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Author: Schulze, Agnes × Has files: Yes × Type: Article × Type: Text ×

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Now showing 1 - 10 of 21
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    Synthesis of Modified Poly(vinyl Alcohol)s and Their Degradation Using an Enzymatic Cascade
    (Weinheim : Wiley-VCH, 2023) von Haugwitz, Gerlis; Donnelly, Kian; Di Filippo, Mara; Breite, Daniel; Phippard, Max; Schulze, Agnes; Wei, Ren; Baumann, Marcus; Bornscheuer, Uwe T.
    Poly(vinyl alcohol) (PVA) is a water-soluble synthetic vinyl polymer with remarkable physical properties including thermostability and viscosity. Its biodegradability, however, is low even though a large amount of PVA is released into the environment. Established physical-chemical degradation methods for PVA have several disadvantages such as high price, low efficiency, and secondary pollution. Biodegradation of PVA by microorganisms is slow and frequently involves pyrroloquinoline quinone (PQQ)-dependent enzymes, making it expensive due to the costly cofactor and hence unattractive for industrial applications. In this study, we present a modified PVA film with improved properties as well as a PQQ-independent novel enzymatic cascade for the degradation of modified and unmodified PVA. The cascade consists of four steps catalyzed by three enzymes with in situ cofactor recycling technology making this cascade suitable for industrial applications.
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    Biocatalytic Degradation Efficiency of Postconsumer Polyethylene Terephthalate Packaging Determined by Their Polymer Microstructures
    (Weinheim : Wiley-VCH, 2019) Wei, Ren; Breite, Daniel; Song, Chen; Gräsing, Daniel; Ploss, Tina; Hille, Patrick; Schwerdtfeger, Ruth; Matysik, Jörg; Schulze, Agnes; Zimmermann, Wolfgang
    Polyethylene terephthalate (PET) is the most important mass-produced thermoplastic polyester used as a packaging material. Recently, thermophilic polyester hydrolases such as TfCut2 from Thermobifida fusca have emerged as promising biocatalysts for an eco-friendly PET recycling process. In this study, postconsumer PET food packaging containers are treated with TfCut2 and show weight losses of more than 50% after 96 h of incubation at 70 °C. Differential scanning calorimetry analysis indicates that the high linear degradation rates observed in the first 72 h of incubation is due to the high hydrolysis susceptibility of the mobile amorphous fraction (MAF) of PET. The physical aging process of PET occurring at 70 °C is shown to gradually convert MAF to polymer microstructures with limited accessibility to enzymatic hydrolysis. Analysis of the chain-length distribution of degraded PET by nuclear magnetic resonance spectroscopy reveals that MAF is rapidly hydrolyzed via a combinatorial exo- and endo-type degradation mechanism whereas the remaining PET microstructures are slowly degraded only by endo-type chain scission causing no detectable weight loss. Hence, efficient thermostable biocatalysts are required to overcome the competitive physical aging process for the complete degradation of postconsumer PET materials close to the glass transition temperature of PET.
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    Synthesis of High Crystalline TiO2 Nanoparticles on a Polymer Membrane to Degrade Pollutants from Water
    (Basel : MDPI, 2018-9-5) Fischer, Kristina; Schulz, Paulina; Atanasov, Igor; Abdul Latif, Amira; Thomas, Isabell; Kühnert, Mathias; Prager, Andrea; Griebel, Jan; Schulze, Agnes
    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.
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    Effect of morphology on the photoelectrochemical activity of TiO2 self-organized nanotube arrays
    (Basel : MDPI, 2020) Ennaceri, Houda; Fischer, Kristina; Hanus, Kevin; Chemseddine, Abdelkrim; Prager, Andrea; Griebel, Jan; Kühnert, Mathias; Schulze, Agnes; Abel, Bernd
    In the present work, highly ordered titanium dioxide (TiO2) nanotube anodes were grown using a rapid anodization process. The photoelectrochemical performances of these electrodes strongly depend on the anodization conditions. Parameters such as electrolyte composition, anodization potential and anodization time are shown to affect the geometrical parameters of TiO2 nanotubes. The optimal anodization parameters are determined by photocurrent measurements, linear sweep voltammetry and electrochemical impedance spectroscopy. The thickness of the tube wall and its homogeneity is shown to strongly depend on the anodization potential, and the formation mechanism is discussed. This study permits the optimization of the photocurrent density and contributes to further improvement of the photoelectrochemical water-splitting performance of TiO2 nanotube photoelectrodes. © 2020 by the authors. Licensee MDPI, Basel, Switzerland.
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    Comparison of Photocatalytic Membrane Reactor Types for the Degradation of an Organic Molecule by TiO2-Coated PES Membrane
    (Basel : MDPI, 2020) Regmi, Chhabilal; Lotfi, Shabnam; Espíndola, Jonathan Cawettiere; Fischer, Kristina; Schulze, Agnes; Schäfer, Andrea Iris
    Photocatalytic membrane reactors with different configurations (design, flow modes and light sources) have been widely applied for pollutant removal. A thorough understanding of the contribution of reactor design to performance is required to be able to compare photocatalytic materials. Reactors with different flow designs are implemented for process efficiency comparisons. Several figures-of-merit, namely adapted space-time yield (STY) and photocatalytic space-time yield (PSTY), specific energy consumption (SEC) and degradation rate constants, were used to assess the performance of batch, flow-along and flow-through reactors. A fair comparison of reactor performance, considering throughput together with energy efficiency and photocatalytic activity, was only possible with the modified PSTY. When comparing the three reactors at the example of methylene blue (MB) degradation under LED irradiation, flow-through proved to be the most efficient design. PSTY1/PSTY2 values were approximately 10 times higher than both the batch and flow-along processes. The highest activity of such a reactor is attributed to its unique flow design which allowed the reaction to take place not only on the outer surface of the membrane but also within its pores. The enhancement of the mass transfer when flowing in a narrow space (220 nm in flow-through) contributes to an additional MB removal. © 2020 by the authors. Licensee MDPI, Basel, Switzerland.
