Described herein is a manganese-catalyzed dehydrogenative [4+2] annulation of NH imines and alkynes, a reaction providing highly atom-economical access to diverse isoquinolines. This transformation represents the first example of manganese-catalyzed CH activation of imines; the stoichiometric variant of the cyclomanganation was reported in 1971. The redox neutral reaction produces H2 as the major byproduct and eliminates the need for any oxidants, external ligands, or additives, thus standing out from known isoquinoline synthesis by transition-metal-catalyzed CH activation. Mechanistic studies revealed the five-membered manganacycle and manganese hydride species as key reaction intermediates in the catalytic cycle.
Interactive halides: Bis(tetraoxacalix[2]arene[2]triazine), a conformationally rigid cage molecule of three V‐shaped electron‐deficient clefts, forms 1:1 complexes with fluoride (361 M−1), chloride (146 M−1) and bromide (95 M−1) in acetonitrile. Different anion–π interactions along with multiple hydrogen bonding, halogen bonding and lone‐pair‐electrons–π interactions directed the formation of different molecular assemblies (an example is shown here).
The synthesis of 1-methyl-3-(arylthio)-1H-indoles has been achieved by the photoredox reaction of N-methylindoles with readily available arylsulfonyl chlorides in moderate yields.
An undulated two-dimensional CTC-based covalent organic framework, CTC-COF, was synthesized through solvothermal reaction for the first time. This mesoporous material stacks in an eclipsed mode in the microcrystalline state. CTC-COF has a surface area of 1710 m 2 g À1 , with a pore width of 2.26 nm calculated by the NL-DFT modelling. The bowl-shaped core unit led to a larger surface area than its analogue, COF-5 constructed by planar subunits. This material has higher low pressure hydrogen uptake than other 2D COFs with similar structures, and even close to the 3D COF materials.
Anion-π interactions have been widely studied as new noncovalent driving forces in supramolecular chemistry. However, self-assembly induced by anion-π interactions is still largely unexplored. Herein we report the formation of supramolecular amphiphiles through anion-π interactions, and the subsequent formation of self-assembled vesicles in water. With the π receptor 1 as the host and anionic amphiphiles, such as sodium dodecylsulfate (SDS), sodium laurate (SLA), and sodium methyl dodecylphosphonate (SDP), as guests, the sequential formation of host-guest supramolecular amphiphiles and self-assembled vesicles was demonstrated by SEM, TEM, DLS, and XRD techniques. The intrinsic anion-π interactions between 1 and the anionic amphiphiles were confirmed by crystal diffraction, HRMS analysis, and DFT calculations. Furthermore, the controlled disassembly of the vesicles was promoted by competing anions, such as NO3 (-) , Cl(-) , and Br(-) , or by changing the pH value of the medium.
Under very mild aerobic conditions, azacalix[1]arene[3]pyridine underwent highly efficient C-H activation with Cu(ClO(4))(2).6H(2)O to form a stable aryl-Cu(III) complex which reacted rapidly with various nucleophiles at ambient temperature to afford diverse functionalized azacalix[1]arene[3]pyridine derivatives in excellent yields.
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