ACS Catalysis,
Год журнала:
2024,
Номер
14(21), С. 16205 - 16213
Опубликована: Окт. 18, 2024
The
electrochemical
reduction
of
nitrate
ions
to
valuable
ammonia
enables
the
recovery
pollutants
from
industrial
wastewater,
thereby
synchronously
balancing
nitrogen
cycle
and
achieving
NH3
production.
However,
currently
reported
electrocatalysts
still
suffer
low
yield
rate,
Faradaic
inefficiency,
partial
current
density.
Herein,
a
strategy
based
on
regulation
d-band
center
by
Ru
doping
is
presented
boost
Theoretical
calculations
unravel
that
dopant
in
Ni
metal–organic
framework
shifts
neighboring
sites
upward,
optimizing
adsorption
strength
N-intermediates,
resulting
greatly
enhanced
reaction
performance.
synthesized
Ru-doped
rod
array
electrode
delivers
rate
1.31
mmol
h–1
cm–2
efficiency
91.5%
at
−0.6
V
versus
reversible
hydrogen
electrode,
as
well
good
cycling
stability.
In
view
multielectron
transfer
electrocatalytic
activity,
Zn-NO3–
battery
assembled
this
Zn
anode,
which
high
open-circuit
voltage
1.421
maximum
output
power
density
4.99
mW
cm–2,
demonstrating
potential
application
value.
Deleted Journal,
Год журнала:
2022,
Номер
1, С. e9120010 - e9120010
Опубликована: Май 30, 2022
To
restore
the
natural
nitrogen
cycle
(N-cycle),
artificial
N-cycle
electrocatalysis
with
flexibility,
sustainability,
and
compatibility
can
convert
intermittent
renewable
energy
(e.g.,
wind)
to
harmful
or
value-added
chemicals
minimal
carbon
emissions.
The
background
of
such
N-cycles,
as
fixation,
ammonia
oxidation,
nitrate
reduction,
is
briefly
introduced
here.
discussion
emerging
nanostructures
in
various
conversion
reactions
focused
on
architecture/compositional
design,
electrochemical
performances,
reaction
mechanisms,
instructive
tests.
Energy
device
advancements
for
achieving
more
functions
well
in
situ/operando
characterizations
toward
understanding
key
steps
are
also
highlighted.
Furthermore,
some
recently
proposed
less
discussed
C–N
coupling
summarized.
We
classify
inorganic
sources
that
each
other
under
an
applied
voltage
into
three
types,
namely,
abundant
nitrogen,
toxic
(nitrite),
oxides,
useful
compounds
ammonia,
hydrazine,
hydroxylamine,
goal
providing
critical
insights
strategies
facilitate
development
our
circular
economy.
Advanced Materials,
Год журнала:
2023,
Номер
36(17)
Опубликована: Июнь 9, 2023
Natural
nitrogen
cycle
has
been
severely
disrupted
by
anthropogenic
activities.
The
overuse
of
N-containing
fertilizers
induces
the
increase
nitrate
level
in
surface
and
ground
waters,
substantial
emission
oxides
causes
heavy
air
pollution.
Nitrogen
gas,
as
main
component
air,
used
for
mass
ammonia
production
over
a
century,
providing
enough
nutrition
agriculture
to
support
world
population
increase.
In
last
decade,
researchers
have
made
great
efforts
develop
processes
under
ambient
conditions
combat
intensive
energy
consumption
high
carbon
associated
with
Haber-Bosch
process.
Among
different
techniques,
electrochemical
reduction
reaction
(NO
Advanced Functional Materials,
Год журнала:
2023,
Номер
33(43)
Опубликована: Июнь 25, 2023
Abstract
Ammonia
as
an
irreplaceable
chemical
has
been
widely
demanded
to
keep
the
sustainable
development
of
modern
society.
However,
its
industrial
production
consumes
huge
energy
and
releases
extraordinary
green‐house
gases,
leading
various
environmental
issues.
To
achieve
green
ammonia
is
a
great
challenge
that
extensively
pursued
recently.
In
review,
most
promising
strategy,
electrochemical
nitrate
reduction
reaction
(e‐NO
3
RR)
for
purpose
comprehensively
investigated
give
full
understanding
mechanism
provide
guidance
future
directions.
Particularly,
electrocatalysts
focused
realize
high
yield
rate
Faraday
efficiency
applications.
The
recent‐developed
catalysts,
including
noble
metallic
materials,
alloys,
metal
compounds,
single‐metal‐atom
metal‐free
are
systematically
discussed
review
effects
factors
on
catalytic
performance
in
e‐NO
RR.
