Publikationen

2024
OptoAssay—Light-controlled dynamic bioassay using optogenetic switches

Urban, Nadine | Hörner, Maximilian | Weber, Wilfried | Dincer, Can

DOI:

Circumventing the limitations of current bioassays, we introduce a light-controlled assay, OptoAssay, toward wash- and pump-free point-of-care diagnostics. Extending the capabilities of standard bioassays with light-dependent and reversible interaction of optogenetic switches, OptoAssays enable a bidirectional movement of assay components, only by changing the wavelength of light. Demonstrating exceptional versatility, the OptoAssay showcases its efficacy on various substrates, delivering a dynamic bioassay format. The applicability of the OptoAssay is successfully demonstrated by the calibration of a competitive model assay, resulting in a superior limit of detection of 8 pg ml−1, which is beyond those of conventional ELISA tests. In the future, combined with smartphones, OptoAssays could obviate the need for external flow control systems such as pumps or valves and signal readout devices, enabling on-site analysis in resource-limited settings.

DOI:

Science Advances ,
2024, 10 (39), eadp0911.

OPEN ACCESS
Quantum Sensing Unravels Antioxidant Efficacy Within PCL/Matrigel Skin Equivalents

Wu, Xixi | Koch, Marcus | Perona Martínez, Felipe P. | Schirhagl, Romana | Wlodarczyk-Biegun, Malgorzata K.

DOI:

Skin equivalents (SE) that recapitulate biological and mechanical characteristics of the native tissue are promising platforms for assessing cosmetics and studying fundamental biological processes. Methods to achieve SEs with well-organized structure, and ideal biological and mechanical properties are limited. Here, the combination of melt electrowritten PCL scaffolds and cell-laden Matrigel to fabricate SE is described. The PCL scaffold provides ideal structural and mechanical properties, preventing deformation of the model. The model consists of a top layer for seeding keratinocytes to mimic the epidermis, and a bottom layer of Matrigel-based dermal compartment with fibroblasts. The compressive modulus and the biological properties after 3-day coculture indicate a close resemblance with the native skin. Using the SE, a testing system to study the damage caused by UVA irradiation and evaluate antioxidant efficacy is established. The effectiveness of Tea polyphenols (TPs) and L-ascorbic acid (Laa) is compared based on free radical generation. TPs are demonstrated to be more effective in downregulating free radical generation. Further, T1 relaxometry is used to detect the generation of free radicals at a single-cell level, which allows tracking of the same cell before and after UVA treatment.

DOI:

Small ,
2024, 20 (49), 2403729.

OPEN ACCESS
Engineered bacterial therapeutics with material solutions

Dey, Sourik | Sankaran, Shrikrishnan

DOI:

Recent advances in engineered bacterial therapeutics underscore their potential in treating diseases via targeted, live interventions. Despite their promising performance in early clinical phases, no engineered therapeutic bacteria have yet received approval, primarily due to challenges in proving efficacy while ensuring biosafety. Material science innovations, particularly the encapsulation of bacteria within hydrogels, present a promising avenue to enhance bacterial survival, efficacy, and safety in therapeutic applications. This review discusses this interdisciplinary approach to develop living therapeutic materials. Hydrogels not only safeguard the bacteria from harsh physiological conditions but also enable controlled therapeutic release and prevent unintended bacterial dissemination. The strategic use of encapsulation materials could redefine the delivery and functionality of engineered bacterial therapeutics, facilitating their clinical translation.

DOI:

Trends in Biotechnology ,
2024, 42 (12), 1663-1676.

OPEN ACCESS
Cation selectivity during flow electrode capacitive deionization

Ren, Panyu | Wang, Bin | De Andrade Ruthes, Jean G. | Torkamanzadeh, Mohammad | Presser, Volker

DOI:

Efficient separation of specific ions from aqueous media is crucial for advanced water treatment and resource recovery. Flow electrode capacitive deionization (FCDI) offers potential for selective ion removal through continuous operation. This study evaluates the performance of selective cation separation using a commercial activated carbon slurry in a multi-ion solution of monovalent (Li+, Na+, K+) and bivalent (Ca2+, Mg2+) cations. We assess ion removal and cation selectivity under different operational parameters, such as applied potential, slurry flow rate, and feed water flow rate. Our data show that bivalent cations, namely Ca2+ and Mg2+, are preferentially removal due to their higher charge-to-size ratio, aligning with hydrated ion sizes. The highest separation rate was observed for Ca2+ (5.7 μg cm−2 min−1), and the lowest for Li+ (0.2 μg cm−2 min−1). At the highest applied voltage (1.2 V), charge efficiencies reached 70 %, with an energy consumption of 41 Wh mol−1 for nearly complete cation removal. Optimal conditions were identified with a slurry flow rate of 6 mL min−1, feed water flow rate of 2 mL min−1, activated carbon content of 10 mass%, 1 mass% carbon black, and a cell voltage of 1.2 V. These findings highlight the importance of optimizing operational parameters to enhance ion removal.

