ACS Materials Letters,
Год журнала:
2024,
Номер
7(1), С. 229 - 249
Опубликована: Дек. 16, 2024
Given
the
increasingly
severe
global
climate
change
and
energy
crisis,
conversion
of
carbon
dioxide
(CO2)
into
very
valuable
chemicals
has
been
proposed
as
an
attractive
solution.
The
electrocatalytic
CO2
reduction
reaction
(eCO2RR)
represents
a
remarkably
efficient
pathway
for
reducing
under
mild
conditions.
Metal
cluster-based
crystalline
materials
(MCMs)
have
garnered
significant
interest
in
area
CO2RR
because
their
elevated
concentration
active
sites,
tunable
backbone
structures,
excellent
stability.
These
enable
precise
control
metal
valence
states
charge
transfer
pathways,
offering
variety
pathways
CO2RR.
Herein,
we
examine
utilization
MCMs
eCO2RR
recent
years.
We
cover
fundamental
principles
reduction,
synthesis
approaches
these
materials,
connection
between
structural
characteristics
catalytic
performance.
Additionally,
paper
delves
challenges
opportunities
presented
by
enhancing
efficiency
selectivity.
aim
to
provide
researchers
with
new
perspective
on
field
eCO2RR,
thereby
improving
understanding
relationship
structure
Ultimately,
this
work
seeks
advance
technology
contributing
significantly
sustainable
production
mitigation
greenhouse
gas
emissions.
The
construction
of
coupled
electrolysis
systems
utilizing
renewable
energy
sources
for
electrocatalytic
nitrate
reduction
and
sulfion
oxidation
reactions
(NO3RR
SOR),
is
considered
a
promising
approach
environmental
remediation,
ammonia
production,
sulfur
recovery.
Here,
simple
chemical
dealloying
method
reported
to
fabricate
hierarchical
porous
multi-metallic
spinel
MFe2O4
(M═Ni,
Co,
Fe,
Mn)
dual-functional
electrocatalysts
consisting
Mn-doped
NiFe2O4/CoFe2O4
heterostructure
networks
Ni/Co/Mn
co-doped
Fe3O4
nanosheet
networks.
excellent
NO3RR
with
high
NH3
Faradaic
efficiency
95.2%
at
-0.80
V
versus
reversible
hydrogen
electrode
(vs
RHE)
yield
rate
608.9
µmol
h-1
cm-2
-1.60
vs
RHE,
impressive
SOR
performance
(100
mA
[email protected]
achieved
MFe2O4.
Key
intermediates
such
as
*NO,
*NH2,
are
identified
in
the
process
by
situ
Fourier
transform
infrared
spectroscopy
(in
FTIR).
MFe2O4-assembled
two-electrode
coupling
system
(NO3RR||SOR)
shows
an
ultra-low
cell
voltage
1.14
10
cm-2,
much
lower
than
NO3RR||OER
(oxygen
evolution
reaction,
[email protected]
V),
simultaneously
achieving
two
expected
targets
value-added
generation
recovery,
also
demonstrating
durability
18
h.
This
work
demonstrates
great
potential
ferrite-based
catalysts
remediation.
Abstract
Seawater
splitting
is
one
of
the
desirable
techniques
for
producing
green
hydrogen
from
vast
natural
resource.
Several
reports
about
designing
and
fabricating
efficient
electrocatalysts
to
boost
oxygen
evolution
reaction
have
been
published.
However,
they
mainly
focus
on
electrodes,
electrocatalysts,
cost,
system
stability.
This
article
presents
an
overview
seawater
by
highlighting
most
challenging
issues
that
complicate
electrolysis,
such
as
durability,
guide
future
research
in
this
important
area.
The
strategy
launch
life
cycle
assessments
described
evaluate
short
long‐term
impacts.
Finally,
current
challenges
prospective
solutions
are
discussed.
Abstract
Seawater
electrocatalysis
is
urgently
needed
for
various
energy
storage
and
conversion
systems.
However,
the
adsorption
of
chloride
ions
(Cl
−
)
to
active
sites
can
degrade
oxygen
reduction
reaction
(ORR)
activity
stability,
thus
reducing
catalytic
performance.
In
this
paper,
a
curved
FeN
4
single
atomic
structure
designed
by
utilizing
curvature
engineering,
which
turns
harmful
Cl
into
benefit
on
Fe
site
that
changes
rate
determining
step
ORR
reduces
overall
barrier
according
density
functional
theory
(DFT)
calculation.
Experimental
studies
reveal
prepared
highly‐curved
single‐atom
iron
catalyst
(HC‐Fe
SA
exhibits
excellent
in
different
electrolytes,
with
half‐wave
potentials
0.90
V
0.1
M
KOH,
simulated
seawater,
0.75
natural
respectively.
This
work
opens
up
an
avenue
synthesis
high‐performance
seawater‐based
catalysts
through
regulating
local
curvature.
The
predominant
product
of
CO
electroreduction
(COER)
is
often
acetate,
with
the
Faradaic
efficiency
(FE)
for
ethanol
usually
falling
below
50%.
Herein,
we
propose
a
unique
strategy
to
enhance
selectivity
in
COER,
shifting
it
from
acetate
predominance
toward
generation
via
alloying
atomic
manganese
(Mn)
atoms
face-centered
cubic
(FCC)
copper
(Cu)
catalyst.
By
optimizing
ratio
Mn
Cu,
observe
an
impressive
enhancement
8.8-fold
ethanol-to-acetate
FE
optimal
Mn3Cu97
alloy
compared
unalloyed
FCC-phase
Cu.
demonstrates
remarkable
nearly
70%
at
high
current
density
600
mA
cm-2
membrane
electrode
assembly
electrolyzer.
Further
theoretical
analysis
reveals
that
atomically
dispersed
generate
synergistic
active
sites
and
modulate
adsorption
strength
critical
intermediates
relevant
synthesis,
thereby
facilitating
transition
pathway
pathway.
