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- ItemPreliminary Study on the Application of Temperature Swing Adsorption in Aqueous Phase for Pesticide Removal(London [u.a.] : Institute of Physics, 2018) Aumeier, B.; Dang, H.Q.A.; Wessling, M.Temperature swing adsorption (TSA) is a well-established process for gas purification. In this work, the feasibility of TSA in aqueous phase was studied. This concept could enable in situ adsorbent regeneration and thus fostering sustainable decentralized adsorption processes applied to water treatment. The adsorption processes with the use of granular activated carbon (GAC) have been widely applied to remove the residual amounts of pesticides in water treatment. Amitrole was chosen as a typical pesticide in this study, GAC was selected as the main adsorbent for amitrole removal. Adsorption isotherm experiments were conducted at different temperatures of 20°C, 57°C and 94°C to identify the most appropriate sorptive – sorbent system for dynamic adsorption and TSA research. Once the isotherm experiments were accomplished, breakthrough curve experiments were subsequently investigated. Finally, TSA process was conducted with the activated carbon regeneration at the elevated temperature of 125°C. Consequently, initial obtained results proved the feasibility of the proposed TSA technique for pesticide removal in aqueous phase.
- ItemCriticial Assessment of the Photocatalytic Reduction of Cr(VI) over Au/TiO2(Basel : MDPI, 2018-12-3) Ngo, Anh Binh; Nguyen, Hong Lien; Hollmann, DirkThe purification of drinking water is one of the most urgent challenges in developing countries, for which the efficient removal of traces of heavy metals, e.g., Cr(IV), represents a key technology. This can be achieved via photocatalysis. In this study, we compare the performance of Au/TiO2 to bare TiO2 P25 catalysts. Furthermore, the influence of the sacrificial reagent citric acid under UV-Vis and Vis excitation was investigated and a detailed investigation of the catalysts before and after reaction was performed. During the photocatalytic reduction of Cr(IV) under acidic conditions, both leaching of Au, as well as absorption of Cr, occur, resulting in new catalyst systems obtained in situ.
- ItemBa termination of Ge(001) studied with STM(Bristol : IOP Publishing, 2015) Koczorowski, W.; Grzela, T.; Radny, M.W.; Schofield, S.R.; Capellini, G.; Czajka, R.; Schroeder, T.; Curson, N.J.We use controlled annealing to tune the interfacial properties of a sub-monolayer and monolayer coverages of Ba atoms deposited on Ge(001), enabling the generation of either of two fundamentally distinct interfacial phases, as revealed by scanning tunneling microscopy. Firstly we identify the two key structural phases associated with this adsorption system, namely on-top adsorption and surface alloy formation, by performing a deposition and annealing experiment at a coverage low enough (~0.15 ML) that isolated Ba-related features can be individually resolved. Subsequently we investigate the monolayer coverage case, of interest for passivation schemes of future Ge based devices, for which we find that the thermal evaporation of Ba onto a Ge(001) surface at room temperature results in on-top adsorption. This separation (lack of intermixing) between Ba and Ge layers is retained through successive annealing steps to temperatures of 470, 570, 670 and 770 K although a gradual ordering of the Ba layer is observed at 570 K and above, accompanied by a decrease in Ba layer density. Annealing above 770 K produces the 2D surface alloy phase accompanied by strain relief through monolayer height trench formation. An annealing temperature of 1070 K sees a further change in surface morphology but retention of the 2D surface alloy characteristic. These results are discussed in view of their possible implications for future semiconductor integrated circuit technology.
