Polymer
gels,
renowned
for
unparalleled
chemical
stability
and
self-sustaining
properties,
have
garnered
significant
attention
in
electrocatalysis.
Notably,
organic
polymer
gels
that
exhibit
temperature
sensitivity
incorporate
suitable
polar
nonvolatile
liquids,
enhance
electronic
conductivity,
impart
distinct
morphological
features,
but
remain
largely
unexplored
as
electrocatalysts
oxygen
reduction
reaction
(ORR).
To
address
this
issue,
an
innovative
strategy
is
proposed
synergistic
modulation
of
the
rigidity
mainchain
molecular
skeleton
length
alkyl
sidechains,
enabling
development
organogel
polymers
with
a
sol-gel
temperature-sensitive
phase
transition
promises
high
selectivity
enhanced
activity
electrocatalytic
processes.
shortening
sidechain
can
significantly
affect
gelation
behavior
internal
microstructure
catalyst,
which
modifies
electron
state,
ultimately
impacting
catalytic
gel
catalysts.
In
particular,
phenyl-containing
Ph-FL1
short
sidechains
demonstrates
outstanding
2e
Chemical Science,
Год журнала:
2024,
Номер
15(29), С. 11188 - 11228
Опубликована: Янв. 1, 2024
The
oxygen
reduction
reaction
(ORR)
is
a
key
component
for
many
clean
energy
technologies
and
other
industrial
processes.
However,
the
low
selectivity
sluggish
kinetics
of
ORR
catalysts
have
hampered
conversion
efficiency
real
application
these
new
mentioned
before.
Recently,
tremendous
efforts
been
made
in
mechanism
understanding,
electrocatalyst
development
system
design.
Here,
comprehensive
critical
review
provided
to
present
recent
advances
field
electrocatalytic
ORR.
two-electron
four-electron
transfer
catalytic
mechanisms
evaluation
parameters
are
discussed
first.
Then,
up-to-date
synthetic
strategies
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 5, 2025
Abstract
Limited
by
the
activity‐selectivity
trade‐off
relationship,
electrochemical
activation
of
small
molecules
(like
O
2
,
N
2,
and
CO
)
rapidly
diminishes
Faradaic
efficiencies
with
elevated
current
densities
(particularly
at
ampere
levels).
Nevertheless,
some
catalysts
can
circumvent
this
restriction
in
a
two‐electron
oxygen
reduction
reaction
(2e
−
ORR),
sustainable
pathway
for
activating
to
hydrogen
peroxide
(H
).
Here
we
report
2e
ORR
expedited
fluorine‐bridged
copper
metal–organic
framework
catalyst,
arising
from
water
spillover
effect.
Through
operando
spectroscopies,
kinetic
theoretical
characterizations,
it
demonstrates
that
under
neutral
conditions,
plays
dual
role
accelerating
dissociation
stabilizing
key
*
OOH
intermediate.
Benefiting
spillover,
catalyst
expedite
density
range
0.1–2.0
A
cm
−2
both
high
(99–84.9%)
H
yield
rates
(63.17–1082.26
mg
h
−1
Further,
feasibility
present
system
has
been
demonstrated
scaling
up
unit
module
cell
25
combination
techno‐economics
simulations
showing
production
cost
strongly
dependent
on
densities,
giving
lowest
price
$0.50
kg
2.0
.
This
work
is
expected
provide
an
additional
dimension
leverage
systems
independent
oftraditional
rules.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(52)
Опубликована: Авг. 26, 2024
Abstract
The
electrosynthesis
of
hydrogen
peroxide
(H
2
O
)
via
two‐electron
oxygen
reduction
reaction
(2e
−
‐ORR)
enables
high
energy
utilization
and
distributed
H
production.
Rational
catalyst
design
is
essential
for
achieving
efficient
production,
in
which
fluorine‐modified
carbon
materials
hold
great
potential.
However,
conventional
methods
can
only
induce
limited
loading
fluorine
atoms
carbon‐based
catalysts,
leading
to
unsatisfying
electrochemical
performance.
Herein,
the
fluorine‐containing
active
sites
with
density
2e
‐ORR
selectivity
achieved
by
chained
polytetrafluoroethylene
precursors
onto
conductive
substrates
plasma‐assisted
ball
milling
technique.
Consequently,
defect‐rich
PTFE@CNTs
show
a
over
95%
yield
more
than
35
mol
g
−1
h
.
Furthermore,
production
be
readily
integrated
water
purification
units
decompose
contaminants,
showing
80%
degradation
multiple
dyes
within
1
removal
ratio
antibiotics
4
h.
In
addition,
100%
sterilization
staphylococcus
aureus
on‐site
accumulating
commercial
saline
30
min.
This
defect
engineering
strategy
through
plasma
provides
promising
universal
avenue
toward
designing
highly
electrocatalysts
as
well
other
processes.
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 23, 2024
Abstract
Alloying
has
significantly
upgraded
the
oxygen
reduction
reaction
(ORR)
of
Pd‐based
catalysts
through
regulating
thermodynamics
oxygenated
intermediates.
However,
unsatisfactory
activation
ability
alloys
toward
O
2
molecules
limits
further
improvement
ORR
kinetics.
Herein,
precise
synthesis
nanosheet
assemblies
spin‐polarized
PdCu–Fe
3
4
in‐plane
heterostructures
for
drastically
activating
and
boosting
kinetics
is
reported.
It
demonstrated
that
deliberate‐engineered
not
only
tailor
d
‐band
center
Pd
sites
with
weakened
adsorption
intermediates
but
also
endow
electrophilic
Fe
strong
to
activate
molecules,
which
make
exhibit
highest
specific
activity
among
state‐of‐art
so
far.
In
situ
electrochemical
spectroscopy
theoretical
investigations
reveal
a
tandem
catalytic
mechanism
on
─Fe
initially
molecular
generate
being
transferred
finish
subsequent
proton‐coupled
electron
transfer
steps.
