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- ItemHighly Efficient and Atom Economic Route for the Production of Methyl Acrylate and Acetic Acid from a Biorefinery Side Stream(Washington, DC : American Chemical Society, 2020) El Ouahabi F.; Polyakov M.; Van Klink G.P.M.; Wohlrab S.; Tin S.; De Vries J.G.We report a highly efficient and 100% atom economic synthesis of methyl acrylate and acetic acid via gas phase pyrolysis of methyl 3-acetoxypropionate at 600 °C. The latter can be produced in a single step from methyl levulinate, a side product of Avantium's FDCA process. Copyright © 2020 American Chemical Society.
- ItemPH-Responsive Biohybrid Carrier Material for Phenol Decontamination in Wastewater(Columbus, Ohio : American Chemical Soc., 2018) Pretscher, Martin; Pineda-Contreras, Beatriz A.; Kaiser, Patrick; Reich, Steffen; Schöbel, Judith; Kuttner, Christian; Freitag, Ruth; Fery, Andreas; Schmalz, Holger; Agarwal, SeemaSmart polymers are a valuable platform to protect and control the activity of biological agents over a wide range of conditions, such as low pH, by proper encapsulation. Such conditions are present in olive oil mill wastewater with phenol as one of the most problematic constituents. We show that elastic and pH-responsive diblock copolymer fibers are a suitable carrier for Corynebacterium glutamicum, i.e., bacteria which are known for their ability to degrade phenol. Free C. glutamicum does not survive low pH conditions and fails to degrade phenol at low pH conditions. Our tea-bag like biohybrid system, where the pH-responsive diblock copolymer acts as a protecting outer shell for the embedded bacteria, allows phenol degradation even at low pH. Utilizing a two-step encapsulation process, planktonic cells were first encapsulated in poly(vinyl alcohol) to protect the bacteria against the organic solvents used in the second step employing coaxial electrospinning.
- ItemThe acidity of atmospheric particles and clouds(Katlenburg-Lindau : EGU, 2020) Pye, Havala O.T.; Nenes, Athanasios; Alexander, Becky; Ault, Andrew P.; Barth, Mary C.; Clegg, Simon L.; Collett Jr, Jeffrey L.; Fahey, Kathleen M.; Hennigan, Christopher J.; Herrmann, Hartmut; Kanakidou, Maria; Kelly, James T.; Ku, I-Ting; McNeill, V. Faye; Riemer, Nicole; Schaefer, Thomas; Shi, Guoliang; Tilgner, Andreas; Walker, John T.; Wang, Tao; Weber, Rodney; Xing, Jia; Zaveri, Rahul A.; Zuend, AndreasAcidity, defined as pH, is a central component of aqueous chemistry. In the atmosphere, the acidity of condensed phases (aerosol particles, cloud water, and fog droplets) governs the phase partitioning of semivolatile gases such as HNO3, NH3, HCl, and organic acids and bases as well as chemical reaction rates. It has implications for the atmospheric lifetime of pollutants, deposition, and human health. Despite its fundamental role in atmospheric processes, only recently has this field seen a growth in the number of studies on particle acidity. Even with this growth, many fine-particle pH estimates must be based on thermodynamic model calculations since no operational techniques exist for direct measurements. Current information indicates acidic fine particles are ubiquitous, but observationally constrained pH estimates are limited in spatial and temporal coverage. Clouds and fogs are also generally acidic, but to a lesser degree than particles, and have a range of pH that is quite sensitive to anthropogenic emissions of sulfur and nitrogen oxides, as well as ambient ammonia. Historical measurements indicate that cloud and fog droplet pH has changed in recent decades in response to controls on anthropogenic emissions, while the limited trend data for aerosol particles indicate acidity may be relatively constant due to the semivolatile nature of the key acids and bases and buffering in particles. This paper reviews and synthesizes the current state of knowledge on the acidity of atmospheric condensed phases, specifically particles and cloud droplets. It includes recommendations for estimating acidity and pH, standard nomenclature, a synthesis of current pH estimates based on observations, and new model calculations on the local and global scale. © 2020 Author(s).
- ItemControlled synthesis of mussel-inspired Ag nanoparticle coatings with demonstrated in vitro and in vivo antibacterial properties(Amsterdam [u.a.] : Elsevier Science, 2021) Wang, Xiaowei; Xu, Kehui; Cui, Wendi; Yang, Xi; Maitz, Manfred F.; Li, Wei; Li, Xiangyang; Chen, JialongThe in-situ formation of silver nanoparticles (AgNPs) via dopamine-reduction of Ag+ has been widely utilized for titanium implants to introduce antibacterial properties. In previous studies, the preparation of AgNPs has focused on controlling the feeding concentrations, while the pH of the reaction solution was ignored. Herein, we systematically determined the influence of various pH (4, 7, 10) and Ag+ concentrations (0.01, 0.1 mg/mL) on the AgNPs formation, followed by the evaluation of the antibacterial properties in vitro and in vivo. The results revealed that an alkaline environment was favourable for AgNP formation and resulted in more particles. Although the AgNPs bearing Ti had lower biocompatibilities, it was significantly improved after 7 days of mineralization in simulated body fluid. The outstanding antibacterial property of the AgNPs was well maintained after one day and seven days of implantation. Moreover, 3D micro-CT modelling showed that the pH 10/0.1 group exhibited remarkable osteogenesis, which may be due to their strong antibacterial properties and ability to promote mineralization. Therefore, we have demonstrated that the solution pH was as important as the feeding Ag+ concentration in determining AgNP formation, and it has paved the way for developing various AgNP-loaded surfaces that could meet different antibacterial needs.
