Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Июль 22, 2024
Abstract
Hydrogen
production
from
seawater
remains
challenging
due
to
the
deactivation
of
hydrogen
evolution
reaction
(HER)
electrode
under
high
current
density.
To
overcome
activity-stability
trade-offs
in
transition-metal
sulfides,
we
propose
a
strategy
engineer
sulfur
migration
by
constructing
nickel-cobalt
sulfides
heterostructure
with
nitrogen-doped
carbon
shell
encapsulation
(CN@NiCoS)
electrocatalyst.
State-of-the-art
ex
situ
/
characterizations
and
density
functional
theory
calculations
reveal
restructuring
CN@NiCoS
interface,
clearly
identifying
dynamic
migration.
The
NiCoS
stimulates
creating
vacancies
at
Ni
3
S
2
-Co
9
8
heterointerface,
while
migrated
atoms
are
subsequently
captured
CN
via
strong
C-S
bond,
preventing
sulfide
dissolution
into
alkaline
electrolyte.
Remarkably,
dynamically
formed
sulfur-doped
pairing
sites
significantly
enhances
HER
activity
altering
d
-band
center
near
Fermi
level,
resulting
low
overpotential
4.6
mV
10
mA
cm
−2
freshwater
media,
long-term
stability
up
1000
h.
This
work
thus
provides
guidance
for
design
high-performance
electrocatalyst
engineering
interfacial
atomic
Energy & Environmental Science,
Год журнала:
2022,
Номер
16(3), С. 1035 - 1048
Опубликована: Дек. 21, 2022
A
Pt
1
/(Co,Ni)(OH)
2
/C
single-atom
electro-catalyst
efficiently
splits
water
for
H
generation,
via
balanced
water-dissociation
and
-formation
steps
from
the
synergistic
effect
of
surface-defective
(Co,Ni)(OH)
electronically
tuned
sites.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(14)
Опубликована: Фев. 9, 2023
Oxygen
vacancies-enriched
black
TiO2
is
one
promising
support
for
enhancing
hydrogen
evolution
reaction
(HER).
Herein,
oxygen
vacancies
enriched
supported
sub-nanometer
Pt
clusters
(Pt/TiO2
-OV
)
with
metal
interactions
designed
through
solvent-free
microwave
and
following
low-temperature
electroless
approach
the
first
time.
High-temperature
strong
reductants
are
not
required
then
can
avoid
aggregation
of
decorated
species.
Experimental
theoretical
calculation
verify
that
created
exhibit
synergistic
effects
optimizing
kinetics.
Based
on
it,
Pt/TiO2
presents
remarkable
electrocatalytic
performance
18
mV
to
achieve
10
mA
cm-2
coupled
small
Tafel
slope
12
dec-1
.
This
work
provides
quick
synthetic
strategy
preparing
titanium
dioxide
based
nanomaterials.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(24)
Опубликована: Март 21, 2023
The
development
of
productive
catalysts
for
the
oxygen
evolution
reaction
(OER)
remains
a
major
challenge
requiring
significant
progress
in
both
mechanism
and
material
design.
Conventionally,
thermodynamic
barrier
lattice
oxidation
(LOM)
is
lower
than
that
absorbate
(AEM)
because
former
can
overcome
certain
limitations.
However,
controlling
OER
pathway
from
AEM
to
LOM
by
exploiting
intrinsic
properties
catalyst
challenging.
Herein,
we
incorporated
F
anions
into
vacancies
spinel
ZnCo2
O4
established
link
between
electronic
structure
catalytic
mechanism.
Theoretical
density
calculations
revealed
upshifts
O
2p
center
activates
redox
capability
O,
successfully
triggering
pathway.
Moreover,
high
electronegativity
favourable
balancing
residual
protonation,
which
stabilize
catalyst.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(42)
Опубликована: Сен. 2, 2023
Abstract
Designing
novel
single‐atom
catalysts
(SACs)
supports
to
modulate
the
electronic
structure
is
crucial
optimize
catalytic
activity,
but
rather
challenging.
Herein,
a
general
strategy
proposed
utilize
metalloid
properties
of
trap
and
stabilize
single‐atoms
with
low‐valence
states.
A
series
supported
on
surface
tungsten
carbide
(M‐WC
x
,
M=Ru,
Ir,
Pd)
are
rationally
developed
through
facile
pyrolysis
method.
Benefiting
from
WC
exhibit
weak
coordination
W
C
atoms,
resulting
in
formation
active
centers
similar
metals.
