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- ItemComparison 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 IrisPhotocatalytic 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.
- ItemDesign of a core-shell catalyst : an effective strategy for suppressing side reactions in syngas for direct selective conversion to light olefins(Cambridge : RSC, 2020) Tan, Li; Wang, Fan; Zhang, Peipe; Suzuki, Yuichi; Wu, Yingquan; Chen, Jiangang; Yang, Guohui; Tsubaki, NoritatsuAn elegant catalyst is designedviathe encapsulation of metallic oxide Zn-Cr inside of zeolite SAPO34 as a core-shell structure (Zn-Cr@SAPO) to realize the coupling of methanol-synthesis and methanol-to-olefin reactions. It can not only break through the limitation of the Anderson-Schulz-Flory distribution but can also overcome the disadvantages of physical mixture catalysts, such as excessive CO2formation. The confinement effect, hierarchical structure and extremely short distance between the two active components result in the Zn-Cr@SAPO capsule catalyst having better mass transfer and diffusion with a boosted synergistic effect. Due to the difference between the adsorption energies of the Zn-Cr metallic oxide/SAPO zeolite physical mixture and capsule catalysts, the produced water and light olefins are easily removed from the Zn-Cr@SAPO capsule catalyst after formation, suppressing the side reactions. The light olefin space time yield (STY) of the capsule catalyst is more than twice that of the typical physical mixture catalyst. The designed capsule catalyst has superior potential for scale-up in industrial applications while simultaneously extending the capabilities of hybrid catalysts for other tandem catalysis reactions through this strategy. © The Royal Society of Chemistry 2020.
- ItemAn Approach to Ring Resonator Biosensing Assisted by Dielectrophoresis: Design, Simulation and Fabrication(Basel : MDPI, 2020) Henriksson, Anders; Kasper, Laura; Jäger, Matthias; Neubauer, Peter; Birkholz, MarioThe combination of extreme miniaturization with a high sensitivity and the potential to be integrated in an array form on a chip has made silicon-based photonic microring resonators a very attractive research topic. As biosensors are approaching the nanoscale, analyte mass transfer and bonding kinetics have been ascribed as crucial factors that limit their performance. One solution may be a system that applies dielectrophoretic forces, in addition to microfluidics, to overcome the diffusion limits of conventional biosensors. Dielectrophoresis, which involves the migration of polarized dielectric particles in a non-uniform alternating electric field, has previously been successfully applied to achieve a 1000-fold improved detection efficiency in nanopore sensing and may significantly increase the sensitivity in microring resonator biosensing. In the current work, we designed microring resonators with integrated electrodes next to the sensor surface that may be used to explore the effect of dielectrophoresis. The chip design, including two different electrode configurations, electric field gradient simulations, and the fabrication process flow of a dielectrohoresis-enhanced microring resonator-based sensor, is presented in this paper. Finite element method (FEM) simulations calculated for both electrode configurations revealed ?E2 values above 1017 V2m-3 around the sensing areas. This is comparable to electric field gradients previously reported for successful interactions with larger molecules, such as proteins and antibodies. © 2020 by the authors. Licensee MDPI, Basel, Switzerland.
- ItemTime-resolved structural evolution during the collapse of responsive hydrogels: The microgel-to-particle transition(Washington, DC [u.a.] : Assoc., 2018) Keidel, Rico; Ghavami, Ali; Lugo, Dersy M.; Lotze, Gudrun; Virtanen, Otto; Beumers, Peter; Pedersen, Jan Skov; Bardow, Andre; Winkler, Roland G.; Richtering, WalterAdaptive hydrogels, often termed smart materials, are macromolecules whose structure adjusts to external stimuli. Responsive micro- and nanogels are particularly interesting because the small length scale enables very fast response times. Chemical cross-links provide topological constraints and define the three-dimensional structure of the microgels, whereas their porous structure permits fast mass transfer, enabling very rapid structural adaption of the microgel to the environment. The change of microgel structure involves a unique transition from a flexible, swollen finite-size macromolecular network, characterized by a fuzzy surface, to a colloidal particle with homogeneous density and a sharp surface. In this contribution, we determine, for the first time, the structural evolution during the microgel-to-particle transition. Time-resolved small-angle x-ray scattering experiments and computer simulations unambiguously reveal a two-stage process: In a first, very fast process, collapsed clusters form at the periphery, leading to an intermediate, hollowish core-shell structure that slowly transforms to a globule. This structural evolution is independent of the type of stimulus and thus applies to instantaneous transitions as in a temperature jump or to slower stimuli that rely on the uptake of active molecules from and/or exchange with the environment. The fast transitions of size and shape provide unique opportunities for various applications as, for example, in uptake and release, catalysis, or sensing.
- ItemTime-lapse gravity and levelling surveys reveal mass loss and ongoing subsidence in the urban subrosion-prone area of Bad Frankenhausen, Germany(Göttingen : Copernicus Publ., 2019) Kobe, Martin; Gabriel, Gerald; Weise, Adelheid; Vogel, DetlefWe present results of sophisticated, high-precision time-lapse gravity monitoring that was conducted over 4 years in Bad Frankenhausen (Germany). To our knowledge, this is the first successful attempt to monitor subrosion-induced mass changes in urban areas with repeated gravimetry. The method provides an approach to estimate the mass of dissolved rocks in the subsurface. Subrosion, i.e. leaching and transfer of soluble rocks, occurs worldwide. Mainly in urban areas, any resulting ground subsidence can cause severe damage, especially if catastrophic events, i.e. collapse sinkholes, occur. Monitoring strategies typically make use of established geodetic methods, such as levelling, and therefore focus on the associated deformation processes. In this study, we combine levelling and highly precise time-lapse gravity observations. Our investigation area is the urban area of Bad Frankenhausen in central Germany, which is prone to subrosion, as many subsidence and sinkhole features on the surface reveal. The city and the surrounding areas are underlain by soluble Permian deposits, which are continuously dissolved by meteoric water and groundwater in a strongly fractured environment. Between 2014 and 2018, a total of 17 high-precision time-lapse gravimetry and 18 levelling campaigns were carried out in quarterly intervals within a local monitoring network. This network covers historical sinkhole areas but also areas that are considered to be stable. Our results reveal ongoing subsidence of up to 30.4 mm a−1 locally, with distinct spatiotemporal variations. Furthermore, we observe a significant time-variable gravity decrease on the order of 8 µGal over 4 years at several measurement points. In the processing workflow, after the application of all required corrections and least squares adjustment to our gravity observations, a significant effect of varying soil water content on the adjusted gravity differences was figured out. Therefore, we place special focus on the correlation of these observations and the correction of the adjusted gravity differences for soil water variations using the Global Land Data Assimilation System (GLDAS) Noah model to separate these effects from subrosion-induced gravity changes. Our investigations demonstrate the feasibility of high-precision time-lapse gravity monitoring in urban areas for sinkhole investigations. Although the observed rates of gravity decrease of 1–2 µGal a−1 are small, we suggest that it is significantly associated with subterranean mass loss due to subrosion processes. We discuss limitations and implications of our approach, as well as give a first quantitative estimation of mass transfer at different depths and for different densities of dissolved rocks.