ChemSusChem,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Aug. 19, 2024
Abstract
Electrochemical
nitrate
reduction
to
ammonia
(NRA)
is
a
promising
approach
remove
environmental
pollutants
while
producing
green
NH
3
under
ambient
conditions.
Ag‐based
nanomaterials
have
been
used
in
NRA
but
their
iron
series
elements
(Fe,
Co,
Ni)
doping
has
not
explored
yet.
Herein,
an
effective
and
versatile
strategy
of
Ag
nanocrystals
by
for
efficient
presented.
Experimental
results
show
that
with
Fe,
Co
or
Ni
can
improve
the
activity.
Among
catalysts,
AgCo
delivers
best
performance
Faraday
efficiency
(FE)
88.3
%
selectivity
97.4
at−0.23
V
vs
RHE,
which
1.9
6.2
times
higher
than
plain
(46.4
FE
15.8
selectivity),
respectively.
A
highest
NO
−
conversion
rate
(91.8
%)
achieved,
maintains
16.4
ppm
−−
N
4
hours,
meeting
drinking
water
level
(~15
−N).
Moreover,
FE,
selectivity,
do
decay
after
four
consecutive
cycles.
It
found
effectively
induce
change
d‐band
center
optimized
NRA.
This
work
reveals
effects
on
shows
potential
practical
application
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(36)
Published: April 23, 2024
Abstract
Electrocatalytic
reduction
of
NO
2
−
to
NH
3
(NO
RR)
presents
a
fascinating
approach
for
simultaneously
migrating
pollutants
and
producing
valuable
.
In
this
study,
single‐atom
Rh‐alloyed
copper
(CuRh
1
)
is
explored
as
highly
active
selective
catalyst
toward
the
RR.
Combined
theoretical
calculations
in
situ
FTIR/EPR
spectroscopic
experiments
uncover
synergistic
effect
Rh
Cu
promote
RR
energetics
CuRh
through
tandem
catalysis
pathway,
which
activates
preliminary
adsorption
hydrogenation
→
*NO
*NOOH
*NO),
while
generated
on
then
transferred
substrate
promotes
rate‐determining
step
*NHO
synthesis.
As
result,
equipped
flow
cell
an
unprecedented
yield
rate
2191.6
µmol
h
−1
cm
−2
‐Faradaic
efficiency
98.9%
at
high
current
density
322.5
mA
,
well
long‐term
stability
100
electrolysis.
ACS Nano,
Journal Year:
2024,
Volume and Issue:
18(20), P. 13141 - 13149
Published: May 8, 2024
Electrocatalytic
reduction
of
NO2–
to
NH3
(NO2RR)
offers
an
effective
method
for
alleviating
pollution
and
generating
valuable
NH3.
Herein,
a
p-block
single-atom
alloy,
namely,
isolated
Sb
alloyed
in
Cu
substrate
(Sb1Cu),
is
explored
as
durable
high-current-density
NO2RR
catalyst.
As
revealed
by
the
theoretical
calculations
operando
spectroscopic
measurements,
we
demonstrate
that
Sb1
incorporation
can
not
only
hamper
competing
hydrogen
evolution
reaction
but
also
optimize
d-band
center
Sb1Cu
intermediate
adsorption
energies
boost
protonation
energetics
NO2–-to-NH3
conversion.
Consequently,
integrated
flow
cell
achieves
outstanding
yield
rate
2529.4
μmol
h–1
cm–2
FENH3
95.9%
at
high
current
density
424.2
mA
cm–2,
well
durability
100
h
electrolysis.
Energy & Fuels,
Journal Year:
2024,
Volume and Issue:
38(13), P. 11815 - 11823
Published: June 12, 2024
Electrocatalytic
N2
reduction
reaction
(NRR)
is
a
low-cost
and
environmental
friendly
strategy
for
NH3
synthesis
but
yet
needs
more
fundamental
applied
research.
Herein,
we
explored
the
NRR
activity
of
bimetal
Nb2Mo2C3Tx
MXene
catalyst
via
both
theoretical
experimental
studies.
Density
functional
theory
calculations
revealed
that
horizontal
adsorption
can
be
most
stable
mode
molecule,
alternating
mechanism
showed
downhill
free
energy
input
all
through
reaction.
More
importantly,
surface
Nb
Mo
terminations
MXenes
facilitate
demonstrate
comparable
to
benchmark
Ru.
In
experiment,
achieved
an
yield
20.77
μg
h–1
mgcat–1
high
Faraday
efficiency
31.0%,
demonstrating
excellent
selectivity
durability.
Internal
carbon
layers
ensured
fast
electron
transfer
avoided
self-aggregation
active
sites.
Structural
defects
also
played
important
role
in
its
because
formation
vast
unsaturated
Nb/Mo
atoms.