Chemoselective hydrogenation of C=C, C=O and C=N bonds in α,β-unsaturated ketones, aldehydes and imines is accomplished at room temperature (27 oC) using the well-defined Mn(I) catalyst and 5.0 bar H2....
A heterogeneous Pd-NPMO hybrid-silica
catalyst is synthesized and
its application for aqueous phase selective hydrogenation of phenol
to cyclohexanone at near ambient temperature (40 °C) and under
atmospheric hydrogen pressure is demonstrated. The homogeneously distributed
Pd nanoparticles on N-bridged hybrid mesoporous organosilica showed
remarkable activity and selectivity for cyclohexanone compared to
the unmodified Pd-SBA-15 catalyst. Control experiments strongly claim
the role of nitrogen domains in the organic framework of hybrid silica
support in stabilizing small Pd nanoparticles and possibly modifying
the Pd sites responsible for catalysis to activate the substrate molecules
in water. The hybrid silica catalyst was stable and reused several
times without any significant drop-in activity, proving the heterogeneity
of the bifunctional Pd catalyst. Based on the density functional theory
study and experimental interventions, a possible reaction mechanism
for the low-temperature phenol hydrogenation explaining the role of
organic domains in the hybrid-silica framework is proposed.
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