TY - CONF A1 - Johann, Sergej A1 - Kohlhoff, Harald A1 - Gawlitza, Kornelia A1 - Bell, Jérémy A1 - Mansurova, Maria A1 - Tiebe, Carlo A1 - Bartholmai, Matthias T1 - Semi-automatic Gas Measurement Device Based on Fluorescent Multi-gas Sensors N2 - This paper describes the development of a semi-automatic gas measurement device presenting potentially a broad range of applications, noteworthy in the agricultural sector. Non-reversible fluorescent molecular sensors were designed and syn-thesized. Upon, integration into a hydrogel matrix with an optimal ratio of co-solvents, the sensors reacting selectively to ammonia were illuminated by excitation light to produce a concentration-correlated fluorescence emission. An automated mechanical-elec-trical device initiates a given gas mixture and thus simulates con-centrations similar to a threshold value. The aim of this project is to develop a sensor or a low-cost method which can monitor low concentrations of harmful gases and aid in their elimination or regulation in livestock housing, barns or stables. T2 - IEEE Sensors 2019 CY - Montreal, Canada DA - 27.10.2019 KW - gas analysis KW - fluorescence KW - embedded sensor KW - spectroscopy KW - environment KW - agricultural economy PY - 2019 SN - 978-1-7281-1634-1 SP - 88 EP - 92 PB - IEEE AN - OPUS4-49506 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Tobias, Charlie A1 - Climent Terol, Estela A1 - Gawlitza, Kornelia A1 - Rurack, Knut T1 - Polystyrene Microparticles with Convergently Grown Mesoporous Silica Shells as a Promising Tool for Multiplexed Bioanalytical Assays N2 - Functional core/shell particles are highly sought after in analytical chemistry, especially in methods suitable for single-particle analysis such as flow cytometry because they allow for facile multiplexed detection of several analytes in a single run. Aiming to develop a powerful bead platform of which the core particle can be doped in a straightforward manner while the shell offers the highest possible sensitivity when functionalized with (bio)chemical binders, polystyrene particles were coated with different kinds of mesoporous silica shells in a convergent growth approach. Mesoporous shells allow us to obtain distinctly higher surface areas in comparison with conventional nonporous shells. While assessing the potential of narrow- as well as wide-pore silicas such as Mobil composition of matter no. 41 (MCM-41) and Santa Barbara amorphous material no. 15 (SBA-15), especially the synthesis of the latter shells that are much more suitable for biomolecule anchoring was optimized by altering the pH and both, the amount and type of the mediator salt. Our studies showed that the best performing material resulted from a synthesis using neutral conditions and MgSO4 as an ionic mediator. The analytical potential of the particles was investigated in flow cytometric DNA assays after their respective functionalization for individual and multiplexed detection of short oligonucleotide strands. These experiments revealed that a two-step modification of the silica surface with amino silane and succinic anhydride prior to coupling of an amino-terminated capture DNA (c-DNA) strand is superior to coupling carboxylic acid-terminated c-DNA to aminated core/shell particles, yielding limits of detection (LOD) down to 5 pM for a hybridization assay, using labeled complementary single-stranded target DNA (t-DNA) 15mers. The potential of the use of the particles in multiplexed analysis was shown with the aid of dye-doped core particles carrying a respective SBA-15 shell. Characteristic genomic sequences of human papillomaviruses (HPV) were chosen as the t-DNA analytes here, since their high relevance as carcinogens and the high number of different pathogens is a relevant model case. The title particles showed a promising performance and allowed us to unequivocally detect the different high- and low-risk HPV types in a single experimental run. KW - Bead-based assay KW - Core-shell particles KW - Human papillomavirus KW - Mesoporous silica KW - Multiplexing PY - 2020 DO - https://doi.org/10.1021/acsami.0c17940 SN - 1944-8244 VL - 13 IS - 1 SP - 207 EP - 218 PB - American Chemical Society CY - Washington, DC AN - OPUS4-51955 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Kimani, Martha Wamaitha A1 - Beyer, S. A1 - El-Schich, Z. A1 - Gawlitza, Kornelia A1 - Rurack, Knut A1 - Gjörloff-Wingren, A. T1 - Imprinted Particles for Direct Fluorescence Detection of Sialic Acid in Polar Media and on Cancer Cells with Enhanced Control of Nonspecific Binding N2 - Glycoproteins are abundant on the cell surface of mammals, providing structural support, modulating cell Membrane properties, and acting as signaling agents. Variation of glycosylation patterns has been found to indicate various disease states, including cell malignancy. Sialic acid (SA) is present as a terminating group on cell-surface glycans, and its overexpression has been linked to several types of cancer. Detection of SA on the cell surface is therefore critical for detection of cancer in its early stages. In this work, a fluorescent molecularly imprinted polymer layer targeting SA was synthesized on the surface of silica-coated polystyrene (PS) particles. Compared to previous works, a PS core supplies a lighter, lower-density support for improved suspension stability and scattering properties. Moreover, their smaller size provides a higher surface-area-to-volume ratio for binding. The incorporation of a fluorescent monomer in the MIP shell allowed for simple and rapid determination of binding specificity in polar media due to a deprotonation−reprotonation interaction mechanism between the fluorescent monomer and SA, which led to spectral changes. Upon titration of the MIP particles with SA in suspension, an increase in fluorescence emission of the particles was observed, with the MIP particles binding SA more selectively compared to the nonimprinted polymer (NIP) control particles. In cell staining experiments performed by flow cytometry, the binding behavior of the MIP particles compared favorably with that of SA-binding lectins. NIPs prepared with a “dummy” template served as a better negative control in cell binding assays due to the favorable inward orientation of template-binding functional groups in the polymer shell, which reduced nonspecific binding. The results show that fluorescent MIPs targeting SA are a promising tool for in vitro fluorescence staining of cancerous cells and for future diagnosis of cancer at early stages. KW - Flow cytometry KW - Sialic acid KW - Fluorescence KW - Molecularly imprinted polymers KW - Cancer cells PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-525216 DO - https://doi.org/10.1021/acsapm.0c01353 VL - 3 IS - 5 SP - 2363 EP - 2373 PB - American Chemical Society AN - OPUS4-52521 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Gawlitza, Kornelia A1 - Bartelmeß, Jürgen A1 - Bartholmai, Matthias A1 - Neumann, Patrick P. A1 - Johann, Sergej A1 - Tiebe, Carlo A1 - Banach, Ulrich A1 - Noske, Reinhard A1 - Rurack, Knut T1 - Fluorescence sensor for the long-term monitoring of gaseous ammonia N2 - Ammonia and its reaction products can cause considerable