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.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(31)
Опубликована: Май 21, 2024
Abstract
The
electrochemical
nitrate
reduction
reaction
(NO
3
RR)
is
able
to
convert
−
)
into
reusable
ammonia
(NH
),
offering
a
green
treatment
and
resource
utilization
strategy
of
wastewater
synthesis.
conversion
NO
NH
undergoes
water
dissociation
generate
active
hydrogen
atoms
nitrogen‐containing
intermediates
hydrogenation
tandemly.
two
relay
processes
compete
for
the
same
sites,
especially
under
pH‐neutral
condition,
resulting
in
suboptimal
efficiency
selectivity
electrosynthesis
from
.
Herein,
we
constructed
Cu
1
‐Fe
dual‐site
catalyst
by
anchoring
single
on
amorphous
iron
oxide
shell
nanoscale
zero‐valent
(nZVI)
RR,
achieving
an
impressive
removal
94.8
%
99.2
neutral
pH
concentration
50
mg
L
−1
−N
conditions,
greatly
surpassing
performance
nZVI
counterpart.
This
superior
can
be
attributed
synergistic
effect
enhanced
adsorption
Fe
sites
strengthened
activation
single‐atom
decreasing
energy
barrier
rate‐determining
step
*NO‐to‐*NOH.
work
develops
novel
fabricating
catalysts
enhance
,
presents
environmentally
sustainable
approach
treatment.
Abstract
Ammonia,
a
vital
component
in
the
synthesis
of
fertilizers,
plastics,
and
explosives,
is
traditionally
produced
via
energy‐intensive
environmentally
detrimental
Haber–Bosch
process.
Given
its
considerable
energy
consumption
significant
greenhouse
gas
emissions,
there
growing
shift
toward
electrocatalytic
ammonia
as
an
eco‐friendly
alternative.
However,
developing
efficient
electrocatalysts
capable
achieving
high
selectivity,
Faraday
efficiency,
yield
under
ambient
conditions
remains
challenge.
This
review
delves
into
decades‐long
research
synthesis,
highlighting
evolution
fundamental
principles,
theoretical
descriptors,
reaction
mechanisms.
An
in‐depth
analysis
nitrogen
reduction
(NRR)
nitrate
(NitRR)
provided,
with
focus
on
their
electrocatalysts.
Additionally,
theories
behind
electrocatalyst
design
for
are
examined,
including
Gibbs
free
approach,
Sabatier
principle,
d
‐band
center
theory,
orbital
spin
states.
The
culminates
comprehensive
overview
current
challenges
prospective
future
directions
development
NRR
NitRR,
paving
way
more
sustainable
methods
production.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(32)
Опубликована: Май 29, 2024
Abstract
Electrochemical
nitrate
reduction
reaction
(NO
3
RR)
is
a
promising
approach
to
achieve
remediation
of
nitrate‐polluted
wastewater
and
sustainable
production
ammonia.
However,
it
still
restricted
by
the
low
activity,
selectivity
Faraday
efficiency
for
ammonia
synthesis.
Herein,
we
propose
an
effective
strategy
modulate
electrolyte
microenvironment
in
electrical
double
layer
(EDL)
mediating
alkali
metal
cations
enhance
NO
RR
performance.
Taking
bulk
Cu
as
model
catalyst,
experimental
study
reveals
that
−
‐to‐NH
performance
different
electrolytes
follows
trend
Li
+
<Cs
<Na
<K
.
Theoretical
studies
illustrate
proton
transport
rate
activity
rate‐determining
step
2
)
increase
order
The
cation
effects
are
also
general
two
typical
nanostructured
catalysts
including
copper/cuprous
oxide
nickel
phosphides,
achieving
near‐100
%
Faradaic
over
99
conversion
NH
Furthermore,
demonstrate
can
be
converted
high‐purity
4
Cl
catalyst
K
‐containing
electrolyte.
Abstract
Electrochemical
conversion
of
nitrate,
a
prevalent
water
pollutant,
to
ammonia
(NH
3
)
is
delocalized
and
green
path
for
NH
production.
Despite
the
existence
different
nitrate
reduction
pathways,
selectively
directing
reaction
pathway
on
road
now
hindered
by
absence
efficient
catalysts.
Single‐atom
catalysts
(SACs)
are
extensively
investigated
in
wide
range
catalytic
processes.
However,
their
application
electrocatalytic
(NO
−
RR)
infrequent,
mostly
due
pronounced
inclination
toward
hydrogen
evolution
(HER).
Here,
Ni
single
atoms
electrochemically
active
carrier
boron,
nitrogen
doped‐graphene
(BNG)
matrix
modulate
atomic
coordination
structure
through
boron‐spanning
strategy
enhance
performance
NO
RR
designed.
Density
functional
theory
(DFT)
study
proposes
that
BNG
supports
with
ionic
characteristics,
offer
surplus
electric
field
effect
as
compared
N‐doped
graphene,
which
can
ease
adsorption.
Consistent
theoretical
studies,
as‐obtained
NiSA@BNG
shows
higher
activity
maximal
yield
rate
168
µg
h
−1
cm
−2
along
Faradaic
efficiency
95%
promising
electrochemical
stability.
This
reveals
novel
ways
rationally
fabricate
SACs'
tunable
electronic
properties
performance.
Energy & Environmental Science,
Год журнала:
2024,
Номер
17(13), С. 4582 - 4593
Опубликована: Янв. 1, 2024
The
synergistic
catalysis
effect
based
on
CoP
and
Cu
3
P
dual-function
active
sites
is
proposed
to
understand
the
mechanism
of
hydrogen
(*H)
adsorbed
intermediates
(*NO
x
)
during
water-splitting
nitrate
reduction.
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Сен. 11, 2024
Abstract
Electrochemical
nitrate
reduction
reaction
(NO
3
RR)
is
a
promising
approach
to
realize
ammonia
generation
and
wastewater
treatment.
However,
the
transformation
from
NO
−
NH
involves
multiple
proton‐coupled
electron
transfer
processes
by‐products
2
,
H
etc.),
making
high
selectivity
challenge.
Herein,
two‐phase
nanoflower
P‐Cu/Co(OH)
electrocatalyst
consisting
of
P‐Cu
clusters
P‐Co(OH)
nanosheets
designed
match
two‐step
tandem
process
)
more
compatible,
avoiding
excessive
accumulation
optimizing
whole
reaction.
Focusing
on
initial
2e
process,
inhibited
*
desorption
Cu
sites
in
gives
rise
appropriate
released
electrolyte.
Subsequently,
exhibits
superior
capacity
for
trapping
transforming
desorbed
during
latter
6e
due
thermodynamic
advantage
contributions
active
hydrogen.
In
1
m
KOH
+
0.1
leads
yield
rate
42.63
mg
h
cm
Faradaic
efficiency
97.04%
at
−0.4
V
versus
reversible
hydrogen
electrode.
Such
well‐matched
achieves
remarkable
synthesis
performance
perspective
catalytic
reaction,
offering
novel
guideline
design
RR
electrocatalysts.
