MNPs@MOF catalysts
obtained by encapsulating metal nanoparticles
(NPs) into metal–organic frameworks (MOFs) show fascinating
performance in heterogeneous catalysis. The improvement of catalytic
activity and reusability of MNPs@MOF catalysts has been a great challenge
for a long time. Herein, we demonstrate well-designed Pd/MOFs, featuring
hollow double-shell structure and magnetic property, exhibiting high
reusability, efficient catalytic activity, and size selectivity for
hydrogenation reaction. The as-synthesized Pd/MOF, denoted as Void nFe3O4@Pd/ZIF-8@ZIF-8, possesses diverse
functional structural features. The hollow cavity can improve mass
transfer; superparamagnetic Fe3O4 NPs embedded
in the inner MOF shell can enhance the separation and recyclability;
Pd NPs are highly dispersed in the matrix of the inner MOF shell,
and the outer MOF shell acts as a protector to prevent the leaching
of Pd NPs and a sieve to achieve size selectivity. As a proof of concept,
the Void nFe3O4@Pd/ZIF-8@ZIF-8
catalyst exhibited excellent performance for the hydrogenation of
styrene at room temperature. The activity only reduced 10% after 20
cycles for the higher conversions (>90%), and the lower conversion
only decreased 3.6% (from 32.5 to 28.9% conversion) after twenty consecutive
cycles, indicating the good and intrinsic reusability of the catalyst.
The proposed structure in this work provides a strategy to effectively
improve the reusability of MNPs@MOF catalysts, which would increase
their practical applications.
Hexadecyl trimethylammonium bromide
(CTAB) micelles were applied
in the synthesis of covalent organic frameworks (COFs) for the first
time to achieve the synthesis of 3D COF from 2D materials. Benzidine,
one raw material for COF, was enclosed in the CTAB micelles because
of the hydrophobic effect, and thus the target COF, which can be formed
immediately with the aid of p-toluenesulfonic acid, grew in a micelle
guided 3D form. The synthesized 3D COF showed a flower-like structure,
whereas the COF synthesized without CTAB showed a smooth structure.
The diameter of the 3D COFs showed direct correlations with CTAB concentrations.
Moreover, the CTAB modified COF also showed a dramatically improved
fluorescence property in comparison with that of normal COFs. The
synthesized 3D COF showed good adsorption performance for UV filters
and alkylphenols with recoveries ranged from 90.2% to 99.8%, and it
also showed good fluorescence response for Pb2+. The utility
of CTAB modified COF was verified in the enrichment of UV filters
and alkylphenols from food packaging material migrants.
A new permanently positively charged stable isotope labeling (SIL) agent pair, 4-(((2,5-dioxopyrrolidin-1yl)oxy)carbonyl)-N,N,N-trimethylbenzenaminium iodide(DPTBA) and its deuterated counterpart d 3 -DPTBA, was designed and synthesized. The SIL agents were applied to the liquid chromatography−tandem mass spectrometry analysis of alkylphenols. Light labeled standards and heavy labeled samples were mixed and analyzed simultaneously. Matrix effect which mainly occurred during the ionization process was minimized because of the identical ionization processes between samples and standards. Meanwhile, derivatization made alkylphenols be positively charged, and thus the sensitivity was enhanced. The limits of detection were in the range of 1.5−1.8 ng/L, and the limits of quantitation were in the range of 4.8−6.1 ng/L. The developed method was applied to analyze alkylphenols migrated from plastics to edible oils. The recoveries for all analytes were in the range of 88.6−95.3%, while the matrix effects for all analytes were in the range of 96.2−99.6%.
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