Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Фев. 10, 2024
Abstract
Nitrate
(NO
3
‒
)
pollution
poses
significant
threats
to
water
quality
and
global
nitrogen
cycles.
Alkaline
electrocatalytic
NO
reduction
reaction
RR)
emerges
as
an
attractive
route
for
enabling
removal
sustainable
ammonia
(NH
synthesis.
However,
it
suffers
from
insufficient
proton
(H
+
supply
in
high
pH
conditions,
restricting
-to-NH
activity.
Herein,
we
propose
a
halogen-mediated
H
feeding
strategy
enhance
the
alkaline
RR
performance.
Our
platform
achieves
near-100%
NH
Faradaic
efficiency
(pH
=
14)
with
current
density
of
2
A
cm
–2
enables
over
99%
–
conversion
efficiency.
We
also
convert
high-purity
4
Cl
near-unity
efficiency,
suggesting
practical
approach
valorizing
pollutants
into
valuable
products.
Theoretical
simulations
situ
experiments
reveal
that
Cl-coordination
endows
shifted
d
-band
center
Pd
atoms
construct
local
-abundant
environments,
through
arousing
dangling
O-H
dissociation
fast
*H
desorption,
*NO
intermediate
hydrogenation
finally
effective
conversion.
Nature Communications,
Год журнала:
2022,
Номер
13(1)
Опубликована: Дек. 22, 2022
Abstract
The
development
of
electrocatalysts
capable
efficient
reduction
nitrate
(NO
3
−
)
to
ammonia
(NH
is
drawing
increasing
interest
for
the
sake
low
carbon
emission
and
environmental
protection.
Herein,
we
present
a
CuCo
bimetallic
catalyst
able
imitate
bifunctional
nature
copper-type
nitrite
reductase,
which
could
easily
remove
NO
2
via
collaboration
two
active
centers.
Indeed,
Co
acts
as
an
electron/proton
donating
center,
while
Cu
facilitates
x
adsorption/association.
bio-inspired
nanosheet
electrocatalyst
delivers
100
±
1%
Faradaic
efficiency
at
ampere-level
current
density
1035
mA
cm
−2
−0.2
V
vs
.
Reversible
Hydrogen
Electrode.
NH
production
rate
reaches
high
activity
4.8
mmol
h
−1
(960
g
cat
).
A
mechanistic
study,
using
electrochemical
in
situ
Fourier
transform
infrared
spectroscopy
shell-isolated
nanoparticle
enhanced
Raman
spectroscopy,
reveals
strong
synergy
between
Co,
with
sites
promoting
hydrogenation
adsorbed
*H
species.
well-modulated
coverage
*NO
led
simultaneously
selectivity
yield.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(13)
Опубликована: Фев. 3, 2023
We
demonstrate
the
great
feasibility
of
MBenes
as
a
new
class
tandem
catalysts
for
electrocatalytic
nitrate
reduction
to
ammonia
(NO3
RR).
As
proof
concept,
FeB2
is
first
employed
model
MBene
catalyst
NO3
RR,
showing
maximum
NH3
-Faradaic
efficiency
96.8
%
with
corresponding
yield
25.5
mg
h-1
cm-2
at
-0.6
V
vs.
RHE.
Mechanistic
studies
reveal
that
exceptional
RR
activity
arises
from
catalysis
mechanism,
is,
B
sites
activate
NO3-
form
intermediates,
while
Fe
dissociate
H2
O
and
increase
*H
supply
on
promote
intermediate
hydrogenation
enhance
-to-NH3
conversion.
Advanced Materials,
Год журнала:
2023,
Номер
35(19)
Опубликована: Март 5, 2023
Involving
eight
electron
transfer
process
and
multiple
intermediates
of
nitrate
(NO3-
)
reduction
reaction
leads
to
a
sluggish
kinetic
low
Faradaic
efficiency,
therefore,
it
is
essential
get
an
insight
into
the
mechanism
develop
highly
efficient
electrocatalyst.
Herein,
series
reduced-graphene-oxide-supported
RuCu
alloy
catalysts
(Rux
Cux
/rGO)
are
fabricated
used
for
direct
NO3-
NH3
.
It
found
that
Ru1
Cu10
/rGO
shows
ammonia
formation
rate
0.38
mmol
cm-2
h-1
(loading
1
mg
efficiency
98%
under
ultralow
potential
-0.05
V
versus
Reversible
Hydrogen
Electode
(RHE),
which
comparable
Ru
catalyst.
The
activity
can
be
attributed
synergetic
effect
between
Cu
sites
via
relay
catalysis,
in
exclusively
NO2-
exhibits
superior
In
addition,
doping
tunes
d-band
center
effectively
modulates
adsorption
energy
,
promotes
This
electrocatalysis
strategy
opens
new
avenue
developing
multifunctional
catalysts.
Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Май 2, 2023
Abstract
Oxygen
evolution
reaction
catalysts
capable
of
working
efficiently
in
acidic
media
are
highly
demanded
for
the
commercialization
proton
exchange
membrane
water
electrolysis.
Herein,
we
report
a
Zn-doped
RuO
2
nanowire
array
electrocatalyst
with
outstanding
catalytic
performance
oxygen
under
conditions.
Overpotentials
as
low
173,
304,
and
373
mV
achieved
at
10,
500,
1000
mA
cm
−2
,
respectively,
robust
stability
reaching
to
h
10
.
Experimental
theoretical
investigations
establish
clear
synergistic
effect
Zn
dopants
vacancies
on
regulating
binding
configurations
oxygenated
adsorbates
active
centers,
which
then
enables
an
alternative
Ru−Zn
dual-site
oxide
path
reaction.
Due
change
pathways,
energy
barrier
rate-determining
step
is
reduced,
over-oxidation
Ru
sites
alleviated.
As
result,
activity
significantly
enhanced.
Energy & Environmental Science,
Год журнала:
2023,
Номер
16(6), С. 2611 - 2620
Опубликована: Янв. 1, 2023
The
grain
boundary
defect
engineered
Ni
nanoparticles
has
been
explored
for
boosting
selective
nitrate
electroreduction
to
ammonia,
and
its
NH
3
generation
rate
is
much
higher
than
those
of
the
reported
copper
or
noble
metal-based
catalysts.
Advanced Functional Materials,
Год журнала:
2023,
Номер
33(29)
Опубликована: Апрель 23, 2023
Abstract
Ammonia
is
not
only
an
important
feedstock
for
chemical
industry
but
also
a
carbon‐free
energy
carrier
and
safe
storage
media
hydrogen.
Due
to
the
advantages
compared
Haber–Bosch
process,
electrochemical
NO
3
−
‐to‐NH
conversion
via
nitrate
reduction
reaction
(NO
RR)
received
attention.
Recently,
“green
hydrogen”
generated
from
water
electrolysis
shows
promise
become
future
limited
by
safety
of
transportation.
This
review
proposes
can
store
renewable
electric
into
NH
,
which
potential
solution
solving
puzzle
Moreover,
theoretical
insights
RR
electrocatalyst
design
are
discussed.
Finally,
challenges
opportunities
in
this
field
elucidated.
provides
novel
perspective
accelerates
development
effective
electrocatalysts
conversion.
