ACS ES&T Engineering,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 24, 2024
Palladium–indium
(PdIn)
is
a
well-established
bimetallic
composition
for
reductively
degrading
nitrate
anions,
one
of
the
most
ubiquitous
contaminants
in
groundwater.
However,
scarcity
and
variable
price
these
rare-earth
platinum
group
critical
metals
may
hinder
their
use
water
treatment.
Nickel
(Ni),
nonprecious
metal
same
element
as
Pd,
could
partially
replace
lower
Pd
usage
if
resulting
trimetallic
sufficiently
catalytically
active.
Herein,
we
report
synthesis
reduction
catalysis
activated
carbon-supported
"In-on-Pd-on-Ni"
catalysts
(InPdNi/AC).
While
InPd/AC
(0.05
wt
%
In,
1.3
Pd)
was
expectedly
active,
InPdNi/AC
containing
In
amount,
much
less
(0.1
%),
1
Ni
>17
more
active
(kcat
≈
20
vs
349
L
min–1
gsurface
metal–1).
X-ray
photoelectron
spectroscopy
(XPS)
density
functional
theory
(DFT)
calculations
showed
that
gained
electron
from
Ni,
correlating
to
increased
activity.
Ammonium
byproduct
selectivity
(18%
at
50%
conversion)
compared
(48%),
suggestive
higher
surface
coverage
NO
or
its
greater
reactivity
with
NO2–,
which
led
N2.
Accounting
catalyst
precursor,
manufacturing
costs,
spent
recovery,
calculated
incorporation
lowered
net
cost
significantly
(from
$1028/kg
$170/kg).
The
lowered,
by
∼26
times,
stirred
tank
reactor
sized
treatment
capacity
case.
results
demonstrate
partial
replacement
precious
an
earth-abundant
leads
efficiency
denitrification
catalyst,
via
material
strategy
should
be
beneficial
other
clean-water
catalytic
systems.
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Сен. 11, 2024
Abstract
Electrochemical
nitrate
reduction
reaction
(NO
3
RR)
is
a
promising
approach
to
realize
ammonia
generation
and
wastewater
treatment.
However,
the
transformation
from
NO
−
NH
involves
multiple
proton‐coupled
electron
transfer
processes
by‐products
2
,
H
etc.),
making
high
selectivity
challenge.
Herein,
two‐phase
nanoflower
P‐Cu/Co(OH)
electrocatalyst
consisting
of
P‐Cu
clusters
P‐Co(OH)
nanosheets
designed
match
two‐step
tandem
process
)
more
compatible,
avoiding
excessive
accumulation
optimizing
whole
reaction.
Focusing
on
initial
2e
process,
inhibited
*
desorption
Cu
sites
in
gives
rise
appropriate
released
electrolyte.
Subsequently,
exhibits
superior
capacity
for
trapping
transforming
desorbed
during
latter
6e
due
thermodynamic
advantage
contributions
active
hydrogen.
In
1
m
KOH
+
0.1
leads
yield
rate
42.63
mg
h
cm
Faradaic
efficiency
97.04%
at
−0.4
V
versus
reversible
hydrogen
electrode.
Such
well‐matched
achieves
remarkable
synthesis
performance
perspective
catalytic
reaction,
offering
novel
guideline
design
RR
electrocatalysts.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(45)
Опубликована: Май 28, 2024
Abstract
The
past
decades
have
seen
considerable
imbalances
in
the
nitrogen
cycle
due
to
excessive
use
of
nitrate
agriculture
and
industry.
Electrocatalytic
reduction
(NO
3
RR)
(N
2
)
holds
significant
potential
for
addressing
pollution
wastewater
but
suffers
from
nitrite
formation
sluggish
hydrogeneration
process.
Here
a
single
atom
alloy
(SAA)
catalyst
featuring
atomically
dispersed
Ru
on
2D
Ni
metal
(Ru
1
Ni),
proving
remarkable
performance
−
–N
conversion
(≈93%)
N
selectivity
(≈99%))
through
co‐catalytic
metal‐support
interactions
(CMSI)
effect
is
reported.
Significantly,
SAA
achieves
NO
RR
removal
capacity
as
high
11.1
mg
L
−1
h
cm
−2
with
20
cycles
stability
(9
per
cycle),
surpassing
most
previously
reported
works.
core
boosting
lies
synergistically
promoted
activation
accelerated
hydrogenation
oxide
intermediates
site
substrate,
respectively,
revealed
by
various
situ
experiments
theoretical
simulations.
DFT
calculations
indicate
electron
transfer
substrate
more
robust
interaction
between
Ru–Ni
comparison
that
Ni–Ni.
