ACS Catalysis,
Год журнала:
2022,
Номер
13(1), С. 837 - 847
Опубликована: Дек. 28, 2022
Developing
cost-effective
electrocatalysts
and
elucidating
the
in
situ
catalytic
mechanism
of
urea
oxidation
reaction
(UOR)
is
a
cornerstone
for
developing
urea-based
technology.
Amorphous–crystalline
(A–C)
heterostructures
have
attracted
extensive
attention
owing
to
their
highly
exposed
active
sites
superior
stability.
However,
complicated
synthesis
approach
inefficient
A–C
boundary
severely
limit
industrial
application
UOR
electrolysis.
In
this
study,
simple
hydrothermal
method
was
reported
fabricate
novel
heterostructure
nanoarrays
comprising
NiSe
nanorods
evenly
integrated
with
nickel-terephthalic
acid
(Ni-TPA)
nanosheets.
electrocatalyst,
conductive
facilitate
axial
charge
transfer
interconnection
network.
TPA-induced
formation
crystalline–amorphous
exposes
more
regulates
electronic
structure
Ni.
As
expected,
optimal
Ni-TPA@NiSe/NF
electrode
presents
low
potential
1.37
V
deliver
100
mA
cm–2
while
maintaining
impressively
robust
stability
at
high
current
densities
least
40
h.
electrochemical
Raman
spectroscopy
differential
mass
spectrometry
analyses
reveal
that
activity
originates
from
NiOOH
species
terminal
product
nitrogen
generated
via
intramolecular
N–N
coupling
molecule.
More
importantly,
study
offers
deep
insights
into
designing
fabricating
effective
abundant
grain
boundaries.
Nano-Micro Letters,
Год журнала:
2023,
Номер
15(1)
Опубликована: Фев. 16, 2023
The
electrocatalytic
water
splitting
technology
can
generate
high-purity
hydrogen
without
emitting
carbon
dioxide,
which
is
in
favor
of
relieving
environmental
pollution
and
energy
crisis
achieving
neutrality.
Electrocatalysts
effectively
reduce
the
reaction
barrier
increase
efficiency.
Facet
engineering
considered
as
a
promising
strategy
controlling
ratio
desired
crystal
planes
on
surface.
Owing
to
anisotropy,
with
different
orientations
usually
feature
facet-dependent
physical
chemical
properties,
leading
differences
adsorption
energies
oxygen
or
intermediates,
thus
exhibit
varied
activity
toward
evolution
(HER)
(OER).
In
this
review,
brief
introduction
basic
concepts,
fundamental
understanding
mechanisms
well
key
evaluating
parameters
for
both
HER
OER
are
provided.
formation
facets
comprehensively
overviewed
aiming
give
scientific
theory
guides
realize
dominant
planes.
Subsequently,
three
strategies
selective
capping
agent,
etching
coordination
modulation
tune
summarized.
Then,
we
present
an
overview
significant
contributions
facet-engineered
catalysts
HER,
OER,
overall
splitting.
particular,
highlight
that
density
functional
calculations
play
indispensable
role
unveiling
structure–activity
correlation
between
plane
catalytic
activity.
Finally,
remaining
challenges
provided
future
prospects
designing
advanced
electrocatalysts
discussed.
EcoEnergy,
Год журнала:
2023,
Номер
1(2), С. 425 - 436
Опубликована: Дек. 1, 2023
Abstract
Introducing
oxygen
atoms
into
nickel‐based
alloys
is
an
effective
strategy
for
constructing
water
dissociation
sites
hydrogen
evolution
reaction
(HER).
However,
controlling
content
to
realize
the
best
match
of
and
adsorption
challenging.
Herein,
we
exploit
self‐integration
process
MoNi
alloy
in
molten
salts
introduce
atoms,
which
ultimately
leads
localized
generation
robust
NiO
x
H
y
around
alloys.
Interestingly,
Mo
further
doped
(Mo‐NiO
)
construct
active
center
due
high
mobility
ionic
solutions.
Owing
covering
space
confinement
salt,
exactly
decorated
with
Mo‐NiO
nanosheets.
