@article{BandodkarMolinnusMirzaetal.2014, author = {Bandodkar, Amay J. and Molinnus, Denise and Mirza, Omar and Guinovart, Tomas and Windmiller, Joshua R. and Valdes-Ramirez, Gabriela and Andrade, Francisco J. and Sch{\"o}ning, Michael Josef and Wang, Joseph}, title = {Epidermal tattoo potentiometric sodium sensors with wireless signal transduction for continuous non-invasive sweat monitoring}, series = {Biosensors and bioelectronics}, volume = {54}, journal = {Biosensors and bioelectronics}, publisher = {Elsevier}, address = {Amsterdam}, issn = {1873-4235 (E-Journal); 0956-5663 (Print)}, doi = {10.1016/j.bios.2013.11.039}, pages = {603 -- 609}, year = {2014}, abstract = {This article describes the fabrication, characterization and application of an epidermal temporary-transfer tattoo-based potentiometric sensor, coupled with a miniaturized wearable wireless transceiver, for real-time monitoring of sodium in the human perspiration. Sodium excreted during perspiration is an excellent marker for electrolyte imbalance and provides valuable information regarding an individual's physical and mental wellbeing. The realization of the new skin-worn non-invasive tattoo-like sensing device has been realized by amalgamating several state-of-the-art thick film, laser printing, solid-state potentiometry, fluidics and wireless technologies. The resulting tattoo-based potentiometric sodium sensor displays a rapid near-Nernstian response with negligible carryover effects, and good resiliency against various mechanical deformations experienced by the human epidermis. On-body testing of the tattoo sensor coupled to a wireless transceiver during exercise activity demonstrated its ability to continuously monitor sweat sodium dynamics. The real-time sweat sodium concentration was transmitted wirelessly via a body-worn transceiver from the sodium tattoo sensor to a notebook while the subjects perspired on a stationary cycle. The favorable analytical performance along with the wearable nature of the wireless transceiver makes the new epidermal potentiometric sensing system attractive for continuous monitoring the sodium dynamics in human perspiration during diverse activities relevant to the healthcare, fitness, military, healthcare and skin-care domains.}, language = {en} } @article{PoghossianJablonskiMolinnusetal.2020, author = {Poghossian, Arshak and Jablonski, Melanie and Molinnus, Denise and Wege, Christina and Sch{\"o}ning, Michael Josef}, title = {Field-Effect Sensors for Virus Detection: From Ebola to SARS-CoV-2 and Plant Viral Enhancers}, series = {Frontiers in Plant Science}, volume = {11}, journal = {Frontiers in Plant Science}, number = {Article 598103}, publisher = {Frontiers}, address = {Lausanne}, doi = {10.3389/fpls.2020.598103}, pages = {1 -- 14}, year = {2020}, abstract = {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.}, language = {en} } @article{SiqueiraMolinnusBegingetal.2014, author = {Siqueira, Jose R. and Molinnus, Denise and Beging, Stefan and Sch{\"o}ning, Michael Josef}, title = {Incorporating a hybrid urease-carbon nanotubes sensitive nanofilm on capacitive field-effect sensors for urea detection}, series = {Analytical chemistry}, volume = {86}, journal = {Analytical chemistry}, number = {11}, publisher = {ACS Publications}, address = {Columbus}, issn = {1520-6882 (E-Journal); 0003-2700 (Print); 0096-4484 (Print)}, doi = {10.1021/ac500458s}, pages = {5370 -- 5375}, year = {2014}, abstract = {The ideal combination among biomolecules and nanomaterials is the key for reaching biosensing units with high sensitivity. The challenge, however, is to find out a stable and sensitive film architecture that can be incorporated on the sensor's surface. In this paper, we report on the benefits of incorporating a layer-by-layer (LbL) nanofilm of polyamidoamine (PAMAM) dendrimer and carbon nanotubes (CNTs) on capacitive electrolyte-insulator-semiconductor (EIS) field-effect sensors for detecting urea. Three sensor arrangements were studied in order to investigate the adequate film architecture, involving the LbL film with the enzyme urease: (i) urease immobilized directly onto a bare EIS [EIS-urease] sensor; (ii) urease atop the LbL film over the EIS [EIS-(PAMAM/CNT)-urease] sensor; and (iii) urease sandwiched between the LbL film and another CNT layer [EIS-(PAMAM/CNT)-urease-CNT]. The surface morphology of all three urea-based EIS biosensors was investigated by atomic force microscopy (AFM), while the biosensing abilities were studied by means of capacitance-voltage (C/V) and dynamic