The ion insertion properties of MoS2 continue to be of widespread interest for energy storage. While much of the current work on MoS2 has been focused on the high capacity four‐electron reduction reaction, this process is prone to poor reversibility. Traditional ion intercalation reactions are highlighted and it is demonstrated that ordered mesoporous thin films of MoS2 can be utilized as a pseudocapacitive energy storage material with a specific capacity of 173 mAh g−1 for Li‐ions and 118 mAh g−1 for Na‐ions at 1 mV s−1. Utilizing synchrotron grazing incidence X‐ray diffraction techniques, fast electrochemical kinetics are correlated with the ordered porous structure and with an iso‐oriented crystal structure. When Li‐ions are utilized, the material can be charged and discharged in 20 seconds while still achieving a specific capacity of 140 mAh g−1. Moreover, the nanoscale architecture of mesoporous MoS2 retains this level of lithium capacity for 10 000 cycles. A detailed electrochemical kinetic analysis indicates that energy storage for both ions in MoS2 is due to a pseudocapacitive mechanism.
A major challenge in the field of water electrolysis is the scarcity of oxygen-evolving catalysts that are inexpensive, highly corrosion-resistant, suitable for large-scale applications and able to oxidize water at high current densities and low overpotentials. Most unsupported, non-precious metals oxygen-evolution catalysts require at least ~350 mV overpotential to oxidize water with a current density of 10 mA/cm2 in 1 M alkaline solution. Here we report on a robust nanostructured porous NiFe-based oxygen evolution catalyst made by selective alloy corrosion. In 1 M KOH, our material exhibits a catalytic activity towards water oxidation of 500 mA/cm2 at 360 mV overpotential and is stable for over eleven days. This exceptional performance is attributed to three factors. First, the small size of the ligaments and pores in our mesoporous catalyst (~10 nm) results in a high BET surface area (43 m2/g) and therefore a high density of oxygen-evolution catalytic sites per unit mass. Second, the open porosity facilitates effective mass transfer at the catalyst/electrolyte interface. Third and finally, the high bulk electrical conductivity of the mesoporous catalyst allows for effective current flow through the electrocatalyst, making it possible to use thick films with a high density of active sites and ~3×104 cm2 of catalytic area per cm2 of electrode area. Our mesoporous catalyst is thus attractive for alkaline electrolyzers where water-based solutions are decomposed into hydrogen and oxygen as the only products, driven either conventionally or by photovoltaics.
Tau protein was scanned for highly amyloidogenic sequences in amphiphilic motifs (X)nZ, Z(X)nZ (n≥2) or (XZ)n (n≥2), where X is a hydrophobic residue and Z is a charged or polar residue. N-acetyl peptides homologous to these sequences were used to study aggregation. Transmission electron microscopy (TEM) showed 7 peptides, in addition to well known primary nucleating sequences c275VQIINK (AcPHF6*) and Ac306VQIVYK (AcPHF6), formed fibers, tubes, ribbons or rolled sheets. Of the peptides shown by TEM to form amyloid, Ac10VME, AcPHF6*, Ac375KLTFR, and Ac393VYK were found to enhance the fraction of β-structure of AcPHF6 formed at equilibrium, and Ac375KLTFR was found to inhibit AcPHF6 and AcPHF6* aggregation kinetics in a dose-dependent manner, consistent with its participation in a hybrid steric zipper model. Single site mutants were generated which transformed predicted amyloidogenic sequences in tau into non-amyloidogenic ones. A M11K mutant had fewer filaments and showed a decrease in aggregation kinetics and an increased lag time compared to wild type tau, while a F378K mutant showed significantly more filaments. Our results infer that sequences throughout tau, in addition to PHF6 and PHF6*, can seed amyloid formation or affect aggregation kinetics or thermodynamics.
This work aims to improve the poor cycle lifetime of silicon-based anodes for Li-ion batteries by tuning microstructural parameters such as pore size, pore volume, and specific surface area in chemically synthesized mesoporous silicon. Here we have specifically produced two different mesoporous silicon samples from the magnesiothermic reduction of ordered mesoporous silica in either argon or forming gas. In situ X-ray diffraction studies indicate that samples made in Ar proceed through a MgSi intermediate, and this results in samples with larger pores (diameter ≈ 90 nm), modest total porosity (34%), and modest specific surface area (50 m g). Reduction in forming gas, by contrast, results in direct conversion of silica to silicon, and this produces samples with smaller pores (diameter ≈ 40 nm), higher porosity (41%), and a larger specific surface area (70 m g). The material with smaller pores outperforms the one with larger pores, delivering a capacity of 1121 mAh g at 10 A g and retains 1292 mAh g at 5 A g after 500 cycles. For comparison, the sample with larger pores delivers a capacity of 731 mAh g at 10 A g and retains 845 mAh g at 5 A g after 500 cycles. The dependence of capacity retention and charge storage kinetics on the nanoscale architecture clearly suggests that these microstructural parameters significantly impact the performance of mesoporous alloy type anodes. Our work is therefore expected to contribute to the design and synthesis of optimal mesoporous architectures for advanced Li-ion battery anodes.
Polyaniline is known for reversible acidic doping. However, despite extensive work, little experimental evidence exists for the initial doping mechanism mainly due to the difficulty of synthesizing polyaniline with a uniform chain length. In this study, we partially dope aniline tetramers in order to investigate the initial stage of doping in both solution and the solid state. In solution, we discovered a method for visualizing the doping level due to solvent density differences. The optical results in both the liquid and solid state suggest that the partially doped aniline tetramers are physical mixtures of aniline tetramer in the emeraldine base and emeraldine salt forms. Electron paramagnetic resonance confirms the formation of spinless bipolarons as the major carriers. Therefore, we postulate that the doping mechanism proceeds via a continual increase in the number of doubly doped tetraanilines.
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