Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Авг. 6, 2024
Abstract
Ammonia,
as
a
high‐energy‐density
carrier
for
hydrogen
storage,
is
in
great
demand
worldwide.
Electrocatalytic
nitrate
reduction
reaction
(NO
3
RR)
provides
green
NH
production
process.
However,
the
complex
pathways
NO
RR
to
and
difficulty
controlling
intermediate
products
limit
Herein,
by
incorporating
atomic‐level
bismuth
(Bi)
into
CuCo
2
O
4
hollow
carbon
nanofibers,
catalytic
activity
of
electrocatalyst
enhanced.
The
maximum
Faradaic
efficiency
Bi
1
‐CuCo
95.53%,
with
an
yield
448.74
µmol
h
−1
cm
−2
at
−0.8
V
versus
RHE.
Density
Functional
Theory
calculations
show
that
presence
lowers
barrier
hydrogenation
step
from
*NO
H,
while
promoting
mass
transfer
on
release
*NH
reactivation
surface‐active
sites.
Differential
charge
density
also
after
doping,
supplied
catalyst
−
increases
0.62
0.72
e
‐
,
thus
reasoned
enhanced
activity.
established
nitrate‐Zn
battery
shows
energy
2.81
mW
implying
potential
application.
Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Дек. 5, 2023
Abstract
Most
current
research
is
devoted
to
electrochemical
nitrate
reduction
reaction
for
ammonia
synthesis
under
alkaline/neutral
media
while
the
investigation
of
acidic
conditions
rarely
reported.
In
this
work,
we
demonstrate
potential
TiO
2
nanosheet
with
intrinsically
poor
hydrogen-evolution
activity
selective
and
rapid
conditions.
Hybridized
iron
phthalocyanine,
resulting
catalyst
displays
remarkably
improved
efficiency
toward
formation
owing
enhanced
adsorption,
suppressed
hydrogen
evolution
lowered
energy
barrier
rate-determining
step.
Then,
an
alkaline-acid
hybrid
Zn-nitrate
battery
was
developed
high
open-circuit
voltage
1.99
V
power
density
91.4
mW
cm
–2
.
Further,
environmental
sulfur
recovery
can
be
powered
by
above
hydrazine-nitrate
fuel
cell
simultaneously
hydrazine/nitrate
conversion
electricity
generation.
This
work
demonstrates
attractive
electrosynthesis
broadens
field
conversion.
Advanced Materials,
Год журнала:
2024,
Номер
36(14)
Опубликована: Янв. 26, 2024
Abstract
Electrocatalytic
nitrate
reduction
reaction
(NO
3
RR)
toward
ammonia
synthesis
is
recognized
as
a
sustainable
strategy
to
balance
the
global
nitrogen
cycle.
However,
it
still
remains
great
challenge
achieve
highly
efficient
production
due
complex
proton‐coupled
electron
transfer
process
in
NO
RR.
Here,
controlled
of
RuMo
alloy
nanoflowers
(NFs)
with
unconventional
face‐centered
cubic
(fcc)
phase
and
hexagonal
close‐packed/fcc
heterophase
for
RR
reported.
Significantly,
fcc
NFs
demonstrate
high
Faradaic
efficiency
95.2%
large
yield
rate
32.7
mg
h
−1
cat
at
0
−0.1
V
(vs
reversible
hydrogen
electrode),
respectively.
In
situ
characterizations
theoretical
calculations
have
unraveled
that
possess
highest
d‐band
center
superior
electroactivity,
which
originates
from
strong
Ru─Mo
interactions
intrinsic
activity
phase.
The
optimal
electronic
structures
supply
adsorption
key
intermediates
suppression
competitive
evolution,
further
determines
remarkable
performance.
successful
demonstration
high‐performance
zinc‐nitrate
batteries
suggests
their
substantial
application
potential
electrochemical
energy
systems.
