Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(34)
Published: April 5, 2024
Abstract
Electrochemical
nitrogen
reduction
reaction
(NRR)
for
ammonia
synthesis
has
attracted
great
interest
in
recent
years,
which
presents
a
carbon‐free
alternative
to
the
energy‐intensive
Haber–Bosch
process.
Besides,
NRR
also
provides
promising
coverage
route
of
renewable
energy
since
NH
3
is
considered
second
generation
hydrogen
while
possessing
established
technologies
liquefaction,
storage,
and
transport.
However,
there
are
long‐term
challenges
catalyst
design
due
its
low
intrinsic
activity
unsatisfied
selectivity.
Fortunately,
by
conducting
extensive
explorations
this
field,
much
progress
achieved
boosting
performance.
Herein,
from
view
atomic/electronic
level,
three
promotion
effects
summarized
(i.e.,
electron
effect,
geometry
ligand
effect),
tackle
Representative
studies
with
taking
fully
advantages
reviewed,
realized
remarkable
Finally,
future
research
directions
prospects
discussed.
It
highly
expected
that
review
will
enable
advancement
catalysts
promote
further
development
electrochemical
NRR.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(15), P. 10934 - 10942
Published: April 6, 2024
Hydroxylamine
(HA,
NH2OH)
is
a
critical
feedstock
in
the
production
of
various
chemicals
and
materials,
its
efficient
sustainable
synthesis
great
importance.
Electroreduction
nitrate
on
Cu-based
catalysts
has
emerged
as
promising
approach
for
green
ammonia
(NH3)
production,
but
electrosynthesis
HA
remains
challenging
due
to
overreduction
NH3.
Herein,
we
report
first
work
ketone-mediated
using
water.
A
metal–organic-framework-derived
Cu
catalyst
was
developed
catalyze
reaction.
Cyclopentanone
(CP)
used
capture
situ
form
CP
oxime
(CP-O)
with
C═N
bonds,
which
prone
hydrolysis.
could
be
released
easily
after
electrolysis,
regenerated.
It
demonstrated
that
CP-O
formed
an
excellent
Faradaic
efficiency
47.8%,
corresponding
formation
rate
34.9
mg
h–1
cm–2,
remarkable
carbon
selectivity
>99.9%.
The
hydrolysis
release
regeneration
also
optimized,
resulting
96.1
mmol
L–1
stabilized
solution,
significantly
higher
than
direct
reduction.
Detailed
characterizations,
control
experiments,
theoretical
calculations
revealed
surface
reconstruction
reaction
mechanism,
showed
coexistence
Cu0
Cu+
facilitated
protonation
reduction
*NO2
*NH2OH
desorption,
leading
enhancement
production.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(14), P. 10044 - 10051
Published: April 1, 2024
The
electrochemical
NO
reduction
reaction
(NORR)
is
a
promising
approach
for
both
nitrogen
cycle
regulation
and
ammonia
synthesis.
Due
to
the
relatively
low
concentration
of
source
poor
solubility
in
solution,
mass
transfer
limitation
serious
but
easily
overlooked
issue.
In
this
work,
porous
carbon-supported
ultrafine
Cu
clusters
grown
on
nanowire
arrays
(defined
as
Cu@Cu/C
NWAs)
are
prepared
low-concentration
NORR.
A
high
Faradaic
efficiency
(93.0%)
yield
rate
(1180.5
μg
h–1
cm–2)
realized
NWAs
at
−0.1
V
vs
reversible
hydrogen
electrode
(RHE),
which
far
superior
those
other
reported
performances
under
similar
conditions.
construction
carbon
support
can
effectively
decrease
diffusion
kinetics
promote
coverage
subsequent
highly
effective
conversion.
Moreover,
favorable
metal–support
interaction
between
enhances
adsorption
decreases
barrier
*HNO
formation
comparison
with
that
pure
NWAs.
Overall,
whole
NORR
be
fully
strengthened
concentrations.
