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Wrenn posted an update 9 months, 1 week ago
Comprehensive understanding of the catalyst corrosion dynamics is a prerequisite for the development of an efficient cathode catalyst in proton-exchange membrane fuel cells. To reach this aim, the behavior of fuel cell catalysts must be investigated directly under reaction conditions. CPI-613 Dehydrogenase inhibitor Herein, we applied a strategic combination of in situ/online techniques in situ electrochemical atomic force microscopy, in situ grazing incidence small angle X-ray scattering, and electrochemical scanning flow cell with online detection by inductively coupled plasma mass spectrometry. This combination of techniques allows in-depth investigation of the potential-dependent surface restructuring of a PtNi model thin film catalyst during potentiodynamic cycling in an aqueous acidic electrolyte. The study reveals a clear correlation between the upper potential limit and structural behavior of the PtNi catalyst, namely, its dealloying and coarsening. The results show that at 0.6 and 1.0 VRHE upper potentials, the PtNi catalyst essentially preserves its structure during the entire cycling procedure. The crucial changes in the morphology of PtNi layers are found to occur at 1.3 and 1.5 VRHE cycling potentials. Strong dealloying at the early stage of cycling is substituted with strong coarsening of catalyst particles at the later stage. The coarsening at the later stage of cycling is assigned to the electrochemical Ostwald ripening process.The use of living microorganisms integrated within electrochemical devices is an expanding field of research, with applications in microbial fuel cells, microbial biosensors or bioreactors. We describe the use of porous nanocomposite materials prepared by DNA polymerization of carbon nanotubes (CNTs) and silica nanoparticles (SiNPs) for the construction of a programmable biohybrid system containing the exoelectrogenic bacterium Shewanella oneidensis. We initially demonstrate the electrical conductivity of the CNT-containing DNA composite by employment of chronopotentiometry, electrochemical impedance spectroscopy, and cyclic voltammetry. Cultivation of Shewanella oneidensis in the conductive materials shows that the exoelectrogenic bacteria populate the matrix of the conductive composite, while nonexoelectrogenic Escherichia coli remain on its surface. Moreover, the ability to use extracellular electron transfer pathways is positively correlated with the number of cells within the conductive synthetic biofilm matrix. The Shewanella-containing composite remains stable for several days and shows electrochemical activity, indicating that the conductive backbone is capable of extracting the metabolic electrons produced by the bacteria under strictly anoxic conditions and conducting them to the anode. Programmability of this biohybrid material system is demonstrated by on-demand release and degradation induced by a short-term enzymatic stimulus. We believe that the application possibilities of such biohybrid materials could even go beyond microbial biosensors, bioreactors, and fuel cell systems.Lasso peptides are a class of ribosomally synthesized and post-translationally modified peptides (RiPPs) that feature a unique lariat-knot topology. Canucin A, a post-translationally hydroxylated lasso peptide, was recently discovered via activation of its otherwise silent biosynthetic gene cluster in Streptomyces canus. The biosynthesis of canucin A, notably the introduction of a hydroxyl group at the β-carbon of the terminal aspartate residue, is the topic of the current report. We combine genetic and biochemical experiments to show that an iron/2-oxoglutarate-dependent enzyme, CanE, installs the hydroxyl group onto the precursor peptide in vivo and in vitro. Moreover, we show that hydroxylation occurs prior to macrocyclization and that the RiPP recognition element (RRE), encoded within the gene cluster to facilitate the initial proteolytic reaction, also increases the yield of hydroxylation, hinting at a dual role for the RRE. Our results have implications for the combinatorial biosynthesis of lasso peptides.Inspired by mucus, which provides an ideal supramolecular model and whose fluid-like (viscous) and solid-like (elastic) behaviors can be adjusted to meet different physiological requirements, we report oil-regulated supramolecular adhesives by the co-assembly of polyurea oligomers and carvacrol oils. The adhesive is crosslinked by weak but abundant hydrogen bonds, which can be regulated by the incorporated carvacrol oils through the competition of intermolecular hydrogen bonds, presenting a unique set of mucus-mimicking features including oil-regulated mechanics, processability, reusable adhesivity, and extreme longevity in both air and water. Owing to the intrinsic bactericidal effect of the carvacrol oils, the developed adhesives can serve as potent antibacterial coatings with both rapid contact killing (99.9% killing within 15 min) and long-term controlled release abilities (up to 70 days), enabling versatile antibacterial applications in diverse conditions. We envision that these adhesives will be useful in buildings and architectures, community and public facilities, food storage and packaging technologies, functional textiles, and practical biomedical fields.The morphology, crystal size, and trap density of perovskite films significantly affect the luminescent properties of perovskite light-emitting diodes (PeLEDs). Recently, numerous studies have been conducted on ligands that surround the surface of perovskite crystals and passivate the trap sites to improve the performance of PeLEDs. In this study, a 4-aminobenzonitrile (ABN) ligand improved the performance of methylammonium lead bromide (MAPbBr3)-based PeLEDs by reducing the MAPbBr3 crystal size to the nanoscale and reducing the trap density. Moreover, the properties of PeLEDs with ABN were further improved using a surface-modified hole-transport layer (HTL) with a hydrophilic polymer. Finally, a bright green PeLED was fabricated, which exhibited the maximum luminance of 3350 cd/m2 with an external quantum efficiency of 8.85%. Therefore, it is believed that the use of proper ligands for the perovskite layer and the optimization of the charge-transport layer have great potential for the development of high-performance PeLEDs.