ACS Sustainable Chemistry & Engineering,
Год журнала:
2024,
Номер
12(16), С. 6093 - 6101
Опубликована: Март 12, 2024
The
electrocatalytic
CO2
reduction
reaction
(CO2RR)
to
produce
multicarbon
(C2+)
products
such
as
ethylene
(C2H4)
is
a
promising
method
achieve
carbon
neutrality,
but
it
very
difficult
due
the
high
activation
barrier
of
and
low
selectivity
CO2RR
especially
for
C2+
products.
Herein,
copper
single
atoms
(Cu-SAs)
were
confined
into
nanospace
an
iridium
porphyrin-based
metal–organic
framework
(Ir-PCN-222)
form
(MOF)
composite
(Cu-SAs@Ir-PCN-222-PA)
with
dual
active
sites
Ir-porphyrin
Cu-SAs
through
precoordination
confinement
strategy.
Catalytic
results
disclosed
that
Cu-SAs@Ir-PCN-222-PA
could
drive
C2H4
faradaic
efficiency
(FE)
(70.9%)
current
density
20.4
mA·cm–2.
When
H-cell
was
replaced
by
flow
cell,
be
increased
161
mA·cm–2
still
FE
(66.9%).
Mechanism
studies
suggested
in
Cu-SAs@Ir-PCN-222-PA-catalyzed
electroreduction
reaction,
CO
first
generated
on
then
moved
adsorbed
*CO
intermediate
nearby
Cu-SAs,
after
that,
C–C
coupling
process
carried
out
provide
product
C2H4.
This
work
offers
new
kind
MOF
electrocatalysts
generate
Energy & Environmental Science,
Год журнала:
2023,
Номер
16(7), С. 2759 - 2803
Опубликована: Янв. 1, 2023
The
catalytic
transformation
of
CO
2
into
valuable
fuels/chemicals
is
a
promising
and
economically
profitable
process
because
it
offers
an
alternative
toward
fossil
feedstocks
the
benefit
transforming
cycling
on
scale-up.
Advanced Materials,
Год журнала:
2023,
Номер
36(2)
Опубликована: Июль 13, 2023
Single-atom
catalysts
(SACs)
have
attracted
considerable
attention
in
heterogeneous
catalysis
because
of
their
well-defined
active
sites,
maximum
atomic
utilization
efficiency,
and
unique
unsaturated
coordinated
structures.
However,
effectiveness
is
limited
to
reactions
requiring
sites
containing
multiple
metal
atoms.
Furthermore,
the
loading
amounts
single-atom
must
be
restricted
prevent
aggregation,
which
can
adversely
affect
catalytic
performance
despite
high
activity
individual
The
introduction
nanoscale
particles
(NMPs)
into
SACs
(NMP-SACs)
has
proven
an
efficient
approach
for
improving
performance.
A
comprehensive
review
urgently
needed
systematically
introduce
synthesis,
characterization,
application
NMP-SACs
mechanisms
behind
superior
This
first
presents
classifies
different
through
NMPs
enhance
SACs.
It
then
summarizes
currently
reported
synthetic
strategies
state-of-the-art
characterization
techniques
NMP-SACs.
Moreover,
electro/thermo/photocatalysis,
reasons
are
discussed.
Finally,
challenges
perspectives
future
design
advanced
addressed.
ACS Catalysis,
Год журнала:
2023,
Номер
13(10), С. 6630 - 6640
Опубликована: Май 1, 2023
The
rational
construction
of
single-atom-modified
porous
metal–organic
frameworks
(MOFs)
for
efficient
CO2
photoconversion
is
a
promising
avenue,
yet
the
one
that
poses
significant
challenge.
In
this
study,
we
demonstrate
successful
Ni
single-atom-immobilized
ZIF-8
with
an
ordered
hierarchical
(macro–micro)
pore
structure
highly
photocatalytic
reduction
to
CO.
interpenetrated
macroporous
in
microporous
built
up
by
employing
polystyrene
(PS)
opal
as
hard
template,
while
high
stability
framework
achieved
through
double-solvent-induced
crystallization.
enables
rapid
mass
transport
and
strong
adsorption
CO2,
single
atoms
active
sites
electron-trapping
optimize
reaction
energy
hinder
competitive
H2
evolution.
As
result,
achieves
activity
4.2
mmol
g–1
h–1
CO
yield
electronic
selectivity
94%,
which
shows
47-fold
ZIF-8.
This
work
highlights
significance
constructing
MOFs
single-atom-active
improve
photoreduction
realizing
carbon
neutralization.
Advanced Materials,
Год журнала:
2023,
Номер
36(3)
Опубликована: Окт. 2, 2023
Abstract
It
is
very
important
to
understand
the
structure–performance
relationship
of
metal
catalysts
by
adjusting
microstructure
at
atomic
scale.
The
distance
has
an
essential
influence
on
composition
environment
active
atom,
which
a
key
factor
for
design
targeted
with
desired
function.