Both
physical
characterization
density
functional
theory
calculation
prove
that
electron
transport,
capability,
are
finely
tuned
benefited
from
O
doping,
thus
greatly
expediting
HER
kinetics.
exhibits
a
much
lower
overpotential
33
mV
at
10
cm
−2
alkaline
electrolyte,
even
superior
Pt/C
benchmark.
Moreover,
final
requires
low
57
acidic
media.
This
enhancement
ascribed
successful
assembly
foam
elicited
by
salt.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(17)
Опубликована: Март 2, 2023
The
construction
of
high-activity
and
low-cost
electrocatalysts
is
critical
for
efficient
hydrogen
production
by
water
electrolysis.
Herein,
we
developed
an
advanced
electrocatalyst
anchoring
well-dispersed
Ir
nanoparticles
on
nickel
metal-organic
framework
(MOF)
Ni-NDC
(NDC:
2,6-naphthalenedicarboxylic)
nanosheets.
Benefiting
from
the
strong
synergy
between
MOF
through
interfacial
Ni-O-Ir
bonds,
synthesized
Ir@Ni-NDC
showed
exceptional
electrocatalytic
performance
evolution
reaction
(HER),
oxygen
(OER)
overall
splitting
in
a
wide
pH
range,
superior
to
commercial
benchmarks
most
reported
electrocatalysts.
Theoretical
calculations
revealed
that
charge
redistribution
bridge
induced
optimization
H2
O,
OH*
H*
adsorption,
thus
leading
accelerated
electrochemical
kinetics
HER
OER.
This
work
provides
new
clue
exploit
bifunctional
pH-universal
splitting.
Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Июль 14, 2023
Electrochemical
hydrogen
evolution
reaction
in
neutral
media
is
listed
as
the
most
difficult
challenges
of
energy
catalysis
due
to
sluggish
kinetics.
Herein,
Ir-HxWO3
catalyst
readily
synthesized
and
exhibits
enhanced
performance
for
reaction.
HxWO3
support
functioned
proton
sponge
create
a
local
acid-like
microenvironment
around
Ir
metal
sites
by
spontaneous
injection
protons
WO3,
evidenced
spectroscopy
electrochemical
analysis.
Rationalize
revitalized
lattice-hydrogen
species
located
interface
are
coupled
with
Had
atoms
on
metallic
surfaces
via
thermodynamically
favorable
Volmer-Tafel
steps,
thereby
fast
Elaborated
demonstrates
activity
low
overpotential
20
mV
at
10
mA
cm-2
Tafel
slope
28
dec-1,
which
even
comparable
those
acidic
environment.
The
concept
exemplified
this
work
offer
possibilities
tailoring
regulate
catalytic
pathway.
Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Март 31, 2023
Developing
robust
nonprecious-metal
electrocatalysts
with
high
activity
towards
sluggish
oxygen-evolution
reaction
is
paramount
for
large-scale
hydrogen
production
via
electrochemical
water
splitting.
Here
we
report
that
self-supported
laminate
composite
electrodes
composed
of
alternating
nanoporous
bimetallic
iron-cobalt
alloy/oxyhydroxide
and
cerium
oxynitride
(FeCo/CeO2-xNx)
heterolamellas
hold
great
promise
as
highly
efficient
alkaline
reaction.
By
virtue
three-dimensional
architecture
to
offer
abundant
accessible
electroactive
CoFeOOH/CeO2-xNx
heterostructure
interfaces
through
facilitating
electron
transfer
mass
transport,
FeCo/CeO2-xNx
exhibit
superior
electrocatalysis
in
1
M
KOH,
ultralow
Tafel
slope
~33
mV
dec-1.
At
overpotential
low
360
mV,
they
reach
>3900
mA
cm-2
retain
exceptional
stability
at
~1900
>1000
h,
outperforming
commercial
RuO2
some
representative
oxygen-evolution-reaction
catalysts
recently
reported.
These
properties
make
them
attractive
candidates
electrolysis
generation.
Nano-Micro Letters,
Год журнала:
2023,
Номер
15(1)
Опубликована: Апрель 10, 2023
Abstract
The
sluggish
kinetics
of
both
hydrogen
evolution
reaction
(HER)
and
oxygen
(OER)
generate
the
large
overpotential
in
water
electrolysis
thus
high-cost
production.
