Latest ArticlesMetal organic framework (MOF) has been confirmed as the promising precursor to develop the conversion-typed anode materials of sodium-ion batteries (SIBs) because of the tunable structure design and simple functional modification. Here, we prepare the ultrasmall Ni3S2 nanocrystals embedded into N-doped porous carbon nanoparticles using the scalable Ni-MOF as precursor (denoted as Ni3S2@NPC). The ultrasmall size of Ni3S2 can work for accelerated electron/ion transfer to facilitate the electrochemical reaction kinetics. Moreover, the robust conductivity network originated from N-doped porous carbon nanoparticles can not only improve the electron conductivity, but also enhance the electrode integrity and stability of the electrode/electrolyte interface. In addition, the N heteroatoms provide extra Na storage sites. Accordingly, the electrode delivers the obviously competitive capacities and high-power output with respect to the currently reported Ni3S2/C composites. This study provides a scalable and universal strategy to develop the advanced transition metal sulfides for practically feasible SIBs.
Zinc-ion hybrid super-capacitors are regarded as promising safe energy storage systems. However, the relatively low volumetric energy density has become the main bottlenecks in practical applications of portable electronic devices. In this work, the zinc-ion hybrid super-capacitor with high volumetric energy density and superb cycle stability had been constructed which employing the high-density three-dimensional graphene hydrogel as cathode and Zn foil used as anode in 1 mol/L ZnSO4 electrolyte. Benefiting from the abundant ion transport paths and the abundant active sites for graphene hydrogel with high density and porous structure, the zinc-ion hybrid super-capacitor exhibited an extremely high volumetric energy density of 118.42 Wh/L and a superb power density of 24.00 kW/L, as well as an excellent long cycle life (80% retention after 30,000 cycles at 10 A/g), which was superior to the volumetric energy density of the reported zinc-ion hybrid super-capacitors. This device, based on the fast ion adsorption/desorption on the capacitor-type graphene cathode and reversible Zn2+ plating/stripping on the battery-type Zn anode, which will inspire the development of zinc-ion hybrid super-capacitor in miniaturized devices.
By taking the functional advantages of both pyrazolate and carboxylate ligands, a unique dual-functional pyrazolate-carboxylate ligand acid, 4-(3,6-di(pyrazol-4-yl)-9-carbazol-9-yl)benzoic acid (H3PCBA) was designed and synthesized. Using it, a new Co(II)-based metal-organic framework (MOF), Co3(PCBA)2(H2O)2 (BUT-75) has been constructed. It revealed a (3,6)-connected net based on the 6-connected linear trinuclear metal node, and showed good chemical stability in a wide pH range from 3 to 12 at room temperature, as well as in boiling water. Due to the presence of rich exposed Co(II) sites in pores, BUT-75 presented high selective CO2 adsorption capacity over N2 at 298 K. Simultaneously, it demonstrated fine catalytic performance for the cycloaddition of CO2 with epoxides into cyclic carbonates under ambient conditions. This work has not only enriched the MOF community through integrating diverse functionalities into one ligand but also contributed a versatile platform for CO2 fixation, thereby pushing MOF chemistry forward by stability enhancement and application expansion.
In this work, titanium-capped cobalt clathrochelates have been applied as secondary building units (SBUs) for the construction of supramolecular rings. Two heterometallic wheel-like [Ti6Co12] complexes based on cobalt clathrochelates, [C6H15N4]2[TiCo2(μ2-Oipr)(Oipr)2(Dmg)3]6 (2, Dmg=dimethylglyoxime) and H6[TiCo2(μ2-Oipr)(Oipr)2(Dmg)3]6 (3), have been successfully synthesized and characterized. The supramolecular stacking modes of these wheels are largely dependent on the applied synthetic conditions, which further impact their gas adsorption properties.