constant-capacitance (ConCap) measureaments at urea concentrations ranging from 0.1 mM to 100 mM. The EIS-urease and EIS-(PAMAM/CNT)-urease sensors showed similar sensitivity (∼18 mV/decade) and a nonregular signal behavior as the urea concentration increased. On the other hand, the EIS-(PAMAM/CNT)-urease-CNT sensor exhibited a superior output signal performance and higher sensitivity of about 33 mV/decade. The presence of the additional CNT layer was decisive to achieve a urea based EIS sensor with enhanced properties. Such sensitive architecture demonstrates that the incorporation of an adequate hybrid enzyme-nanofilm as sensing unit opens new prospects for biosensing applications using the field-effect sensor platform.}, language = {en} } @article{BertzSchoeningMolinnusetal.2024, author = {Bertz, Morten and Sch{\"o}ning, Michael Josef and Molinnus, Denise and Homma, Takayuki}, title = {Influence of temperature, light, and H₂O₂ concentration on microbial spore inactivation: in-situ Raman spectroscopy combined with optical trapping}, series = {Physica status solidi (a) applications and materials science}, journal = {Physica status solidi (a) applications and materials science}, number = {Early View}, publisher = {Wiley-VCH}, address = {Berlin}, issn = {1862-6319 (Online)}, doi = {10.1002/pssa.202300866}, pages = {8 Seiten}, year = {2024}, abstract = {To gain insight on chemical sterilization processes, the influence of temperature (up to 70 °C), intense green light, and hydrogen peroxide (H₂O₂) concentration (up to 30\% in aqueous solution) on microbial spore inactivation is evaluated by in-situ Raman spectroscopy with an optical trap. Bacillus atrophaeus is utilized as a model organism. Individual spores are isolated and their chemical makeup is monitored under dynamically changing conditions (temperature, light, and H₂O₂ concentration) to mimic industrially relevant process parameters for sterilization in the field of aseptic food processing. While isolated spores in water are highly stable, even at elevated temperatures of 70 °C, exposure to H₂O₂ leads to a loss of spore integrity characterized by the release of the key spore biomarker dipicolinic acid (DPA) in a concentration-dependent manner, which indicates damage to the inner membrane of the spore. Intensive light or heat, both of which accelerate the decomposition of H₂O₂ into reactive oxygen species (ROS), drastically shorten the spore lifetime, suggesting the formation of ROS as a rate-limiting step during sterilization. It is concluded that Raman spectroscopy can deliver mechanistic insight into the mode of action of H₂O₂-based sterilization and reveal the individual contributions of different sterilization methods acting in tandem.}, language = {en} } @article{MolinnusIkenJohnenetal.2022, author = {Molinnus, Denise and Iken, Heiko and Johnen, Anna Lynn and Richstein, Benjamin and Hellmich, Lena and Poghossian, Arshak and Knoch, Joachim and Sch{\"o}ning, Michael Josef}, title = {Miniaturized pH-Sensitive Field-Effect Capacitors with Ultrathin Ta₂O₅ Films Prepared by Atomic Layer Deposition}, series = {physica status solidi (a) applications and materials science}, volume = {219}, journal = {physica status solidi (a) applications and materials science}, number = {8}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1862-6319}, doi = {10.1002/pssa.202100660}, pages = {7 Seiten}, year = {2022}, abstract = {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.}, language = {en} } @article{BertzMolinnusSchoeningetal.2023, author = {Bertz, Morten and Molinnus, Denise and Sch{\"o}ning, Michael Josef and Homma, Takayuki}, title = {Real-time monitoring of H₂O₂ sterilization on individual bacillus atrophaeus spores by optical sensing with trapping Raman spectroscopy}, series = {Chemosensors}, volume = {8}, journal = {Chemosensors}, number = {11}, publisher = {MDPI}, address = {Basel}, issn = {2227-9040}, doi = {10.3390/chemosensors11080445}, pages = {Artikel 445}, year = {2023}, abstract = {Hydrogen peroxide (H₂O₂), a strong oxidizer, is a commonly used sterilization agent employed during aseptic food processing and medical applications. To assess the sterilization efficiency with H₂O₂, bacterial spores are common microbial systems due to their remarkable robustness against a wide variety of decontamination strategies. Despite their widespread use, there is, however, only little information about the detailed time-resolved mechanism underlying the oxidative spore death by H₂O₂. In this work, we investigate chemical and morphological