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.
Energy & Environmental Science,
Год журнала:
2023,
Номер
17(1), С. 49 - 113
Опубликована: Ноя. 7, 2023
This
perspective
highlights
recent
advancements
in
innovative
strategies
to
provide
valuable
insights
into
the
potential
for
energy-saving
hydrogen
production
through
water
electrolysis.
Advanced Materials,
Год журнала:
2023,
Номер
36(4)
Опубликована: Окт. 10, 2023
Abstract
As
one
of
the
most
promising
approaches
to
producing
high‐purity
hydrogen
(H
2
),
electrochemical
water
splitting
powered
by
renewable
energy
sources
such
as
solar,
wind,
and
hydroelectric
power
has
attracted
considerable
interest
over
past
decade.
However,
electrolysis
process
is
seriously
hampered
sluggish
electrode
reaction
kinetics,
especially
four‐electron
oxygen
evolution
at
anode
side,
which
induces
a
high
overpotential.
Currently,
emerging
hybrid
strategy
proposed
integrating
thermodynamically
favorable
electro–oxidation
reactions
with
cathode,
providing
new
opportunity
for
energy–efficient
H2
production.
To
achieve
highly
efficient
cost–effective
toward
large–scale
practical
H
production,
much
work
been
continuously
done
exploit
alternative
anodic
oxidation
cutting–edge
electrocatalysts.
This
review
will
focus
on
recent
developments
production
coupled
reactions,
including
choice
substrates,
investigation
electrocatalytic
materials,
deep
understanding
underlying
mechanisms.
Finally,
some
insights
into
scientific
challenges
now
standing
in
way
future
advancement
technique
are
shared,
hope
inspiring
further
innovative
efforts
this
rapidly
growing
field.
Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Сен. 12, 2023
Electrooxidation
of
biomass
platforms
provides
a
sustainable
route
to
produce
valuable
oxygenates,
but
the
practical
implementation
is
hampered
by
severe
carbon
loss
stemming
from
inherent
instability
substrates
and/or
intermediates
in
alkaline
electrolyte,
especially
under
high
concentration.
Herein,
based
on
understanding
non-Faradaic
degradation,
we
develop
single-pass
continuous
flow
reactor
(SPCFR)
system
with
ratio
electrode-area/electrolyte-volume,
short
duration
time
reactor,
and
separate
feeding
substrate
solution,
thus
largely
suppressing
degradation.
By
constructing
nine-stacked-modules
SPCFR
system,
achieve
electrooxidation
glucose-to-formate
5-hydroxymethylfurfural
(HMF)-to-2,5-furandicarboxylic
acid
(FDCA)
conversion
efficiency
(SPCE;
81.8%
95.8%,
respectively)
selectivity
(formate:
76.5%,
FDCA:
96.9%)
at
concentrations
562.8
mM,
556.9
mM).
Furthermore,
demonstrate
kilogram-scale
electrosynthesis
potassium
diformate
(0.7
kg)
wood
soybean
oil,
FDCA
(1.17
HMF.
This
work
highlights
importance
providing
opportunities
for
scalable
upgrading
using
electrochemical
technology.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Март 18, 2024
Abstract
Preventing
the
deactivation
of
noble
metal-based
catalysts
due
to
self-oxidation
and
poisonous
adsorption
is
a
significant
challenge
in
organic
electro-oxidation.
In
this
study,
we
employ
pulsed
potential
electrolysis
strategy
for
selective
electrocatalytic
oxidation
glycerol
glyceric
acid
over
Pt-based
catalyst.
situ
Fourier-transform
infrared
spectroscopy,
quasi-in
X-ray
photoelectron
finite
element
simulations
reveal
that
could
tailor
catalyst’s
surface
micro-environment.
This
prevents
overaccumulation
poisoning
intermediate
species
frees
up
active
sites
re-adsorption
OH
adsorbate
glycerol.
The
results
higher
selectivity
(81.8%)
than
constant-potential
electrocatalysis
with
0.7
V
RHE
(37.8%).
work
offers
an
efficient
mitigate
electrocatalysts.
Electrochemical
valorization
of
polyethylene
terephthalate
(PET)
waste
streams
into
commodity
chemicals
offers
a
potentially
sustainable
route
for
creating
circular
plastic
economy.
However,
PET
wastes
upcycling
valuable
C2
product
remains
huge
challenge
by
the
lack
an
electrocatalyst
that
can
steer
oxidation
economically
and
selectively.
Here,
it
is
reported
catalyst
comprising
Pt
nanoparticles
hybridized
with
γ-NiOOH
nanosheets
supported
on
Ni
foam
(Pt/γ-NiOOH/NF)
favors
electrochemical
transformation
real-word
hydrolysate
glycolate
high
Faradaic
efficiency
(>
90%)
selectivity
across
wide
reactant
(ethylene
glycol,
EG)
concentration
ranges
under
marginal
applied
voltage
0.55
V,
which
be
paired
cathodic
hydrogen
production.
