Synthesis, characterization, crystal and molecular structure analysis of N-(2,4-dimethylphenyl)-6-methyl-4-(3-nitrophenyl)-2-oxo-1,2,3,4-tetrahydropyrimidine-5-carboxamide

A novel dihydropyrimidine (DHPM) derivative bearing a carbamoyl moiety was synthesized by an efficient three-component Biginelli reaction and was characterized spectroscopically and finally confirmed by X-ray diffraction studies. The title compound C₂₀H₂₀N₄O₄ crystallizes in the monoclinic space group P2₁/c with cell parameters a=12.8970(12) Å, b=13.6210(11) Å, c=11.8420(13) Å, β=115.860(3)°, Z=4 and V=1872.0(3) Å³. The conformation of the dihydropyrimidine ring is unusual; it is planar instead of the usual boat-like conformation. The 3-nitrophenyl ring is orthogonal to the 3,4-DHPM ring. The carbonyl group is in an anti-clinal conformation.     

Formal synthesis of 14-membered unsymmetrical bis-macrolactone, (−)-colletodiol

Formal synthesis of 14-membered unsymmetrical bis-macrolactone, (?)-colletodiol was accomplished from homopropargylic alcohol derivative. Building of the two different hydroxy acid fragments from the same intermediate of homoallylic alcohol was particularly advantageous. A Sharpless asymmetric dihydroxylation, homologation of carbon chain, a Pinnick oxidation, and a macrolactonization to assemble the 14-membered macrodiolide were the additional salient features of this convergent synthesis.     

B ?→ K 1*? (1270)(→ ρ 0 K ?) ? + ? ? in LEET

Flavor changing neutral current (FCNC) decays of the B-meson are a very useful tool for studying possible physics scenarios beyond the standard model (SM), where of the many FCNC modes radiative, purely leptonic and semi-leptonic decays of the B-meson are relatively clean tests. Within this context, the BELLE collaboration has measured the process B→K ^* γ and also searched for the B→K ₁(1270)γ process. Theoretical analyses of these processes are yielding similar values of the relevant form factors. In this work we have used this upper bound in studying the angular correlations for the related semi-leptonic decay mode B ⁻→K ₁⁻(1270)(→ρ ⁰ K ⁻)ℓ ⁺ ℓ ⁻, where we have used the form factors that have already been estimated for the B→K ₁(1270)γ mode. Note that the additional form factors that are required were calculated using large energy effective theory (LEET).     

Transition-Metal Acetate-Promoted Intramolecular Nitrene Insertion to Vinylogous Carbonates for Divergent Synthesis of Azirinobenzoxazoles and Benzoxazines

Synthesis and isolation of highly unstable azirinobenzoxazole and benzoxazines in a chemodivergent fashion from aryl azido vinylogous carbonates by simple change in transition metal acetate is described. Thermal or rhodium(II) acetate-mediated decomposition of these azides gave dihydroazirino benzoxazole. Their nickel(II) acetate-promoted reaction gave 4-dihydro-2H-benzoxazines, whereas copper(II) acetate led to the corresponding oxidized imine derivatives. Benzaoxazine derivative could be kinetically resolved using a proline-catalyzed Mannich reaction. The benzoxazines were rapidly elaborated to angularly fused tetracyclic systems and coumarin-fused derivatives in a “one pot” fashion.     

Synergistic effect of cellulose nanowhiskers reinforcement and dicarboxylic acids crosslinking towards polyvinyl alcohol properties

In the presented work, a significant increase in the tensile strength of the PVA composite material is reported. The obtained best value of 122 MPa and 14.6% swelling shows the excellent synergistic effect of both crosslinker and reinforcement material. The composite films were prepared by simple mechanical dispersion of reinforcement material, bacterial cellulose nanowhiskers (BCNW) into PVA solution followed by crosslinking with diacids, succinic acid (SuA), and adipic acid (AdA). The effect of aliphatic carbon chain length of crosslinker on thermal, mechanical, and water uptake properties is evaluated and discussed in detail. Neat PVA had the strength of 37.3 MPa. With 5% reinforcement of BCNW, that is, without crosslinking, it exhibited 97% increase, that is, 74.5 MPa. With crosslinking of 15 mmol of SuA and AdA PVA films for 2 h had excellent thermal properties with swelling percentage of 19 and 26.6% and tensile strength of 103 and 67 MPa, respectively. The best result obtained was for 5% BCNW–PVA films crosslinked with 15 mmol SuA. These results were explained on the basis of synergetic crosslinking and extended hydrogen bonding between PVA and reinforcement material. The composite films can be used as biological implants, a membrane for pervaporation and filtration system, etc. © 2016 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2016 , 54, 2515–2525     

