Advanced Science,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 24, 2024
Abstract
Semiconductor‐based
photoelectrochemical
(PEC)
organic
transformations
usually
show
radical
characteristics,
in
which
the
reaction
selectivity
is
often
difficult
to
precisely
control
due
nonselectivity
of
radicals.
Accordingly,
several
simple
reactions
(e.g.,
oxidations
alcohols,
aldehydes,
and
other
small
molecules)
have
been
widely
studied,
while
more
complicated
processes
like
C─C
coupling
remain
challenging.
Herein,
a
synergistic
heterogeneous/homogeneous
PEC
strategy
developed
achieve
controllable
radical‐induced
mediated
by
copper‐coordination
effect
at
semiconductor/electrolyte
interfaces,
additionally
exerts
significant
impact
on
product
regioselectivity.
Through
experimental
studies
theoretical
simulations,
this
study
reveals
that
copper‐chloride
complex
effectively
regulates
formation
chloride
radicals,
typical
hydrogen
atom
transfer
agent,
semiconductor
surfaces
stabilizes
heterogeneous
interfaces
suppressing
surface
passivation.
Taking
Minisci
(the
between
2‐phenylquinoline
cyclohexane)
as
model,
yield
target
reaches
up
90%
TiO
2
photoanodes
with
95%
long‐term
stability
over
100
h.
Moreover,
such
exhibits
broad
scope
can
be
used
for
functionalization
various
heteroaromatic
hydrocarbons.
ACS Sensors,
Год журнала:
2024,
Номер
9(5), С. 2684 - 2694
Опубликована: Май 2, 2024
Semiconductor-based
photoelectrochemical
(PEC)
test
protocols
offer
a
viable
solution
for
developing
efficient
individual
health
monitoring
by
converting
light
and
chemical
energy
into
electrical
signals.
However,
slow
reaction
kinetics
electron–hole
complexation
at
the
interface
limit
their
practical
application.
Here,
we
reported
triple-engineered
CdS
nanohierarchical
structures
(CdS
NHs)
modification
scheme
including
morphology,
defective
states,
heterogeneous
structure
to
achieve
precise
of
neurotransmitter
dopamine
(DA)
in
plasma
noninvasive
body
fluids.
By
precisely
manipulating
Cd–S
precursor,
achieved
control
over
ternary
NHs
obtained
well-defined
layered
self-assembled
through
surface
carbon
treatment.
The
integration
defect
states
thin
layer
effectively
established
carrier
directional
transfer
pathways,
thereby
enhancing
sites
improving
conversion
efficiency.
microelectrode
fabricated
demonstrated
remarkable
negative
response
toward
DA,
enabling
development
miniature
self-powered
PEC
device
quantification
human
saliva.
Additionally,
utilization
density
functional
theory
calculations
elucidated
structural
characteristics
DA
state
CdS,
thus
establishing
crucial
theoretical
groundwork
optimizing
polymerization
process
DA.
present
study
offers
potential
engineering
approach
high
efficiency
semiconductors
as
well
proposing
novel
concept
designing
sensitive
testing
strategies.
Abstract
Selective
oxidation
of
amines
to
imines
through
electrocatalysis
is
an
attractive
and
efficient
way
for
the
chemical
industry
produce
nitrile
compounds,
but
it
limited
by
difficulty
designing
catalysts
lack
understanding
mechanism
catalysis.
Herein,
we
demonstrate
a
novel
strategy
generation
oxyhydroxide
layers
on
two‐dimensional
iron‐doped
layered
nickel
phosphorus
trisulfides
(Ni
1−
x
Fe
PS
3
)
during
benzylamine
(BA).
In‐depth
structural
surface
characterizations
electrocatalytic
process
combined
with
theoretical
calculations
reveal
that
Ni
(1−
undergoes
reconstruction
under
alkaline
conditions
form
metal
oxyhydroxide/phosphorus
trichalcogenide
(NiFeOOH/Ni
heterostructure.
Interestingly,
generated
heterointerface
facilitates
BA
low
onset
potential
1.39
V
Faradaic
efficiency
53%
benzonitrile
(BN)
synthesis.
Theoretical
further
indicate
as‐formed
NiFeOOH/Ni
heterostructure
could
offer
optimum
free
energy
adsorption
BN
desorption,
resulting
in
promising
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Июнь 18, 2024
Abstract
Steering
on
the
intrinsic
active
site
of
an
electrode
material
is
essential
for
efficient
electrochemical
biomass
upgrading
to
valuable
chemicals
with
high
selectivity.
Herein,
we
show
that
in-situ
surface
reconstruction
a
two-dimensional
layered
CdPS
3
nanosheet
electrocatalyst,
triggered
by
electrolyte,
facilitates
5-hydroxymethylfurfural
(HMF)
hydrogenation
2,5-bis(hydroxymethyl)furan
(BHMF)
under
ambient
condition.