damage of human health and ecosystems, increasing the necessity for reliable and reversible sensors to monitor traces of gaseous ammonia in ambient air directly on-site or in the field. Although various types of gas sensors are available, fluorescence sensors have gained importance due to advantages such as high sensitivity and facile miniaturization. Here, we present the development of a sensor material for the detection of gaseous ammonia in the lower ppm to ppb range by incorporation of a fluorescent dye, which shows reversible fluorescence modulations as a function of analyte concentration, into a polymer matrix to ensure the accumulation of ammonia. A gas standard generator producing standard gas mixtures, which comply with the metrological traceability in the desired environmentally relevant measurement range, was used to calibrate the optical sensor system. To integrate the sensor material into a mobile device, a prototype of a hand-held instrument was developed, enabling straightforward data acquisition over a long period. T2 - Colloquium of Optical Spectrometry (COSP) 2017 CY - Berlin, Germany DA - 27.11.2017 KW - Ammonia gas sensor KW - Fluorescence KW - Air quality monitoring KW - Standard gas generator KW - Miniaturized sensor device PY - 2017 AN - OPUS4-43143 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Gawlitza, Kornelia A1 - Tiebe, Carlo A1 - Banach, Ulrich A1 - Noske, Reinhard A1 - Bartholmai, Matthias A1 - Rurack, Knut T1 - Novel sensor for long-term monitoring of ammonia in gas phase N2 - Pollution through emission of toxic gases is of utmost environmental concern, raising the interest in developing reliable gas sensors. Exemplarily, ammonia and its conversion products can provoke considerable damage on human health and ecosystems. Hence, there is a need for reliable and reversible sensor materials to monitor traces of gaseous ammonia in ambient air, which at best can be used on-site for field measurements. Although various types of sensors such as potentiometric, amperometric, and biological sensors are available for detecting trace amounts of gases, fluorescent sensors have gained importance due to several advantages such as high sensitivity, possible miniaturization, as well as potential multiplexing. Herein, we present the development of a sensor material for gaseous ammonia in the lower ppm or even ppb range using optical fluorescence as transduction mechanism due to its intrinsically high sensitivity and high spatial resolution.[1] Therefore, a fluorescent dye, which shows reversible fluorescence enhancement in the presence of the analyte was incorporated into a polymer matrix, the latter to ensure the accumulation of ammonia. To calibrate the designed optical sensor system a gas standard generator was used, producing standard gas mixtures, which comply with the metrological traceability for ammonia gas standards in the desired environmentally relevant measurement range.[2] Beside the development of a highly sensitive, selective, and reversible sensor, the integration of such systems into mobile sensor devices is addressed. Therefore, a prototype of a miniaturized hand-held instrument was developed enabling a straightforward and long-term read-out of the measurement signal. T2 - 13. Dresdner Sensor Symposium (13. DSS) CY - Dresden, Germany DA - 04.12.2017 KW - Ammonia gas sensor KW - Fluorescence KW - Air quality monitoring KW - Standard gas generator KW - Minitaurized sensor device PY - 2017 AN - OPUS4-43351 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Gawlitza, Kornelia A1 - Tiebe, Carlo A1 - Banach, Ulrich A1 - Noske, Reinhard A1 - Bartholmai, Matthias A1 - Rurack, Knut T1 - Novel sensor for long-term monitoring of ammonia in gas phase N2 - Because ammonia and its reaction products can cause considerable damage to human health and ecosystems, there is a need for reliably operating and reversibly interacting sensor materials to monitor traces of gaseous ammonia in ambient air, which at best can be used on-site for in-the-field measurements. Herein, the development of a sensor material for gaseous ammonia in the lower ppm to ppb range using optical fluorescence as transduction mechanism is presented. A fluorescent dye, which shows reversible fluorescence enhancement in the presence of ammonia is incorporated into a polymer matrix, the latter to ensure the accumulation of ammonia. The sensor material is integrated into a prototype of a miniaturized sensor device, facilitating long-term operation. To calibrate the optical sensor system a gas standard generator, producing standard gas mixtures, is used, leading to a sensitivity down to lower ppm concentrations of ammonia. T2 - 13. Dresdner Sensor-Symposium 2017 CY - Dresden, Germany DA - 04.12.2017 KW - Ammonia gas sensor KW - Fluorescence KW - Air quality monitoring KW - Standard gas generator KW - Miniaturized sensor device PY - 2017 DO - https://doi.org/10.5162/13dss2017/P4.02 SP - P4.02, 272 EP - 276 AN - OPUS4-43352 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Gawlitza, Kornelia T1 - Wieviel Schmutz ist rein? Über das Arbeiten im Reinraum N2 - Um verlässliche Methoden für die medizinische Diagnostik und Umweltanalytik zu entwickeln sowie Zellen zu kultivieren, ist staub- bzw. keimfreies Arbeiten in einem Reinraum erforderlich. Aber was ist ein Reinraum? Viele stellen sich hier sterile Räume, keine Fenster und Personen in weißen Anzügen und Schutzmaske vor. Hier können die Besucher einen Blick hinter die Kulissen werfen und erfahren, was die Eigenschaften und Bedingungen eines Reinraumes sind und welche Anforderungen an die dort Beschäftigten gestellt werden. KW - Reinraum PY - 2017 UR - http://www.aktuelle-wochenschau.de/main-navi/aktuelle-wochenschau-2017/kw49-wieviel-schmutz-ist-rein-ueber-das-arbeiten-im-reinraum.html SP - 1 EP - 2 AN - OPUS4-43355 LA - deu AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Tiebe, Carlo A1 - Banach, Ulrich A1 - Hübert, Thomas A1 - Gawlitza, Kornelia A1 - Bartholmai, Matthias T1 - Development of a gas standard generator N2 - Pollution through emission of toxic gases is an increasing problem for the environment. It affects similarly agricultural, industrial and urban areas. In future, environmental emissions in ambient air must be monitored at even lower concentrations as nowadays. One environmental relevant compound is ammonia and its conversion product ammonium that have strong negative impact on human health and ecosystems. Most ammonia measurements in ambient air are performed in the range below 1000 nmol·mol-1 and thus there is a need for reliable traceable ammonia gas standards and in addition in situ analytical procedures for monitoring (in ambient air to avoid that thresholds are exceeded). Therefore, the use of reference materials is necessary for development accompanying test or for calibration, e. g. of structure-integrated sensors and mobile multi-gas sensors. The developed gas standard generator produces gas mixtures that comply with the metrological traceability for ammonia gas standards in the desired environmentally relevant measurement range. The method is based on the permeation of ammonia through a membrane at constant temperature