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.