Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(18)
Опубликована: Март 1, 2022
Generally,
in
terms
of
electrocatalytic
CO2
reduction,
single-atom
catalysts
show
high
selectivities
yet
low
current
densities
whereas
conventional
nanoparticle
exhibit
relatively
but
selectivities.
This
work
combines
the
advantages
two
classes
by
constructing
a
Ni-Gd-N-doped
carbon
black
electrocatalyst
within
which
NiI
active
sites
are
exposed
outside
layers
and
Ni
nanoparticles
encapsulated
inside
layers.
The
Gd
atoms
can
not
only
influence
local
electron
3d
orbitals,
thus
strengthening
electronic
activity,
also
tailor
sizes
nanoparticles,
thereby
minimizing
activity
toward
hydrogen
evolution.
Accordingly,
this
yields
both
CO
faradaic
efficiency
(97
%)
large
density
(308
mA
cm-2
),
alongside
an
outstanding
stability
(100
h).
Advanced Energy Materials,
Год журнала:
2023,
Номер
13(13)
Опубликована: Фев. 12, 2023
Abstract
The
electrocatalytic
CO
2
reduction
reaction
(CO
RR)
to
fuels
driven
by
electrocatalysts
is
a
viable
strategy
for
efficient
utilization
of
emitted
.
RR
involves
multiple‐steps,
including
adsorption,
activation,
hydrogenation,
etc.
At
present,
copper‐tin
alloy
catalysts
have
shown
the
capability
reduce
formic
acid
or
formate.
However,
their
poor
adsorption
and
activation
capacities
molecules,
as
well
sluggish
kinetics
in
*H
supply
restrict
proton‐coupled
electron
transfer
processes
produce
acid.
In
order
solve
above
problems,
ultra‐small
SnO
/Cu
6
Sn
5
/CuO
nanocatalysts
with
superscalar
phase
boundaries
are
fabricated
laser
sputtering.
introduction
enhances
,
while
CuO
promotes
H
O
decomposition
provides
abundant
intermediates,
resulting
tandem
catalytic
sites
on
composite
thus
leading
excellent
activity
high
selectivity
Faradic
efficiency
(FE
HCOOH
)
at
electrode
reaches
90.13%
along
current
density
25.2
mA
cm
−2
−0.95
V
versus
reversible
hydrogen
electrode.
role
multiphase
constructed
oxides
confirmed
situ
infrared
spectroscopy
kinetic
isotope
effects
experiments,
which
consistent
design
concept.
ACS Applied Materials & Interfaces,
Год журнала:
2023,
Номер
15(13), С. 16673 - 16679
Опубликована: Март 24, 2023
The
electrochemical
carbon-dioxide
reduction
reaction
(CO2RR)
to
high-value
multi-carbon
(C2+)
chemicals
provides
a
hopeful
approach
store
renewable
energy
and
close
the
carbon
cycle.
Although
copper-based
catalysts
with
porous
architecture
are
considered
potential
electrocatalysts
for
CO2
C2+
chemicals,
challenges
remain
in
achieving
high
selectivity
partial
current
density
simultaneously
practical
application.
Here,
Cu
cavity
structure
by
situ
electrochemical-reducing
Cu2O
cavities
developed
high-performance
conversion
of
fuels.
as-described
exhibit
Faradaic
efficiency
75.6
±
1.8%
605
14
mA
cm-2,
respectively,
at
low
applied
(-0.59
V
vs
RHE)
microfluidic
flow
cell.
Furthermore,
Raman
tests
finite
element
simulation
indicated
that
can
enrich
local
concentration
CO
intermediates,
thus
promoting
C-C
coupling
process.
More
importantly,
should
be
major
through
*CO-*CHO
pathway
as
demonstrated
spectra
functional
theory
calculations.
This
work
provide
ideas
insights
into
designing
producing
compounds
highlight
important
effect
characterization
uncovering
mechanism.
Advanced Materials,
Год журнала:
2024,
Номер
36(16)
Опубликована: Янв. 10, 2024
Abstract
Single‐atom
catalysts
(SACs)
are
demonstrated
to
show
exceptional
reactivity
and
selectivity
in
catalytic
reactions
by
effectively
utilizing
metal
species,
making
them
a
favorable
choice
among
the
different
active
materials
for
energy
conversion.
