Advanced Materials,
Год журнала:
2024,
Номер
36(37)
Опубликована: Май 19, 2024
Abstract
The
conversion
of
carbon
dioxide
(CO
2
)
into
value‐added
chemicals
with
two
or
more
carbons
(C
2+
is
a
promising
strategy
that
cannot
only
mitigate
anthropogenic
CO
emissions
but
also
reduce
the
excessive
dependence
on
fossil
feedstocks.
In
recent
years,
atomically
dispersed
metal
catalysts
(ADCs),
including
single‐atom
(SACs),
dual‐atom
(DACs),
and
single‐cluster
(SCCs),
emerged
as
attractive
candidates
for
fixation
reactions
due
to
their
unique
properties,
such
maximum
utilization
active
sites,
tunable
electronic
structure,
efficient
elucidation
catalytic
mechanism,
etc.
This
review
provides
an
overview
significant
progress
in
synthesis
characterization
ADCs
utilized
photocatalytic,
electrocatalytic,
thermocatalytic
toward
high‐value
C
compounds.
To
provide
insights
designing
chemical
originating
from
,
key
factors
influence
activity
selectivity
are
highlighted.
Finally,
relevant
challenges
opportunities
discussed
inspire
new
ideas
generation
‐based
products
over
ADCs.
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(49), С. 26783 - 26790
Опубликована: Ноя. 28, 2023
The
electroreduction
of
CO2
into
value-added
liquid
fuels
holds
great
promise
for
addressing
global
environmental
and
energy
challenges.
However,
achieving
highly
selective
yielding
multi-carbon
oxygenates
through
the
electrochemical
reduction
reaction
(eCO2RR)
is
a
formidable
task,
primarily
due
to
sluggish
asymmetric
C-C
coupling
reaction.
In
this
study,
novel
metal-organic
framework
(CuSn-HAB)
with
unprecedented
heterometallic
Sn···Cu
dual
sites
(namely,
pair
SnN2O2
CuN4
bridged
by
μ-N
atoms)
was
designed
overcome
limitation.
CuSn-HAB
demonstrated
an
impressive
Faradic
efficiency
(FE)
56(2)%
eCO2RR
alcohols,
current
density
68
mA
cm-2
at
low
potential
-0.57
V
(vs
RHE).
Notably,
no
significant
degradation
observed
over
continuous
35
h
operation
specified
density.
Mechanistic
investigations
revealed
that,
in
comparison
copper
site,
site
exhibits
higher
affinity
oxygen
atoms.
This
enhanced
plays
pivotal
role
facilitating
generation
key
intermediate
*OCH2.
Consequently,
compared
homometallic
Cu···Cu
(generally
ethylene
product),
were
proved
be
more
thermodynamically
favorable
between
*CO
*OCH2,
leading
formation
*CO-*OCH2,
which
ethanol
product.
Abstract
Hydrogen‐bonded
organic
frameworks
(HOFs)
are
emerging
porous
materials
that
show
high
structural
flexibility,
mild
synthetic
conditions,
good
solution
processability,
easy
healing
and
regeneration,
recyclability.
Although
these
properties
give
them
many
potential
multifunctional
applications,
their
unstable
due
to
the
presence
of
only
weak
reversible
hydrogen
bonds.
In
this
work,
development
history
synthesis
methods
HOFs
reviewed,
categorize
design
concepts
strategies
improve
stability.
More
importantly,
significant
latest
HOF‐related
research
for
addressing
energy
environmental
issues,
work
discusses
advances
in
storage
conversion,
substance
generation
isolation,
detection
degradation
transformation,
biological
applications.
Furthermore,
a
discussion
coupling
orientation
HOF
cross‐cutting
fields
environment
is
presented
first
time.
Finally,
current
challenges,
opportunities,
advance
applications
discussed.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 10, 2025
Abstract
Reducing
carbon
dioxide
（CO
2
）to
high‐value
products
using
green
renewable
energy
is
a
promising
approach
for
addressing
and
greenhouse
effect
issues.
Consequently,
electrocatalytic
CO
reduction
reaction
(CO
RR)
technology
has
become
current
research
hotspot.
Since
the
discovery
of
high
activity
selectivity
copper
in
RR,
atomically
dispersed
Cu
catalysts
have
garnered
widespread
attention
due
to
their
efficient
atom
utilization,
unique
electronic
structure,
outstanding
catalytic
performance.
However,
great
challenge
remains
providing
rational
catalyst
design
principles
achieve
regulation
product
distribution.
A
clear
understanding
materials
an
in‐depth
interpretation
mechanism
as
well
elucidation
strategy
progress
toward
different
are
keys
building
solving
above
problem.
Therefore,
this
review
starts
with
introduction
advanced
characterization
techniques
reveal
structure
mechanisms.
Then,
various
optimization
strategies
applications
producing
targeted
summarized
discussed.
Finally,
perspectives
on
RR
field
future
development
offered.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 10, 2025
The
electrochemical
coupling
of
CO2
and
NO3–
on
copper-based
catalysts
presents
a
sustainable
strategy
for
urea
production
while
simultaneously
addressing
wastewater
denitrification.
However,
the
inefficient
random
adsorption
copper
surface
limits
interaction
key
carbon
nitrogen
intermediates,
thereby
impeding
efficient
C–N
coupling.
In
this
study,
we
demonstrate
that
residual
lattice
oxygen
in
oxide-derived
nanosheets
(OL-Cu)
can
effectively
tune
electron
distribution,
thus
activating
neighboring
atoms
generating
electron-deficient
(Cuδ+)
sites.
These
Cuδ+
sites
enhance
stabilize
*CO
which
enables
directional
at
adjacent
This
mechanism
shortens
pathway
achieves
yield
up
to
298.67
mmol
h–1
g–1
−0.7
V
versus
RHE,
with
an
average
Faradaic
efficiency
31.71%
high
current
density
∼95
mA
cm–2.
situ
spectroscopic
measurements
confirmed
formation
tracked
evolution
intermediates
(i.e.,
*CO,
*NO,
*OCNO,
*NOCONO)
during
synthesis.
Density
functional
theory
calculations
revealed
promote
coadsorption
*NO3,
as
well
*OCNO
significantly
improving
kinetics.
study
underscores
critical
role
facilitating
selectivity.
Catalysts,
Год журнала:
2025,
Номер
15(3), С. 199 - 199
Опубликована: Фев. 20, 2025
The
electroreduction
of
CO2
(CO2RR)
is
a
promising
and
environmentally
sustainable
approach
to
closing
the
carbon
cycle.
However,
achieving
high
activity
selectivity
for
multicarbon
(C2₊)
products
remains
significant
challenge
due
complexity
reaction
pathways.
In
this
study,
porous
carbon-supported
copper
catalysts
(CuHCS)
with
pore
sizes
120
nm
(CuHCS120)
500
(CuHCS500)
were
synthesized
tailor
microenvironment
at
electrode–electrolyte
interface
enhance
product
selectivity.
CuHCS120
achieved
maximum
faradaic
efficiency
(FE)
C2₊
46%,
double
that
CuHCS500
(23%).
contrast,
showed
higher
FE
CO
(36%)
compared
(14%)
same
potential.
In-depth
ex
situ
in
investigations
revealed
smaller
pores
promote
enrichment
adsorption
*CO
intermediates,
thereby
enhancing
C–C
coupling
formation
products.
These
findings
underscore
critical
role
structural
confinement
modulating
catalytic
provide
valuable
insights
rational
design
advanced
CO2RR.
