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Author: Schulze, Agnes × Type: Text ×

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Now showing 1 - 10 of 21
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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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    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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    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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    Enzymatic degradation of polyethylene terephthalate nanoplastics analyzed in real time by isothermal titration calorimetry
    (Amsterdam [u.a.] : Elsevier Science, 2021) Vogel, Kristina; Wei, Ren; Pfaff, Lara; Breite, Daniel; Al-Fathi, Hassan; Ortmann, Christian; Estrela-Lopis, Irina; Venus, Tom; Schulze, Agnes; Harms, Hauke; Bornscheuer, Uwe T.; Maskow, Thomas
    Plastics are globally used for a variety of benefits. As a consequence of poor recycling or reuse, improperly disposed plastic waste accumulates in terrestrial and aquatic ecosystems to a considerable extent. Large plastic waste items become fragmented to small particles through mechanical and (photo)chemical processes. Particles with sizes ranging from millimeter (microplastics, <5 mm) to nanometer (nanoplastics, NP, <100 nm) are apparently persistent and have adverse effects on ecosystems and human health. Current research therefore focuses on whether and to what extent microorganisms or enzymes can degrade these NP. In this study, we addressed the question of what information isothermal titration calorimetry, which tracks the heat of reaction of the chain scission of a polyester, can provide about the kinetics and completeness of the degradation process. The majority of the heat represents the cleavage energy of the ester bonds in polymer backbones providing real-time kinetic information. Calorimetry operates even in complex matrices. Using the example of the cutinase-catalyzed degradation of polyethylene terephthalate (PET) nanoparticles, we found that calorimetry (isothermal titration calorimetry-ITC) in combination with thermokinetic models is excellently suited for an in-depth analysis of the degradation processes of NP. For instance, we can separately quantify i) the enthalpy of surface adsorption ∆AdsH = 129 ± 2 kJ mol−1, ii) the enthalpy of the cleavage of the ester bonds ∆EBH = −58 ± 1.9 kJ mol−1 and the apparent equilibrium constant of the enzyme substrate complex K = 0.046 ± 0.015 g L−1. It could be determined that the heat production of PET NP degradation depends to 95% on the reaction heat and only to 5% on the adsorption heat. The fact that the percentage of cleaved ester bonds (η = 12.9 ± 2.4%) is quantifiable with the new method is of particular practical importance. The new method promises a quantification of enzymatic and microbial adsorption to NP and their degradation in mimicked real-world aquatic conditions.
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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.
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    Water softening using a light-responsive, spiropyran-modified nanofiltration membrane
    (Basel : MDPI, 2019) Das, Rasel; Kuehnert, Mathias; Sadat Kazemi, Asieh; Abdi, Yaser; Schulze, Agnes
    A 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.
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    Reduction of biofouling of a microfiltration membrane using amide functionalities-Hydrophilization without changes in morphology
    (Basel : MDPI, 2020) Breite, Daniel; Went, Marco; Prager, Andrea; Kühnert, Mathias; Schulze, Agnes
    A major goal of membrane science is the improvement of the membrane performance and the reduction of fouling effects, which occur during most aqueous filtration applications. Increasing the surface hydrophilicity can improve the membrane performance (in case of aqueous media) and decelerates membrane fouling. In this study, a PES microfiltration membrane (14,600 L m−2 h−1 bar−1) was hydrophilized using a hydrophilic surface coating based on amide functionalities, converting the hydrophobic membrane surface (water contact angle, WCA: ~90°) into an extremely hydrophilic one (WCA: ~30°). The amide layer was created by first immobilizing piperazine to the membrane surface via electron beam irradiation. Subsequently, a reaction with 1,3,5-benzenetricarbonyl trichloride (TMC) was applied to generate an amide structure. The presented approach resulted in a hydrophilic membrane surface, while maintaining permeance of the membrane without pore blocking. All membranes were investigated regarding their permeance, porosity, average pore size, morphology (SEM), chemical composition (XPS), and wettability. Soxhlet extraction was carried out to demonstrate the stability of the applied coating. The improvement of the modified membranes was demonstrated using dead-end filtration of algae solutions. After three fouling cycles, about 60% of the initial permeance remain for the modified membranes, while only ~25% remain for the reference.
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    TiO2 as Photosensitizer and Photoinitiator for Synthesis of Photoactive TiO2-PEGDA Hydrogel Without Organic Photoinitiator
    (Lausanne : Frontiers Media, 2018-8-7) Glass, Sarah; Trinklein, Betsy; Abel, Bernd; Schulze, Agnes
    The replacement of potentially toxic photoinitiators is of increasing interest regarding the synthesis of biomaterials by photopolymerization. Therefore, we present a new method for the preparation of UV polymerized hydrogels with TiO2 as a photoinitiator. Titania is known to be an excellent photoactive compound which is non-toxic, inert, and cheap. The so-formed hydrogels possess excellent mechanical properties, a high swelling ratio, and high thermal stability. Furthermore, no TiO2 is released from the hydrogels. Thus, the material is highly suitable for medical applications. Additionally, the present TiO2 in the hydrogels remains photoactive as demonstrated by degradation of methylene blue. This enables the application of TiO2-hydrogels in photodynamic therapy.
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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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    Tailoring Membrane Surface Charges: A Novel Study on Electrostatic Interactions during Membrane Fouling
    (Basel : MDPI, 2015) Breite, Daniel; Went, Marco; Prager, Andrea; Schulze, Agnes
    In this work we aim to show that the overall surface potential is a key factor to understand and predict anti-fouling characteristics of a polymer membrane. Therefore, polyvinylidene fluoride membranes were modified by electron beam-induced grafting reactions forming neutral, acidic, alkaline or zwitterionic structures on the membrane surface. The differently charged membranes were investigated regarding their surface properties using diverse analytical methods: zeta potential, static and dynamic water contact angle, scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS). Porosimetry measurements proved that there is no pore blocking due to the modifications. Monodisperse suspensions of differently charged polystyrene beads were synthesized by a radical emulsion polymerization reaction and were used as a model fouling reagent, preventing comparability problems known from current literature. To simulate membrane fouling, different bead suspensions were filtered through the membranes. The fouling characteristics were investigated regarding permeation flux decline and concentration of model fouling reagent in filtrate as well as by SEM. By considering electrostatic interactions equal to hydrophobic interactions we developed a novel fouling test system, which enables the prediction of a membrane’s fouling tendency. Electrostatic forces are dominating, especially when charged fouling reagents are present, and can help to explain fouling characteristics that cannot be explained considering the surface wettability.