ACS Nano,
Journal Year:
2024,
Volume and Issue:
18(8), P. 6202 - 6214
Published: Feb. 12, 2024
The
development
of
cost-effective
electrocatalysts
with
an
optimal
surface
affinity
for
intermediates
is
essential
sustainable
hydrogen
fuel
production,
but
this
remains
insufficient.
Here
we
synthesize
Ni2P/MoS2-CoMo2S4@C
heterometallic
based
on
the
high-nuclearity
cluster
{Co24(TC4A)6(MoO4)8Cl6},
in
which
Ni2P
nanoparticles
were
anchored
to
MoS2-CoMo2S4@C
nanosheets
via
strong
interfacial
interactions.
Theoretical
calculations
revealed
that
introduction
phases
induces
significant
disturbances
electronic
configuration
Ni2P/MoS2-CoMo2S4@C,
resulting
more
relaxed
d–d
orbital
electron
transfers
between
metal
atoms.
Moreover,
continuous
transport
was
established
by
formation
multiple
heterojunction
interfaces.
optimized
electrocatalyst
exhibited
ultralow
overpotentials
198
and
73
mV
oxygen
evolution
reactions,
respectively,
alkaline
media,
at
10
mA
cm–2.
alkali
electrolyzer
constructed
using
required
a
cell
voltage
only
1.45
V
(10
cm–2)
drive
overall
water
splitting
excellent
long-term
stability.
Energy & Environmental Science,
Journal Year:
2023,
Volume and Issue:
17(1), P. 49 - 113
Published: Nov. 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.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(43)
Published: Sept. 6, 2023
Metal-organic
frameworks
(MOFs)
have
been
increasingly
applied
in
oxygen
evolution
reaction
(OER),
and
the
surface
of
MOFs
usually
undergoes
structural
transformation
to
form
metal
oxyhydroxides
serve
as
catalytically
active
sites.
However,
controllable
regulation
reconstruction
process
remains
a
great
challenge.
Here
we
report
defect
engineering
strategy
facilitate
during
OER
with
enhanced
activity.
Defective
(denoted
NiFc'x
Fc1-x
)
abundant
unsaturated
sites
are
constructed
by
mixing
ligands
1,1'-ferrocene
dicarboxylic
acid
(Fc')
defective
ferrocene
carboxylic
(Fc).
series
more
prone
be
transformed
compared
non-defective
(NiFc').
Moreover,
as-formed
derived
from
contain
vacancies.
NiFc'Fc
grown
on
nickel
foam
exhibits
excellent
catalytic
activity
an
overpotential
213
mV
at
current
density
100
mA
cm-2
,
superior
that
undefective
NiFc'.
Experimental
results
theoretical
calculations
suggest
vacancies
adsorption
oxygen-containing
intermediates
centers,
thus
significantly
improving
Advanced Energy Materials,
Journal Year:
2023,
Volume and Issue:
14(9)
Published: Dec. 27, 2023
Abstract
Lithium–sulfur
batteries
(Li–S)
are
recognized
as
the
next
generation
of
secondary
due
to
their
satisfactory
theoretical
specific
capacity
and
energy
density.
However,
a
series
problems
such
disordered
migration
behavior,
sluggish
redox
kinetics,
serious
shuttle
effect
lithium
polysulfides
(LiPSs)
greatly
limit
commercial
application.
Herein,
nanoreactors
encapsulate
heterostructure
guarantee
sulfur
conversion
in
hosts
where
consists
FeP
with
moderate
adsorption
ability,
excellent
catalytic
active
low
work
function,
Fe
3
O
4
strong
ability
high
function.
This
rational
configuration
controls
direction
interface
built‐in
electric
field
(BIEF)
between
catalyst
adsorbent,
realizing
successive
“trapping‐directional
migration‐conversion”
reaction
mechanism
species.
Thanks
BIEF
bridge
connect
trapping
site
site,
/FeP@C─S
cathode
delivers
an
ultrahigh
initial
1402
mAh
g
−1
at
0.1
C
remains
more
than
450
5
after
350
cycles.
Even
loading
5.20
mg
cm
−2
,
it
displayed
970
.
provided
effective
strategy
design
high‐performance
electrocatalysts
for
Li–S
batteries.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(16)
Published: Feb. 29, 2024
Abstract
Alkaline
water
electrolysis
(AWE)
plays
a
crucial
role
in
the
realization
of
hydrogen
economy.
The
design
and
development
efficient
stable
bifunctional
catalysts
for
both
evolution
reaction
(HER)
oxygen
(OER)
are
pivotal
to
achieving
high‐efficiency
AWE.
Herein,
WC
1‐x
/Mo
2
C
nanoparticle‐embedded
carbon
nanofiber
(WC
C@CNF)
with
abundant
interfaces
is
successfully
designed
synthesized.
Benefiting
from
electron
transfer
behavior
Mo
,
electrocatalysts
C@CNF
exhibit
superior
HER
OER
performance.
