Tom Breugelmans

An Electrochemical Impedimetric Aptasensing Platform for Sensitive and Selective Detection of Small Molecules Such as Chloramphenicol

We report on the aptadetection of chloramphenicol (CAP) using electrochemical impedance spectroscopy. The detection principle is based on the changes of the interfacial properties of the electrode after the interaction of the ssDNA aptamers with the target molecules. The electrode surface is partially blocked due to the formation of the aptamer-CAP complex, resulting in an increase of the interfacial electron-transfer resistance of the redox probe detected by electrochemical impedance spectroscopy or cyclic voltammetry. We observed that the ratio of polarization resistance had a linear relationship with the concentrations of CAP in the range of 1.76–127 nM, and a detection limit of 1.76 nM was obtained. The covalent binding of CAP-aptamer on the electrode surface combined with the unique properties of aptamers and impedimetric transduction leads to the development of a stable and sensitive electrochemical aptasensor for CAP.

Influence of the Morphology of Electrodeposited Nanoparticles on the Activity of Organic Halide Reduction

Influence of the Morphology of Electrodeposited Nanoparticles on the Activity of Organic Halide Reduction Bart Geboes, Bart Vanrenterghem, Jon Ustarroz, Danny Pauwels, Sotiris Sotiropoulos, Annick Hubin and Tom Breugelmans a University of Antwerp, Research Group Advanced Reactor Technology, Salesianenlaan 90, 2660 Hoboken, Belgium b Vrije Universiteit Brussel, Research Group Electrochemical and Surface Engineering, Pleinlaan 2, 1050 Brussels, Belgium c Aristotle University of Thessaloniki, Department of Chemistry, University Campus, Thessaloniki 54124, Greece tom.breugelmans@uantwerpen.be

A membrane microcontactor as a tool for integrated sample preparation

A membrane microcontactor suitable to perform liquid-liquid extraction as well as evaporation in order to conduct enrichment steps in sample preparation of organ samples has been designed, fabricated, and characterized. Spacers of 100- or 200-μm high were constructed in a metal substrate with a channel width of 13 mm and the extraction kinetics in these channels was evaluated. The spacers were designed such that at the entrance and exit region a uniform flow distribution could take place and that a uniform flow profile could be guaranteed along the channel, hence allowing a large freedom in sample volume to be processed. The extraction and evaporation kinetic behavior of the device was first evaluated by extraction of a drug candidate (4-(2,5-dimethyl-pyrrol-1-y1)-2-hydroxybenzoic acid). To evaluate the device under more challenging working conditions, a homogenized mice kidney sample containing the drug candidate that was administered in life condition was cleaned and enriched with the extraction and evaporation modules and characterized by high-performance liquid chromatography, yielding an overall analysis time of 15-20 min per sample only. The system has the potential to be operated in a continuous fashion, making it appealing to be implemented in screening or high-throughput applications.

Electrodeposition of Highly Porous Pt Nanoparticles Studied by Quantitative 3D Electron Tomography: Influence of Growth Mechanisms and Potential Cycling on the Active Surface Area

Nanoporous Pt nanoparticles (NPs) are promising fuel cell catalysts due to their large surface area and increased electrocatalytic activity toward the oxygen reduction reaction (ORR). Herein, we report on the influence of the growth mechanisms on the surface properties of electrodeposited Pt dendritic NPs with large surface areas. The electrochemically active surface was studied by hydrogen underpotential deposition (H UPD) and compared for the first time to high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM) quantitative 3D electron tomography of individual nanoparticles. Large nucleation overpotential leads to a large surface coverage of roughened spheroids, which provide a large roughness factor (Rf) but low mass-specific electrochemically active surface area (EASA). Lowering the nucleation overpotential leads to highly porous Pt NPs with pores stretching to the center of the structure. At the expense of smaller Rf, the obtained EASA values of these structures are in the range of those of large surface area supported fuel cell catalysts. The active surface area of the Pt dendritic NPs was measured by electron tomography, and it was found that the potential cycling in the H adsorption/desorption and Pt oxidation/reduction region, which is generally performed to determine the EASA, leads to a significant reduction of that surface area due to a partial collapse of their dendritic and porous morphology. Interestingly, the extrapolation of the microscopic tomography results in macroscopic electrochemical parameters indicates that the surface properties measured by H UPD are comparable to the values measured on individual NPs by electron tomography after the degradation caused by the H UPD measurement. These results highlight that the combination of electrochemical and quantitative 3D surface analysis techniques is essential to provide insights into the surface properties, the electrochemical stability, and, hence, the applicability of these materials. Moreover, it indicates that care must be taken with widely used electrochemical methods of surface area determination, especially in the case of large surface area and possibly unstable nanostructures, since the measured surface can be strongly affected by the measurement itself.

A novel active-passive sampling approach for measuring time-averaged concentrations of pollutants in water

Passive sampling with in situ devices offers several advantages over traditional sampling methods (i.e., discrete spot sampling), however, data interpretation from conventional passive samplers is hampered by difficulties in estimating the thickness of the diffusion layer at the sampler/medium interface (δ), often leading to inaccurate determinations of target analyte concentrations. In this study, the performance of a novel device combining active and passive sampling was investigated in the laboratory. The active-passive sampling (APS) device is comprised of a diffusion cell fitted with a pump and a flowmeter. Three receiving phases traditionally used in passive sampling devices (i.e., chelex resin, Oasis HLB, and silicone rubber), were incorporated in the diffusion cell and allowed the simultaneous accumulation of cationic metals, polar, and non-polar organic compounds, respectively. The flow within the diffusion cell was accurately controlled and monitored, and, combined with diffusion coefficients measurements, enabled the average δ to be estimated. Strong agreement between APS and time-averaged total concentrations measured in discrete water samples was found for most of the substances investigated. Accuracies for metals ranged between 87 and 116%, except Cu and Pb (∼50%), whilst accuracies between 64 and 101%, and 92 and 151% were achieved for polar and non-polar organic compounds, respectively. These results indicate that, via a well-defined in situ preconcentration step, the proposed APS approach shows promise for monitoring the concentration of a range of pollutants in water.