and pressure. The resulting ammonia penetrant gas flow is then mixed with a carrier gas flow to generate a gas standard flow of known concentration. The dynamic rage is enlarged by using a two dilution steps. Depending on the permeation rate, generable molar fractions are possible in the range nmol·mol-1 to a few µmol·mol-1. We present the design of an ammonia gas standard generator and first results of the characterisation of its individual components supporting the uncertainty assessment according to GUM for stable gas concentrations in this range. The relative uncertainty of the generated ammonia gas standard is smaller than 4 % (k = 2). T2 - Colloquium of Optical Spectrometry (COSP) CY - Berlin, Germany DA - 27.11.2017 KW - Gas standard generator KW - Permeation method KW - Ammonia PY - 2017 AN - OPUS4-43337 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Johann, Sergej A1 - Bartholmai, Matthias A1 - Neumann, Patrick P. A1 - Tiebe, Carlo A1 - Gawlitza, Kornelia A1 - Bartelmeß, Jürgen T1 - Adaptable multi-sensor device for gas detection N2 - Innovation is the catalyst for the technology of the future. It is important to develop new and better technologies that can continuously monitor the environmental impact, e.g., for air quality control or emission detection. In the recently at BAM developed Universal Pump Sensor Control (UPSC3) module, different components and sensors are fused. The combination of the individual components makes the UPSC3 module an excellent monitoring and reference system for the development and characterization of gas specific sensors. Measurements over long periods are possible, for mixed gas loads or for certain gas measurements. The system is part of a mobile sensor network of several sensor units, which can also be used as standalone systems. The motivation and objective of this research is to develop gas sensors based on fluorescence detection with range of ppm / ppb. For this task a reference system is required, which contains volatile organic compound (VOC) sensors for reference data from different scenarios. The integrated multi-sensor unit can measure different gases through the integrated 3-fold VOC sensor, which can be adapted to the addressed scenario. . The system-integrated flow control, with pump and flow sensor, allows the gas molecules to be transported directly to the VOC sensor. The entire measurement is permanently stored on an integrated memory card. If the previously determined limit range is exceeded, an alarm is generated. The system is an important tool towards further developments in the field of gas sensors and is primarily used for the validation of chemically based gas sensors. T2 - Colloquium of Optical Spectrometry (COSP) 2017 CY - Berlin, Germany DA - 27.11.2017 KW - Gas detection KW - Multi sensor device KW - Pump control KW - VOC PY - 2017 AN - OPUS4-43193 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Neumann, Patrick P. A1 - Johann, Sergej A1 - Tiebe, Carlo A1 - Gawlitza, Kornelia A1 - Bartelmeß, Jürgen A1 - Bartholmai, Matthias A1 - Hüllmann, Dino A1 - Krentel, Daniel A1 - Kluge, Martin A1 - Kohlhoff, Harald A1 - Lilienthal, A.J. T1 - Airborne Remote Gas Sensing and Mapping N2 - Leaking methane (CH4) from infrastructures, such as pipelines and landfills, is critical for the environment but can also pose a safety risk. To enable a fast detection and localization of these kind of leaks, we developed a novel robotic platform for aerial remote gas sensing. Spectroscopic measurement methods for remote sensing of selected gases lend themselves for use on mini-copters, which offer a number of advantages for inspection and surveillance over traditional methods. No direct contact with the target gas is needed and thus the influence of the aerial platform on the measured gas plume can be kept to a minimum. This allows to overcome one of the major issues with gas-sensitive mini-copters. On the other hand, remote gas sensors, most prominently Tunable Diode Laser Absorption Spectroscopy (TDLAS) sensors have been too bulky given the payload and energy restrictions of mini-copters. Here, we present the Unmanned Aerial Vehicle for Remote Gas Sensing (UAV-REGAS), which combines a novel lightweight TDLAS sensor with a 3-axis aerial stabilization gimbal for aiming on a versatile hexacopter. The proposed system can be deployed in scenarios that cannot be addressed by currently available robots and thus constitutes a significant step forward for the field of Mobile Robot Olfaction (MRO). It enables tomographic reconstruction of gas plumes and a localization of gas sources. We also present first results showing its performance under realistic conditions. T2 - Colloquium of Optical Spectrometry (COSP) 2017 CY - Berlin, Germany DA - 27.11.2017 KW - Tunable Diode Laser Absorption Spectroscopy (TDLAS) KW - UAV-REGAS KW - Mobile Robot Olfaction KW - Tomographic reconstruction of gas plumes KW - Localization of gas sources PY - 2017 AN - OPUS4-43204 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Bartelmeß, Jürgen A1 - Gawlitza, Kornelia A1 - Bartholmai, Matthias A1 - Rurack, Knut A1 - Kohlhoff, Harald A1 - Kraus, Werner A1 - Mansurova, Maria A1 - Bell, Jérémy T1 - Developments towards the fluorescence based sensing of hazardous gases N2 - Fluorescence based sensing is a versatile approach for the trace analysis outside of the laboratory, requiring suitable sensor materials and their integration into sensing devices. The versatility of fluorophores as probes, especially in terms of the possibility to tailor their optical as well as their recognition properties by synthetic modifications in a wide range, renders them a superior active component for the preparation of optical sensor devices. Recent works at BAM in this field include, for example, the detection of nerve gas agents, illustrating impressively the aforementioned benefits of fluorophores in optical sensing applications. In the interdisciplinary approach presented here, we target hazardous gases such as ammonia, benzene, and hydrogen sulfide, next to others, which pose a major threat to human health and environmental safety and for which the availability of a sensitive and reliable detection method is highly desirable. The dyes presented follow a “turn-on” fluorescence schematic which allows for the selective and sensitive detection of the respective gaseous analyte. The immobilization of the probe in polymeric matrices is then the next step toward the fabrication of a prototype device for molecular sensing. T2 - Colloquium of Optical Spectrometry (COSP) 2017 CY - Berlin, Germany DA - 27.11.2017 KW - Gas sensing KW - Fluorescence KW - KonSens PY - 2017 AN - OPUS4-43209 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Bartholmai, Matthias A1 - Neumann, Patrick P. A1 - Johann, Sergej A1 - Tiebe, Carlo A1 - Gawlitza, Kornelia A1 - Bartelmeß, Jürgen T1 - KonSens - Kommunizierende Sensorsysteme für die Bauteil- und Umweltüberwachung N2 - In the KonSens Project, sensor systems are developed, validated, and operated in form of functional models for the application areas Structure Integrated Sensors and Mobile Multi-gas Sensors. Key aspects are the detection and evaluation of corrosion