TY - JOUR A1 - Welden, Melanie A1 - Poghossian, Arshak A1 - Vahidpour, Farnoosh A1 - Wendlandt, Tim A1 - Keusgen, Michael A1 - Wege, Christina A1 - Schöning, Michael Josef T1 - Towards multi-analyte detection with field-effect capacitors modified with tobacco mosaic virus bioparticles as enzyme nanocarriers JF - Biosensors N2 - Utilizing an appropriate enzyme immobilization strategy is crucial for designing enzyme-based biosensors. Plant virus-like particles represent ideal nanoscaffolds for an extremely dense and precise immobilization of enzymes, due to their regular shape, high surface-to-volume ratio and high density of surface binding sites. In the present work, tobacco mosaic virus (TMV) particles were applied for the co-immobilization of penicillinase and urease onto the gate surface of a field-effect electrolyte-insulator-semiconductor capacitor (EISCAP) with a p-Si-SiO₂-Ta₂O₅ layer structure for the sequential detection of penicillin and urea. The TMV-assisted bi-enzyme EISCAP biosensor exhibited a high urea and penicillin sensitivity of 54 and 85 mV/dec, respectively, in the concentration range of 0.1–3 mM. For comparison, the characteristics of single-enzyme EISCAP biosensors modified with TMV particles immobilized with either penicillinase or urease were also investigated. The surface morphology of the TMV-modified Ta₂O₅-gate was analyzed by scanning electron microscopy. Additionally, the bi-enzyme EISCAP was applied to mimic an XOR (Exclusive OR) enzyme logic gate. KW - urease KW - enzyme-logic gate KW - bi-enzyme biosensor KW - capacitive field-effect sensor KW - tobacco mosaic virus (TMV) KW - penicillinase Y1 - 2022 U6 - http://dx.doi.org/10.3390/bios12010043 SN - 2079-6374 N1 - This article belongs to the Special Issue "Biosensors: 10th Anniversary Feature Papers" VL - 12 IS - 1 PB - MDPI CY - Basel ER - TY - JOUR A1 - Molinnus, Denise A1 - Janus, Kevin Alexander A1 - Fang, Anyelina C. A1 - Drinic, Aleksander A1 - Achtsnicht, Stefan A1 - Köpf, Marius A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Thick-film carbon electrode deposited onto a biodegradable fibroin substrate for biosensing applications JF - Physica status solidi (a) N2 - This study addresses a proof-of-concept experiment with a biocompatible screen-printed carbon electrode deposited onto a biocompatible and biodegradable substrate, which is made of fibroin, a protein derived from silk of the Bombyx mori silkworm. To demonstrate the sensor performance, the carbon electrode is functionalized as a glucose biosensor with the enzyme glucose oxidase and encapsulated with a silicone rubber to ensure biocompatibility of the contact wires. The carbon electrode is fabricated by means of thick-film technology including a curing step to solidify the carbon paste. The influence of the curing temperature and curing time on the electrode morphology is analyzed via scanning electron microscopy. The electrochemical characterization of the glucose biosensor is performed by amperometric/voltammetric measurements of different glucose concentrations in phosphate buffer. Herein, systematic studies at applied potentials from 500 to 1200 mV to the carbon working electrode (vs the Ag/AgCl reference electrode) allow to determine the optimal working potential. Additionally, the influence of the curing parameters on the glucose sensitivity is examined over a time period of up to 361 days. The sensor shows a negligible cross-sensitivity toward ascorbic acid, noradrenaline, and adrenaline. The developed biocompatible biosensor is highly promising for future in vivo and epidermal applications. KW - biocompatible materials KW - biodegradable electronic devices KW - biosensors KW - carbon electrodes KW - glucose Y1 - 2022 U6 - http://dx.doi.org/10.1002/pssa.202200100 SN - 1862-6319 N1 - Corresponding author: Michael J. Schöning VL - 219 IS - 23 SP - 1 EP - 9 PB - Wiley-VCH CY - Weinheim ER - TY - CHAP A1 - Welden, Melanie A1 - Severins, Robin A1 - Poghossian, Arshak A1 - Wege, Christina A1 - Siegert, Petra A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Studying the immobilization of acetoin reductase with Tobacco mosaic virus particles on capacitive field-effect sensors T2 - 2022 IEEE International Symposium on Olfaction and