Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Дек. 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.
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(30)
Опубликована: Май 27, 2024
Abstract
Electrochemical
water
splitting
is
a
promising
technique
for
the
production
of
high‐purity
hydrogen.
Substituting
slow
anodic
oxygen
evolution
reaction
with
an
oxidation
that
thermodynamically
more
favorable
enables
energy‐efficient
Moreover,
this
approach
facilitates
degradation
environmental
pollutants
and
synthesis
value‐added
chemicals
through
rational
selection
small
molecules
as
substrates.
Strategies
small‐molecule
electrocatalyst
design
are
critical
to
electrocatalytic
performance,
focus
on
achieving
high
current
density,
selectivity,
Faradaic
efficiency,
operational
durability.
This
perspective
discusses
key
factors
required
further
advancement,
including
technoeconomic
analysis,
new
reactor
system
design,
meeting
requirements
industrial
applications,
bridging
gap
between
fundamental
research
practical
product
detection
separation.
aims
advance
development
hybrid
electrolysis
applications.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Апрель 18, 2024
Abstract
Local
electron
density
manipulation
can
optimize
the
adsorption
and
desorption
nature
of
catalysts
leading
to
enhanced
catalytic
activity
for
water
oxidation.
Construction
a
Mott–Schottky
barrier
allows
transition
in
because
their
different
Fermi
levels.
Herein,
Pt@NiFc‐MOF
heterojunction
is
constructed,
which
electrons
are
transferred
from
NiFc‐MOF
Pt
as
triggered
by
formed
built‐in
electric
field
at
interface.
The
as‐prepared
reveals
exceptional
performance
toward
hydrazine
oxidation
reaction
(HzOR),
hydrogen
evolution
(HER),
overall
splitting
(OHzS)
ampere‐level
current
densities.
advanced
configured
also
be
further
evidenced
concept
direct
liquid
N
2
H
4
/H
O
fuel
cell
(Pt@NiFc‐MOF//Pt
Net),
yielding
maximum
power
415.2
mW
cm
‒2
80°C
work
stably
190
h
500
mA
(at
25°C).
One
more
function
clarified
well,
that
it
purify
hydrazine‐rich
wastewater
718
6
ppb
(less
than
U.S.
Environmental
Protection
Agency
10
ppb)
120
min
.
This
represents
breakthrough
interface
engineering
metal–organic
frameworks
(MOFs)
industry‐level
generation
its
beyond.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Июль 14, 2024
Abstract
Electrochemical
urea
oxidation
offers
a
sustainable
avenue
for
H
2
production
and
wastewater
denitrification
within
the
water-energy
nexus;
however,
its
wide
application
is
limited
by
detrimental
cyanate
or
nitrite
instead
of
innocuous
N
.
Herein
we
demonstrate
that
atomically
isolated
asymmetric
Ni–O–Ti
sites
on
Ti
foam
anode
achieve
selectivity
99%,
surpassing
connected
symmetric
Ni–O–Ni
counterparts
in
documented
Ni-based
electrocatalysts
with
below
55%,
also
deliver
evolution
rate
22.0
mL
h
–1
when
coupled
to
Pt
counter
cathode
under
213
mA
cm
–2
at
1.40
V
RHE
These
sites,
featuring
oxygenophilic
adjacent
Ni,
favor
interaction
carbonyl
over
amino
groups
urea,
thus
preventing
premature
resonant
C⎓N
bond
breakage
before
intramolecular
N–N
coupling
towards
evolution.
A
prototype
device
powered
commercial
Si
photovoltaic
cell
further
developed
solar-powered
on-site
urine
processing
decentralized
production.
Inorganic Chemistry,
Год журнала:
2024,
Номер
63(12), С. 5642 - 5651
Опубликована: Март 12, 2024
Urea
oxidation
reaction
(UOR)
is
one
of
the
potential
routes
in
which
urea-rich
wastewater
used
as
a
source
energy
for
hydrogen
production.
Metal–organic
frameworks
(MOFs)
have
promising
applications
electrocatalytic
processes,
although
there
are
still
challenges
identifying
MOFs'
molecular
regulation
and
obtaining
practical
catalytic
systems.
The
current
study
sought
to
synthesize
[Zn6(IDC)4(OH)2(Hprz)2]n
(Zn-MOF)
with
three
symmetrically
independent
Zn(II)
cations
connected
via
linear
N-donor
piperazine
(Hprz),
rigid
planar
imidazole-4,5-dicarboxylate
(IDC3–),
−OH
ligands,
revealing
3,4T1
topology.
optimized
noble-metal-free
Zn0.33V0.66-MOF/NF
electrocatalysts
show
higher
robustness
performance
compared
those
parent
Zn
monometallic
MOF/NF
electrode
other
bimetallic
MOFs
different
Zn–V
molar
ratios.
low
1.42
V
(vs
RHE)
at
50
mA
cm–2
1.0
M
KOH
0.33
urea
required
by
developed
Zn0.33V0.66-MOF
makes
its
application
UOR
more
feasible.
availability
exposed
active
sites,
ion
diffusion
path,
conductivity
result
from
distinctive
configuration
synthesized
electrocatalyst,
highly
stable
capable
synergistic
effects,
consequently
enhancing
desired
reaction.
research
contributes
introducing
practical,
cost-effective,
sustainable
solution
decompose
produce
hydrogen.
Catalysis Reviews,
Год журнала:
2024,
Номер
unknown, С. 1 - 61
Опубликована: Май 28, 2024
Nowadays,
extensive
efforts
have
been
devoted
to
the
fabrication
and
design
of
metalbased
catalysts
with
high
activity,
selectivity,
stability.
Theoretical
experimental
investigations
empowered
construction
a
variety
techniques
tune
catalytic
efficiency
by
monitoring
their
size,
morphology,
composition,
crystal
structure.
Multimetal
(MMCs)
provide
revolutionary
synergistic
effect
between
metals,
which
is
promising
strategy
enhance
catalysts'
productivity
product
selectivity.
The
purpose
this
article
familiarize
readers
most
uptodate
information
regarding
synthesis
classification
MMCs.
key
roles
MMCs
electrocatalysts
in
applications
such
as
CO2
conversion
via
electrochemical
reduction
reaction
(ECO2RR),
H2
evolution
(HER),
O2
(OER),
(ORR),
N2
(NRR),
methanol
oxidation
(MOR),
ethanol
(EOR),
formic
acid
(FAOR),
urea
(UOR)
are
summarized.
This
review
also
addressed
challenges
prospects
for
multimetallic
catalyst
design,
characterization,
applications.
will
clear
roadmap
research
progress
electrocatalytic
ACS Nano,
Год журнала:
2024,
Номер
18(52), С. 35654 - 35670
Опубликована: Дек. 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
