ACS Sustainable Chemistry & Engineering,
Год журнала:
2024,
Номер
unknown
Опубликована: Дек. 12, 2024
Electrochemical
CO2
reduction
(ECR)
to
high
value-added
feedstocks
is
a
sustainable
way
address
energy
and
environmental
issues.
However,
there
still
exists
bottleneck
in
comprehending
the
structure–activity
relationship
of
catalysts
for
ECR.
Herein,
we
demonstrated
that
simultaneous
tuning
surface-adsorbed
hydroxyl
group
(OHad)
coverage
oxygen
vacancy
(OV)
amount
on
In2O3
surface
was
an
effective
approach
derive
excellent
formate
Faradaic
efficiency
(FE)
above
80%
at
wide
potential
range
from
−1.0
−1.5
V
versus
reversible
hydrogen
electrode
(vs
RHE)
with
promising
durability.
experiments
theoretical
analyses
revealed
synergistic
effect
OHad
OV
could
smartly
optimize
adsorption
sites,
accelerate
electron
transfer,
stabilize
*CO2•–
*OCHO
intermediates,
thus
facilitate
ECR
activity.
This
result
will
contribute
understanding
critical
role
these
species
ECR,
which
can
offer
valuable
insights
into
rational
catalyst
design
comprehensive
utilization
efficiency.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 24, 2025
The
electrocatalytic
conversion
of
carbon
dioxide
(CO2)
to
ethylene
(C2H4)
holds
great
promise
for
sustainable
chemical
synthesis,
yet
achieving
industrially
relevant
production
rates
remains
a
significant
challenge.
Through
computational
screening,
we
have
identified
praseodymium
(Pr)
single-atom
alloy
embedded
in
copper
(Cu)
catalyst
(Pr@Cu)
that
exhibits
superior
CO2
activation
and
remarkably
low
energy
barrier
asymmetric
*CO-*CHO
coupling,
primarily
by
facilitating
the
*CHO
intermediate
formation.
Our
optimized
catalyst,
Pr@Cu-2
(6
wt
%
Pr),
achieves
C2H4
Faradaic
efficiency
(FE)
64.2%
at
-1.6
V
versus
reversible
hydrogen
electrode
(RHE)
under
high
current
density
1200
mA
cm-2
reduction
reaction
(CO2RR).
Furthermore,
when
integrated
into
100
cm2
membrane
assembly
(MEA)
electrolyzer,
demonstrates
robust
performance,
maintaining
continuous
rate
21.3
mL
min-1
20
A
over
200
h.
This
work
provides
fundamental
insights
role
Pr
alloys
CO2RR
highlights
their
potential
scalable
electrosynthesis.
C-N
coupling
is
crucial
for
constructing
amides
and
amines
involves
various
fields,
including
medicine,
chemical
industries,
agriculture,
energy.
With
the
rapid
development
of
electrocatalytic
continuous
improvement
catalytic
performance,
this
field
has
aroused
extensive
research
interest.
A
comprehensive
review
urgently
needed
to
summarize
structure-activity
relationship,
key
challenges,
future
directions.
This
provides
a
concise
overview
recent
advancements
from
nanocatalysis
single
metal
site
catalysis
reactions.
We
mechanisms
using
different
nitrogen
sources
further
analyze
influences
active
centers
coordination
environments
on
thereby
elucidating
relationship.
Moreover,
we
discuss
dynamic
structural
evolution
sites
during
reaction.
Finally,
present
current
challenges
perspectives
in
field.
aims
provide
valuable
insights
into
advanced
nano/single
catalysts
reactions
along
with
deeper
understanding
mechanisms.
Abstract
Electrolyte
plays
crucial
roles
in
electrochemical
CO
2
reduction
reaction
(e‐CO
RR),
yet
how
it
affects
the
e‐CO
RR
performance
still
being
unclarified.
In
this
work,
is
reported
that
Sn‐Zn
hybrid
oxide
enables
excellent
‐to‐HCOO
−
conversion
KHCO
3
with
a
HCOO
Faraday
efficiency
≈89%,
yield
rate
≈0.58
mmol
cm
−2
h
−1
and
stability
up
to
≈60
at
−0.93
V,
which
are
higher
than
those
NaHCO
K
SO
4
.
Systematical
characterizations
unveil
surface
reconstruction
on
greatly
depends
electrolyte
using:
Sn‐SnO
/ZnO,
ZnO
encapsulated
/ZnO
/Zn‐ZnO
reconstructed
by
,
respectively.
The
improved
highly
attributed
can
enhance
charge
transportation,
promote
adsorption
optimize
configuration,
accumulate
protons
enhancing
water
adsorption/cleavage
limit
hydrogen
evolution.
findings
may
provide
insightful
understanding
relationship
between
guide
design
of
novel
electrocatalyst
for
effective
reduction.
ACS Sustainable Chemistry & Engineering,
Год журнала:
2024,
Номер
unknown
Опубликована: Дек. 12, 2024
Electrochemical
CO2
reduction
(ECR)
to
high
value-added
feedstocks
is
a
sustainable
way
address
energy
and
environmental
issues.
However,
there
still
exists
bottleneck
in
comprehending
the
structure–activity
relationship
of
catalysts
for
ECR.
Herein,
we
demonstrated
that
simultaneous
tuning
surface-adsorbed
hydroxyl
group
(OHad)
coverage
oxygen
vacancy
(OV)
amount
on
In2O3
surface
was
an
effective
approach
derive
excellent
formate
Faradaic
efficiency
(FE)
above
80%
at
wide
potential
range
from
−1.0
−1.5
V
versus
reversible
hydrogen
electrode
(vs
RHE)
with
promising
durability.
experiments
theoretical
analyses
revealed
synergistic
effect
OHad
OV
could
smartly
optimize
adsorption
sites,
accelerate
electron
transfer,
stabilize
*CO2•–
*OCHO
intermediates,
thus
facilitate
ECR
activity.
This
result
will
contribute
understanding
critical
role
these
species
ECR,
which
can
offer
valuable
insights
into
rational
catalyst
design
comprehensive
utilization
efficiency.