changes of individual Bacillus atrophaeus spores undergoing oxidative damage using optical sensing with trapping Raman microscopy in real-time. The time-resolved experiments reveal that spore death involves two distinct phases: (i) an initial phase dominated by the fast release of dipicolinic acid (DPA), a major spore biomarker, which indicates the rupture of the spore's core; and (ii) the oxidation of the remaining spore material resulting in the subsequent fragmentation of the spores' coat. Simultaneous observation of the spore morphology by optical microscopy corroborates these mechanisms. The dependence of the onset of DPA release and the time constant of spore fragmentation on H₂O₂ shows that the formation of reactive oxygen species from H₂O₂ is the rate-limiting factor of oxidative spore death.}, language = {en} } @article{MuschallikMolinnusJablonskietal.2020, author = {Muschallik, Lukas and Molinnus, Denise and Jablonski, Melanie and Kipp, Carina Ronja and Bongaerts, Johannes and Pohl, Martina and Wagner, Torsten and Sch{\"o}ning, Michael Josef and Selmer, Thorsten and Siegert, Petra}, title = {Synthesis of α-hydroxy ketones and vicinal (R, R)-diols by Bacillus clausii DSM 8716ᵀ butanediol dehydrogenase}, series = {RSC Advances}, volume = {10}, journal = {RSC Advances}, publisher = {Royal Society of Chemistry (RSC)}, address = {Cambridge}, issn = {2046-2069}, doi = {10.1039/D0RA02066D}, pages = {12206 -- 12216}, year = {2020}, abstract = {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.}, language = {en} } @article{MolinnusJanusFangetal.2022, author = {Molinnus, Denise and Janus, Kevin Alexander and Fang, Anyelina C. and Drinic, Aleksander and Achtsnicht, Stefan and K{\"o}pf, Marius and Keusgen, Michael and Sch{\"o}ning, Michael Josef}, title = {Thick-film carbon electrode deposited onto a biodegradable fibroin substrate for biosensing applications}, series = {Physica status solidi (a)}, volume = {219}, journal = {Physica status solidi (a)}, number = {23}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1862-6319}, doi = {10.1002/pssa.202200100}, pages = {1 -- 9}, year = {2022}, abstract = {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.}, language = {en} } @article{MolinnusDrinicIkenetal.2021, author = {Molinnus, Denise and Drinic, Aleksander and Iken, Heiko and Kr{\"o}ger, Nadja and Zinser, Max and Smeets, Ralf and K{\"o}pf, Marius and Kopp, Alexander and Sch{\"o}ning, Michael Josef}, title = {Towards a flexible electrochemical biosensor fabricated from biocompatible Bombyx mori silk}, series = {Biosensors and Bioelectronics}, volume = {183}, journal = {Biosensors and Bioelectronics}, number = {Art. 113204}, publisher = {Elsevier}, address = {Amsterdam}, issn = {0956-5663}, doi = {10.1016/j.bios.2021.113204}, year = {2021}, language = {en} } @article{MolinnusBegingLowisetal.2020, author = {Molinnus, Denise and Beging, Stefan and Lowis, Carsten and Sch{\"o}ning, Michael Josef}, title = {Towards a multi-enzyme capacitive field-effect biosensor by comparative study of drop-coating and nano-spotting technique}, series = {Sensors}, volume = {20}, journal = {Sensors}, number = {17}, publisher = {MDPI}, address = {Basel}, isbn = {1424-8220}, doi = {10.3390/s20174924}, pages = {Artikel 4942}, year = {2020}, abstract = {Multi-enzyme immobilization onto a capacitive field-effect biosensor by nano-spotting technique is presented. The nano-spotting technique allows to immobilize different enzymes simultaneously on the sensor surface with high spatial resolution without additional photolithographical patterning. The amount of applied enzymatic cocktail on the sensor surface can be tailored. Capacitive electrolyte-insulator-semiconductor (EIS) field-effect sensors with Ta2O5 as pH-sensitive transducer layer have been chosen to immobilize the three different (pL droplets) enzymes penicillinase, urease, and glucose oxidase. Nano-spotting immobilization is compared to conventional drop-coating method by defining different geometrical layouts on the sensor surface (fully, half-, and quarter-spotted). The drop diameter is varying between 84 µm and 102 µm, depending on the number of applied drops (1 to 4) per spot. For multi-analyte detection, penicillinase and urease are simultaneously nano-spotted on the EIS sensor. Sensor characterization was performed by C/V (capacitance/voltage) and ConCap (constant capacitance) measurements. Average penicillin, glucose, and urea sensitivities for the spotted enzymes were 81.7 mV/dec, 40.5 mV/dec, and 68.9 mV/dec, respectively.}, language = {en} }