processes in reinforced concrete structures as well as the detection and quantification of very low concentrations of toxic gases in air. The adaption of sensor principles from the lab into real-life application including appropriate communication techniques is a major task. In recent years, Structural Health Monitoring have gained in importance, since growing age of buildings and infrastructure as well as increasing load requirements demand for reliable surveillance methods. In this regard, the project follows two strategies: First, the development and implementation of completely embedded sensor systems consisting of RFID-tag and in situ sensors, and their further application potential (e.g. for precast concrete elements, roadways, wind power plants, and maritime structures). Secondly, the development of a long-term stable, miniaturized, fiber optic sensor for a ratiometric and referenced measurement of the pH-value in concrete based on fluorescence detection as an indicator for carbonation and corrosion. Environmental pollution through emission of toxic gases becomes an increasing problem not only in agriculture (e.g. biogas plants) and industry but also in urban areas. This leads to increasing demand to monitor environmental emissions as well as ambient air and industrial air components in many scenarios and in even lower concentrations than nowadays. The selectivity of luminescence-based sensors is enabled by the combination of the sensing dye and the material, which is used as accumulation medium for concentration of the analyte. This principle allows for developing gas sensors with high selectivity and sensitivity of defined substances. Additional benefits, particularly of fluorescence-based sensors, are their capability for miniaturization and potential multiplex mode. Objective is the development and implementation of sensors based on fluorescence detection for defined toxic gases (ammonia, hydrogen sulfide, ozone, and benzene) with sensitivity in the low ppm or even ppb range. Additionally, the integration of such sensors in mobile sensor devices is addressed. T2 - Colloquium of Optical Spectrometry (COSP) 2017 CY - Berlin, Germany DA - 27.11.2017 KW - RFID sensors KW - Sensors in concrete KW - Gas sensors KW - Mobile sensors KW - Fluorescence sensors PY - 2017 AN - OPUS4-43183 LA - mul AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Gawlitza, Kornelia A1 - Fischer, Tobias A1 - Rurack, Knut T1 - Chemical functionalization for quantitative spectroscopic labeling on macroscopically flat surfaces N2 - This chapter highlights the application of chemical derivatization (CD) to facilitate the quantification of surface functional groups being an important issue for a wide field of applications. The selective attachment of a chemical label to a surface functional group being afterwards exclusively detectable by a highly sensitive technique overcomes the problem of characterizing low amounts of functional groups on macroscopically flat surfaces. The most frequently employed methods include CD X-ray photoelectron spectroscopy, ultraviolet/visible absorption, and fluorescence spectroscopy, as well as time-of-flight secondary ion mass spectrometry. Herein, the basic conditions for the different techniques regarding the specific surface functional group which need to be quantified are discussed. Additionally, the substrate highly influences the compatibility of the corresponding method. Because not just the quantification but also the preparation of the desired application is important, a summary of different preparation methods for glass, polymer and gold substrates is presented. KW - Chemical derivatization KW - Fluorescence KW - Surface group quantification KW - Time-of-flight secondary ion mass spectrometry KW - UV/vis spectroscopy KW - X-ray photoelectron spectroscopy PY - 2018 SN - 978-0-12-409547-2 DO - https://doi.org/10.1016/B978-0-12-409547-2.13191-9 SP - 1 PB - Elsevier AN - OPUS4-43767 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Climent Terol, Estela A1 - Biyikal, Mustafa A1 - Gawlitza, Kornelia A1 - Dropa, T. A1 - Urban, M. A1 - Costero, A. M. A1 - Martínez-Mánez, Ramon A1 - Rurack, Knut T1 - Determination of the chemical warfare agents Sarin, Soman and Tabun in natural waters employing fluorescent hybrid silica materials N2 - A novel mesoporous silica material containing boron–dipyrromethene (BODIPY) moieties (I) is employed for the detection of nerve agent simulants (NASs) and the organophosphate nerve or chemical warfare agents (CWAs) Sarin (GB), Soman (GD), and Tabun (GA) in aqueous environments. The reactive BODIPY dye with an optimum positioned hydroxyl group undergoes acylation reactions with phosph(on)ate substrates, yielding a bicyclic ring. Due to aggregation of the dyes in water, the sensitivity of the free dye in solution is very low. Only after immobilization of the BODIPY moieties into the silica substrates is aggregation inhibited and a sensitive determination of the NASs diethyl cyanophosphonate (DCNP), diethyl chlorophosphate (DCP) and diisopropyl fluorophosphate (DFP) possible. The signaling mode is a strong quenching of the fluorescence, reaching LODs in the pM range. The best performing hybrid material was singled out from a library of hybrid silicas varying in morphology and surface functionalization. The response to actual CWAs such as GB, GD, and GA has also been tested, offering similar behavior as for the simulants. The proposed reaction mechanism has been verified by investigation of other model materials, containing for instance BODIPY moieties without an optimum hydroxyl group (III) or a BODIPY dye with an all-aliphatic counterpart (IV). The latter can only form a monocyclic reaction product, showing much less reactivity as I. Assays with other possible competitors have been additionally carried out, showing favorably low cross-reactivities. Finally, the determination of NASs in several natural waters has been demonstrated. KW - Nerve agent simulants KW - Mesoporous silica materials KW - Fluorescence detection PY - 2017 UR - http://www.sciencedirect.com/science/article/pii/S0925400517303428 DO - https://doi.org/10.1016/j.snb.2017.02.115 SN - 0925-4005 VL - 246 SP - 1056 EP - 1065 PB - Elsevier B.V. AN - OPUS4-39739 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Ritter, B. A1 - Haida, P. A1 - Fink, F. A1 - Krahl, T. A1 - Gawlitza, Kornelia A1 - Rurack, Knut A1 - Scholz, G. A1 - Kemnitz, E. T1 - Novel and easy access to highly luminescent Eu and Tb doped ultra-small CaF2, SrF2 and BaF2 nanoparticles – structure and luminescence N2 - A universal fast and easy access at room temperature to transparent sols of nanoscopic Eu3+ and Tb3+ doped CaF2, SrF2 and BaF2 particles via the fluorolytic sol–gel synthesis route is presented. Monodisperse quasi-spherical nanoparticles with sizes of 3–20 nm are obtained with up to 40% rare earth doping showing red or green luminescence. In the beginning luminescence quenching effects are only observed for the highest content, which demonstrates the unique and outstanding properties of these materials. From CaF2:Eu10 via SrF2:Eu10 to BaF2:Eu10 a steady increase of the luminescence intensity and lifetime