ACS Nano,
Год журнала:
2023,
Номер
17(10), С. 9338 - 9346
Опубликована: Май 4, 2023
Main
group
indium
materials
have
been
known
as
promising
electrocatalysts
for
two-electron-involved
carbon
dioxide
reduction
to
produce
formate,
which
is
a
key
energy
vector
in
many
industrial
reactions.
However,
the
synthesis
of
two-dimensional
(2D)
monometallic
nonlayered
remains
great
challenge.
Here,
we
present
facile
electrochemical
strategy
transform
2D
coordination
polymer
into
elemental
nanosheets.
In
customized
flow
cell,
reconstructed
metallic
exhibits
high
Faradaic
efficiency
(FE)
96.3%
formate
with
maximum
partial
current
density
exceeding
360
mA
cm-2
and
negligible
degradation
after
140
h
operation
1
M
KOH
solution,
outperforming
state-of-the-art
indium-based
electrocatalysts.
Moreover,
ex
situ
analysis
characterizations
demonstrate
that
enhanced
exposure
active
sites
mass/charge
transport
at
CO2
gas-catalyst-electrolyte
triple-phase
interface
restrained
electrolyte
flooding
are
contributing
producing
stabilizing
radical
anion
intermediates,
thus
leading
superior
catalytic
performance.
Chemical Society Reviews,
Год журнала:
2023,
Номер
52(5), С. 1723 - 1772
Опубликована: Янв. 1, 2023
Defective
two-dimensional
(2D)
materials
show
huge
potential
for
energy-related
fields.
This
review
overviews
the
formation/evolution
mechanisms
and
engineering
strategies
of
defects
in
2D
materials,
which
enable
enhanced
electrode
reaction
kinetics.
Energy & Environmental Science,
Год журнала:
2023,
Номер
17(1), С. 49 - 113
Опубликована: Ноя. 7, 2023
This
perspective
highlights
recent
advancements
in
innovative
strategies
to
provide
valuable
insights
into
the
potential
for
energy-saving
hydrogen
production
through
water
electrolysis.
Energy & Environmental Science,
Год журнала:
2023,
Номер
16(11), С. 4714 - 4758
Опубликована: Янв. 1, 2023
This
review
analyzes
advanced
catalysts
and
C
2+
synthesis
mechanisms
based
on
theoretical
explorations
in
situ
/
operando
characterizations.
Triphasic
interface
optimization
is
discussed
for
the
potential
of
industry-compatible
stability.
Advanced Materials,
Год журнала:
2023,
Номер
35(13)
Опубликована: Янв. 10, 2023
CO2
electroreduction
is
of
great
significance
to
reduce
emissions
and
complete
the
carbon
cycle.
However,
unavoidable
carbonate
formation
low
utilization
efficiency
in
neutral
or
alkaline
electrolytes
hinder
its
application
at
commercial
scale.
The
development
reduction
under
acidic
conditions
provides
a
promising
strategy,
but
inhibition
hydrogen
evolution
reaction
difficult.
Herein,
first
work
design
Ni-Cu
dual
atom
catalyst
supported
on
hollow
nitrogen-doped
reported
for
pH-universal
CO.
shows
high
CO
Faradaic
≈99%
acidic,
neutral,
electrolytes,
partial
current
densities
reach
190
±
11,
225
10,
489
14
mA
cm-2
,
respectively.
In
particular,
reaches
64.3%,
which
twice
as
that
conditions.
Detailed
study
indicates
existence
electronic
interaction
between
Ni
Cu
atoms.
atoms
push
d-band
center
further
toward
Fermi
level,
thereby
accelerating
*COOH.
addition,
operando
characterizations
density
functional
theory
calculation
are
used
elucidate
possible
mechanism
electrolytes.
Chemical Reviews,
Год журнала:
2023,
Номер
123(17), С. 10530 - 10583
Опубликована: Авг. 17, 2023
Electrosynthesis
of
value-added
chemicals,
directly
from
CO2,
could
foster
achievement
carbon
neutral
through
an
alternative
electrical
approach
to
the
energy-intensive
thermochemical
industry
for
utilization.
Progress
in
this
area,
based
on
electrogeneration
multicarbon
products
CO2
electroreduction,
however,
lags
far
behind
that
C1
products.
Reaction
routes
are
complicated
and
kinetics
slow
with
scale
up
high
levels
required
commercialization,
posing
significant
problems.
In
review,
we
identify
summarize
state-of-art
progress
synthesis
a
multiscale
perspective
discuss
current
hurdles
be
resolved
generation
reduction
including
atomistic
mechanisms,
nanoscale
electrocatalysts,
microscale
electrodes,
macroscale
electrolyzers
guidelines
future
research.
The
review
ends
cross-scale
links
discrepancies
between
different
approaches
extensions
performance
stability
issues
arise
industrial
environment.