Computational
studies
combined
experimental
characterizations
elucidate
Pt/γ-NiOOH
interface
substantial
charge
accumulation
gives
rise
to
optimized
adsorption
energy
EG
decreased
barrier
potential
determining
step.
A
techno-economic
analysis
demonstrates
that,
nearly
same
amount
resource
investment,
electroreforming
strategy
towards
production
raise
revenue
up
2.2
times
relative
conventional
chemical
process.
This
work
may
thus
serve
as
framework
process
net-zero
carbon
footprint
economic
viability.
ACS Catalysis,
Год журнала:
2023,
Номер
13(15), С. 10394 - 10404
Опубликована: Июль 25, 2023
Electrochemical
reformation
of
nitrate
wastewater
and
poly(ethylene
terephthalate)
(PET)
plastic
waste
into
ammonia
(NH3)
fine
chemicals
is
a
sustainable
strategy
for
resource
utilization.
Herein,
co-production
system
glycolic
acid
(GA,
degradable
polymer
monomer)
constructed
by
coupling
reduction
ethylene
glycol
(EG,
in
PET
hydrolysate)
oxidation.
Low-crystalline
CoOOH
(LC-CoOOH/CF)
Pd
nanothorns
(Pd
NTs/NF)
grown
situ
on
the
metal
foam
substrates
are
employed
as
cathode
anode,
respectively.
The
high
density
amorphous
regions
LC-CoOOH/CF
enables
enhanced
adsorption
provides
abundant
active
sites,
ultimately
leading
to
an
Faradic
efficiency
(FE)
97.38
±
1.0%
at
−0.25
V
vs
reversible
hydrogen
electrode
(RHE).
Meanwhile,
unique
nanothorn
morphology
endows
NTs/NF
with
high-curvature
tip,
triggering
tip
effect
(TE)
promote
highly
selective
oxidation
EG
GA.
Furthermore,
two-electrode
system,
NH3
GA
operated
low
energy
consumption
(onset
voltage:
0.5
V),
much
lower
than
traditional
electrolysis
process
(1.4
V).
This
study
method
utilization
co-produce
value-added
chemicals.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Апрель 4, 2024
Abstract
Electrocatalytic
conversion
of
organic
small
molecules
is
a
promising
technique
for
value-added
chemical
productions
but
suffers
from
high
precious
metal
consumption,
poor
stability
electrocatalysts
and
tedious
product
separation.
Here,
Pd/NiMoO
4
/NF
electrocatalyst
with
much
lowered
Pd
loading
amount
(3.5
wt.%)
has
been
developed
efficient,
economic,
ultra-stable
glycolate
synthesis,
which
shows
Faradaic
efficiency
(98.9%),
yield
(98.8%),
ultrahigh
(1500
h)
towards
electrocatalytic
ethylene
glycol
oxidation.
Moreover,
the
obtained
glycolic
acid
converted
to
sodium
by
in-situ
acid-base
reaction
in
NaOH
electrolyte,
atomic
efficient
needs
no
additional
addition
weak
adsorption
on
catalyst
surface
plays
significant
role
avoiding
excessive
oxidation
achieving
selectivity.
This
work
may
provide
instructions
design
as
well
separation
conversions
alcohols.
ACS Catalysis,
Год журнала:
2024,
Номер
14(7), С. 4865 - 4926
Опубликована: Март 18, 2024
Rapid
industrialization
and
development
have
led
to
a
tremendous
increase
in
the
use
of
various
types
plastic
commodities
daily
life.
For
past
several
years,
pollution
has
become
global
issue,
posing
serious
threat
mankind.
The
primary
issue
with
increasing
is
lack
proper
management
which
created
huge
havoc
environment.
From
initial
phase
waste
management,
been
discarded,
recycled,
downcycled,
or
dumped
into
landfills
large
proportion,
causing
extreme
damage
ecosystem.
Conventionally,
treated
via
thermal
processes
such
as
pyrolysis
incineration
plants
require
amount
capital
and,
therefore,
harms
aim
circular
economy.
Chemical
upcycling
gaining
attention
high-potential
catalytic
strategy
convert
plastics,
polyethylene
terephthalate,
polyethylene,
polystyrene,
etc.
fuels,
functionalized
polymers,
other
value-added
chemicals
having
direct
impact
on
affordability
viability.
In
this
review,
we
focused
photocatalysis,
electrocatalysis,
photoelectrocatalysis
effective
efficient
technologies.
These
approaches
can
lower
dependence
nonrenewable
resources
are
more
environmentally
friendly
contrast
conventional
approaches.
This
review
elaborately
discusses
pros
cons
provides
detailed
overview
potential
renewable
energy-driven
for
conversion
wastes
valuable
fuels
commodity
chemicals,
along
challenges
future
directions
emerging
approach
treatment.