With increasing demand for renewable energy, graphene-like BC3 monolayer as high performance electrode materials for lithium and sodium batteries are drawing more attention recently. However, its structural stability, potassium storage properties and strain effect on adsorptionproperties of alkali metal ions have not been reported yet. In this work, phonon spectra, AIMD simulations and elastic constants of graphene-like BC3 monolayer are investigated. Our results show that graphene-like BC3 monolayer possesses excellent structural stability and the maximum theoretical potassium storage capacity can reach up to 1653 mAh/g with the corresponding open circuit voltages 0.66 V. Due to potassium atom can be effectively adsorbed at the most energetically favorable h-CC site with obvious charge transfer, making adsorbed graphene-like BC3 monolayer change from semiconductor to metal which is really good for electrode utilization. Moreover, the migrations potassium atom on the graphene-like BC3 monolayer is rather fast with the diffusion barriers as low as 0.12 eV, comparing lithium atom with a relatively large diffusion barrier of 0.46 eV. Additionally, the tensile strains applied on the graphene-like BC3 monolayer have marginal effect on the adsorption and diffusion performances of lithium, sodium and potassium atoms.
A new family of isostructural 3d-4f polymetallic complexes, formulated as [Cu6Ln5(μ3−OH)9 (C4H8O2N)6(C5H4ON)6(H2O)9]·(ClO4)6·(H2O)22 (Ln = Pr, 1; Nd, 2; Sm, 3; Eu, 4; Gd, 5), was successfully isolated through the simple hydrolysis reaction of 2-aminoisobutyric acid, 2-hydroxypyridine, Cu(CH3COO)2·H2O, and Ln(ClO4)3·6H2O. Notably, the [Cu6Ln5] clusters with high molecular symmetry of D3h are rare examples of 2-aminoisobutyric acid-based 3d-4f clusters. The successful theoretical modeling of 5 yielded that the Gd-Gd exchange is of order 0.2 K, whereas the Gd-Cu exchange is an order of magnitude larger. Magnetization data collected for complex 5 yield a magnetic entropy change (−ΔSm) of 19.6 J kg−1 K−1 at 3 K and 7 T, which may be attributed to the weak magnetic interactions between the component metal ions.
The N-heterocyclic carbene (NHC)-catalyzed reactions involving two-electron reaction pathway have been well-established. However, the development of NHC-catalyzed radical reactions is still in its infancy in terms of reaction types and enantioselectivity. In the past decade, several elegant NHC-catalyzed radical reactions have been developed, including NHC-catalyzed oxidation of aldehydes to esters, reductive coupling reactions using Breslow intermediate as SET reductant and NHC-catalyzed reactions via radical homoenolates, dienoaltes and trienolates. This review summarizes the recent advances in NHC-catalyzed reactions involving radical intermediates.
Transition metal-catalyzed carbene transfer reaction is one of the most notable advances for C−C bond formation reactionsduring the past decade, which has been widely employed in the preparation of C3-substituted indoles. Here, we described an efficient example of catalyst- and metal-free aminoboration of alkynes and C−C bond formation with diazo compounds to produce C3-substituted indoles. Diverse alkynylanilines and diazo compounds can be utilized for this tandem transformation under mild reaction conditions, resulting in broad functional group compatibility. Additionally, this metal-free strategy can be extended to construct substituted benzofurans.
Light utilization is one of the key factors for the improvement of photocatalytic performance. Herein, we design C-TiO2 hollow nanoshells with strong Mie resonance for enhanced photocatalytic hydrogen evolution in a dye-sensitized system under visible light irradiation (λ≥420 nm). By tuning the inner diameters of hollow nanoshells, the Mie resonance in hollow nanoshells is adjusted for better excitation of dye molecules, which thus greatly enhances the light utilization in visible light region. This work shows the potential of Mie resonance in nanoshells can be an alternative strategy to increase the light utilization for photocatalysis.
Chemoselective amine bioconjugation has long been a challenge for native protein modification. Inspired by Thiele's seminal discovery, Li and co-workers recently developed an ortho-phthalaldehyde (OPA) based reagent for labeling the amino group of a protein. Here we report an expeditious and scalable synthesis of a Li—Thiele reagent featuring an arene construction strategy. The reagent contains an alkyne side chain as a handle for secondary modification.
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