ACS Sustainable Chemistry & Engineering,
Journal Year:
2024,
Volume and Issue:
12(15), P. 5979 - 5990
Published: April 1, 2024
The
electrochemical
nitrate
reduction
reaction
(NO3RR)
emerges
as
a
promising
method
for
ammonia
(NH3)
production,
which
faces
the
dilemma
of
inhibiting
hydrogen
evolution
(HER)
and
promoting
active
(Hads)
supply
hydrogenation
nitrogen
intermediates.
Here,
core–shell
structure
engineering
strategy
is
developed
Cu2–xS/MoS2,
where
strong
Hads
adsorption
storage
capacity
can
accelerate
As
result,
an
eminent
NH3
yield
0.178
mmol
h–1
cm–2
Faradaic
efficiency
84.5%
were
achieved.
A
series
tests
demonstrate
that
tuning
Cu2–xS/MoS2
interface
improve
activity
conversion
NO2–,
while
avoiding
HER
effectively
retain
Hads.
density
functional
theory
calculation
further
demonstrates
has
*H
retention
ability
to
promote
NO3RR
process.
This
work
offers
novel
perspective
on
manipulation
generation
NO3RR.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
14(28)
Published: March 3, 2024
Abstract
Electrochemically
reducing
nitrate
(NO
3
−
),
a
common
water
pollutant,
to
valuable
ammonia
(NH
)
offers
green,
sustainable,
and
decentralized
route
for
synthesis.
Electrochemical
reduction
reaction
RR)
involves
two
crucial
steps:
deoxygenation
followed
by
nitrite
hydrogenation;
in
particular,
the
hydrogenation
is
rate‐determining
step
(RDS)
NO
RR.
In
this
work,
an
atomically
dispersed
cobalt‐phosphorus
(Co─P)
catalytic
pair
(CP)
with
strong
electronic
coupling
reported.
The
Co
site
Co─P
CP
effectively
activates
,
while
P
facilitates
dissociation
release
H
+
synergistically
enhancing
thermodynamic
kinetic
performance
of
electrochemical
ammonia.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(27)
Published: April 23, 2024
Electrocatalytic
reduction
of
nitrate
to
ammonia
provides
a
green
alternate
the
Haber-Bosch
method,
yet
it
suffers
from
sluggish
kinetics
and
low
yield
rate.
The
follows
tandem
reaction
nitrite
subsequent
hydrogenation
generate
ammonia,
Faraday
efficiency
(FE)
is
limited
by
competitive
hydrogen
evolution
reaction.
Herein,
we
design
heterostructure
catalyst
remedy
above
issues,
which
consists
Ni
nanosphere
core
Ni(OH)
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(32)
Published: May 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.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Sept. 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.
