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10. Immobilization of Bi2WO6 on Polymer Membranes for Photocatalytic Removal of Micropollutants from Water – A Stable and Visible Light Active Alternative.

Author

Fischer, Kristina, Abdul Latif, Amira, Griebel, Jan, Prager, Andrea, Shayestehpour, Omid, Zahn, Stefan, and Schulze, Agnes

Abstract

In this work, bismuth tungstate Bi2WO6 is immobilized on polymer membranes to photocatalytically remove micropollutants from water as an alternative to titanium dioxide TiO2. A synthesis method for Bi2WO6 preparation and its immobilization on a polymer membrane is developed. Bi2WO6 is characterized using X‐ray diffraction and UV–vis reflectance spectroscopy, while the membrane undergoes analysis through scanning electron microscopy, X‐ray photoelectron spectroscopy, and degradation experiments. The density of states calculations for TiO2 and Bi2WO6, along with PVDF reactions with potential reactive species, are investigated by density functional theory. The generation of hydroxyl radicals OH• is investigated via the reaction of coumarin to umbelliferone via fluorescence probe detection and electron paramagnetic resonance. Increasing reactant concentration enhances Bi2WO6 crystallinity. Under UV light at pH 7 and 11, the Bi2WO6 membrane completely degrades propranolol in 3 and 1 h, respectively, remaining stable and reusable for over 10 cycles (30 h). Active under visible light with a bandgap of 2.91 eV, the Bi2WO6 membrane demonstrates superior stability compared to a TiO2 membrane during a 7‐day exposure to UV light as Bi2WO6 does not generate OH• radicals. The Bi2WO6 membrane is an alternative for water pollutant degradation due to its visible light activity and long‐term stability. [ABSTRACT FROM AUTHOR]

Published
2024
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20. Reagent-Free Immobilization of Industrial Lipases to Develop Lipolytic Membranes with Self-Cleaning Surfaces

Author

Schmidt, Martin, Prager, Andrea, Schönherr, Nadja, Gläser, Roger, Schulze, Agnes, Schmidt, Martin, Prager, Andrea, Schönherr, Nadja, Gläser, Roger, and Schulze, Agnes

Abstract

Biocatalytic membrane reactors combine the highly efficient biotransformation capability of enzymes with the selective filtration performance of membrane filters. Common strategies to immobilize enzymes on polymeric membranes are based on chemical coupling reactions. Still, they are associated with drawbacks such as long reaction times, high costs, and the use of potentially toxic or hazardous reagents. In this study, a reagent-free immobilization method based on electron beam irradiation was investigated, which allows much faster, cleaner, and cheaper fabrication of enzyme membrane reactors. Two industrial lipase enzymes were coupled onto a polyvinylidene fluoride (PVDF) flat sheet membrane to create self-cleaning surfaces. The response surface methodology (RSM) in the design-of-experiments approach was applied to investigate the effects of three numerical factors on enzyme activity, yielding a maximum activity of 823 118 U m2 (enzyme concentration: 8.4 g L1, impregnation time: 5 min, irradiation dose: 80 kGy). The lipolytic membranes were used in fouling tests with olive oil (1 g L1 in 2 mM sodium dodecyl sulfate), resulting in 100% regeneration of filtration performance after 3 h of self-cleaning in an aqueous buffer (pH 8, 37 C). Reusability with three consecutive cycles demonstrates regeneration of 95%. Comprehensive membrane characterization was performed by determining enzyme kinetic parameters, permeance monitoring, X-ray photoelectron spectroscopy, FTIR spectroscopy, scanning electron microscopy, and zeta potential, as well as water contact angle measurements.