Accordingly,
strategies,
defects
engineering,
coordination
environment
modulating,
surface
controlling,
hybridization,
carefully
improve
performance,
such
intrinsic
activity
selectivity.
Finally,
perspectives
challenges
given
out.
This
shall
insightful
advanced
systems
efficiently
industry.
ACS Applied Materials & Interfaces,
Год журнала:
2022,
Номер
14(41), С. 46595 - 46602
Опубликована: Окт. 5, 2022
Electrocatalytic
nitrate
reduction
reaction
(NO3RR)
affords
a
bifunctional
character
in
the
carbon-free
ammonia
synthesis
and
remission
of
pollution
water.
Here,
we
fabricated
Co3O4
nanosheet
array
with
cobalt
vacancies
on
carbon
cloth
(vCo-Co3O4/CC)
by
situ
etching
aluminum-doped
Co3O4/CC,
which
exhibits
an
excellent
Faradaic
efficiency
97.2%
large
NH3
yield
as
high
517.5
μmol
h-1
cm-2,
better
than
pristine
Co3O4/CC.
Theoretical
calculative
results
imply
that
can
tune
local
electronic
environment
around
Co
sites
Co3O4,
increasing
charge
reducing
electron
cloud
density
sites,
is
thus
conducive
to
adsorption
NO3-
for
greatly
enhanced
reduction.
Furthermore,
vCo-Co3O4
(311)
facet
presents
NO3RR
activity
low
energy
barrier
about
0.63
eV
potential-determining
step,
much
smaller
(1.3
eV).
Energy & Environmental Science,
Год журнала:
2023,
Номер
16(6), С. 2483 - 2493
Опубликована: Янв. 1, 2023
Electron-deficient
Ru
sites
at
Ru/Co(OH)
2
heterointerfaces
weaken
the
d–p
orbital
hybridization
ability
and
further
facilitate
desorption
of
ammonia
intermediates,
thereby
achieving
ultrahigh
nitrate
electroreduction
activity
towards
ammonia.
Advanced Functional Materials,
Год журнала:
2022,
Номер
33(6)
Опубликована: Ноя. 28, 2022
Abstract
Electrocatalytic
nitrate
(NO
3
−
)
reduction
reaction
(NITRR)
is
an
inspiring
route
for
ammonia
(NH
synthesis
at
ambient
condition.
The
metallic
Cu‐based
material
with
low
cost
and
high
activity
one
of
the
most
promising
electrocatalysts
NITRR.
However,
due
to
weaker
atomic
H
*
‐providing
capacity,
produced
intermediate—nitrite
tends
accumulate
on
its
surface,
leading
unsatisfactory
NH
selectivity
Faradic
efficiency
(FE).
Herein,
a
novel
facile
O
2
/Ar
plasma
oxidation
subsequent
electro‐reduction
strategy
developed
synthesize
kind
metastable
phase
Cu.
Excitingly,
Cu
demonstrates
superior
NITRR
performance
conventional
4
+
(97.8%)
FE
(99.8%).
Density
function
theory
(DFT)
calculations
reveal
that
upshift
d
‐band
center
near
Fermi
level
in
contributes
enhanced
activity,
while
relatively
strong
adsorption
facilitates
conversion
from
NO
/NO
NOOH
/NOH
thus
ensures
FE.
Furthermore,
when
evaluated
as
cathode
Zn‐NO
battery,
power
density
(7.56
mW
cm
−2
yield
(76
µmol
h
−1
are
achieved
by
battery.
Sustainable Energy & Fuels,
Год журнала:
2022,
Номер
6(18), С. 4130 - 4136
Опубликована: Янв. 1, 2022
Oxygen
vacancy-enriched
Co
3
O
4
nanosheet
arrays
enable
ambient
electrosynthesis
of
NH
via
nitrate
reduction,
achieving
a
faradaic
efficiency
96.9%
and
yield
12
157
μg
h
−1
cm
−2
in
0.1
M
NaOH
with
NO
−
.
Energy & Environmental Science,
Год журнала:
2023,
Номер
16(2), С. 663 - 672
Опубликована: Янв. 1, 2023
Highly
efficient
electrochemical
nitrate
reduction
could
be
key
for
sustainable
ammonia
production.
Our
NiFe
LDH/Cu
foam
electrode
exhibits
an
NH
3
selectivity
of
95.8%
with
98.5%
conversion.