Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 16, 2024
Abstract
Synthesis
of
high‐loading
atomic‐level
dispersed
catalysts
for
highly
efficient
electrochemical
CO
2
reduction
reaction
(eCO
RR)
to
ethylene
(C
H
4
)
in
neutral
electrolyte
remain
challenging
tasks.
To
address
common
aggregation
issues,
a
host‐guest
strategy
is
employed,
by
using
metal‐azolate
framework
(
MAF‐4
with
nanocages
as
the
host
and
dinuclear
Cu(I)
complex
guest,
form
precursors
pyrolysis
into
series
nitrogen‐doped
porous
carbons
(NPCs)
varying
loadings
dual
copper
sites,
namely
NPC
‐Cu
‐21
(21.2
wt%),
‐11
(10.6
‐7
(6.9
wt%).
Interestingly,
loading
sites
increased
from
6.9
21.2
wt%,
partial
current
density
eCO
RR
yield
C
also
gradually
38.7
93.6
mA
cm
−2
.
In
0.1
m
KHCO
3
electrolyte,
at
−1.4
V
versus
reversible
hydrogen
electrode
vs
RHE),
exhibits
excellent
performance
Faradaic
efficiency
52%
180
Such
can
be
attributed
presence
ultrahigh‐loading
which
promotes
C─C
coupling
formation
products.
The
findings
demonstrate
confinement
effect
conducive
preparation
catalysts.
Chemical Society Reviews,
Год журнала:
2024,
Номер
53(10), С. 5149 - 5189
Опубликована: Янв. 1, 2024
This
review
summarizes
promising
strategies
including
the
design
of
catalysts
and
construction
coupled
electrocatalytic
reaction
systems,
aimed
at
achieving
selective
production
various
products
from
CO
2
electroreduction.
Nano-Micro Letters,
Год журнала:
2023,
Номер
15(1)
Опубликована: Июль 11, 2023
Electrochemical
carbon
dioxide
reduction
reaction
(CO2RR)
provides
a
promising
way
to
convert
CO2
chemicals.
The
multicarbon
(C2+)
products,
especially
ethylene,
are
of
great
interest
due
their
versatile
industrial
applications.
However,
selectively
reducing
ethylene
is
still
challenging
as
the
additional
energy
required
for
C-C
coupling
step
results
in
large
overpotential
and
many
competing
products.
Nonetheless,
mechanistic
understanding
key
steps
preferred
pathways/conditions,
well
rational
design
novel
catalysts
production
have
been
regarded
approaches
achieving
highly
efficient
selective
CO2RR.
In
this
review,
we
first
illustrate
CO2RR
(e.g.,
adsorption/activation,
formation
*CO
intermediate,
step),
offering
conversion
ethylene.
Then
alternative
pathways
conditions
competitive
products
(C1
other
C2+
products)
investigated,
guiding
further
development
generation.
Engineering
strategies
Cu-based
CO2RR-ethylene
summarized,
correlations
mechanism/pathways,
engineering
selectivity
elaborated.
Finally,
major
challenges
perspectives
research
area
proposed
future
practical
Abstract
Modifying
the
coordination
or
local
environments
of
single‐,
di‐,
tri‐,
and
multi‐metal
atom
(SMA/DMA/TMA/MMA)‐based
materials
is
one
best
strategies
for
increasing
catalytic
activities,
selectivity,
long‐term
durability
these
materials.
Advanced
sheet
supported
by
metal
atom‐based
have
become
a
critical
topic
in
fields
renewable
energy
conversion
systems,
storage
devices,
sensors,
biomedicine
owing
to
maximum
utilization
efficiency,
precisely
located
centers,
specific
electron
configurations,
unique
reactivity,
precise
chemical
tunability.
Several
offer
excellent
support
are
attractive
applications
energy,
medical
research,
such
as
oxygen
reduction,
production,
hydrogen
generation,
fuel
selective
detection,
enzymatic
reactions.
The
strong
metal–metal
metal–carbon
with
metal–heteroatom
(i.e.,
N,
S,
P,
B,
O)
bonds
stabilize
optimize
electronic
structures
atoms
due
interfacial
interactions,
yielding
activities.
These
provide
models
understanding
fundamental
problems
multistep
This
review
summarizes
substrate
structure‐activity
relationship
different
active
sites
based
on
experimental
theoretical
data.
