Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(30)
Опубликована: Май 14, 2024
Transition-metal
carbides
with
metallic
properties
have
been
extensively
used
as
electrocatalysts
due
to
their
excellent
conductivity
and
unique
electronic
structures.
Herein,
NbC
nanoparticles
decorated
carbon
nanofibers
(NbC@CNFs)
are
proposed
an
efficient
robust
catalyst
for
electrochemical
synthesis
of
ammonia
from
nitrate/nitrite
reduction,
which
achieves
a
high
Faradaic
efficiency
(FE)
94.4
%
large
yield
30.9
mg
h
Industrial
ammonia
production
mainly
relies
on
the
conventional
Haber–Bosch
process
accompanied
by
high
energy
consumption
and
plentiful
carbon
dioxide
emissions,
which
triggered
recent
interest
to
explore
more
energy‐efficient
environmentally
benign
alternatives.
Very
recently,
electrochemical
nitrite
reduction
in
an
aqueous
medium
promises
new
opportunities
for
advanced,
energy‐efficient,
sustainable
at
ambient
conditions.
The
formation
rate
Faradic
efficiency
are
strongly
associated
with
adopted
electrocatalysts;
therefore,
striving
high‐efficient
electrocatalysts
is
key
via
reaction.
Herein,
a
critical
overview
of
advances
reaction
presented,
highlighting
latest
innovative
heterogenous
including
noble
metal
catalysts,
transition‐metal‐based
their
compounds.
Meanwhile,
possible
pathway
electroreduction
ammonia,
detection,
catalytic
activity
descriptor
briefly
summarized.
Finally,
perspective
research
challenges
that
convert
outlined,
increasing
contributions
route
realizing
neutral
footprint.
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.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(11)
Опубликована: Янв. 23, 2024
Abstract
During
the
electrocatalytic
NO
3
−
reduction
reaction
(NO
RR)
under
neutral
condition,
activation
of
H
2
O
to
generate
H*
and
inhibition
inter‐H*
species
binding,
are
critically
important
but
remain
challenging
for
suppressing
non‐desirable
hydrogen
evolution
(HER).
Here,
a
Mn‐doped
Co(OH)
(named
as
Mn‐Co(OH)
)
has
been
synthesized
by
in
situ
reconstruction
electrolyte,
which
is
able
dissociate
molecules
inhibits
binding
between
each
other
owing
increased
interatomic
spacing
Mn‐doping.
The
electrocatalyst
offers
faradaic
efficiency
(FE)
high
98.9±1.7%
at
−0.6
V
vs.
reversible
electrode
(RHE)
an
energy
(EE)
49.90±1.03%
NH
production
RR,
among
highest
recently
reported
state‐of‐the‐art
catalysts
electrolyte.
Moreover,
negligible
degradation
−200
mA
cm
−2
found
least
500
h,
longest
catalytic
durations
ever
reported.
This
work
paves
novel
approach
design
synthesis
efficient
RR
electrocatalysts.
Abstract
The
electrocatalytic
synthesis
of
C–N
coupling
compounds
from
CO
2
and
nitrogenous
species
not
only
offers
an
effective
avenue
to
achieve
carbon
neutrality
reduce
environmental
pollution,
but
also
establishes
a
route
synthesize
valuable
chemicals,
such
as
urea,
amide,
amine.
This
innovative
approach
expands
the
application
range
product
categories
beyond
simple
carbonaceous
in
reduction,
which
is
becoming
rapidly
advancing
field.
review
summarizes
research
progress
urea
synthesis,
using
N
,
NO
−
3
species,
explores
emerging
trends
electrosynthesis
amide
amine
nitrogen
species.
Additionally,
future
opportunities
this
field
are
highlighted,
including
amino
acids
other
containing
bonds,
anodic
reactions
water
oxidation,
catalytic
mechanism
corresponding
reactions.
critical
captures
insights
aimed
at
accelerating
development
electrochemical
reactions,
confirming
superiority
method
over
traditional
techniques.