Electronic Nose (ISOEN) N2 - A capacitive electrolyte-insulator-semiconductor (EISCAP) biosensor modified with Tobacco mosaic virus (TMV) particles for the detection of acetoin is presented. The enzyme acetoin reductase (AR) was immobilized on the surface of the EISCAP using TMV particles as nanoscaffolds. The study focused on the optimization of the TMV-assisted AR immobilization on the Ta 2 O 5 -gate EISCAP surface. The TMV-assisted acetoin EISCAPs were electrochemically characterized by means of leakage-current, capacitance-voltage, and constant-capacitance measurements. The TMV-modified transducer surface was studied via scanning electron microscopy. KW - Tobacco mosaic virus KW - acetoin KW - capacitive field-effect biosensor KW - enzyme immobilization Y1 - 2022 SN - 978-1-6654-5860-3 (Online) SN - 978-1-6654-5861-0 (Print) U6 - http://dx.doi.org/10.1109/ISOEN54820.2022.9789657 N1 - IEEE International Symposium on Olfaction and Electronic Nose (ISOEN), 29 May 2022 - 01 June 2022, Aveiro, Portugal. PB - IEEE ER - TY - JOUR A1 - Pourshahidi, Ali Mohammad A1 - Engelmann, Ulrich M. A1 - Offenhäusser, Andreas A1 - Krause, Hans-Joachim T1 - Resolving ambiguities in core size determination of magnetic nanoparticles from magnetic frequency mixing data JF - Journal of Magnetism and Magnetic Materials N2 - Frequency mixing magnetic detection (FMMD) has been widely utilized as a measurement technique in magnetic immunoassays. It can also be used for the characterization and distinction (also known as “colourization”) of different types of magnetic nanoparticles (MNPs) based on their core sizes. In a previous work, it was shown that the large particles contribute most of the FMMD signal. This leads to ambiguities in core size determination from fitting since the contribution of the small-sized particles is almost undetectable among the strong responses from the large ones. In this work, we report on how this ambiguity can be overcome by modelling the signal intensity using the Langevin model in thermodynamic equilibrium including a lognormal core size distribution fL(dc,d0,σ) fitted to experimentally measured FMMD data of immobilized MNPs. For each given median diameter d0, an ambiguous amount of best-fitting pairs of parameters distribution width σ and number of particles Np with R2 > 0.99 are extracted. By determining the samples’ total iron mass, mFe, with inductively coupled plasma optical emission spectrometry (ICP-OES), we are then able to identify the one specific best-fitting pair (σ, Np) one uniquely. With this additional externally measured parameter, we resolved the ambiguity in core size distribution and determined the parameters (d0, σ, Np) directly from FMMD measurements, allowing precise MNPs sample characterization. Y1 - 2022 U6 - http://dx.doi.org/10.1016/j.jmmm.2022.169969 SN - 0304-8853 VL - 563 IS - In progress, Art. No. 169969 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Engelmann, Ulrich M. A1 - Pourshahidi, Mohammad Ali A1 - Shalaby, Ahmed A1 - Krause, Hans-Joachim T1 - Probing particle size dependency of frequency mixing magnetic detection with dynamic relaxation simulation JF - Journal of Magnetism and Magnetic Materials N2 - Biomedical applications of magnetic nanoparticles (MNP) fundamentally rely on the particles’ magnetic relaxation as a response to an alternating magnetic field. The magnetic relaxation complexly depends on the interplay of MNP magnetic and physical properties with the applied field parameters. It is commonly accepted that particle core size is a major contributor to signal generation in all the above applications, however, most MNP samples comprise broad distribution spanning nm and more. Therefore, precise knowledge of the exact contribution of individual core sizes to signal generation is desired for optimal MNP design generally for each application. Specifically, we present a magnetic relaxation simulation-driven analysis of experimental frequency mixing magnetic detection (FMMD) for biosensing to quantify the contributions of individual core size fractions towards signal generation. Applying our method to two different experimental MNP systems, we found the most dominant contributions from approx. 