Surface modification by graphene oxide:An efficient strategy to improve the performance of activated carbon based supercapacitors

An efficient and cost-effective strategy to modificate the surface of active carbon (AC), form a 3D-conductive network, and therefore improve the electrochemical performance of AC based supercapacitor was developed.     

Pressure controllable phase transition in MoTe2 by the interlayer band occupancy

High pressure can effectively control the phase transition of MoTe₂ in experiment, but the mechanism is still unclear. In this work, we show by first-principles calculations that the phase transition is suppressed and $1T^{\prime }$ phase becomes more stable under high pressure, which originates from the pressure-induced change of the interlayer band occupancies near the Fermi energy. Specifically, the interlayer states of $1T^{\prime }$ phase tend to be fully occupied under high pressure, while they keep partially occupied for the $T_d$ phase. The increase of the band occupancies makes the $1T^{\prime }$ phase more favorable in energy and prevents the structure changing from $1T^{\prime }$ to $T_d$ phase. Moreover, we also analyze the superconductivity under high pressure based on BCS theory by calculating the density of states and phonon spectra. Our results may shed some light on understanding the relationship between the interlayer band occupancy and crystal stability of MoTe₂ under high pressures.     

Catalytic enantioselective synthesis of optically active α-hydroxyl-β,γ-unsaturated acid esters as novel side chains of cerebrosides

Six optically active α-hydroxyl-β,γ-unsaturated acid esters 1a to 1f were synthesised, and they are significant moieties of the cerebrosides. The chiral intermediate alkynol 4 prepared by catalytic asymmetric addition had 99% ee, and which was converted into the target compounds 1a to 1f with high enantiomeric purity.     

Hydrothermal synthesis and characterization of NiS flower-like architectures

Under the influence of thiocyanate anions (SCN^?) and cetyltrimethyl ammonium bromide (CTAB), NiS flower-like architectures were successfully synthesized by a one-step hydrothermal method. The synthesized flower-like architectures, with a multilayered and highly ordered texture, have diameters of several micrometers. X-ray powder diffraction (XRD) shows that the NiS flower-like architectures are rhombohedral crystalline. On the basis of condition-dependent experiments, the diffusion-limited aggregation (DLA) model and cage effect were used to explain the growth process of rhombohedral crystalline NiS flower-like architectures. Magnetic measurements showed that the coercivity (H_c) of the as-obtained NiS flower-like architectures was 102.14 Oe.     

Theoretical study on the origin of enantioselectivity in the primary amine–Brønsted acid catalyzed epoxidation of cyclic enones

Computational studies to determine the origin of enantioselectivity in the (1R,2R)-1,2-diphenylethane-1,2-diamine (DEPN)–Brønsted acid catalyzed epoxidation of 2-cyclohexen-1-one have been performed using density functional theory. Transition states for conjugate addition and ring closure steps of the epoxidations catalyzed by three different catalyst systems were characterized. Our calculations show that the C_sp2H?O H-bond interaction between the benzene ring of the catalyst and H₂O is mainly responsible for the chiral discrimination observed. The Brønsted acid counterion plays a very important role in ensuring high enantioselectivity by improving the rigidity of the transition state structures to allow the efficient formation of the C_sp2H?O H-bond. Moreover, we explain why these two diamine catalysts (1S,2S)-DACH and (1R,2R)-DPEN display consistent enantioselectivities in the catalytic epoxidation of 2-cyclohexen-1-one when combining with three different cocatalysts; achiral TFA, and chiral (R)- and (S)-TRIP.     

A [001]-Oriented Hittorf's Phosphorus Nanorods/Polymeric Carbon Nitride Heterostructure for Boosting Wide-Spectrum-Responsive Photocatalytic Hydrogen Evolution from Pure Water

Red phosphorus is a promising photocatalyst with wide visible-light absorption up to 700 nm, but the fast charge recombination limits its photocatalytic hydrogen evolution reaction (HER) activity. Now, [001]-oriented Hittorf's phosphorus (HP) nanorods were successfully grown on polymeric carbon nitride (PCN) by a chemical vapor deposition strategy. Compared with the bare PCN and HP, the optimized PCN@HP hybrid exhibited a significantly enhanced photocatalytic activity, with HER rates reaching 33.2 and 17.5 μmol h⁻¹ from pure water under simulated solar light and visible light irradiation, respectively. It was theoretically and experimentally indicated that the strong electronic coupling between PCN and [001]-oriented HP nanorods gave rise to the enhanced visible light absorption and the greatly accelerated photoinduced electron–hole separation and transfer, which benefited the photocatalytic HER performance.     

Regulating PdC3/PtC3···thiophene interaction by small molecule doping (AgOTf,CuBr, CuI,CuBr2, PdCl2)

Structural Chemistry - The influences of small molecule doping on PdC3/PtC3···thiophene interaction have been investigated by atoms in molecules (AIM) theory, electron location...