Latest ArticlesThe CpXRh(Ⅲ)-catalyzed asymmetric cascade C-H coupling/intramolecular cyclization of azomethine imines with propargyl carbonates has been developed, affording a variety of chiral tetracyclic indenopyrazolopyrazolone frameworks with good substrate/functional group tolerance and enantioselectivity (up to 97:3 er). Combined experimental studies and DFT calculations revealed the Rh(Ⅲ)-catalyzed stepwise annulation process and clarified the synergy coordination mode of dual directing groups in tuning the selectivity.
An iron-catalyzed coupling reaction of difluoroenol silyl ethers and cyclobutanone oxime esters is described. This protocol provides a convenient access to various previously unknown and potentially useful gem-difluoromethylenated ketonitriles inmoderate to good yields. The transformations of resulting products to other fluorinecontaining products is also documented.
Sodium-ion batteries (SIBs) have gained more scientists' interest, owing to some facts such as the natural abundance of Na, the similarities of physicochemical characteristics between Li and Na. The irreversible Na+ ions consumption during the first cycle of charge/discharge process (due to the formation of the solid electrolyte interface (SEI) on the electrode surface and other irreversible reactions) is the factor that determines high performance SIBs and largely reduces the capacity of the full cell SIBs. Thus, the initial coulombic efficiency (ICE) of SIBs for both anode and cathode materials, is a key parameter for high performance SIBs, and the point is to increase the transport rate of the Na+ ions. Therefore, developing SIBs with high ICE and rate performance becomes vital to boost the commercialization of SIBs. Here we provide a review on the methods to improve the ICE and the rate performance, by summarizing some methods of improving the ICE and rate performance of the anode and cathode materials for SIBs, and end by a conclusion with some perspectives and recommendations.
Film morphology of emissive layers is crucial to the performance and stability of solution-processable organic light-emitting diodes (OLEDs). Compared to the interpenetration of conjugated polymer chain, small molecular emitter with a flexible side chain always presents easily aggregation upon external treatment, and caused π-electronic coupling, which is undesirable for the efficiency and stability of deep-blue OLEDs. Herein, we proposed a side-chain coupling strategy to enhance the film morphological an emission stability of solution-processable small molecular deep-blue emitter. In contrary to "parent" MC8TPA, the crosslinkable styryl and vinyl units were introduced as ended unit at the side-chain of CmTPA and OEYTPA. Interestingly, CmTPA and OEYTPA films present a relatively stable morphology and uniform deep-blue emission after thermal annealing (160 ℃) in the atmosphere, different to the discontinuous MC8TPA annealed film. Besides, compared to the CmTPA and OEYTPA ones, serious polaron formation in the MC8TPA annealed film also negative to the deep-blue emission, according to transient absorption analysis. Therefore, both CmTPA and OEYTPA annealed film obtained at 140 ℃ present an excellent deep-blue ASE behavior with a 445 nm, but absence for MC8TPA ones, associated with the disruption of annealed films. Finally, enhancement of device performance based on CmTPA and OEYTPA film (~40%) after thermal annealing with a similar performance curves also confirmed the assumption above. Therefore, these results also supported the effectiveness of our side-chain coupling strategy for optoelectronic applications.
This work detailed the preparation of a class of water-soluble PNP ligands that differed by the nature of the substitute on phenyl ring of ligands. These ligands were incorporated into water-soluble rhodium-PNP complex catalysts that were used to regioselective hydroformylation of a series of terminal arylalkenes, providing efficient access to rac-α-aryl propionaldehydes in good to excellent yield (up to 97%) and branched-regioselectivity (up to 40:1 b/l ratio). Furthermore, gram-scale and diverse synthetic transformation demonstrated synthetic application of this methodology for non-steroidal antiinflammatory drugs.
Here, a rhodium(Ⅲ)-catalyzed benzo[c]azepine-1, 3(2H)-dione synthesis via tandem C–H alkylation and intramolecular amination of N-methoxylbenzamide with 3-bromo-3, 3-difluoropropene as the alkylation agent is reported. The substituted benzamides and protected indoles are all tolerated, yielding the corresponding products in moderate to good yields. Further study revealed those bioactive compounds such as piperic acid and a key precursor of Roflumilast all perform well, highlighting the synthetic utility of this method.
A bioinspired acid-triggered hemiacetalization/dehydration/[3 + 3]-type cycloaddition cascade process was disclosed, diastereoselectively furnishing furo[2,3-b]chromene skeleton under mild conditions. The viability of this approach was demonstrated by syntheses of a series of furo[2,3-b]chromene and pyrano[2,3-b]chromene derivatives. The successful total syntheses of two lignan-phloroglucinol hybrids, hyperaspidinols A and B, exemplified the synthetic utility of our biomimetic methodology.
The recombination of charge carriers arriving from the random charge movement in semiconductor photocatalysts greatly limits the practical application of solar-driven H2 evolution. The design of photocatalytic systems with spatially oriented charge-transfer is a promising route to achieve high charge-separation efficiency for photocatalysts. Herein, novel sea-urchin-like ReS2 nanosheet/TiO2 nanoparticle heterojunctions (SURTHs) are constructed. The unique sea-urchin-like structure endows the ReS2 cocatalyst with an unusual charge edge-collection effect, which leads to a significant acceleration of charge separation and transfer, as evidenced by the well-designed selective photodeposition of Pt quantum dots in SURTHs. The markedly improved charge transfer capacity contributes to a high photocatalytic H2 evolution rate of 3.71 mmol h-1 g-1 for SURTHs (an apparent quantum efficiency (AQE) of 16.09%), up to 231.9 times by contrast with that of P25 TiO2. This work would provide a new platform for designing the high-efficiency cocatalyst/photocatalyst system with excellent charge transfer capacity.
Electrocatalysis plays an increasingly important role in converting atmospheric molecules (e.g., N2, CO2 and H2O) to value-added products (e.g., NH3, C2H4 and H2). However, developing a simple strategy for preparing catalysts with high performance for the effective conversion of clean energy is still full of challenges. Herein, we describe a straightforward, one-step reduction method to achieve the formation of Pt nanoparticles (NPs) and the vacancy engineering of TiO2–x nanofibers (NFs) simultaneously, which can be accomplished in 5 min. Furthermore, a Pt/TiO2–x nanofibrous aerogel (NA) with an ordered cellular architecture is prepared through a directional freezing technology. The Pt/TiO2–x NA with excellent mechanical properties can be made into a self-supporting electrode for electrocatalytic N2 reduction reaction (NRR), showing high NH3 yield rate (4.81 × 10–10 mol/s cm–2) and Faraday efficiency (14.9%) at –0.35 V vs. RHE.
Development of low-cost electrode materials with long cycle life and high volumetric capacity is important for large-scale applications of lithium-ion batteries (LIBs). Here, an electrode made from Fe2O3 encapsulated with N-doped carbon (Fe2O3@N-C) via ZIF-8 coating and carbonization process is reported. A cavity was generated between the Fe2O3 and N-C material during the carbonization process that is conducive to alleviating the volume expansion of Fe2O3. As a result, the Fe2O3@N-C composite exhibits a high specific capacity (1064 mAh/g at 0.1 A/g) and cycle stability (803.6 mAh/g at 1.0 A/g after 1100 cycles) when used as the LIB anode. In addition, the influence of carbonization under air on the LIB performance was investigated by controllably changing the crystal phase of Fe2O3 and the thickness of the carbon layer. This work provides a new method for the design and fabrication of yolk-shell composite electrodes for LIBs and other applications.
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