INMdok (Leibniz Institute for New Materials)
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Solvation effects on aqueous ion adsorption and electrosorption in carbon micropores
Get PDFMicroporous carbonaceous electrode materials store charge by ion electrosorption onto the electrode surface. Despite significant efforts to understand this phenomenon, a definitive picture of the adsorption mechanisms within these complex nanoscale structures is lacking. Here, we use nuclear magnetic resonance (NMR) spectroscopy to directly observe and quantify aqueous adsorbate partitioning behavior driven by spontaneous physisorption within the micropores. Our results show that the solvation properties of the electrolyte ions influence the ionophilicity/ionophobicity of the adsorbate-carbon system, with ionophilic and ionophobic systems exhibiting distinct behavior concerning the electrolyte loading volume. Micropore diameter is also shown to influence spontaneous electrolyte partitioning behavior and disturb ion solvation. In situ NMR spectroscopy using a working supercapacitor comprising microporous carbon electrodes with aqueous sodium sulfate and aqueous sodium bis(trifluoromethane)sulfonimide electrolytes indicates that spontaneous electrolyte partitioning behavior influences the charge-balancing mechanism. Our results suggest that spontaneously ionophilic systems favor charge-balancing by counter-ion adsorption under an applied voltage, and spontaneously ionophobic systems favor a co-ion ejection mechanism under an applied potential. These results provide new molecular-level insight into the role of electrolyte properties on spontaneous physisorption behavior and charged electrosorption behavior within microporous carbon electrodes
PenTag, a Versatile Platform for Synthesizing Protein-Polymer Biohybrid Materials
Get PDFThe site-specific and covalent conjugation of proteins on solid supports and in hydrogels is the basis for the synthesis of biohybrid materials offering broad applications. Current methods for conjugating proteins to desired targets are often challenging due to unspecific binding, unstable (noncovalent) coupling, or expensive and difficult-to-synthesize ligand molecules. Here, is presented PenTag, an approach for the bioorthogonal, highly specific, and covalent conjugation of a protein to its ligand for various applications in materials sciences. Penicillin-binding protein 3 (PBP3) is engineered and shows that this protein can be used for the stable and spontaneous conjugation of proteins to dyes, polymers, or solid supports. PenTag as a crosslinking tool is applied for synthesizing stimuli-responsive hydrogels or for the development of a biohybrid material system performing computational operations emulating a 4:2 encoder. Based on this broad applicability and the use of a small, cheap, and easy-to-functionalize ligand and a stable, soluble recombinant protein, is seen PenTag as a versatile approach toward biohybrid material synthesis
Functional Integration of Synthetic Cells into 3D Microfluidic Devices for Artificial Organ-On-Chip Technologies
Get PDFMicrofluidics plays a pivotal role in organ-on-chip technologies and in the study of synthetic cells, especially in the development and analysis of artificial cell models. However, approaches that use synthetic cells as integral functional components for microfluidic systems to shape the microenvironment of natural living cells cultured on-chip are not explored. Here, colloidosome-based synthetic cells are integrated into 3D microfluidic devices, pioneering the concept of synthetic cell-based microenvironments for organs-on-chip. Methods are devised to create dense and stable networks of silica colloidosomes, enveloped by supported lipid bilayers, within microfluidic channels. These networks promote receptor-ligand interactions with on-chip cultured cells. Furthermore, a technique is introduced for the controlled release of growth factors from the synthetic cells into the channels, using a calcium alginate-based hydrogel formation within the colloidosomes. To demonstrate the potential of the technology, a modular plug-and-play lymph-node-on-a-chip prototype that guides the expansion of primary human T cells by stimulating receptor ligands on the T cells and modulating their cytokine environment is presented. This integration of synthetic cells into microfluidic systems offers a new direction for organ-on-chip technologies and suggests further avenues for exploration in potential therapeutic applications
OptoAssay—Light-controlled dynamic bioassay using optogenetic switches
Get PDFCircumventing 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
The impact of the tumor microenvironment on the survival of penile cancer patients
Get PDFPeCa is a rare entity with rising incidence rates due to increased infections with human papillomaviruses (HPV). The distinct subtypes of PeCa with an individual pathogenesis demand biomarkers for a precise patient risk assessment regarding disease progression and therapeutic susceptibility. We recently identified promising candidates associated with an HPV-instructed tumor microenvironment (TME) using HPV-positive PeCa cell lines and tissue microarrays (TMA). The capacity of HPV + p63 + PeCa cells to release neutrophil-attracting CXCL-8 provided a molecular link explaining the infiltration of CD15 + myeloid cells in PeCa specimens. The candidate biomarkers HPV, p63, CD15, DKK1, and CD147 linked a tumor-promoting TME with a higher TNM classification reflecting more aggressive and metastasizing cancers. Based on immune-reactive scores (IRS) from TMA staining for these biomarkers, we calculated correlations and conducted association analyses to assess the degree of relationship between all biomarkers. We then conducted Kaplan–Meier survival estimates and Cox regression analyses to delineate the impact on PeCa patient survival. There is a notable predictive potential regarding the survival of patients with biomarker profiles beyond the potency of the individual biomarker. From all candidate biomarkers and biomarker profiles, the combination of CD147 and infiltrating CD15 + cells linked to an active HPV-driven transformation displayed cancer-immune dynamics with dismal prognosis for patients. After deciphering relevant interdependencies, the HPV + CD147 + CD15 + status was the most potent profile predicting metastasis-free survival of PeCa patients. The results of this report underscore the need for analysis of the TME and the development of multi-parameter composite scores that reflect fundamental cancer-immune relationships to tailor therapeutic interventions based on actual cancer immune dynamics