Additionally,
new
synthesis
procedures,
physicochemical
characterizations,
biomedical
discussed.
Finally,
remaining
challenges
developing
efficient
SMA/DMA/TMA/MMA‐based
presented.
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.
Advanced Materials,
Год журнала:
2023,
Номер
35(52)
Опубликована: Ноя. 6, 2023
The
value-added
chemicals,
monoxide,
methane,
ethylene,
ethanol,
ethane,
and
so
on,
can
be
efficiently
generated
through
the
electrochemical
CO2
reduction
reaction
(eCO2
RR)
when
equipped
with
suitable
catalysts.
Among
them,
ethylene
is
particularly
important
as
a
chemical
feedstock
for
petrochemical
manufacture.
However,
despite
its
high
Faradaic
efficiency
achievable
at
relatively
low
current
densities,
substantial
enhancement
of
selectivity
stability
industrial
densities
poses
formidable
challenge.
To
facilitate
implementation
eCO2
RR
production,
it
imperative
to
identify
key
strategies
potential
solutions
comprehending
recent
advancements,
remaining
challenges,
future
directions.
Herein,
latest
innovative
catalyst
design
are
summarized
discussed,
starting
properties
catalysts
such
morphology,
crystalline,
oxidation
state,
defect,
composition,
surface
engineering.
review
subsequently
outlines
related
state-of-the-art
technologies
that
essential
in
driving
forward
into
practical
applications,
capture,
product
separation,
downstream
reactions.
Finally,
greenhouse
model
integrates
conversion,
storage,
utilization
proposed
present
an
ideal
perspective
direction
ethylene.
Abstract
Electrocatalysis
is
a
crucial
method
for
achieving
global
carbon
neutrality,
serving
as
an
essential
means
of
energy
conversion,
and
electrocatalyst
in
the
process
electrocatalysis.
Because
abundant
active
sites,
multi‐component
synergistic
effect
high‐entropy
materials
has
wide
application
prospect
field
Moreover,
due
to
special
structure
materials,
it
possible
obtain
almost
continuous
adsorption
distribution
by
regulating
composition,
which
attracted
extensive
attention
researchers.
This
paper
reviews
properties
types
including
alloys
compounds.
The
synthesis
strategies
are
systematically
introduced,
solid
phase
synthesis,
liquid‐phase
gas‐phase
classified
summarized.
electrocatalysis
summarized,
promotion
strategy
various
catalytic
reaction
processes
Finally,
current
progress
problems
encountered,
future
development
direction
reviewed.
It
emphasized
that
high
flux
density
functional
theory
calculation
guiding
catalyst
design
will
be
great
significance
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(48)
Опубликована: Авг. 22, 2024
Abstract
Thiolate‐protected
Cu
clusters
with
well‐defined
structures
and
stable
low‐coordinated
+
species
exhibit
remarkable
potential
for
the
CO
2
RR
are
ideal
model
catalysts
establishing
structure‐electrocatalytic
property
relationships
at
atomic
level.
However,
extant
employed
in
predominantly
yield
2e
−
products.
Herein,
two
4
(MMI)
8
(
t
BuS)
(MMI=2‐mercapto‐1‐methylimidazole)
prepared
to
investigate
synergistic
effect
of
adjacent
S
sites
on
RR.
can
reduce
deep‐reduced
products
a
91.0
%
Faradaic
efficiency
(including
53.7
CH
)
while
maintaining
stability.
Conversely,
shows
preference
C
2+
products,
achieving
maximum
FE
58.5
current
density
152.1
mA⋅cm
−2
.
In
situ
XAS
ex
XPS
spectra
reveal
preservation
during
RR,
extensively
enhancing
adsorption
capacity
*CO
intermediate.
Moreover,
kinetic
analysis
theoretical
calculations
confirm
that
facilitate
H
O
dissociation
into
*H
species,
which
directly
participate
protonation
process
*CHO.
This
study
highlights
important
role
Cu−S
dual
provides
mechanistic
insights
pathway
ACS Applied Materials & Interfaces,
Год журнала:
2024,
Номер
16(3), С. 3388 - 3395
Опубликована: Янв. 12, 2024
Synergistic
effects
have
been
applied
to
a
variety
of
hybrid
electrocatalysts
improve
their
activity
and
selectivity.
Understanding
the
synergistic
mechanism
is
crucial
for
rational
design
these
types
catalysts.
Here,
we
synthesize
MnCo
