ACS Catalysis,
Journal Year:
2023,
Volume and Issue:
13(16), P. 10968 - 10975
Published: Aug. 4, 2023
Polystyrene
upcycling
to
valuable
commodity
feedstocks
is
essential
for
reducing
plastic
waste.
Photooxidative
degradation
has
emerged
as
a
method
converting
polystyrene
oxidized
aromatic
compounds.
Investigating
the
mechanism
of
photooxidative
understanding
pathways
generating
different
small
molecules.
Here,
we
leveraged
reactivity
differences
between
chlorine
and
bromine
radicals
study
polystyrene.
While
with
radical
yields
primarily
benzoic
acid
(50
mol
%),
shows
an
increased
preference
acetophenone
(4
%
both
products).
After
conducting
several
mechanistic
studies,
discovered
that
activation
3°
C–H
bonds
necessary
form
acetophenone.
However,
production,
second
hydrogen
atom
transfer
from
H–Br
enables
reformation
methyl
group
on
polymer
chain
end.
Lastly,
insights
in
hand,
added
exogenous
sources
increase
concentration
HBr
improved
yield,
becoming
major
product.
We
envision
our
into
will
further
enable
divergent
product
selectivity.
Science,
Journal Year:
2023,
Volume and Issue:
381(6658), P. 666 - 671
Published: Aug. 10, 2023
Conversion
of
plastic
wastes
to
fatty
acids
is
an
attractive
means
supplement
the
sourcing
these
high-value,
high-volume
chemicals.
We
report
a
method
for
transforming
polyethylene
(PE)
and
polypropylene
(PP)
at
~80%
conversion
with
number-average
molar
masses
up
~700
670
daltons,
respectively.
The
process
applicable
municipal
PE
PP
their
mixtures.
Temperature-gradient
thermolysis
key
controllably
degrading
into
waxes
inhibiting
production
small
molecules.
are
upcycled
by
oxidation
over
manganese
stearate
subsequent
processing.
ꞵ-scission
produces
more
olefin
wax
yields
higher
acid-number
than
does
ꞵ-scission.
further
convert
large-market-volume
surfactants.
Industrial-scale
technoeconomic
analysis
suggests
economic
viability
without
need
subsidies.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(3), P. 1847 - 1854
Published: Jan. 12, 2023
To
solve
the
serious
environmental
problem
and
huge
resource
waste
of
plastic
pollution,
we
report
a
tandem
catalytic
conversion
low-density
polyethylene
(LDPE)
into
naphtha,
key
feedstock
for
renewable
production.
Using
β
zeolite
silicalite-1-encapsulated
Pt
nanoparticles
(Pt@S-1),
naphtha
yield
89.5%
is
obtained
with
96.8%
selectivity
C5-C9
hydrocarbons
at
250
°C.
The
acid
sites
crack
long-chain
LDPE
olefin
intermediates,
which
diffuse
within
channels
Pt@S-1
to
encounter
nanoparticles.
hydrogenation
over
confined
metal
matches
cracking
steps
by
selectively
shipping
olefins
right
size,
rapid
diffusion
boosts
formation
narrow-distributed
alkanes.
A
conceptual
upgrading
indicates
it
suitable
closing
loop,
significant
energy
saving
15%
30%
reduced
greenhouse
gas
emissions.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(29), P. 16218 - 16227
Published: July 12, 2023
Recycling
waste
plastics
requires
the
degradation
of
into
small
molecules.
However,
various
products
are
widely
distributed
using
traditional
methods
depolymerizing
polystyrene
(PS)
such
as
catalytic
pyrolysis
and
hydrogenolysis.
Here,
we
creatively
report
a
N-bridged
Co,
Ni
dual-atom
(Co-N-Ni)
catalyst
for
targeted
conversion
PS
to
ethylbenzene
via
pressurized
tandem
fixed-bed
reactor
where
hydropyrolysis
is
coupled
with
downstream
vapor-phase
hydrotreatment.
The
Co-N-Ni
achieves
95
wt
%
92
yield,
significantly
superior
corresponding
single-atom
catalysts,
enables
real
plastics.
Theoretical
calculations
experimental
results
demonstrate
that
d-band
center
metal
atoms
well
regulated
in
catalyst.
Co
site
activates
C═C
bond
more
easily,
while
spatially
optimizes
adsorption
configuration
styrene
molecule
due
electronic
interaction.
This
also
shows
excellent
durability
provides
new
direction
plastic
degradation.
ACS Catalysis,
Journal Year:
2023,
Volume and Issue:
13(6), P. 3575 - 3590
Published: Feb. 27, 2023
Plastic
waste
pollution
is
becoming
one
of
the
most
pressing
environmental
crises
due
to
large-scale
production
without
satisfactory
recycling
schemes,
especially
with
outbreak
COVID-19
pandemic
in
recent
years.
Upcycling
plastic
into
valuable
chemicals
powered
by
solar
energy
presents
a
substantially
untapped
opportunity
turn
treasure.
In
this
review,
fundamental
principles
from
nonselective
degradation
selective
synthesis
are
first
clarified.
Then,
we
aim
outline
representative
advances
photoredox-based
catalytic
conversion.
Particular
emphasis
placed
on
valorization
regarding
versus
synthesis.
Finally,
present
challenges
and
individual
insights
for
further
exploration
conversion
domain.
It
anticipated
that
timely
critical
review
would
provide
an
instructive
direction
foresight
plastics
value-added
chemical
feedstocks,
thus
stimulating
development
circular
sustainable
economy
coming
decades.
Green Chemistry,
Journal Year:
2023,
Volume and Issue:
25(18), P. 6949 - 6970
Published: Jan. 1, 2023
This
review
summarizes
the
emerging
advanced
technologies
including
bio-,
photo-,
electro-,
and
low-temperature
thermocatalysis
for
recycling
upgrading
of
waste
plastics
under
mild
conditions.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: March 10, 2024
Abstract
Covalent
organic
frameworks
(COFs)
attract
significant
attention
due
to
their
ordered,
crystalline,
porous,
metal‐free,
and
predictable
structures.
These
unique
characteristics
offer
great
opportunities
for
the
diffusion
transmission
of
photogenerated
charges
during
photocatalysis.
Currently,
a
considerable
number
COFs
are
used
as
metal‐free
semiconductor
photocatalysts.
This
review
aims
understand
relationships
between
structure
photocatalysis
performance
provides
in‐depth
insight
into
synthetic
strategy
improve
performance.
Subsequently,
focuses
on
structural
motif
in
sustainable
photocatalytic
hydrogen
evolution,
carbon
dioxide
reduction,
peroxide
generation,
compound
transformations.
Last,
conjunction
with
progress
achieved
challenges
yet
be
overcome,
candid
discussion
is
undertaken
regarding
field
COF
photocatalysis,
accompanied
by
presentation
potential
research
avenues
future
directions.
seeks
provide
readers
comprehensive
understanding
pivotal
role
robust
guidance
innovative
utilization
Journal of Materials Chemistry A,
Journal Year:
2023,
Volume and Issue:
11(6), P. 2503 - 2527
Published: Jan. 1, 2023
Plastics
and
microplastics
are
major
environmental
pollutants
due
to
wide
applications
difficult
degradations.
Herein,
we
summarize
several
studies
on
degradations
of
(micro)plastics
value-added
products
intermediates
via
photocatalysis.
Small,
Journal Year:
2023,
Volume and Issue:
19(39)
Published: May 25, 2023
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.