Pyrophosphonate Covalent Organic Frameworks
Get PDFHerein, we report a new family of covalent organic frameworks (COFs), namely pyrophosphonate-COFs, constructed via pyrophosphonate linkages. Pyrophosphonate-COFs can be synthesized via a single-step condensation reaction of the charge-assisted hydrogen-bonded organic framework (HOF) GTUB5, which is constructed from phenylphosphonic acid and 5,10,15,20‐tetrakis[p‐phenylphosphonic acid] porphyrin. The reported pyrophosphonate-COF, which we call GTUB5-COF was synthesized by simply heating its two-linker HOF precursor GTUB5 without using chemical reagents. GTUB5-COF exhibits good water and water vapor stability during the gas sorption measurements. Furthermore, GTUB5-COF exhibits exceptional electrochemical stability in 0.5 M Na2SO4 electrolyte in water. The formation of pyrophosphonate bonds upon heating was confirmed by magic angle spinning nuclear magnetic resonance spectroscopy, Fourier-transform infrared spectroscopy, and mass spectrometry coupled with thermal analysis. The condensed product pyrophosphonate-COF can efficiently adsorb CO2. It has a more favorable heat of adsorption value for CO2 capture at lower pressures than water vapor, making it a suitable candidate for selective CO2 capture in the presence of water vapor. The absorption and emission of GTUB5-COF are governed by localized transitions (Soret and Q bands) within the porphyrin unit, which results in broad-banded fluorescence in the near-infrared range at around 800 nm
Electrochemical recycling of lithium-ion batteries: Advancements and future directions
Get PDFLithium-ion batteries (LIBs) are at the forefront of technological innovation in the current global energy-transition paradigm, driving surging demand for electric vehicles and renewable energy-storage solutions. Despite their widespread use and superior energy densities, the environmental footprint and resource scarcity associated with LIBs necessitate sustainable recycling strategies. This comprehensive review critically examines the existing landscape of battery recycling methodologies, including pyrometallurgical, hydrometallurgical, and direct recycling techniques, along with emerging approaches such as bioleaching and electrochemical separation. Our analysis not only underscores the environmental and efficiency challenges posed by conventional recycling methods but also highlights the promising potential of electrochemical techniques for enhancing selectivity, reducing energy consumption, and mitigating secondary waste production. By delving into recent advancements and juxtaposing various recycling methodologies, we pinpoint electrochemical recycling as a pivotal technology for efficiently recovering valuable metals, such as Li, Ni, Co, and Mn, from spent LIBs in an environmentally benign manner. Our discussion extends to the scalability, economic viability, and future directions of electrochemical recycling, and advocates for their integration into global battery-recycling infrastructure to address the dual challenges of resource depletion and environmental sustainability
Perceptual Constancy in the Speed Dependence of Friction During Active Tactile Exploration
Get PDFFingertip friction is a key component of tactile perception. In active tactile exploaration, friction forces depend on the applied normal force and on the sliding speed chosen. We have investigated wheter humans perceive the speed dependence of friction for textured surface of materials, which show either increase or decrease of the friction coefficient with speed. Participants perceived the decrease or increase when the relative difference in friction coefficient between fast and slow sliding speed was more than 20%. The friction of comparison judgments which were in agreement with the measured difference in friction coefficient did not depend on variations in the applied normal force. The results indicate a perceptual constancy for fingertip friction with respect to self-generated variations of sliding speed and applied normal force
From Theory to Therapy: The Advancements of Extracellular Vesicles in Immunotherapy
Get PDFExtracellular vesicles (EVs) are lipid-membrane-enclosed particles released from cells, playing a pivotal role in cellular communication, particularly within the immune system. The fundamental molecular mechanisms through which EVs offer unique functionality for immunotherapeutic benefits are identified and reviewed. The focus is on three essential features, all rooted in the EV lipid membrane: immune receptor–ligand interactions at the EV membrane interface, the shielding of immunogenic cargo within the EVs, and the fusion of EVs with target cell membranes for direct cargo delivery. From this, how these distinct EV attributes, from their initial description and analysis in immune communication, have led to the development of novel immunotherapeutic strategies is traced. This review delves into how these strategies are applied in various immunotherapies, such as cancer immunotherapy, autoimmune diseases, infections, vaccinations, and graft-versus-host diseases, to modulate communication among different cell types for immune regulation. It is concluded by reviewing clinical trials involving EVs in immunotherapy that have effectively harnessed EVs' unique molecular mechanisms in clinical settings. Research and standardization efforts to maximize the potential impact of EVs on immunotherapy are further suggested
Lighting the way: recent developments and applications in molecular optogenetics
Get PDFMolecular optogenetics utilizes genetically encoded, light-responsive protein switches to control the function of molecular processes. Over the last two years, there have been notable advances in the development of novel optogenetic switches, their utilization in elucidating intricate signaling pathways, and their progress toward practical applications in biotechnological processes, material sciences, and therapeutic applications. In this review, we discuss these areas, offer insights into recent developments, and contemplate future directions