Chemical Communications,
Journal Year:
2024,
Volume and Issue:
60(78), P. 10918 - 10921
Published: Jan. 1, 2024
In
this
study,
we
explore
the
efficacy
of
gold
(Au)
as
a
selective
electrocatalyst
for
reduction
nitrate
to
hydroxylamine,
valuable
nitrogen-based
chemical,
while
also
evaluating
by-product
formation
ammonia.
We
systematically
optimized
various
experimental
parameters
including
concentration,
pH,
and
applied
potential.
found
that
at
an
potential
-0.7
V
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Sept. 24, 2024
Coupling
with
the
nitrate
electroreduction
reaction
(NitRR),
electrosynthesis
of
cyclohexanone
oxime
(CHO,
vital
feedstock
in
nylon-6
industry)
from
provides
a
promising
alternative
to
traditional
energy
consumption
process.
However,
it
still
suffers
low
efficiency
because
selective
production
*NH
Journal of the American Chemical Society,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 2, 2025
Single-atom
Fe-N-C
catalysts
have
attracted
significant
attention
in
the
NOx
reduction
reaction
(NOxRR).
However,
origin
of
their
selectivity
NOxRR
remains
unclear,
impeding
further
advancements
application.
Herein,
we
investigate
potential-driven
competitive
mechanism
for
NH3
and
NH2OH
production
over
single-atom
pyridinic-FeN4
pyrrolic-FeN4
sites
using
constant-potential
density
functional
theory
calculations.
The
is
linked
to
switching
Fe
3d
orbitals
as
they
interact
with
intermediates.
between
determined
by
applied
potentials.
predominantly
generates
at
higher
potentials
(-0.6
-1.2
V,
vs
SHE),
while
favored
lower
(0.6
-0.6
V).
shows
a
similar
potential-dependent
product
distribution,
crossover
potential
-1.0
V.
selectivity-determining
intermediates
(SDIs)
are
*NH2OH
*NH2
+
*OH.
governed
interacting
SDIs,
from
dumbbell-shaped
3dz2
four-leaf
clover-like
3dxz,
3dyz,
3dx2-y2,
which
plays
crucial
role
controlling
distribution
based
on
These
findings
offer
new
insights
into
NOxRR.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Aug. 5, 2024
Abstract
Nano‐single‐atom‐catalysts
have
the
potential
to
combine
respective
advantages
of
both
nano‐catalysts
and
single‐atom‐catalysts
thus
exhibit
enhanced
performance.
Generally,
separation
active
sites
in
space
limits
interaction
between
single
atoms
nanoparticles.
Heterointerface
engineering
has
break
this
limitation.
Regretfully,
studies
on
interface
effect
nanoparticles
are
rarely
reported.
Herein,
an
unprecedented
nano‐single‐atom
heterointerface
composed
Fe
single‐atoms
carbon‐shell‐coated
FeP
(Fe
SAC/FeP@C)
is
demonstrated
as
efficient
electrocatalyst
for
nitrate
reduction
process
from
alkaline
acidic.
Compared
with
typical
nano‐single‐atom‐catalysts
SAC/FePO
4
)
SAC),
constructed
SAC/FeP@C
heterostructure
exhibits
dramatically
nitrate‐to‐ammonia
Especially
acidic
media,
maxmium
Faradaic
efficiency
ammonia
(NH
3
can
reach
95.6
±
0.5%,
a
maximum
NH
yield
36.2
3.1
mg
h
−1
cat
(pH
=
1.2),
which
considerably
higher
than
previously
Density
functional
theory
calculations
situ
spectroscopic
investigations
indicate
that
unique
charge
redistribution
at
interface,
together
optimized
electronic
structure
single‐atoms,
strengthens
intermediate
adsorption
catalytic
activity.
This
work
provides
feasible
strategy
designing
heterointerfaces,
well
valuable
insights
into
conversion
under
environmentally
relevant
wastewater
conditions.