Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 23, 2024
Abstract
Inhibiting
the
deactivation
of
nickel‐based
catalysts
caused
by
self‐oxidation
and
competitive
adsorption
behavior
is
still
a
major
challenge
for
urea
oxidation
reaction
(UOR),
especially
under
industrial‐level
current
densities.
In
this
study,
crystalline
NiSe
2
/amorphous
NiFe‐LDH
(NiSe
/NiFe‐LDH)
heterojunction
catalyst
rationally
constructed
selective
electrocatalytic
UOR.
situ
Raman
spectra
ex
characterization
results
reveal
that
such
structure
can
tailor
impede
accumulation
NiOOH
species
during
UOR
process.
Density
function
theory
simulations
disclose
self‐driven
charge
transport
from
electron‐deficient
region
to
electron‐rich
would
induce
formation
local
electrophilic/nucleophilic
adsorb
electron‐donating
‐NH
electron‐withdrawing
C
=
O
groups,
respectively.
This
optimizes
molecules
hinders
overaccumulation
OH
−
ions
on
surface
/NiFe‐LDH,
which
beneficial
priority
occurrence
over
oxygen
evolution
(OER)
realization
high
selectivity.
Benefiting
tailored
favorable
adsorption,
/NiFe‐LDH
could
act
as
high‐selective
anode
achieve
ultrahigh
800
mAcm
−2
only
at
1.447
V.
Besides,
UV–vis
spectrophotometry
also
unveiled
has
capability
electrochemically
degrade
urea,
offering
great
promise
practical
application
potentials.
ACS Nano,
Journal Year:
2024,
Volume and Issue:
18(52), P. 35654 - 35670
Published: Dec. 11, 2024
Replacing
the
oxygen
evolution
reaction
(OER)
with
urea
oxidation
(UOR)
in
conjunction
hydrogen
(HER)
offers
a
feasible
and
environmentally
friendly
approach
for
handling
urea-rich
wastewater
generating
energy-saving
hydrogen.
However,
deactivation
detachment
of
active
sites
powder
electrocatalysts
reported
hitherto
present
significant
challenges
to
achieving
high
efficiency
sustainability
production.
Herein,
self-supported
bimetallic
nickel
manganese
metal–organic
framework
(NiMn-MOF)
nanosheet
its
derived
heterostructure
composed
NiMn-MOF
decorated
ultrafine
Pt
nanocrystals
(PtNC/NiMn-MOF)
are
rationally
designed.
By
leveraging
synergistic
effect
Mn
Ni,
along
strong
electronic
interaction
between
PtNC
at
interface,
optimized
catalysts
(NiMn-MOF
PtNC/NiMn-MOF)
exhibit
substantially
reduced
potentials
1.459
−0.129
V
reach
1000
mA
cm–2
during
UOR
HER.
Theoretical
calculations
confirm
that
Mn-doping
heterointerface
regulate
d-band
center
catalyst,
which
turn
enhances
electron
transfer
facilitates
charge
redistribution.
This
manipulation
optimizes
adsorption/desorption
energies
reactants
intermediates
both
HER
UOR,
thereby
significantly
reducing
energy
barrier
rate-determining
step
(RDS)
enhancing
electrocatalytic
performance.
Furthermore,
degradation
rates
PtNC/NiMn-MOF
(96.1%)
(90.3%)
higher
than
those
Ni-MOF
most
advanced
catalysts.
work
provides
valuable
insights
designing
applicable
treatment
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 23, 2024
Abstract
Inhibiting
the
deactivation
of
nickel‐based
catalysts
caused
by
self‐oxidation
and
competitive
adsorption
behavior
is
still
a
major
challenge
for
urea
oxidation
reaction
(UOR),
especially
under
industrial‐level
current
densities.
In
this
study,
crystalline
NiSe
2
/amorphous
NiFe‐LDH
(NiSe
/NiFe‐LDH)
heterojunction
catalyst
rationally
constructed
selective
electrocatalytic
UOR.
situ
Raman
spectra
ex
characterization
results
reveal
that
such
structure
can
tailor
impede
accumulation
NiOOH
species
during
UOR
process.
Density
function
theory
simulations
disclose
self‐driven
charge
transport
from
electron‐deficient
region
to
electron‐rich
would
induce
formation
local
electrophilic/nucleophilic
adsorb
electron‐donating
‐NH
electron‐withdrawing
C
=
O
groups,
respectively.
This
optimizes
molecules
hinders
overaccumulation
OH
−
ions
on
surface
/NiFe‐LDH,
which
beneficial
priority
occurrence
over
oxygen
evolution
(OER)
realization
high
selectivity.
Benefiting
tailored
favorable
adsorption,
/NiFe‐LDH
could
act
as
high‐selective
anode
achieve
ultrahigh
800
mAcm
−2
only
at
1.447
V.
Besides,
UV–vis
spectrophotometry
also
unveiled
has
capability
electrochemically
degrade
urea,
offering
great
promise
practical
application
potentials.