ACS Nano,
Год журнала:
2023,
Номер
17(19), С. 18688 - 18705
Опубликована: Сен. 19, 2023
Electrochemical
CO2
reduction
(ECO2R)
with
renewable
electricity
is
an
advanced
carbon
conversion
technology.
At
present,
copper
the
only
metal
to
selectively
convert
into
multicarbon
(C2+)
products.
Among
them,
atomically
dispersed
(AD)
Cu
catalysts
have
received
great
attention
due
relatively
single
chemical
environment,
which
are
able
minimize
negative
impact
of
morphology,
valence
state,
and
crystallographic
properties,
etc.
on
product
selectivity.
Furthermore,
completely
exposed
atomic
sites
not
provide
space
bonding
electrons
for
adsorption
reactants
in
favor
better
catalytic
activity
but
also
ideal
platform
studying
its
reaction
mechanism.
This
review
summarizes
recent
progress
AD
as
a
chemically
tunable
ECO2R,
including
dynamic
evolution,
performance,
prospects
challenges
ECO2R
carefully
discussed.
We
sincerely
hope
that
this
can
contribute
rational
design
enhanced
performance
ECO2R.
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(40), С. 21945 - 21954
Опубликована: Сен. 26, 2023
Cu-based
electrocatalysts
have
great
potential
for
facilitating
CO2
reduction
to
produce
energy-intensive
fuels
and
chemicals.
However,
it
remains
challenging
obtain
high
product
selectivity
due
the
inevitable
strong
competition
among
various
pathways.
Here,
we
propose
a
strategy
regulate
adsorption
of
oxygen-associated
active
species
on
Cu
by
introducing
an
oxophilic
metal,
which
can
effectively
improve
C2+
alcohols.
Theoretical
calculations
manifested
that
doping
Lewis
acid
metal
Al
into
affect
C–O
bond
Cu–C
breaking
toward
selectively
determining
intermediate
(shared
ethanol
ethylene),
thus
prioritizing
pathway.
Experimentally,
Al-doped
catalyst
exhibited
outstanding
Faradaic
efficiency
(FE)
84.5%
with
remarkable
stability.
In
particular,
alcohol
FE
could
reach
55.2%
partial
current
density
354.2
mA
cm–2
formation
rate
1066.8
μmol
h–1.
A
detailed
experimental
study
revealed
improved
strength
oxygen
surface
stabilized
key
*OC2H5,
leading
ethanol.
Further
investigation
showed
this
also
be
extended
other
metals.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(42)
Опубликована: Июнь 14, 2023
Dual-atom
catalysts
(DACs)
have
been
a
new
frontier
in
heterogeneous
catalysis
due
to
their
unique
intrinsic
properties.
The
synergy
between
dual
atoms
provides
flexible
active
sites,
promising
enhance
performance
and
even
catalyze
more
complex
reactions.
However,
precisely
regulating
site
structure
uncovering
dual-atom
metal
interaction
remain
grand
challenges.
In
this
review,
we
clarify
the
significance
of
inter-metal
DACs
based
on
understanding
center
structures.
Three
diatomic
configurations
are
elaborated,
including
isolated
single-atom,
N/O-bridged
dual-atom,
direct
dual-metal
bonding
interaction.
Subsequently,
up-to-date
progress
oxidation
reactions,
hydrogenation/dehydrogenation
electrocatalytic
photocatalytic
reactions
summarized.
structure-activity
relationship
catalytic
is
then
discussed
at
an
atomic
level.
Finally,
challenges
future
directions
engineer
discussed.
This
review
will
offer
prospects
for
rational
design
efficient
toward
catalysis.
Energy & Environmental Science,
Год журнала:
2023,
Номер
16(12), С. 5956 - 5969
Опубликована: Янв. 1, 2023
A
single-atom-based
tandem
photocatalyst
(In
2
O
3
/Cu–O
)
is
fabricated
for
efficient
CO
-to-ethanol
conversion.
The
electronic
interaction
between
Cu
and
In
promotes
C–C
coupling
of
*CO
(on
site)
*COH
Cu–O
to
form
OC–COH
species.