occurs by a factor of ≈2; the photoluminescence quantum yield increases by 29 to 35% due to the lower phonon energy of the matrix. The fast formation process of the particles within fractions of seconds is clearly visualized by exploiting appropriate luminescence processes during the synthesis. Multiply doped particles are also available by this method. Fine tuning of the luminescence properties is achieved by variation of the Ca-to-Sr ratio. Co-doping with Ce3+ and Tb3+ results in a huge increase (>50 times) of the green luminescence intensity due to energy transfer Ce3+ → Tb3+. In this case, the luminescence intensity is higher for CaF2 than for SrF2, due to a lower spatial distance of the rare earth ions. KW - Luminescence materials KW - Alkaline earth metal fluorides KW - Fluorolytic sol–gel synthesis PY - 2017 DO - https://doi.org/10.1039/C6DT04711D VL - 46 IS - 9 SP - 2925 EP - 2936 PB - Royal Society of Chemistry AN - OPUS4-39286 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Climent Terol, Estela A1 - Hecht, Mandy A1 - Witthuhn, Heike A1 - Gawlitza, Kornelia A1 - Rurack, Knut T1 - Cover profile for the article "Mix‐&‐read determination of Mercury(II) at trace levels with hybrid mesoporous silica materials incorporating fluorescent probes by a simple mix‐&‐load technique" N2 - Invited for this month’s cover picture is the group of Dr. Knut Rurack at the Department of Analytical Chemistry; Reference Materials at the Bundesanstalt fuer Materialforschung und -pruefung (BAM) in Berlin (Germany). The cover picture shows how differences in color and fluorescence on a test strip can be easily read out with a mobile device. Two reference spots Frame the sensitive spot that indicates the presence of trace amounts of HgII below the threshold in a natural water sample. This dipstick contains a hybrid material that combines boron-dipyrromethene (BODIPY) probes sterically loaded into specifically tailored mesoporous silica particles, allowing for ultrasensitive HgII detection through enhanced fluorescence in a few seconds. The applicability in real water samples and fish extracts are also studied. KW - Mercury KW - Fluorescence KW - Dip-stick assay KW - Group profile PY - 2018 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-471267 DO - https://doi.org/10.1002/open.201800231 SN - 2191-1363 VL - 7 IS - 12 SP - 932 EP - 933 PB - Wiley-VCH CY - Weinheim AN - OPUS4-47126 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Wagner, Sabine A1 - Bell, Jérémy A1 - Biyikal, Mustafa A1 - Gawlitza, Kornelia A1 - Rurack, Knut T1 - Integrating fluorescent molecularly imprinted polymer (MIP) sensor particles with a modular microfluidic platform for nanomolar smallmolecule detection directly in aqueous samples N2 - Fluorescent sensory MIP (molecularly imprinted polymer) particles were combined with a droplet-based 3D microfluidic system for the selective determination of a prototype small-molecule analyte of environmental concern, 2,4-dichlorophenoxyacetic acid or 2,4-D, at nanomolar concentration directly in water samples. A tailor-made fluorescent indicator cross-linker was thus designed that translates the binding event directly into an enhanced fluorescence signal. The phenoxazinone-type cross-linker was co-polymerized into a thin MIP layer grafted from the surface of silica microparticles following a RAFT (reversible addition-fragmentation chain transfer) polymerization protocol. While the indicator cross-linker outperformed its corresponding monomer twin, establishment of a phase-transfer protocol was essential to guarantee that the hydrogen bond-mediated signalling mechanism between the urea binding site on the indicator cross-linker and the carboxylate group of the analyte was still operative upon real sample analysis. The latter was achieved by integration of the fluorescent core-shell MIP sensor particles into a modular microfluidic platform that allows for an in-line phasetransfer assay, extracting the analyte from aqueous sample droplets into the organic phase that contains the sensor particles. Real-time fluorescence determination of 2,4-D down to 20 nM was realized with the system and applied for the analysis of various surface water samples collected from different parts of the world. KW - Molecular imprinting KW - Microfluidics KW - Fluorescence KW - Core-shell particles KW - Droplets PY - 2018 DO - https://doi.org/10.1016/j.bios.2017.07.053 SN - 0956-5663 VL - 99 IS - 1 SP - 244 EP - 250 PB - Elsevier B.V. CY - Amsterdam AN - OPUS4-42258 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bell, Jérémy A1 - Gawlitza, Kornelia A1 - Rurack, Knut T1 - Mit Tröpfchen Spielen N2 - Mikrofluidische Systeme sind leistungsstarke analytische Tools mit attraktiven Eigenschaften wie miniaturisierter Größe, geringem Reagenzien und Probenverbrauch, schneller Ansprech- und kurzer Messzeit. Der Bedarf solcher leistungsstarken, miniaturisierten und direkt vor Ort anwendbaren Sensorsysteme steigt kontinuierlich, hauptsächlich durch das Bedürfnis der Gesellschaft, schneller, besser und umfassender über kritische Faktoren im Lebens- und Arbeitsumfeld sowie der Umwelt informiert zu sein. KW - Mikrofluidik KW - Sensorpartikel PY - 2018 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-459120 UR - https://www.git-labor.de/forschung/umwelt/mit-troepfchen-spielen VL - 8 IS - 8 SP - 2 EP - 4 PB - Wiley-VCH Verlag GmbH & Co. KGaA CY - Weinheim, Deutschland AN - OPUS4-45912 LA - deu AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bell, Jérémy A1 - Gawlitza, Kornelia A1 - Rurack, Knut T1 - Playing with Droplets N2 - Microfluidic devices are powerful analytical tools with appealing features such as miniaturized size, low reagent and sample consumption, rapid response and short measurement times. As society wants to be ever better, earlier and more comprehensively informed about critical factors in life, work, and the environment, the demand for powerful measurement devices for use outside of the laboratory constantly increases. KW - Microfluidics KW - Sensory particles PY - 2018 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-459131 UR - https://www.laboratory-journal.com/ VL - 4 SP - 2 EP - 4 PB - Wiley-VCH Verlag GmbH & Co. KGaA CY - Weinheim, Deutschland AN - OPUS4-45913 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Climent Terol, Estela A1 - Hecht, Mandy A1 - Witthuhn, Heike A1 - Gawlitza, Kornelia A1 - Rurack, Knut T1 - Mix‐&‐read determination of Mercury(II) at trace levels with hybrid mesoporous silica materials incorporating fluorescent probes by a simple mix‐&‐load technique N2 - The synthesis, characterization, and application of mesoporous materials containing boron–dipyrromethene (BODIPY) moieties that allow the sensitive and selective detection of HgII in aqueous environments by fluorescence enhancement is reported. For this purpose, BODIPY dye I containing a thia‐aza crown ether receptor as the fluorescent probe for the detection of HgII in aqueous environments is encapsulated into mesoporous materials to avoid self‐quenching or aggregation in water. Determination of HgII is accomplished within a few seconds with high selectivity and sensitivity, reaching a limit of detection of 12 