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    Estradiol Removal by Adsorptive Coating of a Microfiltration Membrane
    (Basel : MDPI, 2021) Niavarani, Zahra; Breite, Daniel; Prager, Andrea; Abel, Bernd; Schulze, Agnes
    This work demonstrates the enhancement of the adsorption properties of polyethersulfone (PES) microfiltration membranes for 17β-estradiol (E2) from water. This compound represents a highly potent endocrine-disrupting chemical (EDC). The PES membranes were modified with a hydrophilic coating functionalized by amide groups. The modification was performed by the interfacial reaction between hexamethylenediamine (HMD) or piperazine (PIP) as the amine monomer and trimesoyl chloride (TMC) or adipoyl chloride (ADC) as the acid monomer on the surface of the membrane using electron beam irradiation. The modified membranes and the untreated PES membrane were characterized by scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), water permeance measurements, water contact angle measurements, and adsorption experiments. Furthermore, the effects of simultaneous changes in four modification parameters: amine monomer types (HMD or PIP), acid monomer types (TMC or ADC), irradiation dosage (150 or 200 kGy), and the addition of toluene as a swelling agent, on the E2 adsorption capacity were investigated. The results showed that the adsorption capacities of modified PES membranes toward E2 are >60%, while the unmodified PES membrane had an adsorption capacity up to 30% for E2 under similar experimental conditions, i.e., an enhancement of a factor of 2. Next to the superior adsorption properties, the modified PES membranes maintain high water permeability and no pore blockage was observed. The highlighted results pave the way to develop efficient low-cost, stable, and high-performance adsorber membranes.
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    Membrane 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, Kristina
    To 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
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    Biocatalytic Self-Cleaning Polymer Membranes
    (Basel : MDPI, 2015) Schulze, Agnes; Stoelzer, Astrid; Striegler, Karl; Starke, Sandra; Prager, Andrea
    Polymer membrane surfaces have been equipped with the digestive enzyme trypsin. Enzyme immobilization was performed by electron beam irradiation in aqueous media within a one-step method. Using this method, trypsin was covalently and side-unspecific attached to the membrane surface. Thus, the use of preceding polymer functionalization and the use of toxic solvents or reagents can be avoided. The resulting membranes showed significantly improved antifouling properties as demonstrated by repeated filtration of protein solutions. Furthermore, the biocatalytic membrane can be simply “switched on” to actively degrade a fouling layer on the membrane surface and regain the initial permeability. The membrane pore structure (pore size and porosity) was neither damaged by the electron beam treatment nor blocked by the enzyme loading, ensuring a stable membrane performance.
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    Radiation-Induced Graft Immobilization (RIGI): Covalent Binding of Non-Vinyl Compounds on Polymer Membranes
    (Basel : MDPI, 2021) Schmidt, Martin; Zahn, Stefan; Gehlhaar, Florian; Prager, Andrea; Griebel, Jan; Kahnt, Axel; Knolle, Wolfgang; Konieczny, Robert; Gläser, Roger; Schulze, Agnes
    Radiation-induced graft immobilization (RIGI) is a novel method for the covalent binding of substances on polymeric materials without the use of additional chemicals. In contrast to the well-known radiation-induced graft polymerization (RIGP), RIGI can use non-vinyl compounds such as small and large functional molecules, hydrophilic polymers, or even enzymes. In a one-step electron-beam-based process, immobilization can be performed in a clean, fast, and continuous operation mode, as required for industrial applications. This study proposes a reaction mechanism using polyvinylidene fluoride (PVDF) and two small model molecules, glycine and taurine, in aqueous solution. Covalent coupling of single molecules is achieved by radical recombination and alkene addition reactions, with water radiolysis playing a crucial role in the formation of reactive solute species. Hydroxyl radicals contribute mainly to the immobilization, while solvated electrons and hydrogen radicals play a minor role. Release of fluoride is mainly induced by direct ionization of the polymer and supported by water. Hydrophobic chains attached to cations appear to enhance the covalent attachment of solutes to the polymer surface. Computational work is complemented by experimental studies, including X-ray photoelectron spectroscopy (XPS) and fluoride high-performance ion chromatography (HPIC).
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    Charge Separating Microfiltration Membrane with pH-Dependent Selectivity
    (Basel : MDPI, 2018-12-20) Breite, Daniel; Went, Marco; Prager, Andrea; Kuehnert, Mathias; Schulze, Agnes
    Membrane filters are designed for selective separation of components from a mixture. While separation by size might be the most common approach, other characteristics like charge can also be used for separation as presented in this study. Here, a polyether sulfone membrane was modified to create a zwitterionic surface. Depending on the pH value of the surrounding solution the membrane surface will be either negatively or positively charged. Thus, the charged state can be easily adjusted even by small changes of the pH value of the solution. Charged polystyrene beads were used as model reagent to investigate the pH dependent selectivity of the membrane. It was found that electrostatic forces are dominating the interactions between polystyrene beads and membrane surface during the filtration. This enables a complete control of the membrane’s selectivity according to the electrostatic interactions. Furthermore, differently charged beads marked with fluorescent dyes were used to investigate the selectivity of mixtures of charged components. These different components were successfully separated according to their charged state proving the selectivity of the invented membrane.