Ruthenium-catalysed conversion of oxime ethers into nitriles

The conversion of oxime ethers into nitriles has been achieved under neutral conditions using Ru(CO)(PPh₃)₃H₂ and the bidentate ligand Xantphos as the catalyst.     

Synthesis,characterization, single crystal X-ray diffraction and DFT studies of ethyl 5-methyl-1-phenyl-1H-pyrazole-4-carboxylate

The present study describes the synthesis, spectroscopic, and single crystal X-ray structural analysis of ethyl 5-methyl-1-phenyl-1H-pyrazole-4-carboxylate. The pyrazole ester of formula [C₁₃H₁₄N₂O₂] was prepared from the three-component one-pot condensation reaction of ethyl acetoacetate, N,N-dimethyldimethoxymethanamine, and phenyl hydrazine. The product was crystallized by using ethanol as solvent. The structure of the compound was confirmed by elemental analysis, Fourier transforms infrared (IR), thermogravimetric analysis, UV-visible (UV-Vis), ¹H NMR, and single-crystal X-ray diffraction studies. The gas-phase molecular geometry and the electronic structure-property of the molecule were calculated at the density functional theory. The frontier molecular orbitals, theoretical UV-Vis, and IR stretching vibrations were also reported. The compound crystallizes in the monoclinic system with the space group P2₁/c and Z = 4. The unit cell parameters are a = 12.141(3) Å, b = 13.934(4) Å, c = 7.2777(18) Å, and β = 97.816(14)⁰. The structure is stabilized by an intermolecular interaction of type C-H···O and the structure also involves C-H···π interactions.     

MAC-level Forward Error Correction mechanism for minimum error recovery overhead and retransmission

Wireless transmission suffers from poor wireless channel conditions, such as high bit error rate and error bursts resulting from channel fading and radio interference. The MAC-level Forward Error Correction (MFEC) mechanism is proposed to solve these problems. The MFEC mechanism cannot only adaptively adjust Forward Error Correction (FEC) redundancy, depending on the network condition, but can also retransmit whole packets even if the error packet includes several bit errors. In this paper, an Adaptive MAC-level FEC (AMFEC) mechanism is proposed to improve wireless transmission quality. The AMFEC mechanism relies on the effective packet loss rate model to dynamically adjust MFEC redundancy in order to minimize error recovery overhead. The AMFEC mechanism will retransmit the error of sub-packets and increase FEC redundancy to reduce transmission redundancy. The AMFEC mechanism not only enhances the quality of wireless transmission but also reduces the overhead of retransmission. The experimental results show the AMFEC mechanism is better than conventional MFEC mechanisms.     

Mechanistic Insights into the Self-Assembly of an Acid-Sensitive Photoresponsive Supramolecular Polymer

The supramolecular polymerization of an acid-sensitive pyridyl-based ligand ( L₁ ) bearing a photoresponsive azobenzene moiety was elucidated by mechanistic studies. Addition of trifluoroacetic acid (TFA) led to the transformation of the antiparallel H-bonded fibers of L₁ in methylcyclohexane into superhelical braid-like fibers stabilized by H-bonding of parallel-stacked monomer units. Interestingly, L₁ dimers held together by unconventional pyridine–TFA N⋅⋅⋅H⋅⋅⋅O bridges represent the main structural elements of the assembly. UV-light irradiation caused a strain-driven disassembly and subsequent aggregate reconstruction, which ultimately led to short fibers. The results allowed to understand the mechanism of mutual influence of acid and light stimuli on supramolecular polymerization processes, thus opening up new possibilities to design advanced stimuli-triggered supramolecular systems.