ACS Applied Materials & Interfaces,
Journal Year:
2023,
Volume and Issue:
15(7), P. 9307 - 9314
Published: Feb. 10, 2023
Porous
aromatic
frameworks
(PAFs)
with
rich
metal
coordination
sites
are
highly
effective
support
materials
for
gold
nanoparticles
(AuNPs),
which
would
not
only
prevent
AuNPs
agglomeration
but
also
facilitate
mass
transfer
during
the
catalytic
process.
In
this
work,
PAF-160,
-161,
and
-162
bearing
diphosphine
units
synthesized
via
Friedel–Crafts
alkylation
reaction
to
act
as
efficient
platforms
immobilization.
These
PAFs
possess
high
surface
areas
(up
655
m2
g–1)
together
excellent
stabilities,
different
linkage
lengths
between
P
centers
allow
more
scattered
accessible
coordination.
resultant
Au-PAFs,
uniform
sizes
stabilized
dispersedly.
The
performances
of
these
Au-PAFs
monitored
by
reduction
4-nitrophenol
(4-NP),
all
exhibit
activities
on
4-NP,
especially
Au-PAF-162
apparent
rate
constant
(kapp)
up
0.019
s–1.
Additionally,
reductions
various
nitroarenes
functional
groups
explored
can
convert
most
nitroaromatic
derivatives
corresponding
arylamines
conversions
99%,
in
mechanism
is
proposed.
Furthermore,
a
continuous
device
Au-PAF-160
catalyst
explored,
1-chloro-4-nitrobenzene,
2,6-dichoronitrobenzene
1-chloro-2,4-dinitrobenzene
into
amines
sequence
flow
experiments.
This
work
has
enriched
variety
porous
noble
immobilization
promotes
their
applications
heterogeneous
catalysis.
Chemical Reviews,
Journal Year:
2021,
Volume and Issue:
122(3), P. 3820 - 3878
Published: Dec. 23, 2021
With
the
development
of
advanced
electronic
devices
and
electric
power
systems,
polymer-based
dielectric
film
capacitors
with
high
energy
storage
capability
have
become
particularly
important.
Compared
polymer
nanocomposites
widespread
attention,
all-organic
polymers
are
fundamental
been
proven
to
be
more
effective
choices
in
process
scalable,
continuous,
large-scale
industrial
production,
leading
many
applications.
In
past
decade,
efforts
intensified
this
field
great
progress
newly
discovered
polymers,
production
technologies,
extension
toward
emerging
computational
strategies.
This
review
summarizes
recent
based
on
conventional
as
well
heat-resistant
materials
focus
strategies
enhance
properties
performances.
The
key
parameters
such
constant,
loss,
breakdown
strength,
density,
charge-discharge
efficiency,
thoroughly
studied.
addition,
applications
computer-aided
calculation
including
density
functional
theory,
machine
learning,
genome
rational
design
performance
prediction
dielectrics
reviewed
detail.
Based
a
comprehensive
understanding
developments,
guidelines
prospects
for
future
proposed.
Advanced Materials,
Journal Year:
2020,
Volume and Issue:
32(28)
Published: June 2, 2020
Nanostructures
derived
from
zeolitic-imidazole
frameworks
(ZIFs)
gain
much
interest
in
bifunctional
oxygen
electrocatalysis.
However,
they
are
not
satisfied
well
for
long-life
rechargeable
zinc-air
batteries
due
to
the
limited
single
particle
morphology.
Herein,
preparation
of
an
interconnected
macroporous
carbon
matrix
with
a
well-defined
3D
architecture
by
pyrolysis
silica
templated
ZIF-67
assemblies
is
reported.
The
catalyst
assembled
battery
exhibits
high
power
density
221.1
mW
cm-2
as
excellent
stability
during
500
discharging/charging
cycles,
surpassing
that
commercial
Pt/C
battery.
synergistic
effect
structure
together
abundant
cobalt-nitrogen-carbon
active
sites
justify
electrocatalytic
activity
and
performance.
Considering
advanced
nanostructures
performance,
as-synthesized
hybrid
would
be
promising
other
energy
technologies.
This
work
may
also
provide
significant
concept
view
electrocatalysis
design
Advanced Functional Materials,
Journal Year:
2020,
Volume and Issue:
31(12)
Published: Dec. 6, 2020
Abstract
Direct
knitting
of
nucleophilic
arene
monomers
in
the
presence
electrophilic
cross‐linker,
like
formaldehyde
dimethyl
acetal,
is
proven
to
be
a
cost‐effective
and
versatile
method
for
synthesis
porous
organic
polymers.
The
resulting
hypercrosslinked
polymers
(HCPs)
are
featured
by
hierarchical
structure,
high
surface
area,
pore
volume.
Coordinating
functional
groups
can
easily
installed
with
this
into
rigid
aryl
network.
HCPs
has
therefore
been
widely
used
preparing
heterogeneous
solid
catalysts.
Wise
selection
rational
design
3D
structure
synergy
between
HCP
support
catalytically
active
species
often
lead
efficiency
tailor‐made
catalysts
without
sophisticated
operations.
On
account
all
these
excellent
properties,
enthusiasm
researchers
use
catalysis
increasing
rapidly.
This
review
documents
necessity,
feasibility,
great
contributions
using
as
invaluable
tools
research,
summarizes
state
art
chemistry.
Similar
type
obtained
one‐step
Scholl
reaction
also
included
review.
Advanced Functional Materials,
Journal Year:
2021,
Volume and Issue:
31(45)
Published: Aug. 7, 2021
Abstract
Oxygen
reduction
reaction
(ORR)
is
an
essential
process
for
sustainable
energy
supply
and
sufficient
chemical
production
in
modern
society.