ppt. The determination of trace amounts of HgII in natural waters and in fish extracts is demonstrated by using our sensing material. The incorporation of the material into several μ‐PAD strips yields a portable, cheap, quick, and easy‐to‐handle tool for trace HgII analysis in water. KW - Dyes/pigments KW - Test strips KW - Mesoporous materials KW - Mercury KW - Fluorescence PY - 2018 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-460138 DO - https://doi.org/10.1002/open.201800277 SN - 2191-1363 VL - 7 IS - 12 SP - 957 EP - 968 PB - Wiley-VCH CY - Weinheim AN - OPUS4-46013 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Kyrey, T. A1 - Ganeva, M. A1 - Gawlitza, Kornelia A1 - Witte, J. A1 - von Klitzing, R. A1 - Soltwedel, O. A1 - Di, Z. A1 - Wellert, S. A1 - Holderer, O. T1 - Grazing incidence SANS and reflectometry combined with simulation of adsorbed microgel particles N2 - Adsorbed ethylene glycol based microgel particles on a Silicon surface were studied. Neutron reflectometry (NR) and grazing incidence small-angle neutron scattering (GISANS) were performed to investigate their internal structure. Scattering experiments on soft matter systems such as adsorbed microgels often give only partial Information about the inner structure of the polymer system. In this contribution, we discuss how the detailed inner structure of adsorbed microgel particles can be reconstructed by a combination of the specular Neutron Reflectivity (NR), Grazing Incidence Small Angle Neutron Scattering (GISANS), Atomic Force Microscopy (AFM) and a simulation in the framework of the Distorted Wave Born Approximation. KW - Grazing incidence small-angle neutron scattering KW - Neutron reflectometry KW - BornAgain simulation KW - Adsorbed microgel particles PY - 2018 DO - https://doi.org/10.1016/j.physb.2018.03.049 SN - 0921-4526 VL - 551 SP - 172 EP - 178 PB - Elsevier B.V. AN - OPUS4-47011 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Gawlitza, Kornelia A1 - Wagner, Sabine A1 - Bell, Jérémy A1 - Biyikal, Mustafa A1 - Rurack, Knut T1 - Integrating fluorescent molecularly imprinted polymer (MIP) sensor particles with a microfluidic platform for nanomolar small-molecule detection in water N2 - Besides the traditional areas of application such as separation and enrichment which made molecularly imprinted polymers (MIPs) very attractive, they have emerged as a valuable detection tool in the field of environmental analysis due to the low production costs, high stability, format adaptability and the possibility to imprint and thus specifically recognize a wide variety of target analytes. Regarding optical sensing, however, MIPs have only been used in considerably few applications, especially in fluorescence sensors, basically because of the challenge to incorporate a fluorescently responding moiety into a polymer matrix. One way to overcome this limitation is the coating of a thin MIP layer onto the surface of silica nanoparticles using tailor-made fluorescent indicator monomers or cross-linkers for direct transfer of the binding event into an optical signal. Regarding sensors for environmental monitoring, microfluidic devices utilizing optical detection modules are especially appealing because of their versatility in terms of miniaturization and automation. So far, MIPs have only rarely been used in combination with microfluidic sensor devices. Here, we present the hydrogen bond-mediated optical response of fluorescent MIP sensor particles against a typical small-molecule analyte 2,4-D (2,4-dichlorophen¬oxyacetic acid) which is an important herbicide widely used in agriculture and known to cause adverse health effects when ingested by contaminated water. By combining the sensor particles with droplet-based 3D microfluidics, a microfluidic phase-transfer assay was designed which enables the direct analysis of 2,4-D in river and lake water without sample pre-treatment or clean-up. T2 - Bioinspired Materials conference 2017 CY - Manchester, UK DA - 31.08.2017 KW - MIPs KW - Fluorescence KW - Sensor KW - Water-monitoring PY - 2017 AN - OPUS4-41828 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - RPRT A1 - Sternbaek, L. A1 - Kimani, Martha Wamaitha A1 - Gawlitza, Kornelia A1 - Janicke, B. A1 - Alm, K. A1 - Gjörloff-Wingren, A. T1 - Digital Holographic Cytometry: Macrophage Uptake of Nanoprobes N2 - Digital holographic cytometry (DHC) is a state-of-the-art quantitative Phase imaging (QPI) method that permits time-lapse imaging of cells without induced cellular toxicity. DHC platforms equipped with semi-automated image segmentation and analysis software packages for assessing cell behavior are commercially available. In this study we investigate the possible uptake of nanoprobes in macrophages in vitro over time. KW - Macrophages KW - MIPs KW - Holographic microscopy KW - Sialic acid PY - 2019 VL - 21 SP - 21 EP - 23 PB - Wiley CY - Imaging and Microscopy AN - OPUS4-47793 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Kislenko, Evgeniia A1 - Incel, A. A1 - Gawlitza, Kornelia A1 - Sellergren, B. A1 - Rurack, Knut T1 - Towards molecularly imprinted polymers that respond to and capture phosphorylated tyrosine epitopes using fluorescent bis-urea and bis-imidazolium receptors N2 - Early detection of cancer is essential for successful treatment and improvement in patient prognosis. Deregulation of post-translational modifications (PTMs) of proteins, especially phosphorylation, is present in many types of cancer. Therefore, the development of materials for the rapid sensing of low abundant phosphorylated peptides in biological samples can be of great therapeutic value. In this work, we have synthesised fluorescent molecularly imprinted polymers (fMIPs) for the detection of the phosphorylated tyrosine epitope of ZAP70, a cancer biomarker. The polymers were grafted as nanometer-thin shells from functionalised submicron-sized silica particles using a reversible addition-fragmentation chain-transfer (RAFT) polymerisation. Employing the combination of fluorescent urea and intrinsically cationic bis-imidazolium receptor cross-linkers, we have developed fluorescent sensory particles, showing an imprinting factor (IF) of 5.0. The imprinted polymer can successfully distinguish between phosphorylated and non-phosphorylated tripeptides, reaching lower micromolar sensitivity in organic solvents and specifically capture unprotected peptide complements in a neutral buffer. Additionally, we have shown the importance of assessing the influence of counterions present in the MIP system on the imprinting process and final material performance. The potential drawbacks of using epitopes with protective groups, which can co-imprint with targeted functionality, are also discussed. KW - Functional monomers KW - Molecularly imprinted polymers KW - Phosphorylated peptides KW - Fluorescence KW - Core-shell particles PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-588089 DO - https://doi.org/10.1039/d3tb01474f SN - 2050-750X SP - 1 EP - 10 PB - Royal Society of Chemistry CY - Cambridge AN - OPUS4-58808 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Sun, Yijuan A1 - Pérez-Padilla, Víctor A1 - Valderrey, Virginia A1 - Bell, Jérémy A1 - Gawlitza, Kornelia A1 - Rurack, Knut T1 - Fluorescence Detection of Perfluoroalkyl Carboxylic Acids with a Miniaturised Assay N2 - Per- and polyfluoroalkyl substances (PFAS) are a class of man-made organo-fluorine chemicals that have become environmental contaminants of emerging concern, originating from a variety of materials such as adhesive, stain- and oil-resistant coatings, firefighting foams, etc. The high strength of this C-F bond makes PFAS thermodynamically stable and resistant to (bio)degradation, thus retaining them in the environment over time. Perfluoroalkyl carboxylic acids (PFCAs), one category of the most used PFAS, consist of a fully fluorinated carbon backbone and a charged carboxylic acid headgroup, and have been classified as Substances of Very High Concern (SVHC) and added to the REACH Candidate List due to their persistence in the environment, non-biodegradability and toxicological effects.