This
work
offers
resilient
methodology
rational
design
highly
efficient
electrocatalysts
CMSI
modulation
RR,
illuminating
arena
treatment
cycle.
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(42)
Опубликована: Сен. 25, 2024
Abstract
Using
low
and
optimized
magnetic
field
along
with
electric
is
a
novel
strategy
to
facilitate
electrochemical
nitrite
reduction
reaction
(NO
2
RR).
Herein,
the
assisted
electrocatalytic
ammonia
synthesis
employing
spin‐thrusted
β‐MnPc
at
95
mT
explored.
The
calculated
rate
of
generation
16603.4
µg
h
−1
mg
cat
,
which
almost
twice
that
nonpolarized
manganese
phthalocyanine
(MnPc)
catalyst.
Additionally,
Faradaic
efficiency
(FE)
–0.9
V
versus
RHE
found
be
92.9%,
significantly
higher
compared
MnPc
In
presence
external
field,
catalysts
provide
better
electron
transfer
channel
results
in
lower
charge
resistance
hence
performances.
Density
functional
theory
(DFT)
result
further
verifies
induced
has
potential
barrier
(0.51
eV)
for
protonation
NO*
than
(1.08
eV),
confirms
enhanced
ammonia.
ACS Omega,
Год журнала:
2024,
Номер
9(18), С. 19770 - 19785
Опубликована: Апрель 23, 2024
Over
the
decades,
rise
in
nitrate
levels
ecosystem
has
posed
a
serious
threat
to
continuous
existence
of
humans,
fauna,
and
flora.
The
deleterious
effects
increasing
nitrates
have
led
adverse
health
environmental
implications
form
methemoglobinemia
eutrophication,
respectively.
Different
pathways/routes
for
syntheses
perovskites
their
oxides
were
presented
this
review.
In
recent
times,
electrocatalytic
reduction
emerged
as
most
utilized
technique
conversion
into
ammonia,
an
industrial
feedstock.
According
published
papers,
efficiency
various
used
achieved
high
Faradaic
98%.
Furthermore,
studies
shown
that
there
is
need
improve
chemical
stability
during
scale-up
applications,
well
scalability
applications.
It
is
still
challenging
to
develop
an
effective
strategy
simultaneously
enhance
the
activity
and
stability
of
electrocatalysts
for
electrocatalytic
nitrate
reduction
reaction
(eNO3RR).
Herein,
taking
metallic
cobalt
as
example,
it
demonstrated
that
construction
low-coordinated
nanosheets
(L-Co
NSs)
by
H2
plasma
etching
electrodeposited
(Co
can
greatly
eNO3RR.
Compared
with
Co
NSs,
at
-0.4
V
versus
RHE,
removal
rate,
ammonia
partial
current
density,
yield
are
increased
L-Co
NSs
from
82.14%
98.57%,
476
683
mA
cm-2,
2.11
2.54
mmol
h-1
respectively.
In
addition,
demonstrate
negligible
decay
after
30
cycles
test,
while
show
significant
decline.
situ
electrochemical
characterizations
theoretical
calculations
verify
abundance
vacancies
in
not
only
contribute
optimized
electronic
structure
enhanced
desorption
key
intermediate
boost
but
also
facilitate
transformation
Co(OH)2
Co0
promote
stability.
Furthermore,
exhibit
favorable
performance
removing
simulated
wastewater
air
discharge-electrocatalytic
cascade
system
produce
ammonia.
Environmental Science & Technology,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 6, 2025
Improving
the
reduction
efficiency
and
N2
selectivity
is
important
for
nitrate
decontamination.
A
novel
ternary
ball-milled
Al-Cu-AC
material
reported
to
achieve
a
highly
selective
of
N2.
The
process,
driven
by
continuous
dissolution
zero-valent
aluminum
(ZVAl),
demonstrated
stepwise
scheme.
interesting
shift
in
electron-donating
pathways
was
ascribed
spontaneous
change
microenvironmental
pH
from
neutral
alkaline.
(1:1:5
mass
ratio)
completely
removed
30
mg/L
NO3--N
over
wide
range
(5-9),
achieving
83%
TN
removal
N2-selectivity,
without
detectable
copper
leaching.
atomic
hydrogen
(H*)-mediated
occurring
on
Cu
component
proven
be
crucial
fast
transformation
NO3-
NO2-,
while
non-H*
process
dominated
electrochemical
NO2-
AC
cathode
Al
||
microgalvanic
cells
formed
material.
primary
route
identified
as
*NOH
pathway,
superiority
toward
verified
with
actual
wastewater.
This
study
revealed
how
influenced
ZVAl
provides
new
approach
maximize
performance
metals.