Nature Chemistry,
Journal Year:
2024,
Volume and Issue:
16(7), P. 1184 - 1192
Published: April 12, 2024
Abstract
Polymers
that
degrade
on
demand
have
the
potential
to
facilitate
chemical
recycling,
reduce
environmental
pollution
and
are
useful
in
implant
immolation,
drug
delivery
or
as
adhesives
debond
demand.
However,
polymers
made
by
radical
polymerization,
which
feature
all
carbon-bond
backbones
constitute
most
important
class
of
polymers,
proven
difficult
render
degradable.
Here
we
report
cyclobutene-based
monomers
can
be
co-polymerized
with
conventional
impart
resulting
mechanically
triggered
degradability.
The
cyclobutene
residues
act
mechanophores
undergo
a
ring-opening
reaction,
causes
rearrangement
renders
polymer
chains
cleavable
hydrolysis
under
basic
conditions.
These
broadly
applicable
free
controlled
polymerizations,
introduce
functional
groups
into
backbone
allow
gated
degradation
high-molecular-weight
materials
cross-linked
networks
low-molecular-weight
species.
Green Chemistry,
Journal Year:
2022,
Volume and Issue:
24(23), P. 8899 - 9002
Published: Jan. 1, 2022
This
paper
reviewed
the
entire
life
cycle
of
plastics
and
options
for
management
plastic
waste
to
address
barriers
industrial
chemical
recycling
further
provide
perceptions
on
possible
opportunities
with
such
materials.
Science,
Journal Year:
2022,
Volume and Issue:
377(6614), P. 1561 - 1566
Published: Sept. 29, 2022
The
conversion
of
polyolefins
to
monomers
would
create
a
valuable
carbon
feedstock
from
the
largest
fraction
waste
plastic.
However,
breakdown
main
chains
in
these
polymers
requires
cleavage
carbon–carbon
bonds
that
tend
resist
selective
chemical
transformations.
Here,
we
report
production
propylene
by
partial
dehydrogenation
polyethylene
and
tandem
isomerizing
ethenolysis
desaturated
chain.
Dehydrogenation
high-density
with
either
an
iridium-pincer
complex
or
platinum/zinc
supported
on
silica
as
catalysts
yielded
dehydrogenated
material
containing
up
3.2%
internal
olefins;
combination
second-generation
Hoveyda-Grubbs
metathesis
catalyst
[PdP(
t
Bu)
3
(μ-Br)]
2
isomerization
selectively
degraded
this
unsaturated
polymer
yields
exceeding
80%.
These
results
show
promise
for
application
mild
catalysis
deconstruct
otherwise
stable
polyolefins.
ACS Catalysis,
Journal Year:
2022,
Volume and Issue:
12(8), P. 4659 - 4679
Published: April 5, 2022
Plastics
are
indispensable,
but
their
pollution
is
triggering
a
global
environmental
crisis.
Although
many
end-of-life
catalytic
options
have
involved
converting
plastics
into
valuable
products,
deep
understanding
of
the
relationship
between
polymer
structure
and
recycling
performance
significant
urgently
needed.
Here,
we
start
with
primer
polymeric
chain
structures
on
chemical
discuss
structure–performance
polymer,
catalyst,
reaction.
Specifically,
development
challenges
re/upcycling
waste
PET
polyolefins
discussed
in-depth.
In
addition,
also
present
some
prospects
for
innovations
in
catalyst
synthesis
reaction
engineering
basis
relationship.
The
discussion
ends
brief
perspective
future
plastic
re/upcycling.
Overall,
intelligent
catalysis
design
necessary
incentivizing
relieving
burden
plastics.
Biotechnology Advances,
Journal Year:
2022,
Volume and Issue:
60, P. 107991 - 107991
Published: May 31, 2022
The
global
production
of
plastics
has
continuously
been
soaring
over
the
last
decades
due
to
their
extensive
use
in
our
daily
life
and
industries.