[1-2] Traditional techniques for the analysis of PFCAs include GC-MS, HRMS and HPLC-based approaches, which are laborious, not portable, costly and require trained personnel. In contrast, fluorescence assays can be designed as easy-to-operate, portable and cost-effective methods with high sensitivity and fast response. Integration of fluorescent probes with an adequately miniaturized assay enables a promising alternative for PFCAs analysis. Here, a novel guanidine fluorescent probe has been synthesized and fully characterized for the detection of PFCAs in a biphasic extract-&-detect assay. The fluorescent probe was then incorporated into polymeric matrices supported by a red dye-doped SiO2 nanoparticle to construct a dual-emission sensing platform. Such a system allows precise and selective detection of PFCAs, reducing the interference of competitors, matrix effects and other factors except for the PFCAs. The system was then employed in a droplet-based microfluidic setup which offers a portable and easy to operate detection platform. T2 - IMA 2023 CY - Chania, Greece DA - 18.09.2023 KW - PFAS KW - MIP KW - Fluorescence KW - Microfluidics KW - Fluorezsenz KW - Mikrofluidik PY - 2023 AN - OPUS4-58527 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Sun, Yijuan A1 - Gawlitza, Kornelia A1 - Valderrey, Virginia A1 - Bell, Jérémy A1 - Rurack, Knut T1 - Polymerizable BODIPY probe crosslinker for the molecularly imprinted polymer-based detection of organic carboxylates via fluorescence N2 - This contribution reports the development of a polymerizable BODIPY-type fluorescent probe targeting small-molecule carboxylates for incorporation into molecularly imprinted polymers (MIPs). The design of the probe crosslinker includes a urea recognition site p-conjugated to the 3-position of the BODIPY core and two methacrylate moieties. Titration experiments with a carboxylate-expressing antibiotic, levofloxacin (LEVO), showed a blue shift of the absorption band as well as a broadening and decrease in emission, attributed to hydrogen bonding between the probe’s urea group and the carboxylate group of the antibiotic. Using this probe crosslinker, core–shell particles with a silica core and a thin MIP shell were prepared for the detection of LEVO. The MIP exhibited highly selective recognition of LEVO, with an imprinting factor of 18.1 compared to the non-imprinted polymer. Transmission electron microscopy confirmed the core–shell structure and spectroscopic studies revealed that the receptor’s positioning leads to a unique perturbation of the polymethinic character of the BODIPY chromophore, entailing the favourable responses. These features are fully preserved in the MIP, whereas no such response was observed for competitors such as ampicillin. The sensory particles allowed to detect LEVO down to submicromolar concentrations in dioxane. We have developed here for the first time a BODIPY probe for organic carboxylates and incorporated it into polymers using the imprinting technique, paving the way for BODIPY-type fluorescent MIP sensors. KW - Fluorescence KW - BODIPY probe KW - Molecularly Imprinted Polymers KW - Sensor Materials KW - Dyes KW - Water analysis KW - Advanced materials PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-598629 DO - https://doi.org/10.1039/D3MA00476G SP - 1 EP - 11 PB - Royal Society of Chemistry (RSC) AN - OPUS4-59862 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Gawlitza, Kornelia A1 - Pérez-Padilla, Víctor A1 - Sun, Yijuan A1 - Valderrey, Virginia A1 - Bell, Jérémy A1 - Rurack, Knut T1 - On-Site Detection of PFAAs with Dual Fluorescent MIPs Coupled to a Miniaturized Microfluidics Platform N2 - Per- and polyfluoroalkyl substances (PFAS) represent a class of synthetic organofluorine chemicals extensively utilized in the manufacturing of various materials such as firefighting foams, adhesives, and stain- and oil-resistant coatings. In recent years, PFAS have been considered as emerging environmental contaminants, with particular focus on perfluoroalkyl carboxylic acids (PFCAs), the most prevalent type among PFAS. PFCAs are characterized by a fully fluorinated carbon backbone and a charged carboxylic acid headgroup. Notably, they have been designated as Substances of Very High Concern and added to the REACH Candidate List due to their persistence in the environment, non-biodegradability and toxicological effects. Conventional techniques for the analysis of PFCA, such as GC-MS, HRMS and HPLC-based methods, are laborious, not portable, costly and require skilled personnel. In contrast, fluorescence assays can be designed as easy-to-operate, portable and cost-effective methods with high sensitivity and fast response, especially when analyte binding leads to a specific increase of a probe’s emission. Integration of such probes with a carrier platform and a miniaturized optofluidic device affords a promising alternative for PFCA monitoring. Here, a novel guanidine BODIPY fluorescent indicator monomer has been synthesized, characterized, and incorporated into a molecularly imprinted polymer (MIP) for the specific detection of perfluorooctanoic acid (PFOA). The MIP layer was formed on tris(bipyridine)ruthenium(II) chloride doped silica core particles for optical internal reference and calibration-free assays. Such system allows selective and reliable detection of PFCA from surface water samples, with minimum interference by competitors, matrix effects and other factors. Integration of the assay into an opto-microfluidic setup resulted in a miniaturized and easy-to-operate detection system allowing for micromolar detection of PFOA in less than 15 minutes from surface water sample. T2 - MIP2024: The 12th International Conference on Molecular Imprinting CY - Verona, Italy DA - 18.06.2024 KW - Sensor KW - PFAS KW - Molecularly imprinted polymers KW - Guanidine receptor KW - BODIPY PY - 2024 AN - OPUS4-60438 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Costa, Elena A1 - Climent Terol, Estela A1 - Gawlitza, Kornelia A1 - Wan, Wei A1 - Weller, Michael G. A1 - Rurack, Knut T1 - Optimization of analytical assay performance of antibody-gated indicator-releasing mesoporous silica particles N2 - Antibody-gated indicator delivery (gAID) systems based on mesoporous