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van der Waals (vdW) heterostructures generated by stacking of graphene with other two-dimensional (2D) crystalline sheets have produced a new class of "designer" materials which shows great promise for nanoscience and nanotechnology. However, the 2D sheets are obtained either from nature or synthesized by high-energy procedures, which preclude the design of their structures as well as properties from molecular design on demand. Here, we introduced a rationally designed 2D polymer (one-monomer unit thick, freestanding network composed of periodically linked monomers) as a component for heterostructure construction, and created a 2D polymer-graphene heterostructure. The heterostructure has a high chemical stability, and could be thermally stable up to 400 °C. In the heterostructure, the 2D polymer doped graphene without changing its intrinsic structure, leading to the enhancement of its electric conductivity by a factor of ∼2.5. This piece of work opens the door to tune the properties of graphene heterostructures with rational design for specific applications.Several gas-phase spectroscopic investigations have focused on a better understanding of the nature of weak, non-covalent interactions in model systems. However, their characterization and interpretation are still far from being satisfactory. A promising route to fill this gap is offered by strategies in which high-resolution rotational spectroscopy is deeply integrated with state-of-the-art quantum-chemical methodology to accurately determine intermolecular parameters and interaction energies, with the latter interpreted by means of powerful energy decomposition analyses (EDAs). As a proof of concept of this approach, we have selected the adducts formed by n-propylamine (PA) and iso-propylamine (IPA) with water. Among the stable structures computationally predicted, four (out of five) isomers of the PA-water complex and two isomers (trans and gauche) of the IPA-water adduct have been characterized with supersonic jet Fourier transform microwave spectroscopy. Starting from the experimental rotational constants for different isotopic species, computation of the corresponding vibrational corrections allowed a semi-experimental determination of the intermolecular parameters. Different EDAs point out that in all cases a strong O-HN hydrogen bond is the primary interaction. Accurate computations indicate that the length and ramification of the alkyl chain do not significantly affect the water-amine interactions, which - on the contrary - modify the stability order of PA conformers with respect to the isolated systems.A facile method for post-synthetic exchange of anions in an iron(ii) spin crossover material using mechanochemistry is described. Dry grinding of the [Fe(atrz)3]Cl2 complex (atrz = 4-amino-1,2,4-triazole) in the presence of an excess of sodium halide salt results in the complete exchange of anions and formation of [Fe(atrz)3]Br2 and [Fe(atrz)3]I2 in a solid-state metathesis reaction. The method represents a new strategy for tuning active switching properties such as the transition temperature in spin crossover systems. Formation of stable by-products was identified as a major driving force for exchange and a straightforward method to predict the likely outcome of such reactions using simple thermodynamic considerations is presented.The reaction mechanism of the hydrogenation of ethylene on pristine (Aun, n = 8 and 20) and rhodium-doped (AunRh) gold clusters was unveiled by theoretical calculations. All reaction pathways are predicted and the thermodynamic and kinetic parameters are computed and compared. Doping a rhodium atom on the magic gold cluster surface is effective in reducing the activation barriers for hydrogenation and in creating two competitive pathways with significantly higher turnover frequencies. The lower barriers of hydrogenation on the AunRh clusters were analyzed and explained based on distortion/interaction activation strain (DIAS) analysis. Further insights into the reaction mechanism on both types of clusters are provided by intrinsic bond orbital (IBO) calculations. This theoretical study provides an idea to elucidate the hydrogenation mechanism on Au clusters and the effect of the rhodium dopant on the catalytic process.Non-precious, stable and efficient catalysts for the pH-universal hydrogen evolution reaction (HER) are highly desirable to meet the vast energy demands. Herein, we report a facile and scalable strategy using agaric as a precursor to construct a Mo2C-based HER electrocatalyst consisting of ultrafine Mo2C nanoparticles embedded within biomass-derived 3D N-doped carbon nanorod arrays@nanosheet networks (Mo2C@N-CANs). This electrocatalyst is highly active for the pH-universal hydrogen evolution reaction and requires overpotentials of only 82 mV, 100 mV and 350 mV to drive a current density of -10 mA cm-2 in acidic, alkaline and neutral media, exhibiting stable operation for 3000 cycles and 24 h long-term stability. Theoretical calculations indicate that coupling Mo2C, N and CANs into a hybrid results in producing wrinkles on carbon nanolayers, which changes the direction of sp2 hybrid orbitals to push the Gibbs free energy toward zero. [https://www.selleckchem.com/products/ABT-888.html Veliparib] This result reinforces the presence of a synergy effect between Mo2C and N-CANs in Mo2C@N-CAN catalysts, which leads to their impressive HER performances.Direct C-H functionalization of aryl ethers remains challenging owing to their low reactivity and selectivity. Herein, a novel strategy for nondirected C-H alkenylation of aryl ethers promoted by a dual ligand catalyst was demonstrated. This catalytic system readily achieved the highly efficient alkenylation of alkyl aryl ethers (anisole, phenetole, n-propyl phenyl ether, n-butyl phenyl ether and benzyl phenyl ether), cyclic aryl ethers (1,4-benzodioxan, 2,3-dihydrobenzofuran, dibenzofuran), and diphenyl oxides. Moreover, the proposed methodology was successfully employed for the late-stage modification of complex drugs containing the aryl ether motif. Interestingly, the compounds developed herein displayed fluorescent properties, which would facilitate their biological applications.