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- ItemEffect of cation size of binary cation ionic liquid mixtures on capacitive energy storage(New York, NY [u.a.] : Elsevier, 2023) Seltmann, Anna; Verkholyak, Taras; Gołowicz, Dariusz; Pameté, Emmanuel; Kuzmak, Andrij; Presser, Volker; Kondrat, SvyatoslavIonic liquid mixtures show promise as electrolytes for supercapacitors with nanoporous electrodes. Herein, we investigate theoretically and with experiments how binary electrolytes comprising a common anion and two types of differently-sized cations affect capacitive energy storage. We find that such electrolytes can enhance the capacitance of single nanopores and nanoporous electrodes under potential differences negative relative to the potential of zero charge. For a two-electrode cell, however, they are beneficial only at low and intermediate cell voltages, while a neat ionic liquid performs better at higher voltages. We reveal subtle effects of how the distribution of pores accessible to different types of ions correlates with charge storage and suggest approaches to increase capacitance and stored energy density with ionic liquid mixtures.
- ItemMatrix metalloproteinase-1 decorated polymersomes, a surface-active extracellular matrix therapeutic, potentiates collagen degradation and attenuates early liver fibrosis(New York, NY [u.a.] : Elsevier, 2021) Geervliet, Eline; Moreno, Silvia; Baiamonte, Luca; Booijink, Richell; Boye, Susanne; Wang, Peng; Voit, Brigitte; Lederer, Albena; Appelhans, Dietmar; Bansal, RuchiLiver fibrosis affects millions of people worldwide and is rising vastly over the past decades. With no viable therapies available, liver transplantation is the only curative treatment for advanced diseased patients. Excessive accumulation of aberrant extracellular matrix (ECM) proteins, mostly collagens, produced by activated hepatic stellate cells (HSCs), is a hallmark of liver fibrosis. Several studies have suggested an inverse correlation between collagen-I degrading matrix metalloproteinase-1 (MMP-1) serum levels and liver fibrosis progression highlighting reduced MMP-1 levels are associated with poor disease prognosis in patients with liver fibrosis. We hypothesized that delivery of MMP-1 might potentiate collagen degradation and attenuate fibrosis development. In this study, we report a novel approach for the delivery of MMP-1 using MMP-1 decorated polymersomes (MMPsomes), as a surface-active vesicle-based ECM therapeutic, for the treatment of liver fibrosis. The storage-stable and enzymatically active MMPsomes were fabricated by a post-loading of Psomes with MMP-1. MMPsomes were extensively characterized for the physicochemical properties, MMP-1 surface localization, stability, enzymatic activity, and biological effects. Dose-dependent effects of MMP-1, and effects of MMPsomes versus MMP-1, empty polymersomes (Psomes) and MMP-1 + Psomes on gene and protein expression of collagen-I, MMP-1/TIMP-1 ratio, migration and cell viability were examined in TGFβ-activated human HSCs. Finally, the therapeutic effects of MMPsomes, compared to MMP-1, were evaluated in vivo in carbon-tetrachloride (CCl4)-induced early liver fibrosis mouse model. MMPsomes exhibited favorable physicochemical properties, MMP-1 surface localization and improved therapeutic efficacy in TGFβ-activated human HSCs in vitro. In CCl4-induced early liver fibrosis mouse model, MMPsomes inhibited intra-hepatic collagen-I (ECM marker, indicating early liver fibrosis) and F4/80 (marker for macrophages, indicating liver inflammation) expression. In conclusion, our results demonstrate an innovative approach of MMP-1 delivery, using surface-decorated MMPsomes, for alleviating liver fibrosis.
- ItemTowards efficient production of highly optically pure d-lactic acid from lignocellulosic hydrolysates using newly isolated lactic acid bacteria(New York, NY [u.a.] : Elsevier, 2022) Alexandri, Maria; Hübner, Dennis; Schneider, Roland; Fröhling, Antje; Venus, JoachimThis study presents the production of D-lactic acid with high enantiomeric purity using lignocellulosic hydrolysates from newly isolated lactic acid bacterial (LAB) strains. Six strains, 4 heterofermentative and 2 homofermentative, were investigated for their ability to grow and produce lactic acid on sugar beet pulp (SBP) hydrolysates, containing a mixture of hexose and pentose sugars. Among the strains tested, three were isolates designated as A250, A257 and A15, all of which belonged to the genus Leuconostoc. Only strain A250 could be reliably identified as Leuconostoc pseudomesenteroides based on cluster analysis of Maldi-ToF spectra. All strains produced D-lactic acid in the presence of SBP hydrolysates, but with varying optical purities. The homofermentative strains achieved higher D-lactic acid optical purities, but without assimilating the pentose sugars. Co-cultivation of the homofermentative strain Lactobacillus coryniformis subsp. torquens DSM 20005 together with the heterofermentative isolate A250 led to the production of 21.7 g/L D-lactic acid with 99.3 % optical purity. This strategy enabled the complete sugar utilization of the substrate. Nanofiltration of the SBP hydrolysate enhanced the enantiomeric purity of the D-lactic acid produced from the isolates A250 and A15 by about 5 %. The highest D-lactic acid concentration (40 g/L) was achieved in fed-batch cultures of A250 isolate with nanofiltered SBP, where optical purity was 99.4 %. The results of this study underline the feasibility of a novel isolate as an efficient D-lactic acid producer using lignocellulosic hydrolysates.