Although
synthetic
offer
great
advantages
from
packaging
construction
electronics,
low
biodegradability
induce
serious
plastic
pollution
that
damage
environment,
human
health
make
irreversible
changes
ecological
cycle.
In
particular,
containing
only
carbon-carbon
(C-C)
backbone
are
less
susceptible
degradation
lack
hydrolysable
groups.
representative
polyethylene
(PE)
polystyrene
(PS)
account
for
about
40%
total
production.
Various
chemical
biological
processes
with
potential
have
developed
recycle
reuse,
but
biodegradation
seems
be
most
attractive
eco-friendly
method
combat
this
growing
environmental
problem.
review,
we
first
summarize
current
advances
PE
PS
biodegradation,
including
isolation
microbes
degrading
enzymes
different
sources.
Next,
state-of-the-art
techniques
used
evaluating
monitoring
degradation,
scientific
toolboxes
enzyme
discovery
as
well
challenges
strategies
intensively
discussed.
return,
it
inspires
a
further
technological
exploration
expanding
diversity
species
enzymes,
disclosing
essential
pathways
developing
new
approaches
utilize
waste
feedstock
recycling
upcycling.
ACS Catalysis,
Journal Year:
2022,
Volume and Issue:
12(24), P. 14882 - 14901
Published: Nov. 23, 2022
Polyolefins,
the
largest
used
commodity
plastics
in
world,
find
extensive
application
many
fields.
However,
most
end
up
landfills
or
incineration,
leading
to
severe
ecological
crises,
environmental
pollution,
and
serious
resource
waste
problems.
As
representatives
on
chemical
upcycling
of
polyolefin
fuels
bulk/fine
chemicals,
catalytic
cracking
hydrocracking
based
zeolite
metal/zeolite
composite
catalysts
are
considered
effective
paths
due
their
large
capacity
strong
adaptability
existing
petrochemical
equipment.
After
an
overview
reaction
mechanisms
pyrolysis
cracking,
this
review
aims
comprehensively
discuss
influence
catalyst
structure
(acidity,
pore
structure,
morphology)
activity,
selectivity,
stability
particularly
emphasizing
importance
for
matching
acidity
target
product
formation.
Subsequently,
structure–activity
relationship
between
metal
site
zeolite's
acid
is
also
discussed.
In
end,
emerging
opportunities
challenges
proposed
promote
a
more
efficient
way
upcycling.
ACS Catalysis,
Journal Year:
2022,
Volume and Issue:
12(8), P. 4618 - 4627
Published: April 5, 2022
Nondegradable
polyolefin
plastics
pose
severe
environmental
threats
and
thus
demand
efficient
upcycling
technologies.
In
this
work,
we
discovered
that
low-loading
(≤0.25
wt
%)
Ru/CeO2
exhibits
remarkable
catalytic
performance
in
the
hydrogenolysis
of
polypropylene
(PP),
polyethylene
(PE),
n-C16H34
is
superior
to
high-loading
(≥0.5
Ru/CeO2.
They
possess
high
PP
conversion
efficiency
(sevenfold
increase
over
current
literature
reports),
low
selectivity
toward
undesired
CH4,
good
isomerization
ability.
range,
intrinsic
activity
Ru
increases
as
particle
size
decreases,
opposite
trend
range.
Detailed
characterization
revealed
abrupt
changes
behaviors
coincide
with
species
transitioning
from
well-defined
highly
disordered
structures
domain.
The
were
shown
be
sub-nanometer
cationic.
Mechanistically,
regioselectivity
rate
dependence
on
hydrogen
pressure
C–C
bond
cleavage
are
different
low-
Ru/CeO2,
both
explained
by
higher
coverage
adsorbed
(*H)
This
work
reveals
disordered,
sub-nanometer,
cationic
hydrogenolysis,
opening
immense
opportunities
develop
effective,
selective,
versatile
catalysts
for
plastic
upcycling.
