ACS Applied Nano Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Дек. 19, 2024
Designing
an
affordable
catalyst
for
the
hydrogen
evolution
reaction
(HER)
in
alkaline
media
remains
a
major
challenge.
In
this
study,
we
synthesized
Ru-CoMoO4–x/NF
modified
with
ruthenium
nanoclusters
(Ru
NCs)
and
oxygen
vacancies
(Ovs),
using
nickel
foam
(NF)
as
substrate.
X-ray
photoelectron
spectroscopy
(XPS)
analysis
showed
that
introducing
Ru
effectively
catalyst's
electronic
structure.
A
carefully
controlled
concentration
of
enhanced
stability,
reduced
electrochemical
impedance,
promoted
kinetics,
thereby
improving
intrinsic
activity
Ru-CoMoO4–x/NF.
freshwater
medium,
displayed
low
overpotential
20
mV
to
achieve
current
density
−10
mA
cm–2,
Tafel
slope
41.54
dec–1.
The
maintained
stable
performance
minimal
degradation
after
100
h
constant
voltage
tests
180
multistep
tests.
Moreover,
overall
water-splitting
system,
Ru-CoMoO4–x/NF∥Ru-CoMoO4–x/NF
required
only
1.606
V
drive
−50
cm–2.
This
work
presents
viable
approach
enhancing
HER
electrocatalytic
nonprecious
metal
oxides
through
synergistic
effects
NCs
Ovs.
Advanced Science,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 7, 2025
Abstract
Overall
water
splitting
(OWS)
to
produce
hydrogen
has
attracted
large
attention
in
recent
years
due
its
ecological‐friendliness
and
sustainability.
However,
the
efficiency
of
OWS
been
forced
by
sluggish
kinetics
four‐electron
oxygen
evolution
reaction
(OER).
The
replacement
OER
alternative
electrooxidation
small
molecules
with
more
thermodynamically
favorable
potentials
may
fundamentally
break
limitation
achieve
production
low
energy
consumption,
which
also
be
accompanied
value‐added
chemicals
than
or
electrochemical
degradation
pollutants.
This
review
critically
assesses
latest
discoveries
coupled
various
OWS,
including
alcohols,
aldehydes,
amides,
urea,
hydrazine,
etc.
Emphasis
is
placed
on
corresponding
electrocatalyst
design
related
mechanisms
(e.g.,
dual
hydrogenation
N–N
bond
breaking
hydrazine
C═N
regulation
urea
inhibit
hazardous
NCO
−
NO
productions,
etc.),
along
emerging
reactions
(electrooxidation
tetrazoles,
furazans,
iodide,
quinolines,
ascorbic
acid,
sterol,
trimethylamine,
etc.).
Some
new
decoupled
electrolysis
self‐powered
systems
are
discussed
detail.
Finally,
potential
challenges
prospects
highlighted
aid
future
research
directions.
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Дек. 8, 2024
Abstract
Constructing
built‐in
electric
field
(BIEF)
in
heterojunction
catalyst
is
an
effective
way
to
optimize
adsorption/desorption
of
reaction
intermediates,
while
its
precise
tailor
achieve
efficient
bifunctional
electrocatalysis
remains
great
challenge.
Herein,
the
hollow
Mo/MoS
Vn
nanoreactors
with
tunable
BIEFs
are
elaborately
prepared
simultaneously
promote
hydrogen
evolution
(HER)
and
urea
oxidation
(UOR)
for
sustainable
production.
The
BIEF
induced
by
sulfur
vacancies
can
be
modulated
from
0.79
0.57
0.42
mV
nm
−1
,
exhibits
a
parabola‐shaped
relationship
HER
UOR
activities,
V1
nanoreactor
moderate
presents
best
activity.
Theoretical
calculations
reveal
that
evidently
facilitate
breakage
N─H
bond
UOR.
electrolyzer
assembled
delivers
cell
voltage
1.49
V
at
100
mA
cm
−2
which
437
lower
than
traditional
water
electrolysis,
also
excellent
durability
200
h.
Life
cycle
assessment
indicates
HER||UOR
system
possesses
notable
superiority
across
various
environment
impact
energy
consumption.
This
work
provide
theoretical
experimental
direction
on
rational
design
advanced
materials
energy‐saving
eco‐friendly
Advanced Energy Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 4, 2024
Abstract
Heterostructured
interfaces
are
crucial
to
electrocatalysts
for
water
splitting.