silica nano- and microparticle scaffolds are a promising class of materials for the sensitive chemical detection of small-molecule analytes in simple test formats such as lateral flow assays (LFAs) or microfluidic chips. Their architecture is reminiscent of drug delivery systems, only that reporter molecules instead of drugs are stored in the voids of a porous host particle. In addition, the pores are closed with macromolecular “caps” through a tailored “gatekeeping” recognition chemistry so that the caps are opened when an analyte has reacted with a “gatekeeper”. The subsequent uncapping leads to a release of a large number of indicator molecules, endowing the system with signal amplification features. Particular benefits of such systems are their modularity and adaptability. With the example of the immunochemical detection of type-I pyrethroids by fluorescent dye-releasing gAID systems, the influence of several tuning modes on the optimisation of such hybrid sensory materials is introduced here. In particular, different mesoporous silica supports (from nano- and microparticles to platelets and short fibres), different functionalisation routes and different loading sequences were assessed. The materials’ performances were evaluated by studying their temporal response behaviour and detection sensitivity, including the tightness of pore closure (through the amount of blank release in the absence of analyte) and the release kinetics. Our results indicate that the better the paratope-accommodating Fab region of the antibody “cap” fits into the host material's pore opening, the better the closing/opening mechanism can be controlled. Because such materials are well-suited for LFAs, performance assessment included a test-strip format besides conventional assays in suspension. In combination with dyes as indicators and smartphones for read-out, simple analytical tests for use by untrained personnel directly at a point-of-need such as an aeroplane cabin can be devised, allowing for sensitivities down to the μg kg−1 range in <5 min with case-required selectivities. KW - Antibody-gated indicator delivery KW - Lateral flow assay KW - SBA-15 KW - SBA-16 KW - Type-I pyrethroids KW - Phenothrin KW - Permethrin KW - Etofenprox KW - Amplification KW - Biosensors KW - Immunoassays KW - Mesoporous particles KW - Optical detection PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-517053 DO - https://doi.org/10.1039/d0tb00371a VL - 8 IS - 22 SP - 4950 EP - 4961 PB - Royal Society of Chemistry AN - OPUS4-51705 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Völzke, Jule L. A1 - Hodjat Shamami, Parya A1 - Gawlitza, Kornelia A1 - Feldmann, Ines A1 - Zimathies, Annett A1 - Meyer, Klas A1 - Weller, Michael G. T1 - High-purity corundum as support for affinity extractions from complex samples N2 - Nonporous corundum powder, known as an abrasive material in the industry, was functionalized covalently with protein binders to isolate and enrich specific proteins from complex matrices. The materials based on corundum were characterized by TEM, ESEM, BET, DLS, EDS, and zeta potential measurements. The strong Al-O-P bonds between the corundum surface and amino phosphonic acids were used to introduce functional groups for further conjugations. The common crosslinker glutaraldehyde was compared with a hyperbranched polyglycerol (PG) of around 10 kDa. The latter was oxidized with periodate to generate aldehyde groups that can covalently react with the amines of the surface and the amino groups from the protein via a reductive amination process. The amount of bound protein was quantified via aromatic amino acid analysis (AAAA). This work shows that oxidized polyglycerol can be used as an alternative to glutaraldehyde. With polyglycerol, more of the model protein bovine serum albumin (BSA) could be attached to the surface under the same conditions, and lower non-specific binding (NSB) was observed. As a proof of concept, IgG was extracted with protein A from crude human plasma. The purity of the product was examined by sodium dodecyl sulfate-polyacrylamide gel electrophoresis (SDS-PAGE). A binding capacity of 1.8 mg IgG per gram of corundum powder was achieved. The advantages of corundum include the very low price, extremely high physical and chemical stability, pressure resistance, favorable binding kinetics, convenient handling, and flexible application. KW - Corundum KW - Sapphire KW - Affinity chromatography KW - Antibodies KW - Self-assembled monolayers (SAM) KW - Polyglycerol KW - Dendrimer KW - Nonspecific binding (NSB) KW - Purification KW - Solid-phase extraction (SPE) PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-559342 DO - https://doi.org/10.3390/separations9090252 VL - 9 IS - 9 SP - 1 EP - 13 PB - MDPI CY - Basel AN - OPUS4-55934 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - INPR A1 - Völzke, Jule L. A1 - Hodjat Shamami, Parya A1 - Gawlitza, Kornelia A1 - Feldmann, Ines A1 - Zimathies, Annett A1 - Weller, Michael G. T1 - High-purity corundum as support for affinity extractions from complex samples N2 - Nonporous corundum powder, known as an abrasive material in the industry, was functionalized covalently with protein binders to isolate and enrich specific proteins from complex matrices. The materials based on corundum were characterized by TEM, ESEM, BET, DLS, and zeta potential measurements. The strong Al-O-P bonds between the corundum surface and amino phosphonic acids are used to introduce functional groups for further conjugations. The common cross-linker glutaraldehyde was compared with a hyperbranched polyglycerol (PG) of around 10 kDa. The latter is oxidized with periodate to generate aldehyde groups that can covalently react with the amines of the surface and the amino groups from the protein via a reductive amination process. The amount of bound protein was quantified via aromatic amino acid analysis (AAAA). This work shows that oxidized polyglycerol can be used as an alternative to glutaraldehyde. With polyglycerol, more of the model protein bovine serum albumin (BSA) could be attached to the surface under the same conditions, and lower nonspecific binding (NSB) was observed. As a proof of concept, IgG was extracted with protein A from crude human plasma. The purity of the product was examined by SDS-PAGE. A binding capacity of 1.8 mg IgG per g of corundum powder was achieved. The advantages of corundum are the very low price, extremely high physical and chemical stability, pressure resistance, favorable binding kinetics, and flexible application. KW - Protein KW - Bioseparation KW - Purification KW - Immunoprecipitation KW - Affinity chromatography KW - Polyglycerol KW - Glutaraldehyde KW - Linker KW - Bioconjugation KW - Self-assembled monolayer (SAM) KW - Periodate oxidation KW - Reductive amination KW - Antibodies KW - Igg KW - Immunoglobulins KW - Carrier KW - Solid phase KW - Hyperbranched polymer KW - Aromatic amino acid analysis aaaa PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-555142 DO - https://doi.org/10.20944/preprints202208.0004.v1 SN - 2310-287X SP - 1 EP - 13 PB - MDPI CY - Basel AN - OPUS4-55514 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -