Environmental Science & Technology,
Год журнала:
2023,
Номер
57(38), С. 14482 - 14492
Опубликована: Сен. 12, 2023
It
is
critical
to
discover
a
non-noble
metal
catalyst
with
high
catalytic
activity
capable
of
replacing
palladium
in
electrochemical
reduction.
In
this
work,
highly
efficient
single-atom
Co-N/C
was
synthesized
metal-organic
frameworks
(MOFs)
as
precursor
for
dehalogenation.
X-ray
absorption
spectroscopy
(XAS)
revealed
that
exhibited
Co-N4
configuration,
which
had
more
active
sites
and
faster
charge-transfer
rate
thus
enabled
the
removal
florfenicol
(FLO)
at
wide
pH,
achieving
constant
3.5
2.1
times
N/C
commercial
Pd/C,
respectively.
The
defluorination
dechlorination
efficiencies
were
67.6
95.6%,
respectively,
extremely
low
Co
leaching
(6
μg
L-1),
energy
consumption
(22.7
kWh
kg-1),
turnover
frequency
(TOF)
(0.0350
min-1),
demonstrating
excellent
dehalogenation
performance.
Spiking
experiments
density
functional
theory
(DFT)
verified
site
lowest
barrier
forming
atomic
hydrogen
(H*)
(ΔGH*).
Capture
experiments,
electron
paramagnetic
resonance
(EPR),
tests,
situ
Fourier
transform
infrared
(FTIR)
proved
H*
direct
transfer
responsible
Toxicity
assessment
indicated
FLO
toxicity
decreased
significantly
after
This
work
develops
broad
application
prospects
electrocatalytic
Advanced Functional Materials,
Год журнала:
2023,
Номер
33(43)
Опубликована: Июнь 27, 2023
Abstract
Shuttle
effect
and
sluggish
redox
kinetics
of
sulfur
species
still
hinder
the
practical
application
lithium‐sulfur
batteries
(LSBs).
Herein,
a
strategy
integrating
sub‐nano
catalysts
into
metal‐organic
framework
(MOF)
is
proposed
for
developing
efficient
host
to
tackle
these
issues.
The
designed
MOF
(MOF‐TOC)
endowed
with
TiO
clusters
(TOCs)
in
mesopores
can
act
as
an
reaction
chamber
LSBs.
Systematic
electrochemical
measurements
calculations
demonstrate
that
MOF‐TOC
trap
confine
lithium
polysulfides
(LiPSs)
via
strong
chemical
interaction.
Moreover,
highly
active
TOCs
isolated
different
nanopores
accelerate
bidirectional
through
d‐p
orbital
hybridization
species.
Benefiting
from
merits,
delivers
LSBs
remarkably
improved
areal
capacity
cycling
stability
at
high
loadings
lean
electrolytes.
This
work
gives
insight
rational
design
catalyst‐containing
hosts
will
shed
light
on
development
advanced
catalytic
high‐performance
Chemical Society Reviews,
Год журнала:
2024,
Номер
53(18), С. 9378 - 9418
Опубликована: Янв. 1, 2024
Organic
transformation
by
light-driven
catalysis,
especially,
photocatalysis
and
photothermal
denoted
as
photo(thermal)
is
an
efficient,
green,
economical
route
to
produce
value-added
compounds.
In
recent
years,
owing
their
diverse
structure
types,
tunable
pore
sizes,
abundant
active
sites,
metal-organic
framework
(MOF)-based
catalysis
has
attracted
broad
interest
in
organic
transformations.
this
review,
we
provide
a
comprehensive
systematic
overview
of
MOF-based
for
First,
the
general
mechanisms,
unique
advantages,
strategies
improve
performance
MOFs
are
discussed.
Then,
outstanding
examples
transformations
over
introduced
according
reaction
type.
addition,
several
representative
advanced
characterization
techniques
used
revealing
charge
kinetics
intermediates
presented.
Finally,
prospects
challenges
field
proposed.
This
review
aims
inspire
rational
design
development
materials
with
improved
catalysis.
ACS Catalysis,
Год журнала:
2024,
Номер
14(3), С. 1432 - 1442
Опубликована: Янв. 12, 2024
Defect-rich
Pd/TiO2
catalysts
are
intensively
adopted
in
heterogeneous
hydrogenation
reactions;
however,
the
complexity
of
defect
structure
makes
it
difficult
to
precisely
identify
which
Pd-defect
combination
dominates
catalytic
activity.
Herein,
defective
TiO2
nanoflakes
with
tunable
ratios
Vo
Ti3+
defects
were
synthesized
and
used
construct
Pd–Vo
Pd–Ti3+
active
sites
after
loading
Pd
investigate
role
regulating
structural
properties
catalysts.
Combining
experimental
results
theoretical
calculations,
we
reveal
that
both
act
as
electron
donors
for
induce
strong
metal–support
interaction.
When
compared
defect,
behaves
more
significantly
donates
electrons,
causing
species
on
be
better
dispersed
rich
electrons.
These
unique
features
endow
centers
enhanced
adsorption–activation
ability
toward
C═C
H2
well
reduced
energy
barrier
rate-limiting
step,
thus
improving
intrinsic
The
site
manifests
a
high
turnover
frequency
348
h–1
degree
97%
styrene–butadiene–styrene,
outperforms
(254
78%)
nanoparticle
(217
53%).
This
work
provides
deep
insight
into
metal
sites,
can
guide
development
high-performance
versatile
applications.
Abstract
The
chemical/physical
properties
and
reliable
performance
of
nanoporous
materials
are
strongly
influenced
by
the
particle
size
corresponding
distribution.
Among
many
types
MOFs,
ZIF‐8,
is
still
widely
used
studies
have
been
conducted
to
control
uniformity
ZIF‐8
using
surfactants
organic
solvents.
However,
use
solvents
process
expensive
may
cause
environmental
pollution.
For
first
time,
in
this
paper,
a
surfactant‐free,
size‐controllable,
scalable
green
synthesis
method
particles
reported
four
reaction
parameters
(temperature,
concentration,
pouring
reactant
ratio)
that
affect
formation
nuclei
growth
crystals.
as‐synthesized
nanoparticles
show
great
controllable
sizes
wide
range
147–915
nm.
In
addition,
2
L
large‐scale
with
narrow
distribution
developed
finely
tuned
water
without
any
additives.
To
demonstrate
efficient
utilization
nanopores
according
distribution,
an
adsorption
test
on
nanoparticles.
This
study
will
support
size‐controlled
their
composites
for
achieving
high
emerging
applications.
Chemical Reviews,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 18, 2025
The
electrocatalytic
technique,
as
an
efficient
energy
storage
and
conversion
technology,
has
attracted
significant
attention
to
address
exhaustion
environmental
pollution.
Usually,
the
activity
selectivity
of
reactions
are
largely
dominated
by
dynamic
process
occurring
on
electrocatalysts.
Therefore,
high-performance
electrocatalysts,
which
can
dominate
pathway
barrier
reactions,
great
significance
for
advancement
technique.
Metal-organic
frameworks
(MOFs),
emerging
crystalline
porous
materials,
present
structural
component
advantages
including
well-defined
structure,
high
surface
area,
large
porosity,
diverse
components,
easy
tailorability,
demonstrating
fantastic
potential
precise
fabrication
In
this
Review,
strategies
in
electrocatalysts
based
MOF-related
materials
specifically
introduced
from
aspects
catalytic
site
design
microenvironment
modulation
around
sites.
Furthermore,
representative
progress
achieved
various
applications
employing
MOF-based
is
systematically
summarized,
with
special
emphasis
MOFs
performance
optimization.
Finally,
remaining
challenges
future
perspectives
further
highlighted.
Advanced Functional Materials,
Год журнала:
2023,
Номер
33(40)
Опубликована: Май 31, 2023
Abstract
The
tailored
design
of
hollow
mesoporous
metal−organic
framework
(MOF)
single
crystals
to
realize
the
unimpeded
mass
transport
and
long‐range
carrier
migration
for
advanced
photoelectric
applications
is
attractive
while
being
a
major
challenge.
Here,
kinetically
mediated
micelle
assembly
strategy
presented
synthesize
UiO‐66(Ce)
in
1,3,5‐trimethylbenzene
(TMB)‐H
2
O
emulsion
system
with
Pluronic
F127/P123
as
dual
surfactants.
This
synthesis
features
employment
modulator
acetic
acid,
which
can
coordinate
growth
kinetics
MOFs,
allowing
nucleation
MOF
on
block
polymer
micelles
transforming
self‐assembly
polymer/MOF
composite
monomicelles
from
water
TMB/H
interface
aggregation
oriented
attachment,
thus
ensuring
formation
crystals.
Moreover,
precise
control
cavity
diameter
≈0
≈600
nm,
mesopore
structure
close
radial
dendritic
be
achieved
by
tuning
amount
TMB
ratio
F127/P123.
As
result,
large
mesopores
(≈25
nm)
high
surface
area
(≈1061
m2
g)
exhibit
excellent
photocatalytic
performance
H
generation
owing
enhanced
permeability
suppressed
electron‐hole
combination.