The
unique
metal‐metal
interaction
effectively
stabilizes
single
atoms
improves
orbital
energy
level
distribution
sites.
As
expected,
representative
Ru‐WC
exhibits
superior
mass
activities
7.84
62.52
mg
Ru
−1
for
hydrogen
oxidation
evolution
reactions
(HOR/HER),
respectively.
In‐depth
mechanistic
analysis
demonstrates
that
an
ideal
dual‐sites
cooperative
mechanism
achieves
suitable
adsorption
balance
H
ad
OH
energetically
favorable
Volmer
step.
This
work
offers
new
guidance
precise
construction
highly
SACs.
Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Июнь 24, 2023
Designing
Pt-based
electrocatalysts
with
high
catalytic
activity
and
CO
tolerance
is
challenging
but
extremely
desirable
for
alkaline
hydrogen
oxidation
reaction.
Herein
we
report
the
design
of
a
series
single-atom
lanthanide
(La,
Ce,
Pr,
Nd,
Lu)-embedded
ultrasmall
Pt
nanoclusters
efficient
electro-oxidation
catalysis
based
on
vapor
filling
spatially
confined
reduction/growth
metal
species.
Mechanism
studies
reveal
that
oxophilic
species
in
can
serve
as
Lewis
acid
site
selective
OH-
adsorption
regulate
binding
strength
intermediates
sites,
which
promotes
kinetics
by
accelerating
combination
*H/*CO
thermodynamics,
endowing
electrocatalyst
up
to
14.3-times
higher
mass
than
commercial
Pt/C
enhanced
tolerance.
This
work
may
shed
light
nanocluster-based
energy
conversion.
ACS Catalysis,
Год журнала:
2023,
Номер
13(16), С. 10672 - 10682
Опубликована: Июль 31, 2023
The
acidic
water-splitting
technology
based
on
the
polymer
exchange
membrane
can
produce
hydrogen
efficiently,
continuously,
and
cleanly,
which
is
expected
to
alleviate
energy
crisis.
However,
even
noble
metal-based
electrocatalysts
such
as
IrOx
species
would
dissolve
rapidly
during
oxygen
evolution.
Herein,
we
successfully
assemble
high-density
carbon
nanotubes
(CNTs)
encapsulated
with
IrCo
nanoparticles
(NPs)
cloth
(IrCo@CNT/CC)
using
a
facile
MOF-templated
dicyandiamide-assisted
pyrolysis
strategy.
Benefiting
from
favorable
synergistic
effect
between
Co
Ir
protection
of
CNT,
obtained
IrCo@CNT/CC
only
requires
low
cell
voltage
1.500
V
reach
10
mA
cm–2
for
water
splitting
an
extremely
loading
0.027
mg
exhibits
robust
stability
under
continuous
electrolysis
90
h
in
0.5
M
H2SO4,
ranking
it
among
one
best
bifunctional
splitting.
Detailed
experiments
reveal
that
CNT-encapsulated
NPs
remain
after
evolution
reaction
(HER)
but
transform
into
Co-doped
IrO2
(OER).
Further
DFT
simulation
calculations
confirm
doping
optimize
their
electronic
structures
lower
barriers
HER
OER,
respectively.
Advanced Functional Materials,
Год журнала:
2023,
Номер
34(6)
Опубликована: Ноя. 7, 2023
Abstract
Construction
of
efficient
catalysts
to
couple
biomass
upgrading
with
hydrogen
production
is
significant
for
improving
energy
efficiency,
which
remains
a
challenge.
Herein,
general
method
manufacturing
3D
hierarchical
micro‐nano
arrays
consisting
template
framework
and
nanoparticle‐decorated
nanosheets
reported.
This
strategy
provides
an
opportunity
controllably
tailor
the
interfacial
assembly
on
precursor
materials.
The
obtained
Co@NiMoO‐Ni/NF
exhibits
enhanced
electrocatalytic
performance
oxidation
production.
It
only
needs
1.21
V
achieve
10
mA
cm
−2
5‐hydroxymethylfurfural
electrooxidation
reaction
(HMFOR)
assisted
H
2
evolution
(HER).
good
catalytic
ascribed
intense
interaction
between
(Co)
(NiMoO‐Ni),
tunes
electron
structure
catalyst
optimize
adsorption
behavior
HMFOR/HER
intermediates
promote
bonds
breakage
key
in
process.
work
thus
designing
ideal
upgrading‐coupled