However,
SACs
still
early
stages
of
conversion,
problems
like
agglomeration
low
conversion
efficiency
hampering
their
practical
applications.
Substantial
research
focus
on
support
modifications,
which
vital
SAC
stability
due
intimate
relationship
between
atoms
support.
In
this
review,
category
supports
variety
surface
engineering
strategies
employed
SA
systems
summarized,
including
site
(heteroatom
doping,
vacancy
introducing,
groups
grafting,
coordination
tunning)
structure
(size/morphology
control,
cocatalyst
deposition,
facet
engineering,
crystallinity
control).
Also,
merits
single‐atom
systematically
introduced.
Highlights
comprehensive
summary
discussions
utilization
surface‐engineered
diversified
applications
photocatalysis,
electrocatalysis,
thermocatalysis,
devices.
At
end
potential
obstacles
using
field
discussed.
This
review
aims
guide
rational
design
manipulation
target‐specific
capitalizing
characteristic
benefits
engineering.
Catalysis Science & Technology,
Год журнала:
2020,
Номер
10(9), С. 2711 - 2720
Опубликована: Янв. 1, 2020
We
have
summarized
three
novel
strategies
for
electrocatalytic
carbon
dioxide
reduction,
including
concurrent
CO2
electroreduction,
tandem
electroreduction
and
hybrid
electroreduction.
ChemSusChem,
Год журнала:
2020,
Номер
14(1), С. 73 - 93
Опубликована: Окт. 22, 2020
Single-atom
catalysts
(SACs)
have
attracted
increasing
research
interests
owing
to
their
unique
electronic
structures,
quantum
size
effects
and
maximum
utilization
rate
of
atoms.
Metal
organic
frameworks
(MOFs)
are
good
candidates
prepare
SACs
the
atomically
dispersed
metal
nodes
in
MOFs
abundant
N
C
species
stabilize
single
In
addition,
distance
adjacent
atoms
can
be
turned
by
adjusting
ligands
adding
volatile
centers
promote
formation
isolated
Moreover,
diverse
preparation
dual-atom
(DACs)
improve
loading
optimize
structures
catalysts.
The
applications
derived
DACs
for
electrocatalysis,
including
oxygen
reduction
reaction,
evolution
hydrogen
carbon
dioxide
reaction
nitrogen
systematically
summarized
this
Review.
corresponding
synthesis
strategies,
atomic
electrocatalytic
performances
discussed
provide
a
deep
understanding
MOFs-based
electrocatalysts.
catalytic
mechanisms
presented,
crucial
challenges
perspectives
proposed
further
design
Nano Materials Science,
Год журнала:
2021,
Номер
3(4), С. 344 - 367
Опубликована: Июнь 1, 2021
With
the
rising
global
population,
increasing
energy
demand
and
rapid
climate
change,
great
concerns
have
been
raised
for
environment
security
in
future.
Solar-driven
CO2
reduction
provides
a
promising
way
to
deal
with
crisis
warming,
which
has
widely
concerned.
Photoelectrocatalysis
technology
can
effectively
utilize
solar
avoid
use
high-temperature
high-voltage
by
integrating
vantages
of
both
photocatalysis
electrocatalysis,
exhibits
broad
application
prospect
high
efficiency
excellent
selectivity.
In
this
review,
basic
principles
photocatalysis,
electrocatalysis
photoeletrocatalysis
are
briefly
reviewed,
also
comparing
technical
characteristics
above
technologies.
Different
photoelectrocatalytic
systems
described
compared.
The
several
key
influencing
factors
performance
discussed,
including
interaction
between
reaction
molecules
catalysts,
conditions
influence
photoelectrode.
Then,
advances
on
mechanisms
strategies
enhancement
optimizing
photoexcitation,
charge
separation
surface
were
reviewed.
Besides,
challenges
prospects
will
be
discussed.
Energy & Environmental Science,
Год журнала:
2021,
Номер
15(1), С. 234 - 243
Опубликована: Дек. 1, 2021
A
hydrophobic
core–shell
architecture
was
constructed
to
control
local
H
2
O
availability
on
the
surface
of
copper-based
materials,
which
could
provide
a
maximum
generation
rate
−434
mA
cm
−2
towards
CH
4
.