Single‐atom
catalysts
(SACs)
exhibit
great
potential
on
maximum
atomic
efficiency,
high
ORR
activity,
stability,
making
them
attractive
candidates
pursuing
next‐generation
catalysts.
Despite
substantial
efforts
being
made
building
diversiform
single‐atom
active
sites
(SAASs),
the
performance
of
obtained
still
unsatisfactory.
Fortunately,
microenvironment
regulation
SACs
provides
opportunities
to
improve
activity
selectivity
ORR.
In
this
review,
first,
mechanism
pathways
N‐coordinated
SAAS,
electrochemical
evaluation,
characterization
SAAS
are
displayed.
addition,
recent
developments
tuning
systematically
summarized,
especially,
strategies
modulation
introduced
detail
boosting
intrinsic
4e
−
/2e
selectivity.
Theoretical
calculations
cutting‐edge
techniques
united
discussed
fundamental
understanding
synthesis–construction–performance
correlations.
Furthermore,
their
comprehensively
overviewed
acquire
outstanding
SACs.
Lastly,
by
proposing
perspectives
remaining
challenges
infant
engineering,
future
directions
other
analogous
procedures
pointed
out.
Journal of the American Chemical Society,
Journal Year:
2021,
Volume and Issue:
143(37), P. 15453 - 15461
Published: Sept. 10, 2021
Ligands
are
the
most
commonly
used
means
to
control
regioselectivity
of
organic
reactions.
It
is
very
important
develop
new
regioselective
methods
for
synthesis.
In
this
study,
we
designed
and
synthesized
a
single-atomic-site
catalyst
(SAC),
namely,
Cu1-TiC,
with
strong
electronic
metal–support
interaction
(EMSI)
effects
by
studying
various
reaction
mechanisms.
π
cloud
back-donation
alkyne
on
metal
catalytic
intermediate
was
enhanced
during
using
transient
electron-rich
characteristics.
way,
achieved
highly
linear-E-type
conversion
electronically
unbiased
alkynes
completely
avoided
formation
branched
isomers
(ln:br
>100:1,
TON
up
612,
3
times
higher
than
previously
recorded).
The
structural
elements
SACs
were
following
requirements
synthesis
mechanism.
Every
element
in
played
an
role
This
demonstrated
that
EMSI,
which
normally
thought
be
responsible
improvement
efficiency
durability
heterogeneous
catalysis,
now
first
shows
exciting
potential
regulating
homogeneous
catalysis.
Angewandte Chemie International Edition,
Journal Year:
2020,
Volume and Issue:
60(8), P. 4125 - 4132
Published: Nov. 17, 2020
Abstract
The
valorization
of
carbon
dioxide
(CO
2
)
to
fine
chemicals
is
one
the
most
promising
approaches
for
CO
capture
and
utilization.
Herein
we
demonstrated
a
series
porous
organometallic
polymers
could
be
employed
as
highly
efficient
recyclable
catalysts
this
purpose.
Synergetic
effects
specific
surface
area,
iridium
content,
adsorption
capability
are
crucial
achieve
excellent
selectivity
yields
towards
N‐formylation
diverse
amines
with
H
under
mild
reaction
conditions
even
at
20
ppm
catalyst
loading.
Density
functional
theory
calculations
revealed
not
only
redox‐neutral
catalytic
pathway
but
also
new
plausible
mechanism
incorporation
key
intermediate
formic
acid
via
proton‐relay
process.
Remarkably,
record
turnover
number
(TON=1.58×10
6
was
achieved
in
synthesis
N,N‐dimethylformamide
(DMF),
solid
can
reused
up
12
runs,
highlighting
their
practical
potential
industry.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
61(26)
Published: April 4, 2022
Polymer
photocatalysts
have
received
growing
attention
in
recent
years
for
photocatalytic
hydrogen
production
from
water.
Most
studies
report
with
sacrificial
electron
donors,
which
is
unsuitable
large-scale
energy
production.
Here
we
show
that
the
palladium/iridium
oxide-loaded
homopolymer
of
dibenzo[b,d]thiophene
sulfone
(P10)
facilitates
overall
water
splitting
to
produce
stoichiometric
amounts
H
Chemical Society Reviews,
Journal Year:
2021,
Volume and Issue:
50(24), P. 13559 - 13586
Published: Jan. 1, 2021
Though
N-heterocyclic
carbenes
(NHCs)
have
emerged
as
diverse
and
powerful
discrete
functional
molecules
in
pharmaceutics,
nanotechnology,
catalysis
over
decades,
the
heterogenization
of
NHCs
their
precursors
for
broader
applications
porous
materials,
like
metal-organic
frameworks
(MOFs),
coordination
polymers
(PCPs),
covalent-organic
(COFs),
organic
(POPs),
organometallic
cages
(POMCs)
was
not
extensively
studied
until
last
ten
years.
By
de
novo
or
post-synthetic
modification
(PSM)
methods,
myriads
containing
building
blocks
were
designed
integrated
into
MOFs,
PCPs,
COFs,
POPs
POMCs
to
form
various
structures
porosities.
Functionalisation
with
significantly
expands
scope
potential
materials
by
tuning
pore
surface
chemical/physical
properties,
providing
active
sites
binding
guest
substrates
realizing
recyclability.
In
this
review,
we
summarise
discuss
recent
progress
on
synthetic
structural
features,
promising
functionalised
materials.
At
end,
a
brief
perspective
encouraging
future
prospects
challenges
contemporary
field
is
presented.
This
review
will
serve
guide
researchers
design
synthesize
more
novel
precursors.