Polymers,
Journal Year:
2022,
Volume and Issue:
14(15), P. 3133 - 3133
Published: July 31, 2022
The
excessive
amount
of
global
plastic
produced
over
the
past
century,
together
with
poor
waste
management,
has
raised
concerns
about
environmental
sustainability.
Plastic
recycling
become
a
practical
approach
for
diminishing
and
maintaining
sustainability
among
management
methods.
Chemical
mechanical
are
typical
approaches
to
waste,
simple
process,
low
cost,
environmentally
friendly
potential
profitability.
Several
materials,
such
as
polypropylene,
polystyrene,
polyvinyl
chloride,
high-density
polyethylene,
low-density
polyurethanes,
can
be
recycled
chemical
approaches.
Nevertheless,
due
waste’s
varying
physical
properties,
separation
becomes
challenge.
Hence,
reliable
effective
technology
is
critical
increasing
value
rate.
Integrating
technologies
would
an
efficient
method
reducing
accumulation
contaminants
by
especially
in
industrial
uses.
This
review
addresses
recent
advances
technology,
mainly
recycling.
article
also
discusses
current
various
materials.
SusMat,
Journal Year:
2022,
Volume and Issue:
2(2), P. 161 - 185
Published: April 1, 2022
Abstract
The
mass
production
of
disposable
polyolefin
products
has
led
to
serious
plastic
pollution
and
an
imbalance
between
manufacturing
recycling.
Given
these
challenges,
the
chemical
upcycling
waste
polyolefins
attracted
extensive
attention
due
its
high
efficiency
economic
benefits.
Herein,
we
review
development
in
heterogeneous
catalysis.
status
quo
recycling
is
first
discussed.
We
then
introduce
advanced
strategies
for
view
different
value‐added
discuss
their
challenges
prospects.
Our
in‐depth
analysis
centers
on
catalytic
mechanism
design
principle
catalysts.
Finally,
outlook
promising
directions
facilitate
degradation
process
via
polymer
catalyst
optimized
engineering.
Innovative
are
expected
promote
polyolefins,
bringing
great
promise
sustainable
society.
ACS Catalysis,
Journal Year:
2022,
Volume and Issue:
12(22), P. 13969 - 13979
Published: Oct. 31, 2022
Hydrogenolysis
of
C–C
bonds
over
Ru-based
catalysts
has
emerged
as
a
deconstruction
strategy
to
convert
single-use
polyolefin
waste
liquid
alkanes
at
relatively
mild
conditions,
but
this
approach
exhibits
limitations,
including
methane
formation
resulting
from
terminal
bond
scission.
In
study,
variety
were
investigated
for
the
reductive
polyethylene
(PE)
and
polypropylene
(PP)
identify
supports
that
promote
nonterminal
We
found
Ru
nanoparticles
supported
on
Brønsted-acidic
zeolites
with
faujasite
(FAU)
Beta
(BEA)
topologies
highly
active
cleavage
in
PE
PP,
exhibiting
improved
yields
suppressed
formation.
For
PE,
supporting
ruthenium
(5
wt
%)
FAU
increased
67%
compared
33%
an
inert
silica
support
%
Ru/SiO2)
200
°C,
16
h,
under
30
bar
H2.
A
dramatic
selectivity
enhancement
toward
hydrocarbons
was
also
observed
PP
Ru/FAU
Ru/BEA
Ru/SiO2.
To
understand
origin
improvement,
combination
ex
situ
operando
characterization
techniques
used
reveal
both
catalyst
structure
acidity
play
key
roles
conversion.
Operando
X-ray
absorption
spectroscopy
studies
model
polyolefins
Ru-supported
varying
levels
revealed
local
chemical
environment
Ru[0]
during
reaction
is
consistent
across
multiple
acidic
supports,
although
onset
reduction
synthesis
varies
different
supports.
These
results,
combined
reactivity
data,
demonstrate
importance
acid-noble
metal
cooperativity
promoting
selective
scission
shifts
mechanism
hydrogenolysis
ideal
hydrocracking.