Here,
multidimensional
nanoporous
interpenetrating-phase
FeNiZn
alloy
FeNi
3
intermetallic
heterostructure
is
situ
constructed
on
NiFe
foam
(FeNiZn/FeNi
@NiFe)
by
dealloying
protocol.
Coupling
with
eminent
synergism
among
specific
constituents
highly
efficient
mass
transport
from
integrated
porous
backbone,
FeNiZn/FeNi
@NiFe
depicts
exceptional
bifunctional
activities
for
splitting
extremely
low
overpotentials
toward
OER
HER
(
η
1000
=
367/245
mV)
as
well
robust
durability
during
400
h
testing
alkaline
solution.
as-built
electrolyzer
anode
cathode
exhibits
record-high
performances
sustainable
output
terms
much
lower
cell
voltage
1.759
1.919
V
to
deliver
current
density
500
mA
cm
−2
long
working
lives.
Density
functional
theory
calculations
disclose
that
interface
interaction
between
generates
modulated
electron
structure
state
optimized
intermediate
chemisorption,
diminishing
energy
barriers
production
splitting.
With
merits
fine
performances,
scalable
fabrication,
cost,
holds
prospective
application
potential
electrocatalyst
splitting."Image
missing"
ACS Catalysis,
Год журнала:
2022,
Номер
12(21), С. 13234 - 13246
Опубликована: Окт. 17, 2022
In
promising
transition
metal
sulfide
catalysts,
the
extraordinary
instability
under
air
exposure
and
oxygen
evolution
reaction
(OER)
catalysis
severely
degrades
their
activity
stability
in
electrochemical
water
splitting
reaction,
inhibiting
practical
applications.
Herein,
guided
by
a
theoretical
mechanism
study,
it
is
disclosed
that
adsorbing
ability
electronic
interaction
for
molecular
will
be
significantly
weakened
nickel
disulfide
(NiS2)
constructing
an
electron-deficient
distribution
on
Ni–S
sites
with
N
atom
introduction,
which
efficiently
inhibits
process
of
O2
adsorption
electrophilic
activation
during
oxidation,
thus
achieving
air-stable
capacity
NiS2.
addition,
calculations
further
reveal
such
redistribution
weaken
OH–
NiS2
inhibit
reconstruction
OER
process.
Inspired
this,
nanosheets
(NiS2
NSs)
are
synthesized
atoms
introduced
to
bridge
Ni
S,
resulting
S
atom-bridged
NSs
(N–NiS2
NSs).
As
expected,
only
28.1%
phase
oxidized
into
sulfate
N–NiS2
after
one
month
13
mV
overpotential
degradation
toward
OER,
while
NSs,
fast
drastic
transformation
undergone,
155
decline.
For
process,
from
sulfides
(oxy)hydroxides
deservedly
inhibited
situ
constructed
N–NiS2/NiOOH
heterostructure
as
active
phase,
exhibits
higher
compared
those
completely
NiOOH-oxidized
NSs.
Rationalized
density
functional
theory
(DFT)
calculations,
features
strong
electron
rearrangement
at
interface,
improving
chemisorption
conductivity
pristine
NiOOH.
Moreover,
strategy
also
valid
other
(TMS)
(such
CoS2
FeS2).
Nano-Micro Letters,
Год журнала:
2024,
Номер
16(1)
Опубликована: Июль 5, 2024
Green
hydrogen
from
electrolysis
of
water
has
attracted
widespread
attention
as
a
renewable
power
source.
Among
several
production
methods,
it
become
the
most
promising
technology.
However,
there
is
no
large-scale
system
currently
that
can
compete
with
conventional
fossil
fuel
production.
Renewable
energy
electrocatalytic
splitting
an
ideal
technology
environmental
cleanliness
protection
and
good
purity,
which
meet
requirements
future
development.
This
review
summarizes
introduces
current
status
by
three
aspects:
electricity,
catalyst
electrolyte.
In
particular,
present
situation
latest
progress
key
sources
power,
catalytic
materials
electrolyzers
for
are
introduced.
Finally,
problems
generation
electrolytic
directions
next-generation
green
in
discussed
outlooked.
It
expected
this
will
have
important
impact
on
field
water.