DOI:

Desalination ,
2024, 592 118161.

OPEN ACCESS
Selenium Disulfide from Sustainable Resources: an Example of „Redneck“ Chemistry with a Pinch of Salt

Tiganescu, Eduard | Safinazlou, Shahrzad | Abdin, Ahmad Yaman | Lilischkis, Rainer | Schäfer, Karl-Herbert | Fink-Straube, Claudia | Nasim, Muhammad Jawad | Jacob, Claus

DOI:

DOI:

Materials ,
2024, 17 (23), 5733.

OPEN ACCESS
Nahezu unendlich lange Polymere mit Ge=Ge-Doppelbindungen

Thömmes, Anna-Lena | Büttner, Thomas | Morgenstern, Bernd | Janka, Oliver | Kickelbick, Guido | Niebuur, Bart-jan | Kraus, Tobias | Gallei, Markus | Scheschkewitz, David

DOI:

Trotz erheblichen Interesses an heteroatomhaltigen konjugierten Polymeren sind Beispiele mit schwereren Elementen des p-Blocks im Konjugationspfad rar. Die kürzlich beschriebene Metathese schwererer acyclischer Diene (HADMET) ermöglichte die Synthese eines Ge=Ge-Doppelbindungen enthaltenden Polymers, wenn auch eines unlöslichen mit begrenztem Polymerisationsgrad. Durch Einführung langer Alkylketten erhielten wir nun lösliche Vertreter mit – nach diffusionsabhängiger NMR-Spektroskopie (DOSY) und dynamischer Lichtstreuung (DLS) – nahezu unendlichen Polymerisationsgraden. UV/Vis und NMR-Daten bestätigen das Vorliegen von σ,π-Konjugation entlang der Silylen-Phenylen-Verknüpfungen zwischen den Ge=Ge-Einheiten. Günstige intermolekulare Dispersionswechselwirkungen führen zu leiterartigen, zylindrischen Aggregaten, wie durch Röntgendiffraktometrie (XRD), Kleinwinkel-Röntgenstreuung (SAXS) und DLS bestätigt. AFM- und TEM-Bilder abgeschiedener dünner Schichten offenbaren eine lamellare Anordnung ausgedehnter Polymerbündel.

DOI:

Angewandte Chemie ,
2024, 136 (51), e202415103.

OPEN ACCESS
Near-Infinite-Chain Polymers with Ge=Ge Double Bonds

Thömmes, Anna-Lena | Büttner, Thomas | Morgenstern, Bernd | Janka, Oliver | Kickelbick, Guido | Niebuur, Bart-Jan | Kraus, Tobias | Gallei, Markus | Scheschkewitz, David

DOI:

Despite considerable interest in heteroatom-containing conjugated polymers, there are only few examples with heavier p-block elements in the conjugation path. The recently reported heavier acyclic diene metathesis (HADMET) allowed for the synthesis of a polymer containing Ge=Ge double bonds—albeit insoluble and with limited degree of polymerization. By incorporation of long alkyl chains, we now obtained soluble representatives, which exhibit degrees of polymerization near infinity according to diffusion-ordered NMR spectroscopy (DOSY) and dynamic light scattering (DLS). UV/Vis and NMR data confirm the presence of σ,π-conjugation across the silylene-phenylene linkers between the Ge=Ge double bonds. Favorable intermolecular dispersion interactions lead to ladder-like cylindrical assemblies as confirmed by X-ray diffraction (XRD), small angle X-ray scattering (SAXS) and DLS. AFM and TEM images of deposited thin films reveal lamellar ordering of extended polymer bundles.

DOI:

Angewandte Chemie International Edition ,
2024, 63 (51), e202415103.

