extracellular acidification is a basic indicator for alterations in two vital metabolic pathways: glycolysis and cellular respiration. Measuring these alterations by monitoring extracellular acidification using cell-based biosensors such as LAPS plays an important role in studying these pathways whose disorders are associated with numerous diseases including cancer. However, the surface of the biosensors must be specially tailored to ensure high cell compatibility so that cells can represent more in vivo-like behavior, which is critical to gain more realistic in vitro results from the analyses, e.g., drug discovery experiments. In this work, O2 plasma patterning on the LAPS surface is studied to enhance surface features of the sensor chip, e.g., wettability and biofunctionality. The surface treated with O2 plasma for 30 s exhibits enhanced cytocompatibility for adherent CHO–K1 cells, which promotes cell spreading and proliferation. The plasma-modified LAPS chip is then integrated into a microfluidic system, which provides two identical channels to facilitate differential measurements of the extracellular acidification of CHO–K1 cells. To the best of our knowledge, it is the first time that extracellular acidification within microfluidic channels is quantitatively visualized as differential (bio-)chemical images. Y1 - 2020 U6 - http://dx.doi.org/10.1016/j.phmed.2020.100030 SN - 2352-4510 VL - 10 IS - 100030 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Jildeh, Zaid B. A1 - Kirchner, Patrick A1 - Oberländer, Jan A1 - Vahidpour, Farnoosh A1 - Wagner, Patrick H. A1 - Schöning, Michael Josef T1 - Development of a package-sterilization process for aseptic filling machines: A numerical approach and validation for surface treatment with hydrogen peroxide JF - Sensor and Actuators A: Physical N2 - Within the present work a sterilization process by a heated gas mixture that contains hydrogen peroxide (H₂O₂) is validated by experiments and numerical modeling techniques. The operational parameters that affect the sterilization efficacy are described alongside the two modes of sterilization: gaseous and condensed H₂O₂. Measurements with a previously developed H₂O₂ gas sensor are carried out to validate the applied H₂O₂ gas concentration during sterilization. We performed microbiological tests at different H₂O₂ gas concentrations by applying an end-point method to carrier strips, which contain different inoculation loads of Geobacillus stearothermophilus spores. The analysis of the sterilization process of a pharmaceutical glass vial is performed by numerical modeling. The numerical model combines heat- and advection-diffusion mass transfer with vapor–pressure equations to predict the location of condensate formation and the concentration of H₂O₂ at the packaging surfaces by changing the gas temperature. For a sterilization process of 0.7 s, a H₂O₂ gas concentration above 4% v/v is required to reach a log-count reduction above six. The numerical results showed the location of H₂O₂ condensate formation, which decreases with increasing sterilant-gas temperature. The model can be transferred to different gas nozzle- and packaging geometries to assure the absence of H₂O₂ residues. Y1 - 2020 U6 - http://dx.doi.org/10.1016/j.sna.2019.111691 SN - 0924-4247 VL - 303 IS - 111691 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Poghossian, Arshak A1 - Schöning, Michael Josef T1 - Capacitive field-effect eis chemical sensors and biosensors: A status report JF - Sensors N2 - Electrolyte-insulator-semiconductor (EIS) field-effect sensors belong to a new generation of electronic chips for biochemical sensing, enabling a direct electronic readout. The review gives an overview on recent advances and current trends in the research and development of chemical sensors and biosensors based on the capacitive field-effect EIS structure—the simplest field-effect device, which represents a biochemically sensitive capacitor. Fundamental concepts, physicochemical phenomena underlying the transduction mechanism and application of capacitive EIS sensors for the detection of pH, ion concentrations, and enzymatic reactions, as well as the label-free detection of charged molecules (nucleic acids, proteins, and polyelectrolytes) and nanoparticles, are presented and discussed. Y1 - 2020 U6 - http://dx.doi.org/10.3390/s20195639 SN - 1424-8220 VL - 20 IS - 19 PB - MDPI CY - Basel ER -