- ItemInteraction between immobilized polyelectrolyte complex nanoparticles and human mesenchymal stromal cells(Auckland : DOVE Medical Press, 2014) Woltmann, B.; Torger, B.; Müller, M.; Hempel, U.Background: Implant loosening or deficient osseointegration is a major problem in patients with systemic bone diseases (eg, osteoporosis). For this reason, the stimulation of the regional cell population by local and sustained drug delivery at the bone/implant interface to induce the formation of a mechanical stable bone is promising. The purpose of this study was to investigate the interaction of polymer-based nanoparticles with human bone marrow-derived cells, considering nanoparticles' composition and surface net charge. Materials and methods: Polyelectrolyte complex nanoparticles (PECNPs) composed of the polycations poly(ethyleneimine) (PEI), poly(L-lysine) (PLL), or (N,N-diethylamino)ethyldextran (DEAE) in combination with the polyanions dextran sulfate (DS) or cellulose sulfate (CS) were prepared. PECNPs' physicochemical properties (size, net charge) were characterized by dynamic light scattering and particle charge detector measurements. Biocompatibility was investigated using human mesenchymal stromal cells (hMSCs) cultured on immobilized PECNP films (5-50 nmol·cm-2) by analysis for metabolic activity of hMSCs in dependence of PECNP surface concentration by MTS (3-[4,5-dimethylthiazol-2-yl]-5-[3-carboxymethoxyphenyl]-2-[4-sulfophenyl]-2H-tetrazolium, inner salt) assay, as well as cell morphology (phase contrast microscopy). Results: PECNPs ranging between ~50 nm and 150 nm were prepared. By varying the ratio of polycations and polyanions, PECNPs with a slightly positive (PEC+NP) or negative (PEC-NP) net charge were obtained. The PECNP composition significantly affected cell morphology and metabolic activity, whereas the net charge had a negligible influence. Therefore, we classified PECNPs into "variant systems" featuring a significant dose dependency of metabolic activity (DEAE/CS, PEI/DS) and "invariant systems" lacking such a dependency (DEAE/DS, PEI/CS). Immunofluorescence imaging of fluorescein isothiocyanate isomer I (FITC)-labeled PECNPs suggested internalization into hMSCs remaining stable for 8 days. Conclusion: Our study demonstrated that PECNP composition affects hMSC behavior. In particular, the PEI/CS system showed biocompatibility in a wide concentration range, representing a suitable system for local drug delivery from PECNP-functionalized bone substitute materials.
- ItemSurface Functionalization by Stimuli-Sensitive Microgels for Effective Enzyme Uptake and Rational Design of Biosensor Setups(Basel : MDPI, 2018) Sigolaeva, Larisa V.; Pergushov, Dmitry V.; Oelmann, Marina; Schwarz, Simona; Brugnoni, Monia; Kurochkin, Ilya N.; Plamper, Felix A.; Fery, Andreas; Richtering, WalterWe highlight microgel/enzyme thin films that were deposited onto solid interfaces via two sequential steps, the adsorption of temperature- and pH-sensitive microgels, followed by their complexation with the enzyme choline oxidase, ChO. Two kinds of functional (ionic) microgels were compared in this work in regard to their adsorptive behavior and interaction with ChO, that is, poly(N-isopropylacrylamide-co-N-(3-aminopropyl)methacrylamide), P(NIPAM-co-APMA), bearing primary amino groups, and poly(N-isopropylacrylamide-co-N-[3-(dimethylamino) propyl]methacrylamide), P(NIPAM-co-DMAPMA), bearing tertiary amino groups. The stimuli-sensitive properties of the microgels in the solution were characterized by potentiometric titration, dynamic light scattering (DLS), and laser microelectrophoresis. The peculiarities of the adsorptive behavior of both the microgels and the specific character of their interaction with ChO were revealed by a combination of surface characterization techniques. The surface charge was characterized by electrokinetic analysis (EKA) for the initial graphite surface and the same one after the subsequent deposition of the microgels and the enzyme under different adsorption regimes. The masses of wet microgel and microgel/enzyme films were determined by quartz crystal microbalance with dissipation monitoring (QCM-D) upon the subsequent deposition of the components under the same adsorption conditions, on a surface of gold-coated quartz crystals. Finally, the enzymatic responses of the microgel/enzyme films deposited on graphite electrodes to choline were tested amperometrically. The presence of functional primary amino groups in the P(NIPAM-co-APMA) microgel enables a covalent enzyme-to-microgel coupling via glutar aldehyde cross-linking, thereby resulting in a considerable improvement of the biosensor operational stability.
- ItemAdsorption characteristics of Er3N@C80on W(110) and Au(111) studied via scanning tunneling microscopy and spectroscopy(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2017-5-23) Schimmel, Sebastian; Sun, Zhixiang; Baumann, Danny; Krylov, Denis; Samoylova, Nataliya; Popov, Alexey; Büchner, Bernd; Hess, ChristianWe performed a study on the fundamental adsorption characteristics of Er3N@C80 deposited on W(110) and Au(111) via room temperature scanning tunneling microscopy and spectroscopy. Adsorbed on W(110), a comparatively strong bond to the endohedral fullerenes inhibited the formation of ordered monolayer islands. In contrast, the Au(111)-surface provides a sufficiently high mobility for the molecules to arrange in monolayer islands after annealing. Interestingly, the fullerenes modify the herringbone reconstruction indicating that the molecule–substrate interaction is of considerable extent. Investigations concerning the electronic structure of Er3N@C80/Au(111) reveals spatial variations dependent on the termination of the Au(111) at the interface.
