Angewandte Chemie,
Journal Year:
2024,
Volume and Issue:
136(42)
Published: July 25, 2024
Abstract
Precisely
controlling
the
microstructure
of
supported
metal
catalysts
and
regulating
metal‐support
interactions
at
atomic
level
are
essential
for
achieving
highly
efficient
heterogeneous
catalysts.
Strong
interaction
(SMSI)
not
only
stabilizes
nanoparticles
improves
their
resistance
to
sintering
but
also
modulates
electrical
between
species
support,
optimizing
catalytic
activity
selectivity.
Therefore,
understating
formation
mechanism
SMSI
its
dynamic
evolution
during
chemical
reaction
scale
is
crucial
guiding
structural
design
performance
optimization
Recent
advancements
in
situ
transmission
electron
microscopy
(TEM)
have
shed
new
light
on
these
complex
phenomena,
providing
deeper
insights
into
dynamics.
Here,
research
progress
TEM
investigation
catalysis
systematically
reviewed,
focusing
dynamics,
reactions,
regulation
methods
SMSI.
The
significant
advantages
technologies
highlighted.
Moreover,
challenges
probable
development
paths
studies
provided.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(48)
Published: Sept. 3, 2024
Abstract
Intramolecular
charge
separation
driving
force
and
linkage
chemistry
between
building
blocks
are
critical
factors
for
enhancing
the
photocatalytic
performance
of
metal‐covalent
organic
framework
(MCOF)
based
photocatalyst.
However,
robust
achieving
both
simultaneously
has
yet
to
be
challenging
despite
ongoing
efforts.
Here
we
develop
a
fully
π‐conjugated
vinylene‐linked
multivariate
donor‐π‐acceptor
MCOF
(D‐π‐A,
termed
UJN‐1)
by
integrating
benzyl
cyanides
linker
with
multiple
functional
electron‐rich
triphenylamine
electron‐deficient
copper‐cyclic
trinuclear
units
(Cu‐CTUs)
moieties,
featuring
strong
intramolecular
force,
extended
conjugation
degree
skeleton,
abundant
active
sites.
The
incorporation
Cu‐CTUs
acceptor
electron‐withdrawing
ability
concomitantly
giant
can
efficiently
accelerate
photogenerated
electrons
transfer
from
Cu‐CTUs,
revealing
experiments
theoretical
calculations.
Benefiting
synergistically
effect
D‐π‐A
configuration
vinylene
linkage,
highly‐efficient
spatial
is
achieved.
Consequently,
UJN‐1
exhibits
an
excellent
CO
formation
rate
114.8
μmol
g
−1
in
4
h
without
any
co‐catalysts
or
sacrificial
reagents
under
visible
light,
outperforming
those
analogous
MCOFs
imine‐linked
(UJN‐2,
28.9
)
COF
Cu‐CTU
sites
(UJN‐3,
50.0
),
emphasizing
role
designing
novel
COFs‐based