20 nm sized particles in the two independent MNP systems. Additional comparison between freely suspended and immobilized MNP also reveals insight in the MNP microstructure, allowing to use FMMD for MNP characterization, as well as to further fine-tune its applicability in biosensing. Y1 - 2022 U6 - http://dx.doi.org/10.1016/j.jmmm.2022.169965 SN - 0304-8853 VL - 563 IS - In progress, Art. No. 169965 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Falkenberg, Fabian A1 - Bott, Michael A1 - Bongaerts, Johannes A1 - Siegert, Petra T1 - Phylogenetic survey of the subtilase family and a data-mining-based search for new subtilisins from Bacillaceae JF - Frontiers in Microbiology N2 - The subtilase family (S8), a member of the clan SB of serine proteases are ubiquitous in all kingdoms of life and fulfil different physiological functions. Subtilases are divided in several groups and especially subtilisins are of interest as they are used in various industrial sectors. Therefore, we searched for new subtilisin sequences of the family Bacillaceae using a data mining approach. The obtained 1,400 sequences were phylogenetically classified in the context of the subtilase family. This required an updated comprehensive overview of the different groups within this family. To fill this gap, we conducted a phylogenetic survey of the S8 family with characterised holotypes derived from the MEROPS database. The analysis revealed the presence of eight previously uncharacterised groups and 13 subgroups within the S8 family. The sequences that emerged from the data mining with the set filter parameters were mainly assigned to the subtilisin subgroups of true subtilisins, high-alkaline subtilisins, and phylogenetically intermediate subtilisins and represent an excellent source for new subtilisin candidates. Y1 - 2022 U6 - http://dx.doi.org/10.3389/fmicb.2022.1017978 SN - 1664-302X VL - 2022 IS - 13 PB - Frontiers CY - Lausanne ER - TY - JOUR A1 - Molinnus, Denise A1 - Iken, Heiko A1 - Johnen, Anna Lynn A1 - Richstein, Benjamin A1 - Hellmich, Lena A1 - Poghossian, Arshak A1 - Knoch, Joachim A1 - Schöning, Michael Josef T1 - Miniaturized pH-Sensitive Field-Effect Capacitors with Ultrathin Ta₂O₅ Films Prepared by Atomic Layer Deposition JF - physica status solidi (a) applications and materials science N2 - Miniaturized electrolyte–insulator–semiconductor capacitors (EISCAPs) with ultrathin gate insulators have been studied in terms of their pH-sensitive sensor characteristics: three different EISCAP systems consisting of Al–p-Si–Ta2O5(5 nm), Al–p-Si–Si3N4(1 or 2 nm)–Ta2O5 (5 nm), and Al–p-Si–SiO2(3.6 nm)–Ta2O5(5 nm) layer structures are characterized in buffer solution with different pH values by means of capacitance–voltage and constant capacitance method. The SiO2 and Si3N4 gate insulators are deposited by rapid thermal oxidation and rapid thermal nitridation, respectively, whereas the Ta2O5 film is prepared by atomic layer deposition. All EISCAP systems have a clear pH response, favoring the stacked gate insulators SiO2–Ta2O5 when considering the overall sensor characteristics, while the Si3N4(1 nm)–Ta2O5 stack delivers the largest accumulation capacitance (due to the lower equivalent oxide thickness) and a higher steepness in the slope of the capacitance–voltage curve among the studied stacked gate insulator systems. KW - atomic layer deposition KW - capacitive field-effect sensors KW - pH sensors KW - ultrathin gate insulators Y1 - 2022 U6 - http://dx.doi.org/10.1002/pssa.202100660 SN - 1862-6319 VL - 219 IS - 8 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Pourshahidi, Ali Mohammad A1 - Achtsnicht, Stefan A1 - Offenhäusser, Andreas A1 - Krause, Hans-Joachim ED - Offenhäusser, Andreas T1 - Frequency Mixing Magnetic Detection Setup Employing Permanent Ring Magnets as a Static Offset Field Source JF - Sensors N2 - Frequency mixing magnetic detection (FMMD) has been explored for its applications in fields of magnetic biosensing, multiplex detection of magnetic nanoparticles (MNP) and the determination of core size distribution of MNP samples. Such applications rely on the application of a static offset magnetic field, which is generated traditionally with an electromagnet. Such a setup requires a current source, as well as passive or active cooling