- ItemProximal Soil Sensing - A Contribution for Species Habitat Distribution Modelling of Earthworms in Agricultural Soils?(San Francisco, California, US : PLOS, 2016) Schirrmann, Michael; Joschko, Monika; Gebbers, Robin; Kramer, Eckart; Zörner, Mirjam; Barkusky, Dietmar; Timmer, JensBackground: Earthworms are important for maintaining soil ecosystem functioning and serve as indicators of soil fertility. However, detection of earthworms is time-consuming, which hinders the assessment of earthworm abundances with high sampling density over entire fields. Recent developments of mobile terrestrial sensor platforms for proximal soil sensing (PSS) provided new tools for collecting dense spatial information of soils using various sensing principles. Yet, the potential of PSS for assessing earthworm habitats is largely unexplored. This study investigates whether PSS data contribute to the spatial prediction of earthworm abundances in species distribution models of agricultural soils. Methodology/Principal Findings: Proximal soil sensing data, e.g., soil electrical conductivity (EC), pH, and near infrared absorbance (NIR), were collected in real-time in a field with two management strategies (reduced tillage / conventional tillage) and sandy to loam soils. PSS was related to observations from a long-term (11 years) earthworm observation study conducted at 42 plots. Earthworms were sampled from 0.5 x 0.5 x 0.2 m³ soil blocks and identified to species level. Sensor data were highly correlated with earthworm abundances observed in reduced tillage but less correlated with earthworm abundances observed in conventional tillage. This may indicate that management influences the sensor-earthworm relationship. Generalized additive models and state-space models showed that modelling based on data fusion from EC, pH, and NIR sensors produced better results than modelling without sensor data or data from just a single sensor. Regarding the individual earthworm species, particular sensor combinations were more appropriate than others due to the different habitat requirements of the earthworms. Earthworm species with soil-specific habitat preferences were spatially predicted with higher accuracy by PSS than more ubiquitous species. Conclusions/Significance: Our findings suggest that PSS contributes to the spatial modelling of earthworm abundances at field scale and that it will support species distribution modelling in the attempt to understand the soil-earthworm relationships in agroecosystems.
- ItemPeptide induced crystallization of calcium carbonate on wrinkle patterned substrate: implications for chitin formation in molluscs(Basel : MDPI, 2013) Weiss, Ingrid M.; Ghatak, Anindita Sengupta; Koch, Markus; Guth, ChristinaWe here present the nucleation and growth of calcium carbonate under the influence of synthetic peptides on topographically patterned poly(dimethylsiloxane) (PDMS) substrates, which have a controlled density of defects between the wrinkles. Experiments with two lysine-rich peptides derived from the extracellular conserved domain E22 of the mollusc chitin synthase Ar-CS1, AKKKKKAS (AS8) and EEKKKKKES (ES9) on these substrates showed their influence on the calcium carbonate morphology. A transition from polycrystalline composites to single crystalline phases was achieved with the peptide AS8 by changing the pH of the buffer solution. We analyzed three different pH values as previous experiments showed that E22 interacts with aragonite biominerals more strongly at pH 7.75 than at pH 9.0. At any given pH, crystals appeared in characteristic morphologies only on wrinkled substrates, and did not occur on the flat, wrinkle-free PDMS substrate. These results suggest that these wrinkled substrates could be useful for controlling the morphologies of other mineral/peptide and mineral/protein composites. In nature, these templates are formed enzymatically by glycosyltransferases containing pH-sensitive epitopes, similar to the peptides investigated here. Our in vitro test systems may be useful to gain understanding of the formation of distinct 3D morphologies in mollusc shells in response to local pH shifts during the mineralization of organic templates.
