Advanced Materials,
Год журнала:
2024,
Номер
36(24)
Опубликована: Март 19, 2024
Abstract
Mother
nature
accomplishes
efficient
ammonia
synthesis
via
cascade
N
2
oxidation
by
lightning
strikes
followed
with
enzyme‐catalyzed
nitrogen
oxyanion
(NO
x
−
,
=
2,3)
reduction.
The
protein
environment
of
enzymatic
centers
for
NO
‐to‐NH
4
+
process
greatly
inspires
the
design
glutathione‐capped
(GSH)
quantum
dots
(QDs)
under
visible
light
(440
nm)
in
tandem
plasma‐enabled
oxidation.
Mechanistic
studies
reveal
that
GSH
induces
positive
shift
surface
charge
to
strengthen
interaction
between
and
QDs.
Upon
irradiation
QDs,
balanced
rapid
hole
electron
transfer
furnish
GS·radicals
2e
/2H
alcohol
H·for
8e
/10H
3
reduction
simultaneously.
For
first
time,
mmol‐scale
is
realized
apparent
yields
5.45%
±
0.64%,
gram‐scale
value‐added
acetophenone
NH
Cl
proceeds
1:4
stoichiometry
stability,
demonstrating
promising
multielectron
multiproton
efficiency
sustainability
nature‐inspired
artificial
photocatalysts.
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
Proceedings of the National Academy of Sciences,
Год журнала:
2023,
Номер
120(32)
Опубликована: Июль 31, 2023
Electrochemical
nitrate
reduction
reaction
(NO
3
RR)
to
ammonia
has
been
regarded
as
a
promising
strategy
balance
the
global
nitrogen
cycle.
However,
it
still
suffers
from
poor
Faradaic
efficiency
(FE)
and
limited
yield
rate
for
production
on
heterogeneous
electrocatalysts,
especially
in
neutral
solutions.
Herein,
we
report
one-pot
synthesis
of
ultrathin
nanosheet-assembled
RuFe
nanoflowers
with
low-coordinated
Ru
sites
enhance
NO
RR
performances
electrolyte.
Significantly,
exhibit
outstanding
FE
92.9%
38.68
mg
h
−1
cat
(64.47
)
at
−0.30
−0.65
V
(vs.
reversible
hydrogen
electrode),
respectively.
Experimental
studies
theoretical
calculations
reveal
that
are
highly
electroactive
an
increased
d-band
center
guarantee
efficient
electron
transfer,
leading
low
energy
barriers
reduction.
The
demonstration
rechargeable
zinc-nitrate
batteries
large-specific
capacity
using
indicates
their
great
potential
next-generation
electrochemical
systems.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(26)
Опубликована: Апрель 22, 2024
Abstract
The
controlled
synthesis
of
metal
nanomaterials
with
unconventional
phases
is
significant
importance
to
develop
high‐performance
catalysts
for
various
applications.
However,
it
remains
challenging
modulate
the
atomic
arrangements
nanomaterials,
especially
alloy
nanostructures
that
involve
different
metals
distinct
redox
potentials.
Here
we
report
general
one‐pot
IrNi,
IrRhNi
and
IrFeNi
nanobranches
hexagonal
close‐packed
(hcp)
phase.
Notably,
as‐synthesized
hcp
IrNi
demonstrate
excellent
catalytic
performance
towards
electrochemical
nitrite
reduction
reaction
(NO
2
RR),
superior
NH
3
Faradaic
efficiency
yield
rate
98.2
%
34.6
mg
h
−1
cat
(75.5
Ir
)
at
0
−0.1
V
(vs
reversible
hydrogen
electrode),
respectively.
Ex/in
situ
characterizations
theoretical
calculations
reveal
Ir−Ni
interactions
within
improve
electron
transfer
benefit
both
activation
active
generation,
leading
a
stronger
trend
NO
RR
by
greatly
reducing
energy
barriers
rate‐determining
step.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
147(9), С. 8012 - 8023
Опубликована: Фев. 18, 2025
The
electrocatalytic
nitrite
reduction
(NO2RR)
converts
nitrogen-containing
pollutants
to
high-value
ammonia
(NH3)
under
ambient
conditions.
However,
its
multiple
intermediates
and
multielectron
coupled
proton
transfer
process
lead
low
activity
NH3
selectivity
for
the
existing
electrocatalysts.
Herein,
we
synthesize
a
solid-solution
copper-zinc
cyanamide
(Cu0.8Zn0.2NCN)
with
localized
structure
distortion
tailored
surface
electrostatic
potential,
allowing
asymmetric
binding
of
NO2-.
It
exhibits
outstanding
NO2RR
performance
Faradaic
efficiency
∼100%
an
yield
22
mg
h-1
cm-2,
among
best
such
process.
Theoretical
calculations
in
situ
spectroscopic
measurements
demonstrate
that
Cu-Zn
sites
coordinated
linear
polarized
[NCN]2-
could
transform
symmetric
[Cu-O-N-O-Cu]
CuNCN-NO2-
[Cu-N-O-Zn]
configuration
Cu0.8Zn0.2NCN-NO2-,
thus
enhancing
adsorption
bond
cleavage.
A
paired
electro-refinery
Cu0.8Zn0.2NCN
cathode
reaches
2000
mA
cm-2
at
2.36
V
remains
fully
operational
industrial-level
400
>140
h
production
rate
∼30
mgNH3
cm-2.
Our
work
opens
new
avenue
tailoring
potentials
using
strategy
advanced
electrocatalysis.
