Metal
organic framework (MOF) derivatives, porous N-doped carbons
(CN), can be used as catalyst carriers owing to their excellent structural
properties. The microstructures of MOF-derived carbon materials are
affected considerably by the atmosphere in which the parent MOFs are
pyrolyzed. In this study, a hierarchically porous N-doped carbon hybrid
of carbon nanotubes and a porous carbon framework (denoted CN-H) was
fabricated by pyrolysis in a H2/Ar atmosphere followed
by acid etching, and subsequently, a Pd@CN-H catalyst was synthesized
by the addition of Pd nanoparticles on the porous N-doped carbon support.
The pyrolysis atmosphere and etching treatment significantly affected
the morphology, specific surface area, meso/macropore ratio, and composition
of the porous N-doped carbon materials, as well as the catalytic properties
of the Pd@CN catalysts for the selective hydrogenation of phenol to
produce cyclohexanone. Nitrogen adsorption–desorption measurements
and inductively coupled plasma atomic absorption spectroscopy analyses
confirmed that pyrolysis in a H2/Ar atmosphere and acid
etching significantly increased the number of meso/macropores in Pd@CN-H,
thus enhancing the Pd loading and phenol adsorption. As a result of
the increased porosity, Pd loading, and phenol adsorption, the cyclohexanone
selectivity and phenol conversion were improved. Furthermore, the
as-fabricated Pd@CN-H catalyst displayed good reusability in recycling
tests. These results provide insights into the synthesis of MOF-derived
hybrid carbon materials and their possible utilization in catalysis.
Covalent organic frameworks (COFs) have emerged as an excellent support for heterogeneous catalysis due to their regular pore structure and high specific surface area. Herein, a series of porous TpPa-1 with different morphologies and structures were achieved by adjusting the ratio of water to acetic acid in the solvent-thermal process,
Zeolite imidazolate frameworks (ZIFs) derivatives, porous N-doped carbon (CN) materials, show outstanding performance when used as catalyst supports. The characteristics of ZIFs affect significantly the microstructure of CN. In this work, a series of CN materials were fabricated through direct pyrolysis of Zn/Co-ZIFs and Pd@ CN catalysts were achieved by loading Pd nanoparticles. The results underline that the Co content in Zn/Co-ZIFs influences considerably the properties of CN and the catalytic activity of Pd@CN for the phenol hydrogenation to cyclohexanone. N 2 adsorption−desorption, CO 2 -TPD, and ICP analyses confirm that the increase of Co in ZIFs can enhance significantly the mesoporous ratio of CN for improving the loading and dispersion of Pd and increase the basic sites of CN materials for improving the phenol adsorption. As a result, significantly enhanced phenol conversion with similar cyclohexanone selectivity is achieved. These findings provide deep insights for the fabrication of ZIF-derived CN materials and their applications in catalysis.
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