Inorganic Chemistry,
Год журнала:
2024,
Номер
63(33), С. 15477 - 15484
Опубликована: Авг. 6, 2024
Transition-metal
phosphides
(TMPs)
have
attracted
extensive
attention
in
energy-related
fields,
especially
for
electrocatalytic
hydrogen
evolution
reaction
(HER).
However,
it
is
imperative
to
develop
a
facile
and
time-consuming
approach
prepare
metal
with
satisfactory
catalytic
performance.
Herein,
nitrogen-doped
CoP-Co
Nano Letters,
Год журнала:
2024,
Номер
24(21), С. 6302 - 6311
Опубликована: Май 15, 2024
Photocatalytic
synthesis
based
on
the
oxygen
reduction
reaction
(ORR)
has
shown
great
promise
for
H2O2
production.
However,
low
activity
and
selectivity
of
2e–
ORR
result
in
a
fairly
efficiency
Herein,
we
propose
strategy
to
enhance
proton-coupled
electron
transfer
(PCET)
process
covalent
organic
frameworks
(COFs),
thereby
significantly
boosting
photosynthesis.
We
demonstrated
that
construction
hydrogen-bonding
network,
achieved
by
anchoring
H3PO4
molecular
network
COF
nanochannels,
can
greatly
improve
both
proton
conductivity
photogenerated
charge
separation
COFs.
Thus,
COF@H3PO4
exhibited
superior
photocatalytic
performance
generating
without
sacrificial
agents,
with
solar-to-chemical
conversion
as
high
0.69%.
Results
indicated
much
more
localized
spatial
distribution
energy
band
density
led
efficient
separation,
small
barrier
rate-limiting
step
from
*OOH
endowed
higher
selectivity.
ABSTRACT
Ruthenium
(Ru)‐based
electrocatalysts
show
great
promise
as
substitutes
for
platinum
(Pt)
the
alkaline
hydrogen
evolution
reaction
(HER)
because
of
their
efficient
water
dissociation
capabilities.
Nevertheless,
strong
adsorption
Ru–OH
intermediates
(Ru‐OH
ad
)
blocks
active
site,
leading
to
unsatisfactory
HER
performance.
In
this
study,
we
report
a
universal
ligand‐exchange
strategy
synthesizing
MOF‐on‐MOF‐derived
FeP–CoP
heterostructure‐anchored
Ru
single‐atom
site
catalyst
(Ru‐FeP‐CoP/NPC).
The
obtained
shows
low
overpotential
(28
mV
at
10
mA
cm
−2
and
high
mass
activity
(9.29
A
mg
−1
100
mV),
surpassing
performance
commercial
Pt/C
by
factor
46.
Theoretical
studies
that
regulating
local
charge
distribution
sites
could
alleviate
surrounding
OH
−
blockages,
accelerating
facilitating
adsorption/desorption,
thus
enhancing
activity.
This
work
aims
inspire
further
design
highly
durable
with
tailored
electronic
properties
high‐purity
production.
Environmental Science & Technology,
Год журнала:
2024,
Номер
58(33), С. 14895 - 14905
Опубликована: Авг. 8, 2024
Breaking
the
activity-selectivity
trade-off
has
been
a
long-standing
challenge
in
catalysis.
Here,
we
proposed
nanoheterostructure
engineering
strategy
to
overcome
metal
phosphide
catalysts
for
oxidative
desulfurization
(ODS)
of
fuels.
Experimental
and
theoretical
results
demonstrated
that
electron
delocalization
was
key
driver
simultaneously
achieve
high
activity
selectivity
molybdenum
(MoP)/tungsten
(WP)
catalyst.
The
not
only
promoted
catalytic
pathway
transition
from
predominant
radicals
singlet
oxygens
H
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Сен. 29, 2024
Abstract
Heterogeneous
interfaces
designed
rationally
in
catalysts
can
induce
geometrical,
compositional,
and
electronic
effects
that
be
applied
to
modulate
catalytically
active
sites
consequently
accelerate
reaction
kinetics.
Here,
a
core‐shell
heterostructure
catalyst
consisting
of
crystalline
molybdenum
phosphide
(MoP)
cores
amorphous
tungsten
oxide
(WO
x
)
shells
on
porous
carbon
nanosheets
(PCN)
is
developed
for
oxidative
desulfurization
(ODS)
fuels.
The
strongly
coupled
heterogeneous
interface
triggers
distinctive
atomic
permeation
effect
induces
substantial
electron
transfer
from
MoP
WO
subsequent
generation
electron‐rich
W
sites,
optimizing
the
adsorption
intermediates
substrates.
resulting
@MoP/PCN)
demonstrates
turnover
frequency
as
high
768.1
h
−1
ODS
at
60
°C,
exceeding
almost
all
state‐of‐the‐art
by
1–2
orders
magnitude.
Moreover,
novel
surface
oxidation
pathway
based
direct
identified
@MoP/PCN‐H
2
O
system,
which
bypasses
formation
reactive
oxygen
species,
endowing
system
with
moderate
redox
potential.
Thus,
@MoP/PCN
exhibits
unprecedented
selectivity,
achieving
100%
removal
thiophenic
sulfides
real
diesel
minimal
consumption
oxidant.