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- ItemSelf-Regenerating Soft Biophotovoltaic Devices(Washington, DC : ACS Publications, 2018) Qiu, Xinkai; Castañeda Ocampo, Olga; de Vries, Hendrik W.; van Putten, Maikel; Loznik, Mark; Herrmann, Andreas; Chiechi, Ryan C.This paper describes the fabrication of soft, stretchable biophotovoltaic devices that generate photocurrent from photosystem I (PSI) complexes that are self-assembled onto Au electrodes with a preferred orientation. Charge is collected by the direct injection of electrons into the Au electrode and the transport of holes through a redox couple to liquid eutectic gallium-indium (EGaIn) electrodes that are confined to microfluidic pseudochannels by arrays of posts. The pseudochannels are defined in a single fabrication step that leverages the non-Newtonian rheology of EGaIn. This strategy is extended to the fabrication of reticulated electrodes that are inherently stretchable. A simple shadow evaporation technique is used to increase the surface area of the Au electrodes by a factor of approximately 106 compared to planar electrodes. The power conversion efficiency of the biophotovoltaic devices decreases over time, presumably as the PSI complexes denature and/or detach from the Au electrodes. However, by circulating a solution of active PSI complexes the devices self-regenerate by mass action/self-assembly. These devices leverage simple fabrication techniques to produce complex function and prove that photovoltaic devices comprising PSI can retain the ability to regenerate, one of the most important functions of photosynthetic organisms. © 2018 American Chemical Society.
- ItemIn-Gel Direct Laser Writing for 3D-Designed Hydrogel Composites That Undergo Complex Self-Shaping(Weinheim : Wiley-VCH, 2017) Nishiguchi, Akihiro; Mourran, Ahmed; Zhang, Hang; Möller, MartinSelf-shaping and actuating materials inspired by biological system have enormous potential for biosensor, microrobotics, and optics. However, the control of 3D-complex microactuation is still challenging due to the difficulty in design of nonuniform internal stress of micro/nanostructures. Here, we develop in-gel direct laser writing (in-gel DLW) procedure offering a high resolution inscription whereby the two materials, resin and hydrogel, are interpenetrated on a scale smaller than the wavelength of the light. The 3D position and mechanical properties of the inscribed structures could be tailored to a resolution better than 100 nm over a wide density range. These provide an unparalleled means of inscribing a freely suspended microstructures of a second material like a skeleton into the hydrogel body and also to direct isotropic volume changes to bending and distortion motions. In the combination with a thermosensitive hydrogel rather small temperature variations could actuate large amplitude motions. This generates complex modes of motion through the rational engineering of the stresses present in the multicomponent material. More sophisticated folding design would realize a multiple, programmable actuation of soft materials. This method inspired by biological system may offer the possibility for functional soft materials capable of biomimetic actuation and photonic crystal application.
- ItemDNA Nanotechnology Enters Cell Membranes(Weinheim : Wiley-VCH, 2019) Huo, Shuaidong; Li, Hongyan; Boersma, Arnold J.; Herrmann, AndreasDNA is more than a carrier of genetic information: It is a highly versatile structural motif for the assembly of nanostructures, giving rise to a wide range of functionalities. In this regard, the structure programmability is the main advantage of DNA over peptides, proteins, and small molecules. DNA amphiphiles, in which DNA is covalently bound to synthetic hydrophobic moieties, allow interactions of DNA nanostructures with artificial lipid bilayers and cell membranes. These structures have seen rapid growth with great potential for medical applications. In this Review, the current state of the art of the synthesis of DNA amphiphiles and their assembly into nanostructures are first summarized. Next, an overview on the interaction of these DNA amphiphiles with membranes is provided, detailing on the driving forces and the stability of the interaction. Moreover, the interaction with cell surfaces in respect to therapeutics, biological sensing, and cell membrane engineering is highlighted. Finally, the challenges and an outlook on this promising class of DNA hybrid materials are discussed.
