ACS Applied Materials & Interfaces,
Journal Year:
2024,
Volume and Issue:
16(13), P. 16062 - 16074
Published: March 25, 2024
Efficient
charge
transfer
and
light-trapping
units
are
pivotal
prerequisites
in
the
realm
of
Ti-based
photoanode
photoelectrochemical
(PEC)
water
splitting.
In
this
work,
we
successfully
synthesized
a
ternary
carbon
quantum
dots/Bi2S3
dots/Nb-doped
TiO2
nanotube
arrays
(CQDs/Bi2S3/TiNbO)
composite
for
PEC
CQDs/Bi2S3/TiNbO
exhibited
considerably
elevated
photocurrent
density
8.80
mA
cm–2
at
1.23
V
vs
reversible
hydrogen
electrode,
which
was
20.00
times
better
than
that
(0.44
cm–2).
Furthermore,
attested
to
exceptional
stability,
maintaining
92.54%
its
initial
current
after
5
h
stability
measurement.
Nb-doping
boosted
electrical
conductivity,
facilitating
solid–liquid
interface.
Moderate
amounts
Bi2S3
dots
(QDs)
CQDs
deposited
on
TiNbO
provided
abundant
active
sites
electrolyte–photoanode
interaction.
Simultaneously,
QDs
synergistically
functioned
as
broaden
light
absorption
range
from
396
530
nm,
stimulating
increased
carrier
generation
within
photoanode.
comparison
with
pristine
TiO,
photoanodes
possessed
superior
ability
promote
interfacial
reactions.
This
study
may
provide
strategy
developing
high-performance
efficient
trapping
highly
driving
solar-to-hydrogen
conversion.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(12)
Published: Jan. 15, 2023
Abstract
Electrochemical
reduction
of
nitrate
to
ammonia
(NO
3
RR)
holds
a
great
promise
for
attaining
both
NH
electrosynthesis
and
wastewater
purification.
Herein,
single‐atom
Bi
alloyed
Pd
metallene
(Bi
1
Pd)
is
reported
as
highly
effective
NO
RR
catalyst,
showing
near
100%
‐Faradaic
efficiency
with
the
corresponding
yield
33.8
mg
h
−1
cm
−2
at
−0.6
V
versus
RHE,
surpassing
those
almost
all
ever
catalysts.
In‐depth
theoretical
operando
spectroscopic
investigations
unveil
that
electronically
couples
its
neighboring
atoms
synergistically
activate
−
destabilize
*NO
on
Pd,
leading
reduced
energy
barrier
potential‐determining
step
(*NO→*NOH)
enhanced
protonation
energetics
‐to‐NH
pathway.
ACS Nano,
Journal Year:
2023,
Volume and Issue:
17(2), P. 1081 - 1090
Published: Jan. 11, 2023
The
electrochemical
nitrate
reduction
to
ammonia
reaction
(NO3RR)
has
emerged
as
an
appealing
route
for
achieving
both
wastewater
treatment
and
production.
Herein,
sub-nm
RuOx
clusters
anchored
on
a
Pd
metallene
(RuOx/Pd)
are
reported
highly
effective
NO3RR
catalyst,
delivering
maximum
NH3-Faradaic
efficiency
of
98.6%
with
corresponding
NH3
yield
rate
23.5
mg
h–1
cm–2
partial
current
density
296.3
mA
at
−0.5
V
vs
RHE.
Operando
spectroscopic
characterizations
combined
theoretical
computations
unveil
the
synergy
enhance
energetics
through
mechanism
hydrogen
spillover
hydrogen-bond
interactions.
In
detail,
activates
NO3–
form
intermediates,
while
dissociates
H2O
generate
*H,
which
spontaneously
migrates
RuOx/Pd
interface
via
process.
Further
interactions
between
spillovered
*H
intermediates
makes
desorb
from
participate
in
intermediate
hydrogenation,
contributing
enhanced
activity
NO3–-to-NH3
conversion.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(13)
Published: Jan. 18, 2023
Abstract
Electrochemical
reduction
of
nitrate
to
ammonia
(NO
3
RR)
has
been
recognized
as
an
appealing
approach
realize
both
sustainable
NH
production
and
waste
removal.
Herein,
from
the
perspective
Lewis
acid‐base
interaction,
a
single‐atom
Fe‐doped
V
2
O
5
(Fe‐V
)
catalyst
enriched
is
designed
with
acid
sites,
which
present
maximum
‐Faradaic
efficiency
97.1%
corresponding
yield
12.5
mg
h
−1
cm
−2
at
–0.7
versus
RHE.
Mechanistic
studies
based
on
theoretical
calculations
operando
spectroscopic
characterizations
identify
creation
Fe‐V
pairs
,
can
synergetically
activate
NO
−
promote
hydrogenation
energetics,
restrain
hydrogen
evolution,
leading
enhanced
RR
activity
selectivity.
ACS Energy Letters,
Journal Year:
2023,
Volume and Issue:
8(3), P. 1281 - 1288
Published: Feb. 3, 2023
Electrocatalytic
NO
reduction
to
NH3
(NORR)
offers
a
prospective
approach
attain
both
harmful
removal
and
efficient
electrosynthesis.
Main-group
p-block
metals
are
promising
NORR
candidates
but
still
lack
adequate
exploration.
Herein,
Sb
single
atoms
confined
in
amorphous
MoO3
(Sb1/a-MoO3)
designed
as
an
catalyst,
exhibiting
the
highest
yield
rate
of
273.5
μmol
h–1
cm–2
NO-to-NH3
Faradaic
efficiency
91.7%
at
−0.6
V
vs
RHE.
In
situ
spectroscopic
characterizations
theoretical
computations
reason
that
outstanding
performance
Sb1/a-MoO3
arises
from
isolated
Sb1
sites,
which
can
optimize
adsorption
*NO/*NHO
lower
reaction
energy
barriers
simultaneously
exhibit
higher
affinity
than
H2O/H
species.
Moreover,
our
strategy
be
extended
prepare
Bi1/a-MoO3,
showing
high
property,
demonstrating
immense
potential
metal
single-atom
catalysts
toward
high-performing
electrocatalysis.
