ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
15(1), P. 529 - 542
Published: Dec. 20, 2024
The
electrochemical
oxidation
of
ethylene
glycol
(EG)
derived
from
polyethylene
terephthalate
(PET)
plastic
into
value-added
chemicals,
coupled
with
hydrogen
evolution,
offers
a
promising
approach
to
addressing
pollution.
However,
the
mechanisms
by
which
adsorption
key
reaction
intermediates
affects
EG
(EGOR)
are
not
well
understood.
To
investigate
this,
we
synthesized
two
model
catalysts:
amorphous-phase
CoNiOOH/NF
and
CoNiOOH–Ni3S2/NF
an
amorphous/crystalline
interface.
Detailed
characterizations
theoretical
calculations
demonstrate
that
interface
in
shifts
d-band
center
upward,
enhancing
*OH
compared
amorphous
CoNiOOH/NF.
Enhanced
is
crucial
for
promoting
C–C
bond
cleavage
subsequent
dehydrogenation.
In
situ
infrared
absorption
spectroscopy
(IRAS)
reveal
formate
(FA)
primarily
formed
through
glycolic
acid,
followed
oxidation.
Notably,
achieves
industrial-level
current
densities
500
mA
cm–2
at
ultralow
potential
1.45
V
vs
RHE,
Faradaic
efficiency
(FE)
96.6%
FA
productivity
3.14
mmol
h–1
1.70
RHE.
This
study
valuable
insights
designing
efficient
heterojunction
catalysts
upcycling
PET
plastics.
Advanced Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 25, 2025
Abstract
To
overcome
the
challenges
of
low
catalytic
activity
and
instability,
a
molecular
weight
engineering
strategy
coupled
with
oxidative
ammonolysis
is
developed
to
synthesize
CoRu‐based
alloy
catalysts
distinct
morphologies
properties
from
biorefinery
lignin.
This
approach
effectively
modulates
intrinsic
active
sites
exposes
unsaturated
nitrogen‐oxygen
structures,
thereby
tailoring
morphology
defect
structure
carbon
layers
in
catalysts.
The
as‐synthesized
CoRu
lignin
precursors
varying
weights
are
designated
as
CoRu@OALC‐EtOAC,
CoRu@OALC‐EtOH,
CoRu@OALC‐Residual.
featuring
defect‐rich
graphitic
carbon‐coated
structure,
exhibited
exceptional
overall
water‐splitting
performance
(1.48
V
at
10
mA
cm
−2
),
significantly
surpassing
Pt/C
||
Ru/C
(1.58
).
In
contrast,
CoRu@OALC‐Residual,
its
amorphous
demonstrated
remarkable
stability
(350
h
100
vastly
outperforming
(6
In‐situ
Raman
spectroscopy
DFT
calculations
revealed
that
adsorb
*
H
intermediates,
accelerating
process.
strong
adsorption
also
induces
layer
rearrangement,
leading
dissolution
oxidation
metal
particles.
provides
universal
method
for
biomass‐derived
catalysts,
establishing
direct
relationship
between
weight,
catalyst
morphology,
electrocatalytic
performance.
The
electrochemical
oxygen
evolution
reaction
(OER)
as
a
rapid
control
step
in
water
splitting
for
hydrogen
production
can
utilise
FeNi-based
catalysts
to
reduce
the
overpotential.
In
considering
disparate
effects
of
crystalline
and
amorphous
phases
on
stability
activity
catalyst,
amorphous/crystalline
heterojunctions
were
formed
by
metal
oxides
employed
catalysts.
this
work,
NiFeOx-modified
Ni3S2-NiO/NF*
heterojunction
nanosheets
(NiFe@Ni3S2-NiO/NF*)
with
three-dimensional
structural
configuration
successfully
prepared
through
two-stage
process
involving
hydrothermal
electrical
treatments.
NiFe@Ni3S2-NiO/NF*,
electrically
activated
in-stiu
exhibit
stable
crystal
structure
regular
morphology,
which
enhances
catalytic
facilitates
exposure
active
sites.
Meanwhile,
nickel-iron
modified
electrodeposition
methods
robust
bond
substrate,
coupled
flexibility,
low
contact
resistance
high
electrocatalytic
activity.
NiFe@Ni3S2-NiO/NF*
electrode
exhibits
remarkable
towards
OER
alkaline
media,
particularly
at
potential
1.49
V
reach
large
current
density
50
mA
cm-2,
along
excellent
long-term
stability.
These
findings
are
significant
importance
providing
novel
insights
design
construction
oxide
Small,
Journal Year:
2025,
Volume and Issue:
unknown
Published: April 24, 2025
Abstract
Single
atomic
sites
(SAs)
face
challenges
in
catalyzing
complex
chemical
processes
involving
multiple
intermediates
due
to
rigid
coordination
environments,
steric
hindrances,
and
limited
activation
behaviors.
Herein,
an
alloying‐mediated
element
repartition
method
is
developed
synthesize
flexible
cesium
single‐atom
catalysts,
anchoring
Cs
single
on
precisely
controlled
amorphous‐MgO/crystalline
NbC
hetero‐phase
nano‐supports.
The
amorphousMgO(a‐MgO)
equipped
1
‐a‐MgO/NbC
achieves
91%
yield
the
cyclization
of
CO
2
with
2‐aminobenzonitrile
within
a
gas–liquid–solid
triphasic
system,
outperforming
its
counterpart
fabricated
crystalline
MgO,
‐c‐MgO/NbC
catalyst
(only
23%).
shows
excellent
tolerance
various
functional
groups
sustainable
catalysis,
especially
removing
traditional
requirement
for
high‐pressure
conditions
additives.
Operando
spectroscopic
characterizations
theoretical
calculations
demonstrate
that
sandwich‐structural
enhances
consecutive
through
vertically
adsorbed
configurations
during
C‐N
coupling
N‐heterocyclic
ring
formation.
SAs
supported
by
a‐MgO
nano‐cushions
allow
adaptability
dynamic
transformations
via
tensile
Cs‐O
compressive
Mg─O
bonds,
ultimately
reducing
energy
barriers
critical
rearrangement
isomerization
steps.
This
study
provides
valuable
insights
into
designing
SACs
overcome
limitations
support
interfaces,
thereby
enhancing
performance
toward
multi‐intermediate
conversion
heterogeneous
catalytic
transformations.