- ItemPorous PEDOT:PSS Particles and their Application as Tunable Cell Culture Substrate(Weinheim : Wiley, 2021) Rauer, Sebastian Bernhard; Bell, Daniel Josef; Jain, Puja; Rahimi, Khosrow; Felder, Daniel; Linkhorst, John; Wessling, MatthiasDue to its biocompatibility, electrical conductivity, and tissue-like elasticity, poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) constitutes a highly promising material regarding the fabrication of smart cell culture substrates. However, until now, high-throughput synthesis of pure PEDOT:PSS geometries was restricted to flat sheets and fibers. In this publication, the first microfluidic process for the synthesis of spherical, highly porous, pure PEDOT:PSS particles of adjustable material properties is presented. The particles are synthesized by the generation of PEDOT:PSS emulsion droplets within a 1-octanol continuous phase and their subsequent coagulation and partial crystallization in an isopropanol (IPA)/sulfuric acid (SA) bath. The process allows to tailor central particle characteristics such as crystallinity, particle diameter, pore size as well as electrochemical and mechanical properties by simply adjusting the IPA:SA ratio during droplet coagulation. To demonstrate the applicability of PEDOT:PSS particles as potential cell culture substrate, cultivations of L929 mouse fibroblast cells and MRC-5 human fibroblast cells are conducted. Both cell lines present exponential growth on PEDOT:PSS particles and reach confluency with cell viabilities above 95 vol.% on culture day 9. Single cell analysis could moreover reveal that mechanotransduction and cell infiltration can be controlled by the adjustment of particle crystallinity.
- ItemWet-Spinning of Biocompatible Core–Shell Polyelectrolyte Complex Fibers for Tissue Engineering(Weinheim : Wiley-VCH, 2020) Cui, Qing; Bell, Daniel Josef; Rauer, Sebastian Bernhard; Wessling, MatthiasPolyelectrolyte complex fibers (PEC fibers) have great potential with regard to biomedical applications as they can be fabricated from biocompatible and water-soluble polyelectrolytes under mild process conditions. The present publication describes a novel method for the continuous fabrication of PEC fibers in a water-based wet-spinning process by interfacial complexation within a core–shell spinneret. This process combines the robustness and flexibility of nonsolvent-induced phase separation (NIPS) spinning processes conventionally used in the membrane industry with the complexation between oppositely charged polyelectrolytes. The produced fibers demonstrate a core–shell structure with a low-density core and a highly porous polyelectrolyte complex shell of ≈800 μm diameter. In the case of chitosan and polystyrene sulfonate (PSS), mechanical fiber properties could be enhanced by doping the PSS with poly(ethylene oxide) (PEO). The resulting CHI/PSS-PEO fibers present a Young modulus of 3.78 GPa and a tensile strength of 165 MPa, which is an excellent combination of elongation at break and break stress compared to literature. The suitability of the CHI/PSS-PEO fibers as a scaffold for cell culture applications is verified by a four-day cultivation of human HeLa cells on PEO-reinforced fibers with a subsequent analysis of cell viability by fluorescence-based live/dead assay. © 2020 The Authors. Published by Wiley-VCH GmbH
- ItemMitigating Water Crossover by Crosslinked Coating of Cation‐Exchange Membranes for Brine Concentration(Weinheim : Wiley, 2021) Rommerskirchen, Alexandra; Roth, Hannah; Linnartz, Christian J.; Egidi, Franziska; Kneppeck, Christian; Roghmans, Florian; Wessling, MatthiasUndesired water crossover through ion-exchange membranes is a significant limitation in electrically driven desalination processes. The effect of mitigating water crossover is twofold: 1) The desalination degree is less reduced due to the unwanted removal of water, and 2) the brine concentration is increased due to decreased dilution by an unwanted crossover of water molecules. Hence, water crossover limits the desalination and concentration efficiency of the processes, while the energy demand to achieve a certain level of desalination or concentration increases. This effect is especially pronounced when treating high salinity solutions, which goes hand in hand with the crossover of many ions through the ion-exchange membranes. A crosslinked coating for cation-exchange membranes (CEMs) is presented in this work, which can significantly mitigate such undesired water crossover. The efficacy is demonstrated using the flow-electrode capacitive deionization process applied for desalination and concentration of saline brines at feed concentrations of 60 and 120 g L−1 NaCl. With just a single coated CEM, the water crossover was reduced by up to 54%.