- ItemSoil pH mapping with an on-the-go sensor(Basel : MDPI, 2011) Schirrmann, Michael; Gebbers, Robin; Kramer, Eckart; Seidel, JanSoil pH is a key parameter for crop productivity, therefore, its spatial variation should be adequately addressed to improve precision management decisions. Recently, the Veris pH ManagerTM, a sensor for high-resolution mapping of soil pH at the field scale, has been made commercially available in the US. While driving over the field, soil pH is measured on-the-go directly within the soil by ion selective antimony electrodes. The aim of this study was to evaluate the Veris pH ManagerTM under farming conditions in Germany. Sensor readings were compared with data obtained by standard protocols of soil pH assessment. Experiments took place under different scenarios: (a) controlled tests in the lab, (b) semicontrolled test on transects in a stop-and-go mode, and (c) tests under practical conditions in the field with the sensor working in its typical on-the-go mode. Accuracy issues, problems, options, and potential benefits of the Veris pH ManagerTM were addressed. The tests demonstrated a high degree of linearity between standard laboratory values and sensor readings. Under practical conditions in the field (scenario c), the measure of fit (r2) for the regression between the on-the-go measurements and the reference data was 0.71, 0.63, and 0.84, respectively. Field-specific calibration was necessary to reduce systematic errors. Accuracy of the on-the-go maps was considerably higher compared with the pH maps obtained by following the standard protocols, and the error in calculating lime requirements was reduced by about one half. However, the system showed some weaknesses due to blockage by residual straw and weed roots. If these problems were solved, the on-the-go sensor investigated here could be an efficient alternative to standard sampling protocols as a basis for liming in Germany.
- ItemEvaluating Soil-Borne Causes of Biomass Variability in Grassland by Remote and Proximal Sensing(Basel : MDPI AG, 2019) Vogel, Sebastian; Gebbers, Robin; Oertel, Marcel; Kramer, EckartOn a grassland field with sandy soils in Northeast Germany (Brandenburg), vegetation indices from multi-spectral UAV-based remote sensing were used to predict grassland biomass productivity. These data were combined with soil pH value and apparent electrical conductivity (ECa) from on-the-go proximal sensing serving as indicators for soil-borne causes of grassland biomass variation. The field internal magnitude of spatial variability and hidden correlations between the variables of investigation were analyzed by means of geostatistics and boundary-line analysis to elucidate the influence of soil pH and ECa on the spatial distribution of biomass. Biomass and pH showed high spatial variability, which necessitates high resolution data acquisition of soil and plant properties. Moreover, boundary-line analysis showed grassland biomass maxima at pH values between 5.3 and 7.2 and ECa values between 3.5 and 17.5 mS m−1. After calibrating ECa to soil moisture, the ECa optimum was translated to a range of optimum soil moisture from 7% to 13%. This matches well with to the plant-available water content of the predominantly sandy soil as derived from its water retention curve. These results can be used in site-specific management decisions to improve grassland biomass productivity in low-yield regions of the field due to soil acidity or texture-related water scarcity.
- ItemCarbonate-based Janus micromotors moving in ultra-light acidic environment generated by HeLa cells in situ(London : Nature Publishing Group, 2016) Guix, Maria; Meyer, Anne K.; Koch, Britta; Schmidt, Oliver G.Novel approaches to develop naturally-induced drug delivery in tumor environments in a deterministic and controlled manner have become of growing interest in recent years. Different polymeric-based microstructures and other biocompatible substances have been studied taking advantage of lactic acidosis phenomena in tumor cells, which decrease the tumor extracellular pH down to 6.8. Micromotors have recently demonstrated a high performance in living systems, revealing autonomous movement in the acidic environment of the stomach or moving inside living cells by using acoustic waves, opening the doors for implementation of such smart microengines into living entities. The need to develop biocompatible motors which are driven by natural fuel sources inherently created in biological systems has thus become of crucial importance. As a proof of principle, we here demonstrate calcium carbonate Janus particles moving in extremely light acidic environments (pH 6.5), whose motion is induced in conditioned acidic medium generated by HeLa cells in situ. Our system not only obviates the need for an external fuel, but also presents a selective activation of the micromotors which promotes their motion and consequent dissolution in presence of a quickly propagating cell source (i.e. tumor cells), therefore inspiring new micromotor configurations for potential drug delivery systems.
- ItemHigh resolution spectroscopy reveals fibrillation inhibition pathways of insulin([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Deckert-Gaudig, Tanja; Deckert, VolkerFibril formation implies the conversion of a protein’s native secondary structure and is associated with several neurodegenerative diseases. A better understanding of fibrillation inhibition and fibril dissection requires nanoscale molecular characterization of amyloid structures involved. Tip-enhanced Raman scattering (TERS) has already been used to chemically analyze amyloid fibrils on a sub-protein unit basis. Here, TERS in combination with atomic force microscopy (AFM), and conventional Raman spectroscopy characterizes insulin assemblies generated during inhibition and dissection experiments in the presence of benzonitrile, dimethylsulfoxide, quercetin, and β-carotene. The AFM topography indicates formation of filamentous or bead-like insulin self-assemblies. Information on the secondary structure of bulk samples and of single aggregates is obtained from standard Raman and TERS measurements. In particular the high spatial resolution of TERS reveals the surface conformations associated with the specific agents. The insulin aggregates formed under different inhibition and dissection conditions can show a similar morphology but differ in their β-sheet structure content. This suggests different aggregation pathways where the prevention of the β-sheet stacking of the peptide chains plays a major role. The presented approach is not limited to amyloid-related reasearch but can be readily applied to systems requiring extremely surface-sensitive characterization without the need of labels.