- ItemIdentification and molecular analysis of interaction sites in the MtSEO-F1 protein involved in forisome assembly(New York, NY [u.a.] : Elsevier, 2020) Rose, Judith; Visser, Franziska; Müller, Boje; Senft, Matthias; Groscurth, Sira; Sicking, Kevin F.; Twyman, Richard M.; Prüfer, Dirk; Noll, Gundula A.Forisomes are large mechanoprotein complexes found solely in legumes such as Medicago truncatula. They comprise several “sieve element occlusion by forisome” (SEO-F) subunits, with MtSEO-F1 as the major structure-forming component. SEO-F proteins possess three conserved domains –an N-terminal domain (SEO-NTD), a potential thioredoxin fold, and a C-terminal domain (SEO-CTD)– but structural and biochemical data are scarce and little is known about the contribution of these domains to forisome assembly. To identify key amino acids involved in MtSEO-F1 dimerization and complex formation, we investigated protein-protein interactions by bimolecular fluorescence complementation and the analysis of yeast two-hybrid and random mutagenesis libraries. We identified a SEO-NTD core region as the major dimerization site, with abundant hydrophobic residues and rare charged residues suggesting dimerization is driven by the hydrophobic effect. We also found that ~45% of the full-length MtSEO-F1 sequence must be conserved for higher-order protein assembly, indicating that large interaction surfaces facilitate stable interactions, contributing to the high resilience of forisome bodies. Interestingly, the removal of 62 amino acids from the C-terminus did not disrupt forisome assembly. This is the first study unraveling interaction sites and mechanisms within the MtSEO-F1 protein at the level of dimerization and complex formation. © 2018
- ItemComparison of bacteria in different metabolic states by micro-Raman spectroscopy(New York, NY [u.a.] : Elsevier, 2022) Shen, Haodong; Rösch, Petra; Thieme, Lara; Pletz, Mathias W.; Popp, JürgenIt was shown that several metabolic states of bacteria with various characteristics such as chemical composition participate in the formation of biofilms. To study the connections and differences among different bacterial metabolic states, five species of bacteria in exponential phase, stationary phase and biofilm have been compared and investigated by micro-Raman spectroscopy. The spectral differences between different metabolic states showed that the chemical composition varied among those metabolic states. Moreover, as can be shown by the spectral differences and principal components (PCs), different species and strains of bacteria behave differently. Furthermore, a principal component analysis (PCA) combined with support vector machines (SVM) was applied to distinguish species of bacteria within the same metabolic states. Our study provides valuable data for the comparison of bacteria between different metabolic states utilizing micro-Raman spectroscopy in combination with chemometrics models.
- ItemVacancy diffusion and its consequences for void growth at the interface of a stripping metal electrode and solid electrolyte(New York, NY [u.a.] : Elsevier, 2023) Shishvan, S.S.; Fleck, N.A.; McMeeking, R.M.; Deshpande, V.S.It is commonly observed that voids can nucleate and grow in the lithium anode of a solid state Li-ion battery at a location adjacent to the solid electrolyte during the stripping (discharge) phase of the battery; a similar phenomenon is observed in sodium-based batteries. It is hypothesised in the current literature that the formation of these voids is due to the coalescence of vacancies that have been generated at the electrode/electrolyte interface when metal atoms are oxidized and transported into the electrolyte: the slow diffusion of the vacancies away from the electrolyte interface into the adjacent electrode results in their coalescence and the consequent growth of voids. These hypotheses are challenged in the current study by using the Onsager formalism to generate a variational principle for vacancy diffusion. Our analysis reveals that no driving force exists for the diffusion of vacancies into a homogeneous metal electrode that thins by stripping. This finding is contrary to models in the literature which have mistakenly assumed that the vanishing flux at the current collector prevents rigid body motion (drift) of the electrode which in turn prevents thinning of the electrode during stripping. Based on our analysis, we conclude that vacancy diffusion within a homogeneous electrode is not responsible for the nucleation and growth of voids at the interface between a stripping metal electrode and a solid electrolyte.