- ItemTurning a Killing Mechanism into an Adhesion and Antifouling Advantage(Weinheim : Wiley-VCH, 2019) Dedisch, Sarah; Obstals, Fabian; los Santos Pereira, Andres; Bruns, Michael; Jakob, Felix; Schwaneberg, Ulrich; Rodriguez‐Emmenegger, CesarMild and universal methods to introduce functionality in polymeric surfaces remain a challenge. Herein, a bacterial killing mechanism based on amphiphilic antimicrobial peptides is turned into an adhesion advantage. Surface activity (surfactant) of the antimicrobial liquid chromatography peak I (LCI) peptide is exploited to achieve irreversible binding of a protein–polymer hybrid to surfaces via physical interactions. The protein–polymer hybrid consists of two blocks, a surface-affine block (LCI) and a functional block to prevent protein fouling on surfaces by grafting antifouling polymers via single electron transfer-living radical polymerization (SET-LRP). The mild conditions of SET-LRP of N-2-hydroxy propyl methacrylamide (HPMA) and carboxybetaine methacrylamide (CBMAA) preserve the secondary structure of the fusion protein. Adsorption kinetics and grafting densities are assessed using surface plasmon resonance and ellipsometry on model gold surfaces, while the functionalization of a range of artificial and natural surfaces, including teeth, is directly observed by confocal microscopy. Notably, the fusion protein modified with poly(HPMA) completely prevents the fouling from human blood plasma and thereby exhibits a resistance to protein fouling that is comparable to the best grafted-from polymer brushes. This, combined with their simple application on a large variety of materials, highlights the universal and scalable character of the antifouling concept. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemBiomineralization of Engineered Spider Silk Protein-Based Composite Materials for Bone Tissue Engineering(Basel : MDPI, 2016) Hardy, John G.; Torres-Rendon, Jose Guillermo; Leal-Egaña, Aldo; Walther, Andreas; Schlaad, Helmut; Cölfen, Helmut; Scheibel, ThomasMaterials based on biodegradable polyesters, such as poly(butylene terephthalate) (PBT) or poly(butylene terephthalate-co-poly(alkylene glycol) terephthalate) (PBTAT), have potential application as pro-regenerative scaffolds for bone tissue engineering. Herein, the preparation of films composed of PBT or PBTAT and an engineered spider silk protein, (eADF4(C16)), that displays multiple carboxylic acid moieties capable of binding calcium ions and facilitating their biomineralization with calcium carbonate or calcium phosphate is reported. Human mesenchymal stem cells cultured on films mineralized with calcium phosphate show enhanced levels of alkaline phosphatase activity suggesting that such composites have potential use for bone tissue engineering.
- ItemA physicochemical perspective of aging from single-cell analysis of ph, macromolecular and organellar crowding in yeast(Cambridge : eLife Sciences Publications, 2020) Mouton, Sara N.; Thaller, David J.; Crane, Matthew M.; Rempel, Irina L.; Terpstra, Owen T.; Steen, Anton; Kaeberlein, Matt; Lusk, C. Patrick; Boersma, Arnold J.; Veenhoff, Liesbeth M.Cellular aging is a multifactorial process that is characterized by a decline in homeostatic capacity, best described at the molecular level. Physicochemical properties such as pH and macromolecular crowding are essential to all molecular processes in cells and require maintenance. Whether a drift in physicochemical properties contributes to the overall decline of homeostasis in aging is not known. Here we show that the cytosol of yeast cells acidifies modestly in early aging and sharply after senescence. Using a macromolecular crowding sensor optimized for long-term FRET measurements, we show that crowding is rather stable and that the stability of crowding is a stronger predictor for lifespan than the absolute crowding levels. Additionally, in aged cells we observe drastic changes in organellar volume, leading to crowding on the µm scale, which we term organellar crowding. Our measurements provide an initial framework of physicochemical parameters of replicatively aged yeast cells. © 2020, eLife Sciences Publications Ltd. All rights reserved.
- ItemModulating the luminance of organic light-emitting diodes: Via optical stimulation of a photochromic molecular monolayer at transparent oxide electrode(Cambridge : RSC Publ., 2020) Ligorio, Giovanni; Cotella, Giovanni F.; Bonasera, Aurelio; Zorn Morales, Nicolas; Carnicella, Giuseppe; Kobin, Björn; Wang, Qiankun; Koch, Norbert; Hecht, Stefan; List-Kratochvil, Emil J.W.; Cacialli, FrancoSelf-assembled monolayers (SAMs) deposited on bottom electrodes are commonly used to tune charge carrier injection or blocking in optoelectronic devices. Beside the enhancement of device performance, the fabrication of multifunctional devices in which the output can be modulated by multiple external stimuli remains a challenging target. In this work, we report the functionalization of an indium tin oxide (ITO) electrode with a SAM of a diarylethene derivative designed for optically control the electronic properties. Following the demonstration of dense SAM formation and its photochromic activity, as a proof-of-principle, an organic light-emitting diode (OLED) embedding the light-responsive SAM-covered electrode was fabricated and characterized. Optically addressing the two-terminal device by irradiation with ultraviolet light doubles the electroluminescence. The original value can be restored reversibly by irradiation with visible light. This expanded functionality is based on the photoinduced modulation of the electronic structure of the diarylethene isomers, which impact the charge carriers' confinement within the emissive layer. This approach could be successfully exploited in the field of opto-communication technology, for example to fabricate opto-electronic logic circuits. © 2020 The Royal Society of Chemistry.