OPEN ACCESS
Life After Death: Re-Purposing End-of-Life Supercapacitors for Electrochemical Water Desalination

Ren, Panyu | Torkamanzadeh, Mohammad | Arnold, Stefanie | Pameté, Emmanuel | Presser, Volker

DOI:

This study explores the potential of re-purposing end-of-life commercial supercapacitors as electrochemical desalination cells, aligning with circular economy principles. A commercial 500-Farad supercapacitor was disassembled, and its carbon electrodes underwent various degrees of modification. The most straightforward modification involved NaOH-etching of the aluminum current collector to produce free-standing carbon films. More advanced modifications included CO2 activation and binder-added wet processing of the electrodes. When evaluated as electrodes for electrochemical desalination via capacitive deionization of low-salinity (20 mM) NaCl solutions, the minimally modified NaOH-etched carbon electrodes achieved an average desalination capacity of 5.8 mg g−1 and a charge efficiency of 80 %. In contrast, the CO2-activated, wet-processed electrodes demonstrated an improved desalination capacity of 7.9 mg g−1 and a charge efficiency above 90 % with stable performance over 20 cycles. These findings highlight the feasibility and effectiveness of recycling supercapacitors for sustainable water desalination applications, offering a promising avenue for resource recovery and re-purposing in pursuing environmental sustainability.

DOI:

Batteries & Supercaps ,
2024, 7 (12), e202400506.

OPEN ACCESS
Harnessing enhanced lithium-ion storage in self-assembled organic nanowires for batteries and metal-ion supercapacitors

Obraztsov, Ievgen | Langer, Rostislav | De Andrade Ruthes, Jean G. | Presser, Volker | Otyepka, Michal | Zboril, Radek | Bakandritsos, Aristides

DOI:

Organic materials have emerged as highly efficient electrodes for electrochemical energy storage, offering sustainable solutions independent from non-renewable resources. In this study, we showcase that mesoscale engineering can dramatically transform the electrochemical features of a molecular organic carboxylic anode. Through a sustainable, energy-efficient and environmentally benign self-assembly strategy, we developed a network of organic nanowires formed during water evaporation directly on the copper current collector, circumventing the need for harmful solvents, typically employed in such processes. The organic nanowire anode delivers high capacity and rate, reaching 1888 mA h g−1 at 0.1 A g−1 and maintaining 508 mA h g−1 at a specific current of 10 A g−1. Moreover, it exhibits superior thermal management during lithiation in comparison to graphite and other organic anodes. Comprehensive electrochemical evaluations and theoretical calculations reveal rapid charge transport mechanisms, with lithium diffusivity rates reaching 5 × 10−9 cm2 s−1, facilitating efficient and rapid interactions with 24 lithium atoms per molecule. Integrated as the negative electrode in a lithium-ion capacitor, paired with a commercially available porous carbon, the cell delivers a specific energy of 156 W h kg−1 at a specific power of 0.34 kW kg−1 and 60.2 W h kg−1 at 19.4 kW kg−1, establishing a benchmark among state-of-the-art systems in the field. These results underscore the critical role of supramolecular organization for optimizing the performance of organic electrode materials for practical and sustainable energy storage technologies.

DOI:

Energy & Environmental Science ,
2024, 17 8874-8884.

OPEN ACCESS
Polyacrylamide Hydrogels as Versatile Biomimetic Platforms to Study Cell-Materials Interactions

Milos, Frano | Del Campo, Aránzazu

DOI:

Polyacrylamide (PAAm) hydrogels are widely adopted as 2D-model soft substrates for investigating cell-material interactions in a controlled in vitro environment. They offer facile synthesis, tunable physico-chemical properties, diverse biofunctionalization routes, optical transparency, mouldability in a range of geometries and shapes, and compatibility with living cells. PAAm hydrogels can be engineered to reconstruct physiologically relevant biointerfaces, like cell-matrix or cell–cell interfaces, featuring biochemical, mechanical, and topographical cues present in the extracellular environment. This Review provides a materials science perspective on PAAm material properties, fabrication, and modification strategies relevant to cell studies, highlighting their versatility and potential to address a wide range of biological questions. Current routes are presented to integrate cell-instructive features, such as 2D patterns, 2.5D surface topographies, or mechanical stiffness gradients. Finally, the recent advances are emphasized toward dynamic PAAm hydrogels with on-demand control over hydrogel properties as well as electrically conductive PAAm hydrogels for bioelectronics.

DOI:

Advanced Materials Interfaces ,
2024, 11 (34), 2400404.

OPEN ACCESS