One of the challenges in material science has been to prepare macro-or mesoporous zeolite. Although examples of their synthesis exist, there is a need for a facile yet versatile approach to such hierarchical structures. Here we report a concept for designing a single quaternary ammonium head amphiphilic template with strong ordered self-assembling ability through p-p stacking in hydrophobic side, which stabilizes the mesostructure to form singlecrystalline mesostructured zeolite nanosheets. The concept is demonstrated for the formation of a new type of MFI (zeolite framework code by International Zeolite Association) nanosheets joined with a 90°rotational boundary, which results in a mesoporous zeolite with highly specific surface area even after calcination. Low binding energies for this selfassembling system are supported by a theoretical analysis. A geometrical matching between the arrangement of aromatic groups and the zeolitic framework is speculated for the formation of single-crystalline MFI nanosheets.
The
separation of acetylene from ethylene is a crucial process
in the petrochemical industry, as even small acetylene impurities
can lead to premature termination of ethylene polymerization. Herein,
we present the synthesis of a robust, crystalline naphthalene diimide
porous aromatic framework via imidization of linear naphthalene-1,4,5,8-tetracarboxylic
dianhydride and triangular tris(4-aminophenyl)amine. The resulting
material, PAF-110, exhibits impressive thermal and long-term structural
stability, as indicated by thermogravimetric analysis and powder X-ray
diffraction characterization. Gas adsorption characterization reveals
that PAF-110 has a capacity for acetylene that is more than twice
its ethylene capacity at 273 K and 1 bar, and it exhibits a moderate
acetylene selectivity of 3.9 at 298 K and 1 bar. Complementary computational
investigation of each guest binding in PAF-110 suggests that this
affinity and selectivity for acetylene arises from its stronger electrostatic
interaction with the carbonyl oxygen atoms of the framework. To the
best of our knowledge, PAF-110 is the first crystalline porous organic
material to exhibit selective adsorption of acetylene over ethylene,
and its properties may provide insight into the further optimized
design of porous organic materials for this key gas separation.
Indole diketopiperazine alkaloids are secondary metabolites of microorganisms that are widely distributed in filamentous fungi, especially in the genera Aspergillus and Penicillium of the phylum Ascomycota or sac fungi. These alkaloids represent a group of natural products characterized by diversity in both chemical structures and biological activities. This review aims to summarize 166 indole diketopiperazine alkaloids from fungi published from 1944 to mid-2015. The emphasis is on diverse chemical structures within these alkaloids and their relevant biological activities. The aim is to assess which of these compounds merit further study for purposes of drug development.
Highly conductive metal selenides are gaining prominence as promising electrode materials in electrochemical energy‐storage fields. However, phase‐pure bimetallic selenides are scarcely retrieved, and their underlying charge‐storage mechanisms are still far from clear. Here, first a solvothermal strategy is devised to purposefully fabricate monodisperse hollow NiCoSe2 (H‐NiCoSe2) sub‐microspheres. Inherent formation of metallic H‐NiCoSe2 is tentatively put forward with comparative structure‐evolution investigations. Interestingly, the fresh H‐NiCoSe2 does not demonstrate striking supercapacitive behaviors when evaluated for electrochemical supercapacitors (ESs). But it exhibits competitive pseudocapacitance of ≈750 F g−1 at a rate of 3 A g−1 with a high loading of 7 mg cm−2 after ≈100 cyclic voltammetry (CV) cycles. With systematic physicochemical/electrochemical analyses, intrinsic energy‐storage mechanism of the H‐NiCoSe2 is convincingly revealed that the electrooxidation‐generated biactive CoOOH/NiOOH phases in aqueous KOH over CV scanning, rather than the H‐NiCoSe2 itself, account for the remarkable pesudocapacitance observed after cycling. An assembled H‐NiCoSe2‐based asymmetric device has delivered an energy density of ≈25.5 Wh kg−1 with a power rate of ≈3.75 kW kg−1, and long‐span cycle life. More significantly, the electrode design and new perspectives here hold profound promise in enriching material synthesis methodologies and in‐depth understanding of the complex charge‐storage process of newly emerging pseudocapacitive materials for next‐generation ESs.
2D conductive metal–organic frameworks (2D c‐MOFs) are promising candidates for efficient electrocatalysts for the CO2 reduction reaction (CO2RR). A nitrogen‐rich tricycloquinazoline (TQ) based multitopic catechol ligand was used to coordinate with transition‐metal ions (Cu2+ and Ni2+), which formed 2D graphene‐like porous sheets: M3(HHTQ)2 (M=Cu, Ni; HHTQ=2,3,7,8,12,13‐Hexahydroxytricycloquinazoline). M3(HHTQ)2 can be regarded as a single‐atom catalyst where Cu or Ni centers are uniformly distributed in the hexagonal lattices. Cu3(HHTQ)2 exhibited superior catalytic activity towards CO2RR in which CH3OH is the sole product. The Faradic efficiency of CH3OH reached up to 53.6 % at a small over‐potential of −0.4 V. Cu3(HHTQ)2 exhibited larger CO2 adsorption energies and higher activities over the isostructural Ni3(HHTQ)2 and the reported archetypical Cu3(HHTP)2. There is a strong dependence of both metal centers and the N‐rich ligands on the electrocatalytic performance.
A conjugated copper(II) catecholate based metal–organic framework (namely Cu‐DBC) was prepared using a D2‐symmetric redox‐active ligand in a copper bis(dihydroxy) coordination geometry. The π‐d conjugated framework exhibits typical semiconducting behavior with a high electrical conductivity of ca. 1.0 S m−1 at room temperature. Benefiting from the good electrical conductivity and the excellent redox reversibility of both ligand and copper centers, Cu‐DBC electrode features superior capacitor performances with gravimetric capacitance up to 479 F g−1 at a discharge rate of 0.2 A g−1. Moreover, the symmetric solid‐state supercapacitor of Cu‐DBC exhibits high areal (879 mF cm−2) and volumetric (22 F cm−3) capacitances, as well as good rate capability. These metrics are superior to most reported MOF‐based supercapacitors, demonstrating promising applications in energy‐storage devices.
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