Environmental Science & Technology,
Год журнала:
2024,
Номер
58(8), С. 4008 - 4018
Опубликована: Фев. 13, 2024
The
electrocatalytic
hydrodehalogenation
(EHDH)
process
mediated
by
atomic
hydrogen
(H*)
is
recognized
as
an
efficient
method
for
degrading
halogenated
organic
pollutants
(HOPs).
However,
a
significant
challenge
the
excessive
energy
consumption
resulting
from
recombination
of
H*
to
H2
production
in
EHDH
process.
In
this
study,
promising
strategy
was
proposed
generate
piezo-induced
H*,
without
external
input
or
chemical
consumption,
degradation
and
dehalogenation
HOPs.
Specifically,
sub-5
nm
Ni
nanoparticles
were
subtly
dotted
on
N-doped
carbon
layer
coating
BaTiO3
cube,
resulted
hybrid
nanocomposite
(Ni-NC@BTO)
can
effectively
break
C-X
(X
=
Cl
F)
bonds
under
ultrasonic
vibration
mechanical
stirring,
demonstrating
high
piezoelectric
driven
efficiencies
toward
various
Mechanistic
studies
revealed
that
efficiently
capture
form
Ni–H*
(Habs)
drive
lower
toxicity
intermediates.
COMSOL
simulations
confirmed
"chimney
effect"
interface
nanoparticle,
which
facilitated
accumulation
H+
enhanced
electron
transfer
formation
improving
surface
charge
piezocatalyst
strengthening
interfacial
electric
field.
Our
work
introduces
environmentally
friendly
HOPs
using
independent
consumption.
Environmental Science & Technology,
Год журнала:
2024,
Номер
58(4), С. 2144 - 2152
Опубликована: Янв. 18, 2024
The
electrocatalytic
nitrate
reduction
reaction
(NO3RR)
has
recently
emerged
as
a
promising
technique
for
readily
converting
aqueous
(NO3–)
pollutants
into
valuable
ammonia
(NH3).
It
is
vital
to
thoroughly
understand
the
mechanism
of
rationally
design
and
construct
advanced
systems
that
can
effectively
selectively
drive
NO3RR.
There
are
several
natural
enzymes
incorporate
molybdenum
(Mo)
activate
NO3–.
Based
on
this,
cadmium
(Cd)
single-atom
anchored
Mo2TiC2Tx
electrocatalyst
(referred
CdSA-Mo2TiC2Tx)
through
NO3RR
generate
NH3
was
designed
demonstrated.
In
an
H-type
electrolysis
cell
at
current
density
42.5
mA
cm–2,
had
Faradaic
efficiency
>95%
impressive
yield
rate
48.5
mg
h–1
cm–2.
Moreover,
conversion
NO3–
CdSA-Mo2TiC2Tx
surface
further
revealed
by
operando
attenuated
total
reflection
Fourier-transform
infrared
spectroscopy
electrochemical
differential
mass
spectrometer.
significantly
outperformed
well
reported
state-of-the-art
catalysts.
Density
functional
theory
calculations
decreased
ability
d-p
orbital
hybridize
with
NH3*
intermediates,
thereby
decreasing
activation
energy
potential-determining
step.
This
work
not
only
highlights
application
prospects
heavy
metal
catalysts
in
but
also
provides
examples
bio-inspired
electrocatalysts
synthesis
NH3.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(45)
Опубликована: Май 28, 2024
Abstract
The
past
decades
have
seen
considerable
imbalances
in
the
nitrogen
cycle
due
to
excessive
use
of
nitrate
agriculture
and
industry.
Electrocatalytic
reduction
(NO
3
RR)
(N
2
)
holds
significant
potential
for
addressing
pollution
wastewater
but
suffers
from
nitrite
formation
sluggish
hydrogeneration
process.
Here
a
single
atom
alloy
(SAA)
catalyst
featuring
atomically
dispersed
Ru
on
2D
Ni
metal
(Ru
1
Ni),
proving
remarkable
performance
−
–N
conversion
(≈93%)
N
selectivity
(≈99%))
through
co‐catalytic
metal‐support
interactions
(CMSI)
effect
is
reported.
Significantly,
SAA
achieves
NO
RR
removal
capacity
as
high
11.1
mg
L
−1
h
cm
−2
with
20
cycles
stability
(9
per
cycle),
surpassing
most
previously
reported
works.
core
boosting
lies
synergistically
promoted
activation
accelerated
hydrogenation
oxide
intermediates
site
substrate,
respectively,
revealed
by
various
situ
experiments
theoretical
simulations.
DFT
calculations
indicate
electron
transfer
substrate
more
robust
interaction
between
Ru–Ni
comparison
that
Ni–Ni.
This
work
offers
resilient
methodology
rational
design
highly
efficient
electrocatalysts
CMSI
modulation
RR,
illuminating
arena
treatment
cycle.
Environmental Science & Technology,
Год журнала:
2024,
Номер
58(8), С. 4008 - 4018
Опубликована: Фев. 13, 2024
The
electrocatalytic
hydrodehalogenation
(EHDH)
process
mediated
by
atomic
hydrogen
(H*)
is
recognized
as
an
efficient
method
for
degrading
halogenated
organic
pollutants
(HOPs).
However,
a
significant
challenge
the
excessive
energy
consumption
resulting
from
recombination
of
H*
to
H2
production
in
EHDH
process.
In
this
study,
promising
strategy
was
proposed
generate
piezo-induced
H*,
without
external
input
or
chemical
consumption,
degradation
and
dehalogenation
HOPs.
Specifically,
sub-5
nm
Ni
nanoparticles
were
subtly
dotted
on
N-doped
carbon
layer
coating
BaTiO3
cube,
resulted
hybrid
nanocomposite
(Ni-NC@BTO)
can
effectively
break
C-X
(X
=
Cl
F)
bonds
under
ultrasonic
vibration
mechanical
stirring,
demonstrating
high
piezoelectric
driven
efficiencies
toward
various
Mechanistic
studies
revealed
that
efficiently
capture
form
Ni–H*
(Habs)
drive
lower
toxicity
intermediates.
COMSOL
simulations
confirmed
"chimney
effect"
interface
nanoparticle,
which
facilitated
accumulation
H+
enhanced
electron
transfer
formation
improving
surface
charge
piezocatalyst
strengthening
interfacial
electric
field.
Our
work
introduces
environmentally
friendly
HOPs
using
independent
consumption.