Advanced Functional Materials,
Год журнала:
2023,
Номер
33(48)
Опубликована: Июль 12, 2023
Abstract
Exploring
efficient
transition‐metal‐based
electrocatalysts
for
oxygen
evolution
reaction
(OER)
is
imperative
but
remain
challenging
sustainable
energy
storage
and
conversion
systems.
Foreign
species
doping
a
significant
regulation
strategy
to
enhance
the
intrinsic
activity
of
host
matrix.
However,
potential
relationship
structure‐activity
caused
by
guest
elements
seldom
tracked
systematically.
In
this
case,
both
theoretical
screening
experimental
verification
are
complementarily
employed
investigate
effects
ten
first‐row
transition
metals
(Sc∼Zn)
on
bimetallic
NiCo
layered
double
hydroxide
(NiCo‐LDH).
As
result,
optimized
Fe‐doped
NiCo‐LDH
identified
as
most
promising
candidate
toward
alkaline
electrocatalytic
OER,
which
exhibits
quasi‐industrial
current
density
1000
mA
cm
−2
at
overpotential
400
mV.
Meanwhile,
it
also
shows
impressively
long‐term
stability
500
h
with
negligible
loss.
Moreover,
in
situ
electrochemical
Raman
spectroscopy
unveils
dynamic
structure
from
pre‐catalytic
state
(Fe‐NiCo‐LDH)
metal
oxyhydroxide
(Fe‐(NiCo)OOH)
during
oxidation
reaction,
ab‐initio
molecular
dynamics
simulations
further
performed
confirm
thermodynamic
activated
Fe‐(NiCo)OOH
phase.
This
work
provides
platform
exploring
critical
role
matrix
developing
industrially
required
OER
electrocatalysts.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Фев. 26, 2024
Tuning
interfacial
electric
fields
provides
a
powerful
means
to
control
electrocatalyst
activity.
Importantly,
can
modify
adsorbate
binding
energies
based
on
their
polarizability
and
dipole
moment,
hence
operate
independently
of
scaling
relations
that
fundamentally
limit
performance.
However,
implementation
such
strategy
remains
challenging
because
typical
methods
the
field
non-uniformly
affects
only
minority
active
sites.
Here
we
discover
uniformly
tunable
modulation
be
achieved
using
model
system
single-atom
catalysts
(SACs).
These
consist
M-N
Energy & Environmental Science,
Год журнала:
2023,
Номер
16(10), С. 4423 - 4431
Опубликована: Янв. 1, 2023
Hydrophobized
nanofibers
of
hierarchical
porosity
as
the
integral
gas
diffusion
electrode
are
demonstrated.
The
GDE
showcases
stable
operation
for
>273
hours
in
neutral
MEA
and
a
single-pass
CO
2
conversion
78%
acidic
MEA.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(14)
Опубликована: Фев. 16, 2024
Abstract
The
acidic
electrochemical
CO
2
reduction
reaction
(CO
RR)
for
direct
formic
acid
(HCOOH)
production
holds
promise
in
meeting
the
carbon‐neutral
target,
yet
its
performance
is
hindered
by
competing
hydrogen
evolution
(HER).
Understanding
adsorption
strength
of
key
intermediates
electrolyte
indispensable
to
favor
RR
over
HER.
In
this
work,
high‐density
Sn
single
atom
catalysts
(SACs)
were
prepared
and
used
as
catalyst,
reveal
pH‐dependent
coverage
*CO
−
intermediatethat
enables
enhanced
towards
HCOOH
production.
At
pH=3,
SACs
could
deliver
a
high
Faradaic
efficiency
(90.8
%)
formation
corresponding
partial
current
density
up
−178.5
mA
cm
−2
.
detailed
situ
attenuated
total
reflection
Fourier
transform
infrared
(ATR‐FTIR)
spectroscopic
studies
that
favorable
alkaline
microenvironment
formed
near
surface
SACs,
even
electrolyte.
More
importantly,
intermediate
unravelled
which
turn
affects
competition
between
HER