Published
2022

29. Highly Efficient One-Step Protein Immobilization on Polymer Membranes Supported by Response Surface Methodology

Author

Schmidt, Martin, Abdul Latif, Amira, Prager, Andrea, Gläser, Roger, Schulze, Agnes, Schmidt, Martin, Abdul Latif, Amira, Prager, Andrea, Gläser, Roger, and Schulze, Agnes

Abstract

Immobilization of proteins by covalent coupling to polymeric materials offers numerous excellent advantages for various applications, however, it is usually limited by coupling strategies, which are often too expensive or complex. In this study, an electron-beambased process for covalent coupling of the model protein bovine serum albumin (BSA) onto polyvinylidene fluoride (PVDF) flat sheet membranes was investigated. Immobilization can be performed in a clean, fast, and continuous mode of operation without any additional chemicals involved. Using the Design of Experiments (DoE) approach, nine process factors were investigated for their influence on graft yield and homogeneity. The parameters could be reduced to only four highly significant factors: BSA concentration, impregnation method, impregnation time, and electron beam irradiation dose. Subsequently, optimization of the process was performed using the Response Surface Methodology (RSM). A one-step method was developed, resulting in a high BSA grafting yield of 955 mgm−2 and a relative standard deviation of 3.6%. High efficiency was demonstrated by reusing the impregnation solution five times consecutively without reducing the final BSA grafting yield. Comprehensive characterization was conducted by X-ray photoelectron spectroscopy (XPS), Fourier-transform infrared spectroscopy (FTIR), and measurements of zeta potential, contact angle and surface free energy, as well as filtration performance. In addition, mechanical properties and morphology were examined using mercury porosimetry, tensile testing, and scanning electron microscopy (SEM).

Published
2021

30. Functionalized and Platinum-Decorated Multi-Layer Oxidized Graphene as a Proton, and Electron Conducting Separator in Solid Acid Fuel Cells

Author

Hatahet, Mhamad Hamza, Wagner, Maximilian, Prager, Andrea, Helmstedt, Ulrike, Abel, Bernd, Hatahet, Mhamad Hamza, Wagner, Maximilian, Prager, Andrea, Helmstedt, Ulrike, and Abel, Bernd

Abstract

In the present article, electrodes containing a composite of platinum on top of a plasma-oxidized multi-layer graphene film are investigated as model electrodes that combine an exceptional high platinum utilization with high electrode stability. Graphene is thereby acting as a separator between the phosphate-based electrolyte and the platinum catalyst. Electrochemical impedance measurements in humidified hydrogen at 240 °C show area-normalized electrode resistance of 0.06 Ω·cm−2 for a platinum loading of ∼60 µgPt·cm−2, resulting in an outstanding mass normalized activity of almost 280 S·mgPt−1, exceeding even state-of-the-art electrodes. The presented platinum decorated graphene electrodes enable stable operation over 60 h with a non-optimized degradation rate of 0.15% h−1, whereas electrodes with a similar design but without the graphene as separator are prone to a very fast degradation. The presented results propose an efficient way to stabilize solid acid fuel cell electrodes and provide valuable insights about the degradation processes which are essential for further electrode optimization.

Published
2021

40. High quality reduced graphene oxide flakes by fast kinetically controlled and clean indirect UV-induced radical reduction

Author

Flyunt, Roman, Knolle, Wolfgang, Kahnt, Axel, Halbig, Christian E., Lotnyk, Andriy, Häupl, Tilmann, Prager, Andrea, Eigler, Siegfried, and Abel, Bernd

Subjects
ddc:540, Naturwissenschaftliche Fakultät
Abstract

This work highlights a surprisingly simple and kinetically controlled highly efficient indirect method for the production of high quality reduced graphene oxide (rGO) flakes via UV irradiation of aqueous dispersions of graphene oxide (GO), in which the GO is not excited directly. While the direct photoexcitation of aqueous GO (when GO is the only light-absorbing component) takes several hours of reaction time at ambient temperature (4 h) leading only to a partial GO reduction, the addition of small amounts of isopropanol and acetone (2% and 1%) leads to a dramatically shortened reaction time by more than two orders of magnitude (2 min) and a very efficient and soft reduction of graphene oxide. This method avoids the formation of non-volatile species and in turn contamination of the produced rGO and it is based on the highly efficient generation of reducing carbon centered isopropanol radicals via the reaction of triplet acetone with isopropanol. While the direct photolysis of GO dispersions easily leads to degradation of the carbon lattice of GO and thus to a relatively low electric conductivity of the films of flakes, our indirect photoreduction of GO instead largely avoids the formation of defects, keeping the carbon lattice intact. Mechanisms of the direct and indirect photoreduction of GO have been elucidated and compared. Raman spectroscopy, XPS and conductivity measurements prove the efficiency of the indirect photoreduction in comparison with the state-of-the-art reduction method for GO (hydriodic acid/trifluoroacetic acid). The rapid reduction times and water solvent containing only small amounts of isopropanol and acetone may allow easy process up-scaling for technical applications and low-energy consumption.