Furthermore,
when
employed
as
anode
cathode
membrane
electrode
assembly
devices,
catalyst
exhibits
enhanced
catalytic
activity
remarkable
stability
100
hours
at
high
current
density
200
mA
cm
−2
towards
overall
splitting.
experimental
characterizations
theoretical
simulation
reveal
that
modulation
d‐band
center
C@CNF,
achieved
through
asymmetric
charge
distribution
resulting
built‐in
electric
field
induced
by
work
function,
enables
optimization
adsorption
strength
hydrogen/oxygen
intermediates,
thereby
promoting
kinetics
This
provides
promising
strategies
designing
highly
active
energy
conversion
fields.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
36(1)
Published: Sept. 23, 2023
Abstract
Developing
bifunctional
electrocatalyst
for
seawater
splitting
remains
a
persistent
challenge.
Herein,
an
approach
is
proposed
through
density
functional
theory
(DFT)
preanalysis
to
manipulate
electron
redistribution
in
Ni
2
P
addressed
by
cation
doping
and
vacancy
engineering.
The
needle‐like
Fe‐doped
with
(Fe‐Ni
Pv)
successfully
synthesized
on
nickel
foam,
exhibiting
superior
hydrogen
evolution
reaction
(HER)
oxygen
(OER)
catalytic
activity
electrolysis
alkaline
condition.
As
result,
Fe‐Ni
Pv
achieves
the
industrially
required
current
densities
of
1.0
3.0
A
cm
−2
at
low
voltages
1.68
1.73
V,
respectively,
60
°C
6.0
m
KOH
circumstances.
theoretical
calculation
experimental
results
collectively
reveal
reasons
enhancement
catalyst
activity.
Specifically,
Fe
vacancies
can
accelerate
reconstruction
OER
active
species
optimize
adsorption
free
energy
(Δ
G
H*
)
HER.
In
addition,
sites
are
identified,
where
greatly
improve
electrical
conductivity
dominant
centers,
meanwhile
atoms
as
centers
study
provides
deep
insight
into
exploration
nickel‐based
phosphide
catalysts
identification
their
real
centers.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(38)
Published: Aug. 1, 2023
The
complexes
of
metal
center
and
nitrogen
ligands
are
the
most
representative
systems
for
catalyzing
hydrogenation
reactions
in
small
molecule
conversion.
Developing
heterogeneous
catalysts
with
similar
active
metal-nitrogen
functional
centers,
nevertheless,
still
remains
challenging.
In
this
work,
we
demonstrate
that
coupling
anti-perovskite
Co4
N
can
be
effective
modulated
by
Cu
doping
to
form
Co3
CuN,
leading
strongly
promoted
process
during
electrochemical
reduction
nitrate
(NO3-
RR)
ammonia.
combination
advanced
spectroscopic
techniques
density
theory
calculations
reveal
dopants
strengthen
Co-N
bond
upshifted
d-band
towards
Fermi
level,
promoting
adsorption
NO3-
*H
facilitating
transition
from
*NO2
/*NO
H/*NOH.
Consequently,
CuN
delivers
noticeably
better
RR
activity
than
pristine
N,
optimal
Faradaic
efficiency
97
%
ammonia
yield
455.3
mmol
h-1
cm-2
at
-0.3
V
vs.
RHE.
This
work
provides
an
strategy
developing
high-performance
catalyst
synthesis.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
36(29)
Published: April 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.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(34)
Published: March 13, 2024
Abstract
The
proton
exchange
membrane
water
electrolysis
system
has
long
been
considered
a
promising
technique
for
the
generation
of
hydrogen
owing
to
its
high
electrolytic
efficiency,
reliability,
and
quick
response
renewable
energy
sources.
At
present,
noble
metals
their
oxides
(e.g.,
Pt,
IrO
2
,
RuO
)
are
widely
used
as
active
electrocatalysts
accelerating
conversion
efficiency
process,
especially
in
acidic
media.
Nevertheless,
scarcity
instability
seriously
impede
large‐scale
application
practice.
In
past
years,
metal‐organic
frameworks
(MOFs)
have
proven
be
an
ideal
platform
designing
efficient
cost‐effective
electrodes
due
unique
physicochemical
properties.
this
review,
fundamental
catalytic
mechanisms
evolution
reaction
(HER)
oxygen
(OER)
media
discussed
first.
Then,
design
strategies
advanced
characterizations
MOF‐based
water‐splitting
catalysts
summarized.
Finally,
recent
research
advances
HER
OER
electrolytes,
along
with
current
challenges
future
opportunities,
provided.
Energy & Environmental Science,
Journal Year:
2024,
Volume and Issue:
17(14), P. 5260 - 5272
Published: Jan. 1, 2024
Self-supporting
Fe
2
O
3
–CeO
nano-heterojunction
electrodes
with
rich
oxygen
vacancies
present
high
catalytic
performance
for
evolution
reaction,
where
defect-engineering
promotes
the
interfacial
interaction
and
activates
lattice
oxygens.