Hendriksenthybo1197

The breaking of multiple symmetries by periodic lattice distortion at a commensurate charge density wave (CDW) state is expected to give rise to intriguing interesting properties. However, accessing the commensurate CDW state on bulk TaS2 crystals typically requires cryogenic temperatures (77 K), which precludes practical applications. Here, we found that heteroepitaxial growth of a 2H-tantalum disulfide bilayer on a hexagonal-boron nitride (h-BN) substrate produces a robust commensurate CDW order at room temperature, characterized by a Moiré superlattice of 3 × 3 TaS2 on a 4 × 4 h-BN unit cell. The CDW order is confirmed by scanning transmission electron microscopy and Raman measurements. Theoretical calculations reveal that the stabilizing energy for the CDW phase of the monolayer and bilayer 2H-TaS2-on-h-BN substrates arises primarily from interfacial electrostatic interactions and, to a lesser extent, interfacial strain. Our work shows that engineering interfacial electrostatic interactions in an ultrathin van der Waals heterostructure constitutes an effective way to enhance CDW order in two-dimensional materials.Crossing losses in silicone optical waveguides are related to the magnitude and spatial extent of the waveguide refractive index gradient. When processing conditions are altered, the refractive index gradient can vary substantially, even when the formulation remains constant. Controlling the refractive index gradient requires control of the concentration of small molecules present within the core and clad layers. Developing a fundamental understanding of how small molecule migration drives changes in crossing loss requires the ability to examine chemical functionality over small length scales, which is a natural fit for atomic force microscopy-infrared spectroscopy (AFM-IR). In this work, AFM-IR spectra from model bilayer stacks are initially examined to understand molecular migration that occurs from heating the core and clad layers. The results of these model studies are then applied to photopatterned waveguide builds, where structure-function relationships are constructed between values of crossing loss and the concentration of C-H and O-H functionalities present in the core and clad layers. Results show that small molecule evaporation and migration are competing processes that need to be controlled to minimize crossing loss.Electrochemical organic oxidation reactions are highly appealing because protons are often effective terminal electron acceptors, thereby avoiding undesirable stoichiometric oxidants. These reactions are often plagued by high overpotentials, however, that greatly limit their utility. Single-electron transfer (SET) from organic molecules generates high-energy radical-cations. Formation of such intermediates often requires electrode potentials far above the thermodynamic potentials of the reaction and frequently causes decomposition and/or side reactions of ancillary functional groups. In this Account, we show how electrocatalytic electron-proton transfer mediators (EPTMs) address this challenge. EPTMs bypass the formation of radical-cation intermediates by supporting mechanisms that operate at electrode potentials much lower (≥1 V) than those of analogous direct electrolysis reactions. The stable aminoxyl radical TEMPO (2,2,6,6-tetramethylpiperidine N-oxyl) is an effective mediator for electrochemical alcohol ical building blocks and preparation of non-natural amino acids. Electrochemical oxidations of benzylic C-H bonds are commonly initiated by SET to generate arene radical cations, but such methods are again plagued by large overpotentials. Mediated electrolysis methods that promote hydrogen-atom-transfer (HAT) from benzylic C-H bonds to Fe-oxo species and phthalimide N-oxyl (PINO) support C-H oxygenation, iodination, and oxidative-coupling reactions. A complementary method merges photochemistry with electrochemistry to achieve amidation of C(sp3)-H bonds. This unique process operates at much lower overpotentials compatible with diverse functional groups. These results have broad implications for organic electrochemistry, highlighting the importance of "overpotential" considerations and the prospects for expanding synthetic utility by using mediators to bypass high-energy outer-sphere electron-transfer mechanisms. Principles demonstrated here for oxidation are equally relevant to electrochemical reductions.Current lithium ion capacitors (LICs) have been severely plagued by the insufficient anion storage capacity of porous carbon. This work reports the exploration of conductive polyaniline (PANi) as an anion intercalation cathode to enhance the PF6- storage via fast doping/undoping reactions. The PANi is electrodeposited on an electrospun carbon nanofiber (CNF) textile (denoted as PANi@CNF), which not only provides a robust support for PANi to increase its pseudocapacity but also renders a free-standing architecture for flexible devices. The PANi@CNF composite with a dominant capacitive storage characteristic reveals high specific capacities of 158.5 mAh gPANi-1 at 1 A g-1 and 118.5 mAh gPANi-1 even at 20 A g-1, which significantly surpasses state-of-the-art porous carbons. First-principle calculations revealed the coordination of PF6- anions with -NH groups of PANi+ via F atoms through ion-dipole electrostatic interaction, which are accompanied by electron transfer. By pairing with CNF as an anode, a thin and flexible LIC was assembled, which achieves maximum energies of 106.5 Wh kg-1 under 769.0 W kg-1 and 64.5 Wh kg-1 under a super high power of 15087.1 W kg-1, together with an impressive cycling stability of 70.3% after 9000 cycles at 10 A g-1. These findings provide a facile strategy for high-energy and flexible LICs via anion storage pseudocapacitive materials.The development of stretchable electronics requires the invention of compatible high-performance power sources, such as stretchable supercapacitors and batteries. Bufalin mouse In this work, two-dimensional (2D) titanium carbide (Ti3C2Tx) MXene is being explored for flexible and printed energy storage devices by fabrication of a robust, stretchable high-performance supercapacitor with reduced graphene oxide (RGO) to create a composite electrode. The Ti3C2Tx/RGO composite electrode combines the superior electrochemical and mechanical properties of Ti3C2Tx and the mechanical robustness of RGO resulting from strong nanosheet interactions, larger nanoflake size, and mechanical flexibility. It is found that the Ti3C2Tx/RGO composite electrodes with 50 wt % RGO incorporated prove to mitigate cracks generated under large strains. The composite electrodes exhibit a large capacitance of 49 mF/cm2 (∼490 F/cm3 and ∼140 F/g) and good electrochemical and mechanical stability when subjected to cyclic uniaxial (300%) or biaxial (200% × 200%) strains.