Abstract
Bismuth‐based
catalysts
are
effective
in
converting
carbon
dioxide
into
formate
via
electrocatalysis.
Precise
control
of
the
morphology,
size,
and
facets
bismuth‐based
is
crucial
for
achieving
high
selectivity
activity.
In
this
work,
an
efficient,
large‐scale
continuous
production
strategy
developed
a
porous
nanospheres
Bi
2
O
3
‐FDCA
material.
First‐principles
simulations
conducted
advance
indicate
that
(111)/(200)
help
reduce
overpotential
electrocatalytic
reduction
reaction
(ECO
RR).
Subsequently,
using
microfluidic
technology
molecular
to
precisely
adjust
amount
2,
5‐furandicarboxylic
acid,
nanomaterials
rich
successfully
synthesized.
Additionally,
morphology
significantly
increases
adsorption
capacity
active
sites
dioxide.
These
synergistic
effects
allow
stably
operate
90
h
flow
cell
at
current
density
≈250
mA
cm
−
,
with
average
Faradaic
efficiency
exceeding
90%.
The
approach
theoretically
guided
synthesis
finely
structured,
efficient
materials
ECO
RR
may
provide
valuable
references
chemical
engineering
intelligent
nanocatalysts.
Chemical Society Reviews,
Год журнала:
2024,
Номер
53(12), С. 6295 - 6321
Опубликована: Янв. 1, 2024
Developing
sophisticated
strategies
to
stabilize
oxidative
metal
catalysts
based
on
the
correlation
between
dynamic
oxidation
state
and
product
profile
is
favorable
for
efficient
electrochemical
CO
2
conversion.
Abstract
Doping
is
a
recognized
method
for
enhancing
catalytic
performance.
The
introduction
of
strains
common
consequence
doping,
although
it
often
overlooked.
Differentiating
the
impact
doping
and
strain
on
performance
poses
significant
challenge.
In
this
study,
Cu‐doped
Bi
catalysts
with
substantial
tensile
are
synthesized.
synergistic
effects
in
bismuth
result
remarkable
CO
2
RR
Under
optimized
conditions,
Cu
1/6
‐Bi
demonstrates
exceptional
formate
Faradaic
efficiency
(>95%)
maintains
over
90%
across
wide
potential
window
900
mV.
Furthermore,
delivers
an
industrial‐relevant
partial
current
density
−317
mA
cm
−2
at
−1.2
V
RHE
flow
cell,
while
maintaining
its
selectivity.
Additionally,
exhibits
long‐term
stability,
surpassing
120
h
−200
.
Through
experimental
theoretical
mechanistic
investigations,
has
been
determined
that
facilitates
adsorption
*CO
,
thereby
reaction
kinetics.
Moreover,
presence
dopants
further
diminishes
energy
barrier
formation
*OCHO
intermediate.
This
study
not
only
offers
valuable
insights
development
effective
through
but
also
establishes
correlations
between
lattice
strains,
properties
catalysts.
Environmental Science & Technology,
Год журнала:
2024,
Номер
58(25), С. 10881 - 10896
Опубликована: Июнь 11, 2024
One
of
the
most
promising
approaches
to
address
global
challenge
climate
change
is
electrochemical
carbon
capture
and
utilization.
Solid
electrolytes
can
play
a
crucial
role
in
establishing
chemical-free
pathway
for
CO2.
Furthermore,
they
be
applied
electrocatalytic
CO2
reduction
reactions
(CO2RR)
increase
utilization,
produce
high-purity
liquid
chemicals,
advance
hybrid
electro-biosystems.
This
review
article
begins
by
covering
fundamentals
processes
capture,
emphasizing
advantages
utilizing
solid
electrolytes.
Additionally,
it
highlights
recent
advancements
use
polymer
electrolyte
or
layer
CO2RR
with
multiple
functions.
The
also
explores
avenues
future
research
fully
harness
potential
electrolytes,
including
integration
performance
assessment
under
realistic
conditions.
Finally,
this
discusses
opportunities
challenges,
aiming
contribute
establishment
green
sustainable
society
through
valorization.
Angewandte Chemie,
Год журнала:
2024,
Номер
136(34)
Опубликована: Июнь 5, 2024
Abstract
Bismuth‐based
materials
have
emerged
as
promising
catalysts
in
the
electrocatalytic
reduction
of
CO
2
to
formate.
However,
reasons
for
reconstruction
Bi‐based
precursors
form
bismuth
nanosheets
are
still
puzzling,
especially
formation
defective
sites.
Herein,
we
prepare
with
vacancy‐rich
defects
(V‐Bi
NS)
by
rapidly
reconstructing
Bi
19
Cl
3
S
27
under
negative
potential.
Theoretical
analysis
reveals
that
introduction
chlorine
induces
generation
intrinsic
electric
field
precursor,
thereby
increasing
electron
transfer
rate
and
further
promoting
metallization
trivalent
bismuth.
Meanwhile,
experimental
tests
verify
has
a
faster
than
.
The
formed
V‐Bi
NS
exhibits
up
96
%
HCOO
−
Faraday
efficiency
400
mA
cm
−2
partial
current
densities,
its
electrochemical
active
surface
area
normalized
formate
density
yield
2.2
times
higher
those
intact
(I‐Bi
NS).
Density
functional
theory
calculations
indicate
vacancies
electron‐rich
aggregation
reduce
activation
energy
*CO
radicals
stabilize
adsorption
key
intermediate
*OCHO,
thus
facilitating
reaction
kinetics
production.
Abstract
Electrochemical
carbon
dioxide
reduction
reaction
(ECO
2
RR)
is
a
promising
approach
to
synthesize
fuels
and
value‐added
chemical
feedstocks
while
reducing
atmospheric
CO
levels.
Here,
high
surface
area
cerium
sulfur‐doped
hierarchical
bismuth
oxide
nanosheets
(Ce@S‐Bi
O
3
)
are
develpoed
by
solvothermal
method.
The
resulting
Ce@S‐Bi
electrocatalyst
shows
maximum
formate
Faradaic
efficiency
(FE)
of
92.5%
current
density
42.09
mA
cm
−2
at
−1.16
V
versus
RHE
using
traditional
H‐cell
system.
Furthermore,
three‐chamber
gas
diffusion
electrode
(GDE)
reactor,
FE
85%
achieved
in
wide
range
applied
potentials
(−0.86
−1.36
vs
RHE)
.
functional
theory
(DFT)
results
show
that
doping
Ce
S
Bi
enhances
production
weakening
the
OH*
H*
species.
Moreover,
DFT
calculations
reveal
*OCHO
dominant
pathway
on
leads
efficient
production.
This
study
opens
up
new
avenues
for
designing
metal
element‐doped
electrocatalysts
improve
catalytic
activity
selectivity
ECO
RR.
