Latest ArticlesA Rh(Ⅰ)-catalyzed highly regio- and enantioselective allylic alkylation of Meldrum acid with racemic allylic substrates bearing alkyl groups has been developed. The applying of chiral bisoxazopinephosphine ligand is essential for the high yields and selectivities. This method provides a rapid access to various chiral β-alkyl-λ, δ-unsaturated carboxylic acids and their derivatives.
One 6-metal Zn-Nd complex [Zn2Nd4L2(OAc)10(OH)2(CH3OH)2] (1) with Schiff base ligand bis(3-methoxysalicylidene)ethylene-1,2-phenylenediamine (H2L) was constructed, and it has nanoscale rectangular structure (8×11×28 Å). Excited by ligand-centered absorption bands, 1 shows NIR emission of Nd3+ ion. Interestingly, 1 exhibits lanthanide luminescent response towards metal ions, especially to alkali metal ions (Li+, Na+ and K+) at ppm level.
The asymmetric synthesis of 16, 17, 20-epi-deserpidine and a derivative of (-)-deserpidine has been achieved. Key features in the assembly of the pentacyclic framework include a visible-light photocatalytic intra-/inter-/intramolecular radical cascade reaction to construct the tetracyclic ABCD ring system in one-pot and an intramolecularaldol reaction to forge the cyclohexane E ring.
Fragrances are widely used in cosmetics, apparel and detergents. However, the rapid evaporation of the aroma shortens the useful life of the aromatic product. Therefore, improving the fragrance retention time of aromatic products and prolonging the service life of aromatic products are the key scientific problems that need to be solved in current aromatic products. In this study, zwitterionic comb-like lipid polymers were synthesized to encapsulate the fragrance molecule linalool. The results showed that the zwitterionic comb lipid molecules were capable of encapsulating more linalool than linear lipid molecules. At the same time, the zwitterionic comb-like lipid molecules also limited the slow release rate of the aroma, thereby increasing the fragrance retention time of the nano-fragrance.
Bis(4-fluorophenyl) substituted oxazole(2,5-Oxz) and C2(5)-C2'(5') linked bioxazole isomers(C2-C2'_BOxz, C2-C5'_BOxz and C5-C5'_BOxz) were concisely synthesized via palladium-catalyzed regioselective and sequential C—H arylation in 1–3 reaction steps along with 20%–83% of total yields from oxazole and 4-bromofluorobenzene.The linking orientation plays a key role in the packing geometry and photophysical properties of C2-C2'_BOxz, C2-C5'_BOxz and C5-C5'_BOxz. These bioxazole isomers in solid state showed significant differences in photoluminescence quantum yields (PLQY) (0.33, 0.25 and 0.04, respectively), delayed fluorescence properties and powder X-ray diffraction (PXRD) patterns, suggesting the divergence in intermolecular interactions. The theoretically calculated gradient isosurfaces and complexation energies indicate the existence of intense π-π interactions between molecular layers, which are in good agreement with the variation trend of optical properties.
Transition metal phosphide (TMP) based electrocatalysts possessing special crystal and electronic structures attract broad attention in the field of electrocatalysis. Immense effort is made to optimize TMP catalysts aiming to satisfy the electrochemical catalysis performance. In this work, an environmentally friendly in situ green phosphating strategy and spatial limiting effect of the RuCo precursor is employed to fabricate the ruthenium nanoclusters anchored on cobalt phosphide hollow microspheres (Ru NCs/Co2P HMs). The obtained Ru NCs/Co2P HMs electrocatalysts exhibit high hydrogen evolution reaction (HER) activity at wide pH ranges, which require an overpotential of 77 mV to achieve the current density of 10 mA/cm2 in 0.5 mol/L H2SO4 and 118 mV in 1.0 mol/L KOH. Besides, the multifunctional Ru NCs/Co2P HMs exhibit good oxygen evolution reaction (OER) activity with an overpotential of 197 mV to reach the current density of 10 mA/cm2 in 0.5 mol/L H2SO4, which is below that of the commercial RuO2 electrocatalyst (248 mV). A two-electrode electrolyzer is assembled as well, in acid electrolyte, it achieves a current density of 10 mA/cm2 at a voltage of 1.53 V, which is superior to that of the benchmark of precious metal-based electrolyzer (1.58 V).
The synthesis of borylated organofluorines is of great interest due to their potential values as synthons in modular construction of fluorine-containing molecules. Reported herein is a rhodium-catalyzed hydroboration of aryl gem-difluoroalkenes leading to a series of α-difluoromethylated benzylborons. The use of cationic rhodium catalyst and a biphosphine ligand with large bite angle was crucial for reactivity by offering good regioselectivity and diminishing the undesired β-F elimination. Preliminary derivatizations of the products were conducted to showcase the utility of this protocol.
Carbon nanotubes (CNTs), as one-dimensional nanomaterials, show great potential in energy conversion and storage due to their efficient electrical conductivity and mass transfer. However, the security risks, time-consuming and high cost of the preparation process hinder its further application. Here, we develop that a negative pressure rather than a following gas environment can promote the generation of cobalt and nitrogen co-doped CNTs (Co/N-CNTs) by using cobalt zeolitic imidazolate framework (ZIF-67) as a precursor, in which the negative pressure plays a key role in adjusting the size of cobalt nanoparticles and stimulating the rearragement of carbon atoms for forming CNTs. Importantly, the obtained Co/N-CNTs, with high content of pyridinic nitrogen and abundant graphitized structure, exhibit superior catalytic activity for oxygen reduction reaction (ORR) with half-wave potential (E1/2) of 0.85 V and durability in terms of the minimum current loss (2%) after the 30, 000 s test. Our development provides a new pathway for large-scale and cost-effective preparation of metal-doped CNTs for various applications.
Metal organic frameworks (MOFs) are a kind of promising materials in many applications, while the fast and controllable synthesis of MOFs is still challenging. Here, taking HKUST-1 as illustration, a micro-plasma electrochemistry (MIPEC) strategy was developed to accelerate the synthesis process of MOFs with micro-plasma acting as cathode. Treating the HKUST-1 precursor solution with micro-plasma cathode could not only transfer the electrons into the solution leading to the deprotonation effect, but also generate radical species to trigger and accelerate the nucleation and growth of MOFs at the plasma-liquid interface. Thus, uniform and nanosize MOFs could be prepared within minutes. The obtained MOFs show similar excellent uranium adsorption properties compared with those obtained by other method, with a highly adsorption capability of uranium with 550 mg/g in minutes. The novel MIPEC strategy developed in this work provides an alternative for controllable synthesis of MOFs, and especially has potential application in accelerating traditional organic synthesis.
Since graphene-based materials have shown great potential in many fields, it is important to explore ultrafast and high-efficient methods to synthesize reduced graphene oxide (rGO) using inexpensive reducing agents under mild conditions. Here, we reported a novel method for the ultrafast chemical reduction of graphene oxide (GO) at room temperature using sodium borohydride (NaBH4), sodium molybdate (Na2MoO4) and hydrochloric acid (HCl). The reduction was carried out within 2 min. A series of characterization results revealed that the obtained reduced graphene oxide has higher reduction degree than that synthesized by NaBH4 alone at high temperature. Moreover, rGO electrode based on the present reducing method exhibited a superior specific capacitance of 139.8 F/g at a current density of 1 A/g, indicating that it can be used as electrode materials for supercapacitors.
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