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- ItemElectron beam-induced immobilization of laccase on porous supports for waste water treatment applications(Basel : MDPI AG, 2014) Jahangiri, E.; Reichelt, S.; Thomas, I.; Hausmann, K.; Schlosser, D.; Schulze, A.The versatile oxidase enzyme laccase was immobilized on porous supports such as polymer membranes and cryogels with a view of using such biocatalysts in bioreactors aiming at the degradation of environmental pollutants in wastewater. Besides a large surface area for supporting the biocatalyst, the aforementioned porous systems also offer the possibility for simultaneous filtration applications in wastewater treatment. Herein a "green" water-based, initiator-free, and straightforward route to highly reactive membrane and cryogel-based bioreactors is presented, where laccase was immobilized onto the porous polymer supports using a water-based electron beam-initiated grafting reaction. In a second approach, the laccase redox mediators 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulphonic acid) (ABTS) and syringaldehyde were cross-linked instead of the enzyme via electron irradiation in a frozen aqueous poly(acrylate) mixture in a one pot set-up, yielding a mechanical stable macroporous cryogel with interconnected pores ranging from 10 to 50 μm in size. The membranes as well as the cryogels were characterized regarding their morphology, chemical composition, and catalytic activity. The reactivity towards waste-water pollutants was demonstrated by the degradation of the model compound bisphenol A (BPA). Both membrane- and cryogel-immobilized laccase remained highly active after electron beam irradiation. Apparent specific BPA removal rates were higher for cryogel-than for membrane-immobilized and free laccase, whereas membrane-immobilized laccase was more stable with respect to maintenance of enzymatic activity and prevention of enzyme leakage from the carrier than cryogel-immobilized laccase. Cryogel-immobilized redox mediators remained functional in accelerating the laccase-catalyzed BPA degradation, and especially ABTS was found to act more efficiently in immobilized than in freely dissolved state.
- ItemMembrane Functionalization in Pilot Scale: Roll‐to‐Roll Electron Beam System with Inline Contact Angle Determination(Weinheim : Wiley-VCH, 2021) Schulze, Agnes; Drößler, Lutz; Weiß, Steffen; Went, Marco; Abdul Latif, Amira; Breite, Daniel; Fischer, KristinaTo increase the permeation performance and antifouling properties of polymer membranes, a one-step reaction using electron irradiation was developed. This process combines the surface activation of the membrane polymer and the simultaneous permanent immobilization of hydrophilic molecules. This technology can be applied to various polymers, flat sheet/hollow fiber membranes and all pore ranges. The roll-to-roll system developed for this enables all process steps including inline analysis for quality control of the membrane surface in a continuously operated system. © 2021 The Authors. Chemie Ingenieur Technik published by Wiley-VCH GmbH
- ItemTailoring the stoichiometry of C3N4 nanosheets under electron beam irradiation(Cambridge : RSC Publ., 2021) Mendes, Rafael G.; Ta, Huy Q.; Yang, Xiaoqin; Bachmatiuk, Alicja; Praus, Petr; Mamakhel, Aref; Iversen, Bo B.; Su, Ren; Gemming, Thomas; Rümmeli, Mark H.Two-dimensional polymeric graphitic carbon nitride (g-C3N4) is a low-cost material with versatile properties that can be enhanced by the introduction of dopant atoms and by changing the degree of polymerization/stoichiometry, which offers significant benefits for numerous applications. Herein, we investigate the stability of g-C3N4 under electron beam irradiation inside a transmission electron microscope operating at different electron acceleration voltages. Our findings indicate that the degradation of g-C3N4 occurs with N species preferentially removed over C species. However, the precise nitrogen group from which N is removed from g-C3N4 (C–N–C, [double bond, length as m-dash]NH or –NH2) is unclear. Moreover, the rate of degradation increases with decreasing electron acceleration voltage, suggesting that inelastic scattering events (radiolysis) dominate over elastic events (knock-on damage). The rate of degradation by removing N atoms is also sensitive to the current density. Hence, we demonstrate that both the electron acceleration voltage and the current density are parameters with which one can use to control the stoichiometry. Moreover, as N species were preferentially removed, the d-spacing of the carbon nitride structure increased. These findings provide a deeper understanding of g-C3N4.
