Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 29, 2025
Abstract
Synergistically
optimizing
electronic
structure
and
exposing
abundant
active
sites
to
significantly
improve
performance
of
transition
metal‐based
electrocatalysts
is
an
urgent
necessity
remains
a
significant
challenge.
Herein,
hybrid
nanotubes
array
rich
P‐vacancy
V‐CoP@Cu
3
P
in
situ
grown
on
copper
foam
(V
‐V‐CoP@Cu
HNTAs/CF)
fabricated
for
overall
water
splitting.
The
combined
experimental
theoretical
calculations
reveal
that
V
doping‐induced
vacancies
lead
the
formation
local
electric
field
within
V‐CoP
heterojunction‐induced
built‐in
field,
which
can
jointly
accelerate
electron
transfer
charge
separation,
thereby
enhancing
reaction
kinetics.
Moreover,
nanotube
not
only
increase
electrochemical
surface
area
offer
superior
mass
transfer,
but
also
possess
superhydrophilic
nature
utilization
efficiency
electrode
surfaces.
Due
these
advantages,
HNTAs/CF
provide
distinguished
HER
OER
activity,
by
employing
as
bifunctional
electrocatalysts,
splitting
device
delivered
current
density
10
mA
cm
−2
at
low
voltage
1.46
maintained
its
activity
without
decay
200
h
1
m
KOH
electrolyte.
Advanced Materials,
Год журнала:
2024,
Номер
36(33)
Опубликована: Июнь 12, 2024
Abstract
Earth‐abundant
metal
oxides
are
usually
considered
as
stable
but
catalytically
inert
toward
hydrogen
evolution
reaction
(HER)
due
to
their
unfavorable
intermediate
adsorption
performance.
Herein,
a
heavy
rare
earth
(Y)
and
transition
(Co)
dual‐doping
induced
lattice
strain
oxygen
vacancy
stabilization
strategy
is
proposed
boost
CeO
2
robust
alkaline
HER.
The
compression
increased
(O
v
)
concentration
in
synergistically
improve
the
water
dissociation
on
O
sites
sequential
at
activated
‐neighboring
sites,
leading
significantly
enhanced
HER
kinetics.
Meanwhile,
Y
doping
offers
effect
by
its
stronger
Y─O
bonding
over
Ce─O,
which
endows
catalyst
with
excellent
stability.
Y,Co‐CeO
electrocatalyst
exhibits
an
ultra‐low
overpotential
(27
mV
10
mA
cm
−2
Tafel
slope
(48
dec
−1
),
outperforming
benchmark
Pt
electrocatalyst.
Moreover,
anion
exchange
membrane
electrolyzer
incorporated
achieves
stability
of
500
h
under
600
.
This
synergistic
sheds
new
light
rational
development
efficient
oxide‐based
electrocatalysts.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 28, 2025
Abstract
Electrochemical
oxidation
of
biomass‐derived
5‐hydroxymethylfurfural
(HMF)
provides
an
environmentally
friendly
route
for
producing
the
sustainable
polymer
monomer
2,5‐furandicarboxylic
acid
(FDCA).
Thus,
precisely
adjusting
synergistic
adsorption
among
key
reactive
species,
such
as
HMF
and
OH
ads
,
on
carefully
designed
catalyst
surface
is
essential
achieving
satisfactory
catalytic
performance
to
FDCA
it
closely
related
strength
configuration
reaction
substrates.
This
kind
regulation
will
ultimately
facilitate
improvement
performance.
In
this
work,
Pt
nanoparticles
modified
CuO
nanowires
(denoted
Pt/CuO@CF)
are
constructed
selective
electrooxidation
under
alkaline
conditions.
The
well‐designed
Pt/CuO@CF
demonstrates
highly
impressive
across
a
range
concentrations,
ranging
from
commonly
used
concentrations
higher
levels
typically
not
explored
(10,
25,
50,
75,
100
m
)
with
high
FE
(all
above
95%)
outstanding
long‐term
stability
(15
cycles).
situ
experimental
characterizations
confirm
that
heterogeneous
interface
between
enhances
enrichment
species
surface.
Theoretical
calculations
reveal
anchored
reduce
barrier
thereby
promoting
FDCA.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 2, 2025
Abstract
Electrochemical
5‐hydroxymethylfurfural
oxidation
reaction
(HMFOR)
offers
a
promising
approach
to
producing
valuable
chemicals
and
facilitating
coupled
H
2
production.
A
significant
challenge
in
the
HMFOR
lies
elucidating
interaction
mechanisms
between
active
sites
(HMF).
However,
unpredictable
reconstruction
of
during
catalytic
process
complicates
understanding
these
mechanisms.
In
this
study,
novel
heterojunction
(CoSe
@NiSe‐CoSe
/NF)
is
synthesized
using
straightforward
hydrothermal
method
combined
with
classical
selenization.
This
demonstrates
exceptional
electrocatalytic
performance
for
direct
HMF
oxidation,
achieving
Faradaic
efficiency
2,5‐furanedicarboxylic
acid
(FDCA)
up
97.9%.