Advanced Materials,
Год журнала:
2023,
Номер
35(51)
Опубликована: Авг. 11, 2023
Electrochemical
CO2
reduction
reaction
(CO2
RR)
offers
a
promising
approach
to
close
the
anthropogenic
carbon
cycle
and
store
intermittent
renewable
energy
in
fuels
or
chemicals.
On
path
commercializing
this
technology,
achieving
long-term
operation
stability
is
central
requirement
but
still
confronts
challenges.
This
motivates
organize
present
review
systematically
discuss
issue
of
RR.
starts
from
fundamental
understanding
on
destabilization
mechanisms
RR,
with
focus
degradation
electrocatalyst
change
microenvironment
during
continuous
electrolysis.
Subsequently,
recent
efforts
catalyst
design
stabilize
active
sites
are
summarized,
where
increasing
atomic
binding
strength
resist
surface
reconstruction
highlighted.
Next,
optimization
electrolysis
system
enhance
by
maintaining
especially
mitigating
flooding
carbonate
problems
demonstrated.
The
manipulation
conditions
also
enables
prolong
RR
lifespan
through
recovering
catalytically
mass
transport
process.
finally
ends
up
indicating
challenges
future
opportunities.
Advanced Functional Materials,
Год журнала:
2023,
Номер
33(16)
Опубликована: Янв. 25, 2023
Abstract
Electrochemical
carbon
dioxide
reduction
reaction
(CO
2
RR)
using
clean
electric
energy
provides
a
sustainable
route
to
generate
highly‐valuable
chemicals
and
fuels,
which
is
beneficial
for
realizing
the
carbon‐neutral
cycle.
Up
now,
achieving
narrow
product
distribution
highly
targeted
selectivity
over
Cu‐based
electrocatalysts
still
big
challenge.
Herein,
sulfur
modification
on
different
crystal
planes
of
cuprous
oxide
(Cu
O)
demonstrated,
results
in
an
improvement
formate
generation
degrees.
Experimental
density
functional
theory
(DFT)
calculations
reveal
that
species
modified
surface
Cu
O
(100)
facet
effectively
lower
formation
key
intermediate
*OCOH
compared
with
(111)
facet.
As
consequence,
p‐Block
elements
effective
strategy
optimize
adsorption
during
CO
RR,
leading
selective
product.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
63(3)
Опубликована: Ноя. 24, 2023
Abstract
Modulating
the
surface
and
spatial
structure
of
host
is
associated
with
reactivity
active
site,
also
enhances
mass
transfer
effect
CO
2
electroreduction
process
(CO
RR).
Herein,
we
describe
development
two‐step
ligand
etch–pyrolysis
to
access
an
asymmetric
dual‐atomic‐site
catalyst
(DASC)
composed
a
yolk–shell
carbon
framework
(Zn
1
Mn
‐SNC)
derived
from
S,N‐coordinated
Zn−Mn
dimers
anchored
on
metal–organic
(MOF).
In
Zn
‐SNC,
electronic
effects
S/N−Zn−Mn−S/N
configuration
are
tailored
by
strong
interactions
between
dual
sites
co‐coordination
S/N
atoms,
rendering
structural
stability
atomic
distribution.
H‐cell,
‐SNC
DASC
shows
low
onset
overpotential
50
mV
high
Faraday
efficiency
97
%
applied
343
mV,
thus
outperforming
counterparts,
in
flow
cell,
it
reaches
current
density
500
mA
cm
−2
at
−0.85
V,
benefitting
accessibility
sites.
DFT
simulations
showed
that
diatomic
site
optimal
adsorption
strength
COOH*
lowers
reaction
energy
barrier,
boosting
intrinsic
RR
activity
DASC.
The
structure‐property
correlation
found
this
study
suggests
new
ideas
for
highly
accessible
catalysts.
Deleted Journal,
Год журнала:
2023,
Номер
3, С. e9120096 - e9120096
Опубликована: Сен. 1, 2023
As
an
important
part
of
carbon
neutralization,
dioxide
electroreduction
reaction
(CO2RR)
can
convert
CO2
into
high
value-added
chemicals
and
fuels
to
realize
the
recycling
resources
solve
problem
environmental
pollution.
Therefore,
exploring
element
species
surface
structure
catalyst
plays
a
central
role
in
improving
performance
catalyst,
enhancing
conversion
efficiency
forming
C1
C2+
products.
Here,
we
summarize
recent
progress
selective
regulation
CO2RR
products
by
different
elements.
In
particular,
emphasize
structure-property
relationship
microenvironment
metal
center
substrate,
heteroatom
doping,
hydrogen
bond
network
metal-free
polymer,
construction
heterogeneous
catalytic
system.
At
same
time,
advances
for
identification
active
sites
mechanistic
studies
on
process
reducing
are
reviewed,
as
well
comprehensive
review
final
Finally,
outline
inevitable
challenges
faced
present
our
own
recommendations
aimed
at
contributing
resource
utilization.