- ItemInsulin adsorption to catheter materials used for intensive insulin therapy in critically ill patients: Polyethylene versus polyurethane - possible cause of variation in glucose control?(Sharjah : Bentham Science Publishers B.V., 2014) Ley, S.C.; Ammann, J.; Herder, C.; Dickhaus, T.; Hartmann, M.; Kindgen-Milles, D.Introduction: Restoring and maintaining normoglycemia by intensified insulin therapy in critically ill patients is a matter of ongoing debate since the risk of hypoglycemia may outweigh positive effects on morbidity and mortality. In this context, adsorption of insulin to different catheter materials may contribute to instability of glucose control. We studied the adsorption of insulin to different tubing materials in vitro and the effects on glycemic control in vivo. Materials and Methods: In vitro experiments: A syringe pump was filled with 50 IU insulin diluted to 50 ml saline. A flow of 2 ml/h was perfused through polyethylene (PET) or polyurethane (PUR) tubing. Insulin concentrations were measured at the end of the tube for 24 hours using Bradford's protein assay. In vivo study: In a randomized double-blinded cross-over design, 10 intensive care patients received insulin via PET and PUR tubes for 24 hours each, targeting blood glucose levels of 80-150 mg/dl. We measured blood glucose levels, the insulin dose required to maintain target levels, and serum insulin and C-peptide levels. Results: In vitro experiments: After the start of the insulin infusion, only 20% (median, IQR 20-27) (PET) and 22% (IQR 16-27) (PUR) of the prepared insulin concentration were measured at the end of the 2 meter tubing. Using PET, after one hour infusion the concentration increased to 34% (IQR 29-36) and did not increase significantly during the next 24 hours (39% (IQR 39-40)). Using PUR, higher concentrations were detected than for PET at every measurement from 1 hour (82% (IQR 70-86)) to 24 hours (79% (IQR 64-87)). In vivo study: Glycemic control was effective and not different between groups. Significantly higher volumes of insulin solution had to be infused with PET compared to PUR (median PET 70.0 (IQR 56-82) ml vs. PUR 42 (IQR 31-63) ml; p=0.0015). Serum insulin concentrations did not decrease significantly one hour after changing to PET or PUR tubing. Conclusion: Polyurethane tubing systems allow application of insulin with significantly lower adsorption rates than polyethylene tubing systems. As a consequence, less insulin solution has to be infused to patients for effective blood glucose control. Tubing material of the insulin infusion may be crucial for safe and effective glycemic control in critically ill patients.
- ItemPolyelectrolyte complex nanoparticles of poly(ethyleneimine) and poly(acrylic acid): Preparation and applications(Basel : MDPI AG, 2011) Müller, M.; Keßler, B.; Fröhlich, J.; Poeschla, S.; Torger, B.In this contribution we outline polyelectrolyte (PEL) complex (PEC) nanoparticles, prepared by mixing solutions of the low cost PEL components poly(ethyleneimine) (PEI) and poly(acrylic acid) (PAC). It was found, that the size and internal structure of PEI/PAC particles can be regulated by process, media and structural parameters. Especially, mixing order, mixing ratio, PEL concentration, pH and molecular weight, were found to be sensible parameters to regulate the size (diameter) of spherical PEI/PAC nanoparticles, in the range between 80-1,000 nm, in a defined way. Finally, applications of dispersed PEI/PAC particles as additives for the paper making process, as well as for drug delivery, are outlined. PEI/PAC nanoparticles mixed directly on model cellulose film showed a higher adsorption level applying the mixing order 1. PAC 2. PEI compared to 1. PEI 2. PAC. Surface bound PEI/PAC nanoparticles were found to release a model drug compound and to stay immobilized due to the contact with the aqueous release medium.
- ItemSimulations of Protein Adsorption on Nanostructured Surfaces([London] : Macmillan Publishers Limited, part of Springer Nature, 2019) Manzi, Berardo M.; Werner, Marco; Ivanova, Elena P.; Crawford, Russell J.; Baulin, Vladimir A.Recent technological advances have allowed the development of a new generation of nanostructured materials, such as those displaying both mechano-bactericidal activity and substrata that favor the growth of mammalian cells. Nanomaterials that come into contact with biological media such as blood first interact with proteins, hence understanding the process of adsorption of proteins onto these surfaces is highly important. The Random Sequential Adsorption (RSA) model for protein adsorption on flat surfaces was modified to account for nanostructured surfaces. Phenomena related to the nanofeature geometry have been revealed during the modelling process; e.g., convex geometries can lead to lower steric hindrance between particles, and hence higher degrees of surface coverage per unit area. These properties become more pronounced when a decrease in the size mismatch between the proteins and the surface nanostructures occurs. This model has been used to analyse the adsorption of human serum albumin (HSA) on a nano-structured black silicon (bSi) surface. This allowed the Blocking Function (the rate of adsorption) to be evaluated. The probability of the protein to adsorb as a function of the occupancy was also calculated.