strategies, which directly sets a limitation based on the portability aspect that is desired for point of care (POC) monitoring applications. In this work, a measurement head is introduced that involves the utilization of two ring-shaped permanent magnets to generate a static offset magnetic field. A steel cylinder in the ring bores homogenizes the field. By variation of the distance between the ring magnets and of the thickness of the steel cylinder, the magnitude of the magnetic field at the sample position can be adjusted. Furthermore, the measurement setup is compared to the electromagnet offset module based on measured signals and temperature behavior. KW - magnetic sensors KW - biosensors KW - frequency mixing magnetic detection KW - magnetic nanoparticles Y1 - 2022 U6 - http://dx.doi.org/10.3390/s22228776 SN - 1424-8220 VL - 22 IS - 22 PB - MDPI CY - Basel ER - TY - JOUR A1 - Poghossian, Arshak A1 - Karschuck, Tobias A1 - Wagner, Patrick A1 - Schöning, Michael Josef T1 - Field-Effect Capacitors Decorated with Ligand-Stabilized Gold Nanoparticles: Modeling and Experiments JF - Biosensors N2 - Nanoparticles are recognized as highly attractive tunable materials for designing field-effect biosensors with enhanced performance. In this work, we present a theoretical model for electrolyte-insulator-semiconductor capacitors (EISCAP) decorated with ligand-stabilized charged gold nanoparticles. The charged AuNPs are taken into account as additional, nanometer-sized local gates. The capacitance-voltage (C–V) curves and constant-capacitance (ConCap) signals of the AuNP-decorated EISCAPs have been simulated. The impact of the AuNP coverage on the shift of the C–V curves and the ConCap signals was also studied experimentally on Al–p-Si–SiO₂ EISCAPs decorated with positively charged aminooctanethiol-capped AuNPs. In addition, the surface of the EISCAPs, modified with AuNPs, was characterized by scanning electron microscopy for different immobilization times of the nanoparticles. KW - aminooctanethiol KW - nanoparticle coverage KW - capacitive model KW - gold nanoparticles KW - field-effect sensor KW - electrolyte-insulator-semiconductor capacitors Y1 - 2022 U6 - http://dx.doi.org/10.3390/bios12050334 SN - 2079-6374 N1 - This article belongs to the Special Issue "Biosensors in Nanotechnology" VL - 12 IS - 5 PB - MDPI CY - Basel ER - TY - JOUR A1 - Welden, Melanie A1 - Severins, Robin A1 - Poghossian, Arshak A1 - Wege, Christina A1 - Bongaerts, Johannes A1 - Siegert, Petra A1 - Keusgen, Michael A1 - Schöning, Michael Josef T1 - Detection of acetoin and diacetyl by a tobacco mosaic virus-assisted field-effect biosensor JF - Chemosensors N2 - Acetoin and diacetyl have a major impact on the flavor of alcoholic beverages such as wine or beer. Therefore, their measurement is important during the fermentation process. Until now, gas chromatographic techniques have typically been applied; however, these require expensive laboratory equipment and trained staff, and do not allow for online monitoring. In this work, a capacitive electrolyte–insulator–semiconductor sensor modified with tobacco mosaic virus (TMV) particles as enzyme nanocarriers for the detection of acetoin and diacetyl is presented. The enzyme acetoin reductase from Alkalihalobacillus clausii DSM 8716ᵀ is immobilized via biotin–streptavidin affinity, binding to the surface of the TMV particles. The TMV-assisted biosensor is electrochemically characterized by means of leakage–current, capacitance–voltage, and constant capacitance measurements. In this paper, the novel biosensor is studied regarding its sensitivity and long-term stability in buffer solution. Moreover, the TMV-assisted capacitive field-effect sensor is applied for the detection of diacetyl for the first time. The measurement of acetoin and diacetyl with the same sensor setup is demonstrated. Finally, the successive detection of acetoin and diacetyl in buffer and in diluted beer is studied by tuning the sensitivity of the biosensor using the pH value of the measurement solution. Y1 - 2022 U6 - http://dx.doi.org/10.3390/chemosensors10060218 SN - 2227-9040 N1 - This article belongs to the Special Issue "Nanostructured Devices for Biochemical Sensing" VL - 10 IS - 6 PB - MDPI CY - Basel ER -