Published
2016

43. Bio-Inspired Polymer Membrane Surface Cleaning

Author

Schulze, Agnes, primary, Breite, Daniel, additional, Kim, Yongkyum, additional, Schmidt, Martin, additional, Thomas, Isabell, additional, Went, Marco, additional, Fischer, Kristina, additional, and Prager, Andrea, additional

Published
2017
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44. Growth, Polymorphism, and Spatially Controlled Surface Immobilization of Biotinylated Variants of IAPP21–27Fibrils

Author

John, Torsten, Bandak, Juhaina, Sarveson, Nilushiya, Hackl, Claudia, Risselada, Herre Jelger, Prager, Andrea, Elsner, Christian, and Abel, Bernd

Abstract

The islet amyloid polypeptide (IAPP) is a regulatory peptide that can aggregate into fibrillar structures associated with type 2 diabetes. In this study, the IAPP21–27segment was modified with a biotin linker at the N-terminus (Btn-GNNFGAIL) to immobilize peptide fibrils on streptavidin-coated surfaces. Key residues for fibril formation of the N-terminal biotinylated IAPP21–27segment were identified by using an alanine scanning approach combined with molecular dynamics simulations, thioflavin T fluorescence measurements, and scanning electron microscopy. Significant contributions of phenylalanine (F23), leucine (L27), and isoleucine (I26) for the fibrillation of the short peptide segment were identified. The fibril morphologies of the peptide variants differed depending on their primary sequence, ranging from flexible and semiflexible to stiff and crystal-like structures. These insights could advance the design of new functional hybrid bionanomaterials and fibril-engineered surface coatings using short peptide segments. To validate this concept, the biotinylated fibrils were immobilized on streptavidin-coated surfaces under spatial control.

Published
2020
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50. Synthesis of High Crystalline TiO2 Nanoparticles on a Polymer Membrane to Degrade Pollutants fromWater.

Author

Fischer, Kristina, Schulz, Paulina, Atanasov, Igor, Latif, Amira Abdul, Thomas, Isabell, Kühnert, Mathias, Prager, Andrea, Griebel, Jan, and Schulze, Agnes

Subjects
PHOTOCATALYSIS, CARBAMAZEPINE, NANOPARTICLES
Abstract

Titanium dioxide (TiO2) is described as an established material to remove pollutants from water. However, TiO2 is still not applied on a large scale due to issues concerning, for example, the form of use or low photocatalytic activity. We present an easily upscalable method to synthesize high active TiO2 nanoparticles on a polyethersulfone microfiltration membrane to remove pollutants in a continuous way. For this purpose, titanium(IV) isopropoxide was mixed with water and hydrochloric acid and treated up to 210 °C. After cooling, the membrane was simply dip-coated into the TiO2 nanoparticle dispersion. Standard characterization was undertaken (i.e., X-ray powder diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy, water permeance, contact angle). Degradation of carbamazepine and methylene blue was executed. By increasing synthesis temperature crystallinity and photocatalytic activity elevates. Both ultrasound modification of nanoparticles and membrane pre-modification with carboxyl groups led to fine distribution of nanoparticles. The ultrasound-treated nanoparticles gave the highest photocatalytic activity in degrading carbamazepine and showed no decrease in degradation after nine times of repetition. The TiO2 nanoparticles were strongly bound to the membrane. Photocatalytic TiO2 nanoparticles with high activity were synthesized. The innovative method enables a fast and easy nanoparticle production, which could enable the use in large-scale water cleaning. [ABSTRACT FROM AUTHOR]

Published
2018
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