Nanoscale,
Год журнала:
2023,
Номер
15(48), С. 19577 - 19585
Опубликована: Янв. 1, 2023
Zn-NO3-
batteries
can
generate
electricity
while
producing
NH3
in
an
environmentally
friendly
manner,
making
them
a
very
promising
device.
However,
the
conversion
of
NO3-
to
involves
proton-assisted
8-electron
(8e-)
transfer
process
with
high
kinetic
barrier,
requiring
high-performance
catalysts
realize
potential
applications
this
technology.
Herein,
we
propose
heterostructured
CoO/CuO
nanoarray
electrocatalyst
prepared
on
copper
foam
(CoO/CuO-NA/CF)
that
electrocatalytically
and
efficiently
convert
at
low
achieves
maximum
yield
296.9
μmol
h-1
cm-2
Faraday
efficiency
(FE)
92.9%
-0.2
V
vs.
reversible
hydrogen
electrode
(RHE).
Impressively,
battery
based
monolithic
CoO/CuO-NA/CF
delivers
60.3
cm-2,
FENH3
82.0%,
power
density
4.3
mW
cm-2.
This
study
provides
paradigm
for
catalyst
preparation
energy-efficient
production
simultaneously
generating
electrical
energy.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(24)
Опубликована: Янв. 17, 2024
Abstract
The
electrochemical
reduction
of
nitrate
to
ammonia
(NO
3
RR)
has
emerged
as
a
promising
but
challenging
orientation
in
sustainable
development.
Cu
is
one
the
most
effective
NO
RR
catalysts.
However,
accumulation
2
−
on
their
surface
erected
bars
further
improvement
efficiency.
Herein,
Cu‐based
electrocatalyst
with
low‐coordinated
atoms
(Cu‐LC)
synthesized
via
instantaneous
ablation
and
rapid
cooling
target
by
pulse
laser
proposed
new
electrocatalyst,
which
exhibits
enhanced
activity
NH
selectivity
97.01%,
yield
rate
0.624
mmol
h
−1
cm
−2
at
−0.8
V
versus
RHE
long‐term
durability,
superior
reported
introduction
sites
upshifts
d‐band
center
near
Fermi
Level,
enhancing
adsorption
key
intermediates
(
*
,
NO)
RR,
also
effectively
regulating
generation
hydrogenation
process,
inhibiting
Cu‐LC
surface,
thus
achieving
efficient
production.
Furthermore,
when
evaluated
cathode
material
Zn–NO
battery,
an
open
circuit
voltage
1.3
power
density
3.1
mW
are
achieved
Cu‐LC‐based
highlighting
multifunctional
system
for
production
energy
supply.
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.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Апрель 1, 2024
Abstract
Reversible
solid-state
hydrogen
storage
of
magnesium
hydride,
traditionally
driven
by
external
heating,
is
constrained
massive
energy
input
and
low
systematic
density.
Herein,
a
single
phase
Mg
2
Ni(Cu)
alloy
designed
via
atomic
reconstruction
to
achieve
the
ideal
integration
photothermal
catalytic
effects
for
stable
solar-driven
MgH
.
With
intra/inter-band
transitions
its
hydrogenated
state,
over
85%
absorption
in
entire
spectrum
achieved,
resulting
temperature
up
261.8
°C
under
2.6
W
cm
−2
Moreover,
reaction
thermodynamically
kinetically
favored,
imbalanced
distribution
light-induced
hot
electrons
within
CuNi
facilitates
weakening
Mg-H
bonds
,
enhancing
“hydrogen
pump”
effect
Ni(Cu)/Mg
Ni(Cu)H
4
The
reversible
generation
upon
repeated
dehydrogenation
process
enables
continuous
roles
stably,
ensuring
direct
action
localized
heat
on
sites
without
any
loss,
thereby
achieving
6.1
wt.%
H
capacity
with
95%
retention
3.5
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(27)
Опубликована: Апрель 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)