- ItemComparison of the molecular properties and morphology of polypropylenes irradiated under different atmospheres and after annealing(Hoboken, NJ [u.a.] : Wiley InterScience, 2006) Krause, Beate; Häußler, Liane; Voigt, DieterElectron-beam irradiation, a well-known way of generating long-chain branching, was used to modify polypropylene. Samples were investigated with differential scanning calorimetry, polarized light microscopy, and size exclusion chromatography. Independently of the atmosphere, postannealing led to the deactivation of residual radicals and to the reduction of the nucleus density. In comparison with the initial polypropylene, the crystallization temperatures increased for nonannealed samples but decreased for annealed samples. Stable products were obtained only by irradiation in nitrogen followed by annealing. A reaction including free radicals with oxygen in the ambient atmosphere led to increasing molar mass degradation and the formation of long-chain branching after Storage. © 2006 Wiley Periodicals, Inc.
- ItemCharacterization of electron beam irradiated polypropylene: Influence of irradiation temperature on molecular and rheological properties(Hoboken, NJ [u.a.] : Wiley InterScience, 2006) Krause, Beate; Voigt, Dieter; Häuβler, Liane; Auhl, Dietmar; Münstedt, HelmutThe aim of the investigations was to analyze the influence of the temperature during the irradiation process of polypropylene on the molar mass, the formation of long chain branching and the final branching topology. A linear isotactic polypropylene homopolymer was modified by electron beam irradiation at different temperatures, with two irradiation doses to insert long chain branching. The Samples were analyzed by size exclusion chromatography coupled with a multiangle laser light scattering detector, by differential scanning calorimetry, and by shear and elongational rheology. The shear and elongational flow behavior isdiscussed in terms of the influence of molecular parameters and used to analyze the topology of the irradiated samples. With increasing temperature, a slight reduction of the molar mass, an increase of long chain branching and an increase of crystallization temperature were found. © 2006 Wiley Periodicals, Inc.
- ItemLong-chain branching of polypropylene by electron-beam irradiation in the molten state(Hoboken, NJ [u.a.] : Wiley InterScience, 2006) Krause, Beate; Stephan, M.; Volkland, S.; Voigt, D.; Häußler, L.; Dorschner, H.The electron-beam irradiation of polymers generates modification effects in the macromolecular structure and material properties. Therefore, irradiation processing is mostly realized in the polymer solid state. In this way, the modification of linear polypropylene may result in long-chain branching of polypropylene macromolecules. The objective of this article is to investigate the effect of a polymer in the molten state during electron-beam irradiation on the macromolecular structure and material properties of polypropylene. For this procedure, a special irradiation vessel (BG3) has been developed in which a rapid transfer of polymer films from the solid state to the molten state and a defined temperature during electron-beam irradiation are realizable. The irradiated samples have been analyzed by high-temperature size exclusion chromatography coupled with a multi-angle laser light scattering detector and differential scanning calorimetry (DSC) measurements. With an increasing irradiation dose, a high reduction of the molar mass and an increasing amount of long-chain branching are found. Compared with irradiation in the solid state, the modification in the molten state leads to a higher degree of branching. The Theological experiments in elongation flow clearly exhibit the existence of long-chain branching. Furthermore, DSC measurements show that the glass-transition temperature and peak temperatures of melting and crystallization decrease. © 2005 Wiley Periodicals, Inc.
- ItemWater softening using a light-responsive, spiropyran-modified nanofiltration membrane(Basel : MDPI, 2019) Das, Rasel; Kuehnert, Mathias; Sadat Kazemi, Asieh; Abdi, Yaser; Schulze, AgnesA novel technique for the covalent attachment of a light-responsive spiropyran onto polyamide thin film composite nanofiltration (NF) membranes in a one-step reaction using low-energy electron beam technology is described. The effect of illumination of the immobilized spiropyran was studied, as well as the resulting membrane properties with respect to MgSO4 retention, water permeability rate, and chlorine resistance. Electron beam irradiation showed a direct effect on the transformation of the rough PA NF membrane surface into a ridge-and-valley structure. Upon UV light irradiation, the spiropyran transformed into zwitterionic merocyanine, which had shown MgSO4 removal of >95% with water permeation rates of 6.5 L/(m2·h·bar). Alternatively, visible light was used to convert merocyanine to spiropyran, which achieved >95% of MgSO4 retention with a water flux of around 5.25 L/(m2·h·bar). The modified NF membranes showed higher chlorine resistance as well as a higher normalized water flux as compared to the reference membrane, without a loss of ion retention. All the NF membranes were characterized by scanning electron microscopy and X-ray photoelectron spectroscopy. This study demonstrates a simple and inexpensive method for the immobilization of molecules onto polymeric membranes, which may be applied in water softening.