The
Raman
spectroscopy
and
comprehensive
post-mortem
catalyst
characterizations
evidence
construction
surface-bounded
CdS
layer
form
/CdS
heterostructure.
This
electrocatalyst
demonstrates
promising
catalytic
activity,
achieving
Faradaic
efficiency
BHMF
reaching
91.3
±
2.3
%
yield
4.96
0.16
mg/h
at
−
0.7
V
versus
reversible
hydrogen
electrode.
Density
functional
theory
calculations
reveal
generated
interface
plays
pivotal
role
in
optimizing
adsorption
HMF*
H*
intermediate,
thus
facilitating
HMF
process.
Furthermore,
reconstructed
heterostructure
cathode,
when
coupled
MnCo
2
O
4.5
anode,
enables
simultaneous
formate
synthesis
from
glycerol
substrates
efficiency.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(46)
Опубликована: Июнь 25, 2024
Abstract
Photoelectrochemical
cells
(PEC)
use
solar
energy
to
generate
green
hydrogen
by
water
splitting
and
have
an
integrated
device
structure.
Achieving
high
solar‐to‐hydrogen
conversion
(STH)
efficiency
along
with
a
long
operational
lifetime
in
these
is
crucial
for
the
production
of
low‐cost
as
viable
source.
Several
functional
components,
such
photo
absorber,
charge
transport,
catalyst
layers
are
interfaced
form
compact
monolithic
device.
In
this
review,
therefore,
engineering
design
individual
components
cells,
interplay
between
them,
their
interfaces
discussed
detail,
factors
determine
overall
performance
cells.
The
main
emphasis
on
halide
perovskite
(HP)
absorbers,
which
emerged
promising
materials
due
superior
optoelectronic
properties.
Recent
advances
development
efficient
stable
perovskite‐based
highlighted
reviewed.
catalysts
effect
pH
supporting
cations
also
examined.
Finally,
scientific
challenges
future
directions
designing
photoelectrochemical
discussed.
This
review
can
help
researchers
further
advance
technology
toward
commercial
hydrogen.
Chemical Reviews,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 21, 2024
Photoelectrochemical
(PEC)
systems
are
essential
for
solar
energy
conversion,
addressing
critical
and
environmental
issues.
However,
the
low
efficiency
in
utilizing
photogenerated
charge
carriers
significantly
limits
overall
conversion.
Consequently,
there
is
a
growing
focus
on
developing
strategies
to
enhance
photoelectrode
performance.
This
review
systematically
explores
recent
advancements
PEC
system
modifications,
spanning
from
atomic
nanoscopic
levels
configuration
engineering.
We
delve
into
relationships
between
structures,
intrinsic
properties,
kinetics
of
carriers,
their
utilization.
Additionally,
we
propose
future
directions
perspectives
more
efficient
systems,
offering
valuable
insights
potential
innovations
field.
Energy & Environmental Science,
Год журнала:
2024,
Номер
17(20), С. 7459 - 7511
Опубликована: Янв. 1, 2024
This
review
provides
a
comprehensive
overview
on
the
mechanism
of
photoelectrochemical
biomass
conversion
and
highlights
extension
dual-function
cells
for
valorization
paired
with
more
valuable
half-reactions.
RSC Advances,
Год журнала:
2025,
Номер
15(1), С. 665 - 673
Опубликована: Янв. 1, 2025
A
photoelectrochemical
enzymatic
biofuel
cell
consisting
of
a
(methyl
violet/Au
nanoparticles)
25
/fluorine-doped
tin
oxide
(FTO)
photoanode
without
conventional
semiconductor(s)
and
bilirubin
oxidase/CuCo
2
O
4
/FTO
bio-photocathode
is
developed.
The
urea
oxidation
reaction
(UOR),
with
its
low
thermodynamic
potential,
offers
a
promising
alternative
to
the
oxygen
evolution
(OER)
for
efficient
hydrogen
production.
However,
sluggish
kinetics
still
demand
development
of
an
electrocatalyst.
In
this
study,
critical
role
Ru
doping
in
Fe₂TiO₅
is
demonstrated
accelerate
UOR
kinetics.
computational
finding
confirmed
feasibility
approach,
guiding
experimental
synthesis
Fe2-xRuxTiO5.
Benefitting
from
surface
properties
and
electronic
structure,
synthesized
material
exhibits
superior
performance
potential
1.30
V
at
current
density
10
mA
cm-2
UOR,
compared
undoped
Fe2TiO5
(1.40
V).
Moreover,
it
demonstrates
favourable
Tafel
slope
52
mV
dec-1
maintains
robust
durability
72
h.
As
findings,
enhanced
activity
can
be
attributed
resulting
structural
distortion
Fe
site
creation
adsorption
thereby
enhancing
via
dual
active
center.
This
study
not
only
broadens
applications
Fe2TiO5-based
materials
beyond
their
traditional
as
photocatalysts
but
also
establishes
them
electrocatalysts
underscoring
versatility
improved