Notably,
it
requires
only
1.29
V
versus
RHE
achieve
current
density
10
mA
cm
−2
HMFOR‐assisted
hydrogen
evolution
(HER).
The
high
activity
primarily
arises
from
interfacial
electron
redistribution.
Specifically,
Co
modulates
band
structure
Ni,
Se
serving
as
intermediary.
modulation
increases
adsorption
energy
reduces
barrier
rate‐determining
step
HMFOR.
research
not
achieves
selective
synthesis
high‐value
but
also
provides
comprehensive
analysis
structure‐performance
relationship
catalyst,
offering
new
pathway
development
efficient
heterogeneous
catalysts.
Nano-Micro Letters,
Год журнала:
2024,
Номер
16(1)
Опубликована: Авг. 22, 2024
Abstract
Electrocatalytic
5-hydroxymethylfurfural
oxidation
reaction
(HMFOR)
provides
a
promising
strategy
to
convert
biomass
derivative
high-value-added
chemicals.
Herein,
cascade
is
proposed
construct
Pd–NiCo
2
O
4
electrocatalyst
by
Pd
loading
on
Ni-doped
Co
3
and
for
highly
active
stable
synergistic
HMF
oxidation.
An
elevated
current
density
of
800
mA
cm
–2
can
be
achieved
at
1.5
V,
both
Faradaic
efficiency
yield
2,5-furandicarboxylic
acid
remained
close
100%
over
10
consecutive
electrolysis.
Experimental
theoretical
results
unveil
that
the
introduction
atoms
modulate
local
electronic
structure
Ni/Co,
which
not
only
balances
competitive
adsorption
OH
–
species,
but
also
promote
Ni
3+
species
formation,
inducing
high
indirect
activity.
We
have
discovered
incorporation
facilitates
2+
pre-oxidation
electrophilic
OH*
generation
contribute
direct
process.
This
work
new
approach
design
advanced
upgrading.
ACS Catalysis,
Год журнала:
2024,
Номер
unknown, С. 17510 - 17524
Опубликована: Ноя. 13, 2024
2,5-Furandicarboxylic
acid
(FDCA)
is
a
promising
biomass-derived
alternative
to
fossil-based
terephthalic
acid.
The
catalytic
oxidation
of
5-hydroxymethylfurfural
(HMF)
FDCA
widely
recognized
as
viable
route
for
producing
at
industrially
relevant
concentrations
(approximately
20
wt
%);
however,
this
has
not
yet
been
achieved.
Toward
goal,
we
report
that
through
controlled
engineering
an
oxygen-vacancy-enriched
Mn/Co
oxide
the
support
Pt
nanoparticles,
heterostructure
Pt/PtO2
with
electron-rich
interfacial
Pt–O–Mn
sites
(Pt/Mn10Co1Ox-VC)
formed,
significantly
enhancing
adsorption
and
activation
O2,
HMF,
its
key
intermediates.
As
result,
selective
both
HMF
(up
40
%)
crude
(10
%
70
purity)
was
achieved
high
yields
ranging
from
83%
95%
under
base-free
conditions,
demonstrating
strong
economic
feasibility
industrial
potential
production.
This
work
highlights
rational
design
structures
efficient
aldehydes
alcohols
bio-based
dicarboxylic
acids
concentrations,
paving
way
serve
sustainable
comonomer
in
polyester
Abstract
Electrochemical
upcycling
of
end‐of‐life
polyethylene
terephthalate
(PET)
using
renewable
electricity
offers
a
route
to
generate
valuable
chemicals
while
processing
plastic
wastes.
However,
it
remains
huge
challenge
design
an
electrocatalyst
with
reliable
structure‐property
relationships
for
PET
valorization.
Herein,
spinel
Co
3
O
4
rich
oxygen
vacancies
improved
activity
toward
formic
acid
(FA)
production
from
hydrolysate
is
reported.
Experimental
investigations
combined
theoretical
calculations
reveal
that
incorporation
V
into
not
only
promotes
the
generation
reactive
hydroxyl
species
(OH
*
)
at
adjacent
tetrahedral
2+
(Co2+
Td),
but
also
induces
electronic
structure
transition
octahedral
3+
(Co3+
Oh)
Oh),
which
typically
functions
as
highly‐active
catalytic
sites
ethylene
glycol
(EG)
chemisorption.
Moreover,
enlarged
Co‐O
covalency
induced
by
facilitates
electron
transfer
EG
OH
via
Co2+
Oh‐O‐Co2+
Td
interaction
and
following
C─C
bond
cleavage
direct
oxidation
glyoxal
intermediate
pathway.
As
result,
‐Co
catalyst
exhibits
high
half‐cell
oxidation,
Faradaic
efficiency
(91%)
productivity
(1.02
mmol
cm
−2
h
−1
FA.
Lastly,
demonstrated
hundred
gram‐scale
formate
crystals
can
be
produced
real‐world
bottles
two‐electrode
electroreforming,
yield
82%.