Angewandte Chemie,
Год журнала:
2024,
Номер
136(26)
Опубликована: Апрель 19, 2024
Abstract
The
electrocatalytic
CO
2
reduction
reaction
(CO
RR)
is
a
sustainable
route
for
converting
into
value‐added
fuels
and
feedstocks,
advancing
carbon‐neutral
economy.
electrolyte
critically
influences
utilization,
rate
product
selectivity.
While
typically
conducted
in
neutral/alkaline
aqueous
electrolytes,
the
RR
faces
challenges
due
to
(bi)carbonate
formation
its
crossover
anolyte,
reducing
efficiency
stability.
Acidic
media
offer
promise
by
suppressing
these
processes,
but
low
Faradaic
efficiency,
especially
multicarbon
(C
2+
)
products,
poor
electrocatalyst
stability
persist.
effective
regulation
of
environment
at
cathode
essential
favor
over
competitive
hydrogen
evolution
(HER)
improve
long‐term
This
review
examines
progress
acidic
RR,
focusing
on
strategies
such
as
design,
electrode
modification
engineering
promote
RR.
Insights
mechanisms
via
situ/operando
techniques
theoretical
calculations
are
discussed,
along
with
critical
future
directions
technology,
offering
guidance
developing
practical
systems
community.
ACS Materials Letters,
Год журнала:
2023,
Номер
5(12), С. 3212 - 3221
Опубликована: Ноя. 6, 2023
The
electrochemical
carbon
dioxide
(CO2)
reduction
reaction
(CO2RR)
has
been
considered
as
a
promising
approach
to
convert
atmospheric
CO2
value-added
chemicals
promote
neutrality.
However,
developing
electrocatalysts
with
superior
activity
and
high
selectivity
toward
individual
products
remains
great
challenge.
Herein
we
report
the
electronic
structure
modulation
of
unconventional
phase
metal
nanomaterials
achieve
highly
efficient
electroreduction.
It
found
that
growing
cerium
oxide
(CeOx)
nanostructures
on
4H/face-centered
cubic
(fcc)
gold
(Au)
nanorods
can
significantly
enhance
their
catalytic
conversion
monoxide.
X-ray
analysis
indicates
change
4H/fcc
Au
after
CeOx
overgrowth.
In-situ
attenuated
total
reflection
infrared
spectroscopy
measurements
reveal
HCO3–
concentration
near
surface
Au-CeOx
heteronanostructures
is
much
higher
than
nanorods,
facilitating
process.
Density
functional
theory
calculations
suggest
activation
effect
nanorod
for
electrocatalytic
CO2RR.
synergy
between
promotes
formation
carboxyl
(*COOH)
species
thus
boosts
CO2RR
performance.
This
work
highlights
importance
rational
regulation
unusual
small
molecules.
Advanced Energy Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Сен. 9, 2024
Abstract
CO
2
reduction
reaction
(CO
RR),
as
a
promising
strategy
for
storing
renewable
energy
and
promoting
carbon
resource
recycling,
is
critical
industrial
development.
Previous
reports
have
extensively
explored
catalyst‐electrolyte
microenvironmental
modulation
to
elucidate
coupling
mechanisms
enhance
catalytic
conversion
multicarbon
products.
Currently,
most
reviews
mainly
focus
on
the
impact
of
microenvironment
in
low‐current
systems
mechanism
exploration
performance
optimization,
yet
few
them
can
integrate
macroscopic
applications
with
microscopic
investigations
explore
relevance
between
development
optimization.
To
address
gap,
this
review
focuses
summarizing
challenges
advancements
high‐current
devices.
By
introducing
models
different
scales
sequentially,
connection
device
clarified.
Then,
various
invalidation
effective
solutions
are
summarized
intuitively
expound
stability.
Meanwhile,
an
intuitive
measure
rationality
modulation,
evaluation
methods
should
be
refined,
which
also
covered
further
detail
below.
Finally,
more
valuable
challenging
prospects
discussed
guiding
transformation
RR.
The
electrocatalytic
carbon
dioxide
reduction
reaction
(CO2RR)
at
industrial-level
current
densities
provides
a
sustainable
approach
to
converting
CO2
into
value-added
fuels
and
feedstocks
using
renewable
electricity.
However,
the
CO2RR
conducted
typically
in
alkaline
neutral
electrolytes
encounters
some
challenges
due
inevitable
between
OH-
ions,
which
undermines
utilization
leads
poor
operational
stability.
Acidic
media
present
viable
alternative
by
reducing
(bi)carbonate
production,
thereby
enhancing
efficiency
stability
CO2RR.
objective
of
this
paper
is
provide
concise
account
recent
advancements
field
acidic
CO2RR,
with
an
emphasis
on
future
developments
opportunities.
Abstract
Electrocatalytic
carbon
dioxide
reduction
reaction
(CO
2
RR)
has
emerged
as
a
promising
and
sustainable
approach
to
cut
emissions
by
converting
greenhouse
gas
CO
value‐added
chemicals
fuels.
Metal–organic
coordination
compounds,
especially
the
copper
(Cu)‐based
which
feature
well‐defined
crystalline
structures
designable
metal
active
sites,
have
attracted
much
research
attention
in
electrocatalytic
RR.
Herein,
recent
advances
of
electrochemical
RR
on
pristine
Cu‐based
compounds
with
different
types
Cu
sites
are
reviewed.
First,
general
pathways
briefly
introduced.
Then
highly
efficient
conversion
various
kinds
(e.g.,
single‐Cu
site,
dimeric‐Cu
multi‐Cu
heterometallic
site)
is
systematically
discussed,
along
corresponding
catalytic
mechanisms.
Finally,
some
existing
challenges
potential
opportunities
for
this
direction
provided
guide
rational
design
metal–organic
their
practical
application
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
64(1)
Опубликована: Сен. 2, 2024
Abstract
Acidic
CO
2
electrolysis
offers
a
promising
strategy
to
achieve
high
carbon
utilization
and
energy
efficiency.
However,
challenges
still
remain
in
suppressing
the
competitive
hydrogen
evolution
reaction
(HER)
improving
product
selectivity.
Although
concentrations
of
potassium
ions
(K
+
)
can
suppress
HER
accelerate
reduction,
they
inevitably
suffer
from
salt
precipitation
problems.
In
this
study,
we
demonstrate
that
sulfonate‐based
polyelectrolyte,
polystyrene
sulfonate
(PSS),
enables
reconstruct
electrode‐electrolyte
interface
significantly
enhance
acidic
electrolysis.
Mechanistic
studies
reveal
PSS
induces
local
K
through
electrostatic
interaction
between
anions
.
situ
spectroscopy
reveals
reshapes
interfacial
hydrogen–bond
(H‐bond)
network,
which
is
attributed
H‐bonds
hydrated
proton,
as
well
steric
hindrance
additive
molecules.
This
greatly
weakens
proton
transfer
kinetics
leads
suppression
undesirable
HER.
As
result,
Faradaic
efficiency
93.9
%
for
be
achieved
at
250
mA
cm
−2
,
simultaneous
with
single‐pass
72.2
on
commercial
Ag
catalysts
acid.
study
highlights
important
role
induced
by
polyelectrolyte
additives
promoting
electrocatalytic
reactions.
