Energy & Environmental Science,
Год журнала:
2022,
Номер
15(6), С. 2397 - 2409
Опубликована: Янв. 1, 2022
In
this
work,
we
designed
a
novel
CuO/Al
2
CuO
4
catalyst
by
phase
and
interphase
engineering
approach,
which
enables
the
electrochemical
conversion
of
carbon
dioxide
to
ethylene
with
ultrahigh
activity
selectivity.
Advanced Functional Materials,
Год журнала:
2021,
Номер
31(47)
Опубликована: Авг. 26, 2021
Abstract
High‐entropy
alloys
(HEAs)
have
attracted
widespread
attention
in
electrocatalysis
due
to
their
unique
advantages
(adjustable
composition,
complex
surface,
high
tolerance,
etc.).
They
allow
for
the
formation
of
new
and
tailorable
active
sites
multiple
elements
adjacent
each
other,
interaction
can
be
tailored
by
rational
selection
element
configuration
composition.
However,
it
needs
further
explored
catalyst
design,
elements,
determination
sites.
This
review
article
focuses
on
important
progress
multi‐sites
HEAs.
The
classification
is
done
basis
catalytic
reaction,
including
hydrogen
evolution
oxygen
reduction
alcohol
oxidation
carbon
dioxide
nitrogen
reaction.
Based
experiments
theories,
a
more
in‐depth
exploration
activity
HEAs
will
conducted,
(the
special
role
catalysis)
effect.
provide
design
some
reactions,
adjust
compositions
improve
intrinsic
activity.
Furthermore,
remaining
challenges
future
directions
promising
research
fields
are
also
provided.
Advanced Functional Materials,
Год журнала:
2021,
Номер
31(37)
Опубликована: Июнь 26, 2021
Abstract
Electrochemical
carbon
dioxide
reduction
reaction
(CO
2
RR)
offers
a
promising
way
of
effectively
converting
CO
to
value‐added
chemicals
and
fuels
by
utilizing
renewable
electricity.
To
date,
the
electrochemical
single‐carbon
products,
especially
monoxide
formate,
has
been
well
achieved.
However,
efficient
conversion
more
valuable
multicarbon
products
(e.g.,
ethylene,
ethanol,
n
‐propanol,
‐butanol)
is
difficult
still
under
intense
investigation.
Here,
recent
progresses
in
using
copper‐based
catalysts
are
reviewed.
First,
mechanism
RR
briefly
described.
Then,
representative
approaches
catalyst
engineering
introduced
toward
formation
RR,
such
as
composition,
morphology,
crystal
phase,
facet,
defect,
strain,
surface
interface.
Subsequently,
key
aspects
cell
for
including
electrode,
electrolyte,
design,
also
discussed.
Finally,
advances
summarized
some
personal
perspectives
this
research
direction
provided.
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.
Angewandte Chemie International Edition,
Год журнала:
2020,
Номер
60(13), С. 7382 - 7388
Опубликована: Дек. 15, 2020
Abstract
The
development
of
efficient
electrocatalysts
for
the
CO
2
reduction
reaction
(CO
RR)
remains
a
challenge.
Demonstrated
here
is
NiSn
atomic‐pair
electrocatalyst
(NiSn‐APC)
on
hierarchical
integrated
electrode,
which
exhibits
synergistic
effect
in
simultaneously
promoting
activity
and
selectivity
RR
to
formate.
atomic
pair
consists
adjacent
Ni
Sn,
each
coordinated
with
four
nitrogen
atoms
(N
4
‐Ni‐Sn‐N
).
as‐prepared
NiSn‐APC
displays
exceptional
formate
turnover
frequency
4752
h
−1
,
productivity
36.7
mol
g
Sn
an
utilization
degree
active
sites
(57.9
%),
are
superior
previously
reported
single‐atomic
catalysts.
Both
experimental
data
density‐functional
theory
calculations
verify
electron
redistribution
imposed
by
Ni,
reduces
energy
barrier
*OCHO
intermediate
makes
this
potential‐determining
step
thermodynamically
spontaneous.
This
catalysis
provides
successful
paradigm
rational
design
preparation
enhanced
performance.
Journal of the American Chemical Society,
Год журнала:
2021,
Номер
143(18), С. 6855 - 6864
Опубликована: Апрель 14, 2021
Electrochemical
CO2
reduction
(CO2RR)
using
renewable
energy
sources
represents
a
sustainable
means
of
producing
carbon-neutral
fuels.
Unfortunately,
low
efficiency,
poor
product
selectivity,
and
rapid
deactivation
are
among
the
most
intractable
challenges
CO2RR
electrocatalysts.
Here,
we
strategically
propose
"two
ships
in
bottle"
design
for
ternary
Zn–Ag–O
catalysts,
where
ZnO
Ag
phases
twinned
to
constitute
an
individual
ultrafine
nanoparticle
impregnated
inside
nanopores
ultrahigh-surface-area
carbon
matrix.
Bimetallic
electron
configurations
modulated
by
constructing
interface,
density
reconfiguration
arising
from
delocalization
enhances
stabilization
*COOH
intermediate
favorable
CO
production,
while
promoting
selectivity
suppressing
HCOOH
generation
altering
rate-limiting
step
toward
high
thermodynamic
barrier
forming
HCOO*.
Moreover,
pore-constriction
mechanism
restricts
bimetallic
particles
nanosized
dimensions
with
abundant
heterointerfaces
exposed
active
sites,
meanwhile
prohibiting
detachment
agglomeration
nanoparticles
during
enhanced
stability.
The
designed
catalysts
realize
60.9%
efficiency
94.1
±
4.0%
Faradaic
CO,
together
remarkable
stability
over
6
days.
Beyond
providing
high-performance
electrocatalyst,
this
work
presents
promising
catalyst-design
strategy
efficient
conversion.
Energy & Environmental Science,
Год журнала:
2021,
Номер
14(3), С. 1194 - 1246
Опубликована: Янв. 1, 2021
Power
to
formic
acidviaCO2hydrogenation
or
electrochemical
CO2reduction
has
great
potential
enable
a
complete
cycle
with
acid
power
for
the
storage
and
utilization
of
low-carbon
electricity
at
scale
multi-gigatonnes
per
year.
ACS Catalysis,
Год журнала:
2020,
Номер
10(19), С. 10803 - 10811
Опубликована: Сен. 2, 2020
Hosting
atomically
dispersed
nitrogen-coordinated
iron
sites
(Fe–N4)
on
graphene
offers
unique
opportunities
for
driving
electrochemical
CO2
reduction
reaction
(CO2RR)
to
CO.
However,
the
strong
adsorption
of
*CO
Fe–N4
site
embedded
in
intact
limits
current
density
due
slow
CO
desorption
process.
Herein,
we
report
how
manipulation
pore
edges
alters
local
electronic
structure
isolated
and
improves
their
intrinsic
reactivity
prompting
generation.
We
demonstrate
that
constructing
holes
basal
plane
support
can
significantly
enhance
its
CO2RR
compared
pore-deficient
graphene-supported
counterpart,
exhibiting
a
Faradaic
efficiency
94%
turnover
frequency
1630
h–1
at
0.58
V
vs
RHE.
Mechanistic
studies
reveal
incorporation
results
downshifting
d-band
center
Fe
sites,
which
weakens
strength
Fe–C
bond
when
intermediate
adsorbs
edge-hosted
Fe–N4,
thus
boosting
evolution
rates.
These
findings
suggest
engineering
renders
way
design
high-performance
single-atom
catalysts.