In
this
review,
we
discuss
and
summarize
strategies
changing
from
three
aspects
relate
their
effects
reactivity
catalysts.
First,
regulating
bond
length
between
coordination
atom
one
single‐atom
site
catalytic
performance
are
introduced.
lengths
affected
strain
effect
support
high‐shell
doping
can
evolve
during
reaction.
Next,
sites
discussed.
Due
space
matching
adsorption
electron
transport,
be
adjusted
shortening
distance.
addition,
arrangement
spacing
surface
atoms
nanocatalysts
studied.
Finally,
comprehensive
summary
outlook
given.
EcoEnergy,
Год журнала:
2023,
Номер
1(2), С. 248 - 295
Опубликована: Дек. 1, 2023
Abstract
In
the
advancing
world
of
graphene,
highly
anisotropic
2D
semiconductor
nanosheets,
notable
for
their
nanometer‐scale
thickness,
have
emerged
as
a
leading
innovation,
displaying
immense
potential
in
exploration
renewable
and
clean
energy
production.
These
garnered
significant
attention
from
researchers.
The
nanosheets
are
marked
by
extraordinary
electronic,
optical,
chemical
attributes,
positioning
them
attractive
foundational
components
heterogeneous
photocatalysts.
This
review
diligently
summarizes
both
seminal
work
ongoing
developments
pertaining
to
application
solar
within
context
photocatalysis.
We
begin
detailing
distinctive
properties
concentrating
on
pivotal
roles
augmenting
photocatalytic
efficiency,
explaining
intrinsic
mechanisms
that
govern
migration
rate
photogenerated
carriers
material's
surface.
Subsequently,
we
delineate
methods
employed
synthesize
typical
nanosheets.
alignment
with
overarching
objective
expanding
light
absorption
capacity
accelerating
charge
transfer,
also
examine
current
research
hybridization
techniques
involving
materials
varied
dimensions,
well
deployment
diverse
applications.
conclude
identifying
promising
avenues
challenges
await
further
this
burgeoning
field.
Advanced Materials,
Год журнала:
2023,
Номер
35(38)
Опубликована: Июнь 26, 2023
Constructing
Van
der
Waals
heterojunction
is
a
crucial
strategy
to
achieve
excellent
photocatalytic
activity.
However,
in
most
heterojunctions
synthesized
by
ex
situ
assembly,
electron
transfer
encounters
huge
hindrances
at
the
interface
between
two
components
due
large
spacing
and
potential
barrier.
Herein,
phosphate-bridged
of
cobalt
phthalocyanine
(CoPc)/tungsten
disulfide
(WS2
)
bridged
phosphate
(xCoPc-nPO4-
-WS2
designed
prepared
traditional
wet
chemistry
method.
By
introducing
small
molecule
into
CoPc
WS2
,
creates
an
"bridge",
resulting
compact
combination
eliminating
space
Therefore,
(PO4-
bridge
can
serve
as
efficient
channel
efficiently
transmit
photoelectrons
from
under
excited
states.
These
are
captured
catalytic
central
Co2+
subsequently
convert
CO2
molecules
CO
CH4
products,
achieving
17-fold
enhancement
on
3CoPc-0.6PO4-
sample
compared
that
pure
.
Introducing
"bridge"
create
provides
new
perspective
designing
photocatalysts
for
reduction
valuable
products.
Advanced Materials,
Год журнала:
2024,
Номер
36(21)
Опубликована: Фев. 7, 2024
Single-atom
nanozymes
(SAzymes)
showcase
not
only
uniformly
dispersed
active
sites
but
also
meticulously
engineered
coordination
structures.
These
intricate
architectures
bestow
upon
them
an
exceptional
catalytic
prowess,
thereby
captivating
numerous
minds
and
heralding
a
new
era
of
possibilities
in
the
biomedical
landscape.
Tuning
microstructure
SAzymes
on
atomic
scale
is
key
factor
designing
targeted
with
desirable
functions.
This
review
first
discusses
summarizes
three
strategies
for
their
impact
reactivity
biocatalysis.
The
effects
choices
carrier,
different
synthesis
methods,
modulation
first/second
shell,
type
number
metal
centers
enzyme-like
activity
are
unraveled.
Next,
attempt
made
to
summarize
biological
applications
tumor
therapy,
biosensing,
antimicrobial,
anti-inflammatory,
other
from
mechanisms.
Finally,
how
designed
regulated
further
realization
diverse
reviewed
prospected.
It
envisaged
that
comprehensive
presented
within
this
exegesis
will
furnish
novel
perspectives
profound
revelations
regarding
SAzymes.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(3), С. 2275 - 2285
Опубликована: Янв. 12, 2024
The
construction
of
structurally
well-defined
supramolecular
hosts
to
accommodate
catalytically
active
species
within
a
cavity
is
promising
way
address
catalyst
deactivation.
resulting
catalysts
can
significantly
improve
the
utilization
catalytic
sites,
thereby
achieving
highly
efficient
chemical
conversion.
In
this
study,
Co-metalated
phthalocyanine
(
