Discovering
and constructing novel and fancy structures is the
goal of many supramolecular chemists. In this work, we propose an
assembly strategy based on the synergistic effect of coordination
and covalent interactions to construct a set of octahedral supramolecular
cages and adjust their degree of distortion. Our strategy innovatively
utilizes the addition of sulfur atoms of a metal sulfide synthon,
[Et4N][Tp*WS3] (A), to an alkynyl
group of a pyridine-containing linker, resulting in a novel vertex
with low symmetry, and of Cu(I) ions. By adjusting the length of the
linker and the position of the reactive alkynyl group, the control
of the deformation degree of the octahedral cages can be realized.
These supramolecular cages exhibit enhanced third-order nonlinear
optical (NLO) responses. The results offer a powerful strategy to
construct novel distorted cage structures as well as control the degree
of distortion of supramolecular geometries.
Hydrogenated nitrogen heterocyclic compounds play a critical
role
in the pharmaceutical, polymer, and agrochemical industries. Recent
studies on partial hydrogenation of nitrogen heterocyclic compounds
have focused on costly and toxic precious metal catalysts. As an important
class of main-group catalysts, frustrated Lewis pairs (FLPs) have
been widely applied in catalytic hydrogenation reactions. In principle,
the combination of FLPs and metal–organic framework (MOF) is
anticipated to efficiently enhance the recyclability performance of
FLPs; however, the previously studied MOF-FLPs showed low reactivity
in the hydrogenation of N-heterocycles compounds.
Herein, we offer a novel P/B type MOF-FLP catalyst that was achieved
via a solvent-assisted linker incorporation approach to boost catalytic
hydrogenation reactions. Using hydrogen gas under moderate pressure,
the proposed P/B type MOF-FLP can serve as a highly efficient heterogeneous
catalyst for selective hydrogenation of quinoline and indole to tetrahydroquinoline
and indoline-type drug compounds in high yield and excellent recyclability.
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