Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Июль 19, 2024
Abstract
The
electrochemical
oxygen
reduction
reaction
(ORR)
to
produce
hydrogen
peroxide
(H
2
O
)
is
appealing
due
its
sustainability.
However,
efficiency
compromised
by
the
competing
4e
−
ORR
pathway.
In
this
work,
we
report
a
hierarchical
carbon
nanosheet
array
electrode
with
single-atom
Ni
catalyst
synthesized
using
organic
molecule-intercalated
layered
double
hydroxides
as
precursors.
exhibits
excellent
2e
performance
under
alkaline
conditions
and
achieves
H
yield
rates
of
0.73
mol
g
cat
−1
h
in
H-cell
5.48
flow
cell,
outperforming
most
reported
catalysts.
experimental
results
show
that
atoms
selectively
adsorb
,
while
nanosheets
generate
reactive
species,
synergistically
enhancing
production.
Furthermore,
coupling
system
integrating
ethylene
glycol
oxidation
significantly
enhances
rate
7.30
producing
valuable
glycolic
acid.
Moreover,
convert
electrolyte
containing
directly
into
downstream
product
sodium
perborate
reduce
separation
cost
further.
Techno-economic
analysis
validates
economic
viability
system.
Advanced Materials,
Год журнала:
2024,
Номер
36(23)
Опубликована: Март 20, 2024
Abstract
The
plastic
waste
issue
has
posed
a
series
of
formidable
challenges
for
the
ecological
environment
and
human
health.
While
conventional
recycling
strategies
often
lead
to
down‐cycling,
electrochemical
strategy
recovering
valuable
monomers
enables
an
ideal,
circular
economy.
Here
corrosion
synthesized
single
atom
Pt
1
/Ni(OH)
2
electrocatalyst
with
part‐per‐million
noble
loading
highly
efficient
selective
upcycling
polyethylene
terephthalate
(PET)
into
chemicals
(potassium
diformate
terephthalic
acid)
green
hydrogen
is
reported.
Electro‐oxidation
PET
hydrolysate,
ethylene
glycol
(EG),
formate
processed
high
Faraday
efficiency
(FE)
selectivity
(>90%)
at
current
density
close
1000
mA
cm
−2
(1.444
V
vs
RHE).
in
situ
spectroscopy
functional
theory
calculations
provide
insights
mechanism
understanding
efficiency.
Remarkably,
electro‐oxidation
EG
ampere‐level
also
successfully
illustrated
by
using
membrane‐electrode
assembly
FEs
integrated
production
500
h
continuous
operation.
This
process
allows
chemical
space‐time
yield
profitable
(588–700
$
ton
−1
PET),
showing
industrial
perspective
on
single‐atom
catalysis
upcycling.
Energy & Environmental Science,
Год журнала:
2024,
Номер
17(12), С. 4205 - 4215
Опубликована: Янв. 1, 2024
A
honeycomb-like
PtAu
alloy
catalyst
has
been
developed
to
modulate
the
adsorption
capacity
of
OH
−
species
and
configuration
glycerol
on
surface
for
electrocatalytic
upgrading
C
3
chemicals.
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Июль 28, 2024
Abstract
Electro‐reforming
of
poly(ethylene
terephthalate)
(PET)
into
valuable
chemicals
is
garnering
significant
attention
as
it
opens
a
mild
avenue
for
waste
resource
utilization.
However,
achieving
high
activity
and
selectivity
C2
products
during
ethylene
glycol
(EG)
oxidation
in
PET
hydrolysate
on
Pd
electrocatalysts
remains
challenging.
The
strong
interaction
between
carbonyl
(*CO)
intermediates
leads
to
undesirable
over‐oxidation
poisoning
sites,
which
hinders
the
highly
efficient
production.
Herein,
nonmetallic
alloying
strategy
employed
fabricate
Pd‐boron
alloy
aerogel
(PdB),
wherein
B
atoms
are
induced
regulate
electron
structure
surface
oxophilicity.
This
approach
allows
remarkable
mass
6.71
A
mg
−1
,
glycolic
acid
(GA)
Faradaic
efficiency
(FE)
93.8%,
stable
100
h
cyclic
electrolysis.
In
situ
experiments
density
functional
theory
calculations
reveal
contributions
inserted
lattice
effective
EG‐to‐GA
conversion.
Interestingly,
heightened
oxophilicity
regulated
electronic
by
incorporation
weakened
*CO
adsorption
enhanced
hydroxyl
species
affinity
accelerate
oxidative
*OH
adspecies
formation,
thereby
synergistically
avoiding
boosting
GA
synthesis.
work
provides
insights
rational
design
high‐performance
synthesis
via
an
oxophilic
motifs
strategy.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Июль 19, 2024
Abstract
The
electrochemical
oxygen
reduction
reaction
(ORR)
to
produce
hydrogen
peroxide
(H
2
O
)
is
appealing
due
its
sustainability.
However,
efficiency
compromised
by
the
competing
4e
−
ORR
pathway.
In
this
work,
we
report
a
hierarchical
carbon
nanosheet
array
electrode
with
single-atom
Ni
catalyst
synthesized
using
organic
molecule-intercalated
layered
double
hydroxides
as
precursors.
exhibits
excellent
2e
performance
under
alkaline
conditions
and
achieves
H
yield
rates
of
0.73
mol
g
cat
−1
h
in
H-cell
5.48
flow
cell,
outperforming
most
reported
catalysts.
experimental
results
show
that
atoms
selectively
adsorb
,
while
nanosheets
generate
reactive
species,
synergistically
enhancing
production.
Furthermore,
coupling
system
integrating
ethylene
glycol
oxidation
significantly
enhances
rate
7.30
producing
valuable
glycolic
acid.
Moreover,
convert
electrolyte
containing
directly
into
downstream
product
sodium
perborate
reduce
separation
cost
further.
Techno-economic
analysis
validates
economic
viability
system.
