The
direct
electrooxidation
reaction
of
ammonia
borane
(ABOR)
as
the
anodic
fuel
cells
(DABFCs)
is
greatly
dependent
on
properties
electrocatalysts.
Both
active
sites
and
charge/mass
transfer
characteristics
are
key
to
promoting
processes
kinetics
thermodynamics,
which
can
further
improve
electrocatalytic
activity.
Hence,
catalyst
double-heterostructured
Ni2
P/Ni2
P2
O7
/Ni12
P5
(d-NPO/NP)
with
optimistic
redistribution
electrons
prepared
for
first
time.
d-NPO/NP-750
obtained
after
pyrolysis
at
750
°C
shows
outstanding
activity
toward
ABOR
an
onset
potential
-0.329
V
vs
RHE
better
than
all
published
catalysts.
density
functional
theory
(DFT)
computations
illustrate
that
/Ni2
P
acts
enhancement
heterostructure
a
high
d-band
center
(-1.60
eV)
low
activation
energy
barrier,
while
conductivity
highest
valence
electrons.
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(21)
Опубликована: Фев. 2, 2024
Abstract
Metal–support
interaction
(MSI)
is
witnessed
as
an
essential
manner
to
stabilize
active
metals
and
tune
catalytic
activity
for
heterogonous
water
splitting.
Kinetically
driving
the
electrolysis
(WE)
appeals
a
rational
MSI
system
with
coupled
electron‐donating/accepting
(e‐D/A)
characters
hydrogen/oxygen
evolution
reactions
(HER/OER).
However,
metal
stabilization
effect
by
will
in
turn
restrict
deblocking
of
e‐D/A
properties
challenge
full
electrocatalytic
optimization.
This
study
profiles
heterostructure
featuring
metastable
Ru
clusters
on
defective
NiFe
hydroxide
(Ru/d‐NiFe
LDH)
support
low‐precious
(≈2
wt%)
platform
efficient
WE.
It
indicated
that
interfacial
oxygen
vacancies
can
deviate
stable
4d
5
orbit
2+δ
state,
regulate
d‐band
center
levels
toward
facilitated
HER/OER
processes.
Resultantly,
Ru/d‐NiFe
LDH
attains
ultralow
overpotentials
at
10
mA
cm
−2
Pt‐beyond
alkaline
HER
(18
mV)
OER
(220
fast
kinetics
durability.
The
symmetrical
electrolyzer
delivers
promising
voltage
1.49
V
1
m
KOH
seawater
splitting
performance.
work
carries
interesting
opportunities
rationalizing
sophisticated
metal‐support
electrocatalysts
through
metal‐site
metastabilization
engineering.
Space
charge
transfer
of
heterostructures
driven
by
the
work-function-induced
built-in
field
can
regulate
electronic
structure
catalysts
and
boost
catalytic
activity.
Herein,
an
epitaxial
heterojunction
catalyst
CoO/Mo2
C
with
interfacial
electron
redistribution
induced
work
functions
(WFs)
is
constructed
for
overall
water
splitting
via
a
novel
top-down
strategy.
Theoretical
simulations
experimental
results
unveil
that
WFs-induced
facilitates
from
CoO
to
Mo2
through
formed
"Co─C─Mo"
bond
at
interface
C,
achieving
redistribution,
further
optimizing
Gibbs
free
energy
primitive
reaction
step
then
accelerating
kinetics
hydrogen
evolution
(HER).
As
expected,
effects
exhibits
excellent
HER
activity
only
needing
overpotential
107
mV
achieve
10
mA
cm-2
stability
60-h
continuous
catalyzing.
Besides,
assembled
behaves
outstanding
performance
toward
(1.58
V
).
This
provides
possibility
designing
materials
based
on
arising
application
in
other
fields.
Advanced Functional Materials,
Год журнала:
2023,
Номер
34(7)
Опубликована: Окт. 30, 2023
Abstract
Owing
to
the
Pt‐like
electrocatalytic
capability
and
moderate
price,
Ru‐based
catalysts
are
considered
as
Pt
alternatives
for
electrochemical
water
splitting.
However,
they
demonstrate
limited
catalytic
performance
under
industrial‐level
current
densities.
Herein,
a
novel
electrocatalyst
with
an
extremely
low
amount
(0.85
wt.%)
of
Ru
nanoclusters
anchored
on
Cr‐doped
Fe‐metal–organic
frameworks
(Ru@Cr─FeMOF)
through
robust
Cr─O─Ru
bond
is
presented.
The
study
unveils
that
such
architecture
facilitates
fast
electron
transfer
manipulates
highest
occupied
d
orbital
d‐band
centers
sites,
favoring
both
oxygen
evolution
reaction
(OER)
hydrogen
(HER)
catalysis.
as‐prepared
catalyst
performs
excellent
activity
21
mV@10
mA
cm
−2
HER
230
mV@50
OER
in
alkaline
solution,
realizes
water‐splitting
at
densities
(1.72
V@1000
),
surpassing
state‐of‐the‐art
literatures.
Advanced Materials,
Год журнала:
2024,
Номер
36(29)
Опубликована: Апрель 29, 2024
Abstract
The
development
of
high‐performance
electrocatalysts
for
energy
conversion
reactions
is
crucial
advancing
global
sustainability.
design
catalysts
based
on
their
electronic
properties
(e.g.,
work
function)
has
gained
significant
attention
recently.
Although
numerous
reviews
electrocatalysis
have
been
provided,
no
such
reports
function‐guided
electrocatalyst
are
available.
Herein,
a
comprehensive
summary
the
latest
advancements
in
diverse
electrochemical
applications
provided.
This
includes
function‐based
catalytic
activity
descriptors,
and
both
monolithic
heterostructural
catalysts.
measurement
function
first
discussed
descriptors
various
fully
analyzed.
Subsequently,
function‐regulated
material‐electrolyte
interfacial
electron
transfer
(IET)
employed
catalyst
design,
methods
regulating
optimizing
performance
discussed.
In
addition,
key
strategies
tuning
function‐governed
material‐material
IET
examined.
Finally,
perspectives
determination,
put
forward
to
guide
future
research.
paves
way
rational
efficient
sustainable
applications.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(12)
Опубликована: Янв. 30, 2024
Although
great
efforts
on
the
delicate
construction
of
a
built-in
electric
field
(BIEF)
to
modify
electronic
properties
active
sites
have
been
conducted,
substantial
impact
BIEF
coupled
with
electrode
potential
electrochemical
reactions
has
not
clearly
investigated.
Herein,
we
designed
an
alkaline
hydrogen
evolution
reaction
(HER)
catalyst
composed
heterogeneous
Ru-CoP
urchin
arrays
carbon
cloth
(Ru-CoP/CC)
strong
guidance
density
functional
theory
(DFT)
calculations.
Impressively,
despite
its
unsatisfactory
activity
at
10
mA
cm
Energy & Environmental Science,
Год журнала:
2024,
Номер
17(5), С. 1725 - 1755
Опубликована: Янв. 1, 2024
This
article
summarizes
the
regulation
strategies
of
Fe-based
MOFs-derived
electrocatalysts
for
ZABs,
and
provides
a
prospect
their
future
development.
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.
