Latest ArticlesAtkamine is a complex marine pyrroloiminoquinone alkaloid that comprises a heptacyclic scaffold bearing five different heterocycles and four contiguous stereocenters, and therefore it is a highly challenging target for synthetic chemists. We herein reported a modular synthetic strategy toward this alkaloid, featuring a formal [5 + 2] annulation and an asymmetric Michael addition. The efficient synthesis of the long-chain aliphatic aldehyde and chiral amino acetal fragments have been achieved. A simplified tetracyclic intermediate bearing the core structure of atkamine has been successfully constructed through the formal [5 + 2] annulation.
Nanoarchitectonics provide versatile opportunities for modifying the properties of coordination polymers (CP) other than molecular engineering. Spatial-controlled etching focuses on the controlled disassembly of the frameworks. The etching method provides an excellent opportunity for tailoring the properties and functions of the CPs. Here, we discuss the mechanism for controlled etching of the CPs and summarized the two main strategies utilized so far. Several examples are illustrated to demonstrate recent developments in this area. Moreover, advantages of the etched CPs are summarized in several important applications, including energy storage, catalysis and nanomedicine.
The P2-type manganese-based Na0.7MnO2 cathode materials attract great interest due to their high theoretical capacity. However, these materials suffer from rapid capacity fading, poor rate performance and severe voltage decay resulting from phase transition and sluggish reaction kinetics. In this work we report a novel Nb-doped Na0.7[Ni0.3Co0.1Mn0.6]1-xNbxO2 with significantly suppressed voltage decay and enhanced cycling stability. The strong Nb-O bond can efficiently stabilize the TMO framework, and the as prepared material demonstrates much lower discharge midpoint voltage decay (0.132 V) than that of pristine one (0.319 V) after 200 cycles. Consequently, a remarkably improved cycling performance with a capacity retention of 87.9% after 200 cycle at 0.5 C is achieved, showing a 2.4 fold improvement as compared to the control sample Na0.7Ni0.3Co0.1Mn0.6O2 (~37% rotation). Even at 2 C, a capacity retention of 68.4% is retained after 500 cycles. Remarkably, the as prepared material can be applied at low temperature of −20 ℃, showing a capacity retention of 81% as compared to that at room temperature.
Hydrous electrolytes with high electrochemical potentials were obtained by hydrating water molecules into solutes to form high Li: water molar ratio electrolytes (HMRE). Solid polyethylene glycol (PEG) were employed to enhance the molar ratio of Li+ to water in the electrolytes while reducing the consumption of Li-salt. The obtained mole ratio of Li+ to water molecules in the hydrous electrolytes was greater than 1:1; however, the mass fraction of Li-salt was reduced to 61% (approximately 5.5 mol/kg, based on water and PEG). Compared with that of water-in-salt electrolytes, the mass fraction of Li-salt could be remarkably reduced by adding solid PEG. The electrochemical stability of the electrolytes improved considerably because of the strong hydration of Li+ by the water molecules. A beneficial passivation effect, arising from the decomposition of the electrolyte, at a wide potential window was observed.
Two new hydrostable two-dimensional (2D) uranyl coordination complexes [(UO2)5(μ3-O)2(nbca)2]·7H2O (1) and [(UO2)3(nbca)2(H2O)3]·2H2O (2) (H3nbca = 5-nitro-1,2,3-benzenetricarboxylic acid) were hydrothermal synthesized. Single-crystal structural refinements reveal that both of the two complexes were formed by the packing of 2D uranyl coordination sheets via the hydrogen bonds. The nbca ligand coordinating to the uranyl polyhedron centers constructed the 2D sheets. There are UO8 hexagonal bipyramids and UO7 pentagonal bipyramids in 1 while only UO7 pentagonal bipyramids in 2. Photocatalytic degradation of rhodamine B (RhB) in aqueous solution was studied. Complex 2 possesses better performance than 1 with 96.2 % of the RhB was degraded in only 60 min. Mechanism studies reveal that the dissolved oxygens are essential to the RhB degradation. The photocurrent density of 2 is more stable than that of 1, which indicating the stronger ability to separate photoexcited electrons and hole pairs of 2.
A convergent approach to 1,5-hydroxy ketones, the general precursors for constructing the C ring of bryostatins, has been developed via a Zn/Cu-promoted conjugate addition of α-hydroxy iodides with enones. The reaction leads to direct formation of the C21-C22 bond and tolerates diverse functionalities at the C17-, C18- and C24-positions. The approach also enables a more concise synthesis of the known C ring intermediate (10 longest linear steps and 14 total steps), in contrast to its previous synthesis (17 longest linear steps and 22 total steps) in our total synthesis of bryostatin 8.
Reported herein is the first example of heterogeneous palladium catalyzed C(sp3)-H bonds arylation by a transient-ligand-directed strategy. Using supported palladium (metallic state) nanopariticles as catalyst, a wide range of aryl iodides undergo the coupling with various o-methylbenzaldehyde derivatives to assemble a library of highly selective and functionalized o-benzylbenzaldehydes. The stability of the catalyst was easily recovered four runs without significant loss of activity. The XPS analysis of the catalyst before and after reaction indicated that the reaction might be carried out by a catalytic cycle starting with Pd0.
The cheap and easily available sodium dithionite and thiourea dioxide have been used as the source of sulfonyl group in the synthesis of sulfones and sulfonamides recently. Compared with other methods for the sulfonylation reactions, the strategies using sodium dithionite or thiourea dioxide provide an alternative and complementary route to diverse sulfonyl compounds. During the reaction process, sulfur dioxide anion radical is the key intermediate, which is usually generated from a single electron transfer under suitable conditions. The advantages using sodium dithionite or thiourea dioxide in the sulfonylation reactions include mild conditions and broad substrate scope with excellent functional group compatibility. Further applications by using sodium dithionite and thiourea dioxide in organic transformations will be anticipated.
To discover novel fluorophores of solution and solid dual-state emission (DSE) materials, unique V-shape furo[2, 3-b]furans have been designed and synthesized by a one-pot method for the first time and their photoluminescent properties have been explored in benzene, THF, DMF and DMSO, as well as in the solid state. As the best example, 2, 5-bis(4-(9H-carbazol-9-yl)phenyl)-6a-amino-3a, 6a-dihydrofuro[2, 3-b] furan-3, 3a, 4-tricarbonitrile (3g) exhibited solution and solid DSE properties in THF, benzene, and in the solid state with quantum yields of 55%, 92%, and 45%, respectively.
In this work, a blue emitter with a 3D rigid structure composed of multiple spirobifluorene (3-Spiro) has been synthesized and characterized. Through a detailed study of the electrochemical and photophysical properties of 3-Spiro, we have evidenced that 3-Spiro can be applied as an active component of organic light-emitting diodes (OLEDs). The device with 5% doping rate of 4CzPNPh exhibits high external quantum efficiency (EQE) of 11%, which proves the potential of 3D rigid structure emitters for OLEDs.
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