Herein,
coral‐like
multiheterostructured
Ni
x
B/Mo
0.8
B
3
(NMB)
nanorods
encapsulated
by
a
boron‐rich
amorphous
layer
prepared
Density‐functional
theory
(DFT)
calculations
indicate
that
the
NMB
interface
adjusts
d
‐band
center
and
electronic
structure
of
molybdenum
sites.
Owing
strong
coupling
between
Ni,
Mo,
at
heterojunction,
large
number
exposed
catalytic
active
sites,
as
well
special
hydrophilic
characteristics
endowed
surrounding
layer,
catalyst
exhibits
remarkable
universal‐pH
hydrogen
evolution
reaction
(HER)
activity
with
low
overpotentials
(
η
)
15,
26,
83
mV
deliver
10
mA
cm
−2
in
basic,
acid,
neutral
media,
respectively,
outstanding
oxygen
(OER)
basic
medium
500
170
420
mV,
respectively.
The
unique
self‐supporting
3D
hierarchical
interconnected
facilitates
mass
transport
thus
leading
high
mechanical
stability
450
200
h
HER
OER
≈1000
.
More
importantly,
excellent
performance
toward
overall‐water
electrolysis
bifunctional
ultralow
cell
voltages
1.45/1.56/1.85
V
@
10/100/1000
,
demonstrating
potential
industrial
splitting
applications.
Applied Physics Reviews,
Год журнала:
2025,
Номер
12(1)
Опубликована: Фев. 6, 2025
Electrochemical
reactions
are
pivotal
for
energy
conversion
and
storage
to
achieve
a
carbon-neutral
sustainable
society,
optimal
electrocatalysts
essential
their
industrial
applications.
Theoretical
modeling
methodologies,
such
as
density
functional
theory
(DFT)
molecular
dynamics
(MD),
efficiently
assess
electrochemical
reaction
mechanisms
electrocatalyst
performance
at
atomic
levels.
However,
its
intrinsic
algorithm
limitations
high
computational
costs
large-scale
systems
generate
gaps
between
experimental
observations
calculation
simulation,
restricting
the
accuracy
efficiency
of
design.
Combining
machine
learning
(ML)
is
promising
strategy
accelerate
development
electrocatalysts.
The
ML-DFT
frameworks
establish
accurate
property–structure–performance
relations
predict
verify
novel
electrocatalysts'
properties
performance,
providing
deep
understanding
mechanisms.
ML-based
methods
also
solution
MD
DFT.
Moreover,
integrating
ML
experiment
characterization
techniques
represents
cutting-edge
approach
insights
into
structural,
electronic,
chemical
changes
under
working
conditions.
This
review
will
summarize
DFT
current
application
status
design
in
various
conversions.
underlying
physical
fundaments,
advancements,
challenges
be
summarized.
Finally,
future
research
directions
prospects
proposed
guide
revolution.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 8, 2025
Electrochemical
H2
production
from
water
favors
low-voltage
molecular
oxidation
to
replace
the
oxygen
evolution
reaction
as
an
energy-saving
and
value-added
approach.
However,
there
exists
a
mismatch
between
high
demand
for
slow
anodic
reactions,
restricting
practical
applications
of
such
hybrid
systems.
Here,
we
propose
bipolar
approach,
with
generation
N–N
oxidatively
coupled
dehydrogenation
(OCD)
3,5-diamino-1H-1,2,4-triazole
(DAT),
in
addition
cathodic
generation.
The
system
requires
relatively
low
potentials
0.872
1.108
V
vs
RHE
reach
10
500
mA
cm–2,
respectively.
H-type
electrolyzer
only
0.946
1.129
deliver
100
respectively,
electricity
consumption
(1.3
kWh
per
m3
H2)
reduced
by
68%,
compared
conventional
splitting.
Moreover,
process
is
highly
appealing
due
absence
traditional
hazardous
synthetic
conditions
azo
compounds
at
anode
crossover/mixing
H2/O2
electrolyzer.
A
flow-type
operates
stably
cm–2
300
h.
Mechanistic
studies
reveal
that
Pt
single
atom
nanoparticle
(Pt1,n)
optimize
adsorption
S
active
sites
over
Pt1,n@VS2
catalysts.
At
anode,
stepwise
−NH2
DAT
then
oxidative
coupling
−N–N–
predominantly
form
while
generating
H2.
present
report
paves
new
way
atom-economical
aminotriazole
green
electrosynthesis
chemicals.
