Angewandte Chemie,
Год журнала:
2024,
Номер
unknown
Опубликована: Сен. 23, 2024
Abstract
Developing
plastics
that
fill
the
need
of
polyolefins
yet
are
more
easily
recyclable
is
a
critical
to
address
plastic
waste
crisis.
However,
most
efforts
in
this
vein
have
focused
on
high‐density
polyethylene
(PE),
while
many
different
types
PE
exist.
To
create
broadly
sustainable
with
modular
properties,
we
present
synthesis,
characterization,
and
demonstration
materials
applications
for
chemically
PE‐like
multiblock
polymers
prepared
from
distinct
hard
soft
blocks
using
ruthenium‐catalyzed
dehydrogenative
polymerization.
By
altering
branching
pattern
within
blocks,
series
were
synthesized
tunable
glass
transition
temperatures
(
T
g
)
maintaining
consistent
high
melting
m
).
A
clear
U‐shape
trend
between
mechanical
properties
was
found,
showcasing
their
potential
as
tailored
spanning
commercial
linear
low‐density
(LLDPE)
(LDPE).
These
offer
adjustable
adhesive
strength
metal
demonstrate
chemical
recyclability
selective
depolymerization
mixed
streams,
promoting
circularity
separation.
Chemical Reviews,
Год журнала:
2024,
Номер
124(5), С. 2327 - 2351
Опубликована: Фев. 26, 2024
Polyethylene
deconstruction
to
reusable
smaller
molecules
is
hindered
by
the
chemical
inertness
of
its
hydrocarbon
chains.
Pyrolysis
and
related
approaches
commonly
require
high
temperatures,
are
energy-intensive,
yield
mixtures
multiple
classes
compounds.
Selective
cleavage
reactions
under
mild
conditions
(
Angewandte Chemie,
Год журнала:
2024,
Номер
136(24)
Опубликована: Апрель 8, 2024
Abstract
Environmentally
friendly
crosslinked
polymer
networks
feature
degradable
covalent
or
non‐covalent
bonds,
with
many
of
them
manifesting
dynamic
characteristics.
These
attributes
enable
convenient
degradation,
facile
reprocessibility,
and
self‐healing
capabilities.
However,
the
inherent
instability
these
crosslinking
bonds
often
compromises
mechanical
properties
networks,
limiting
their
practical
applications.
In
this
context,
environmentally
dual‐crosslinking
(denoted
EF‐DCPNs)
have
emerged
as
promising
alternatives
to
address
challenge.
materials
effectively
balance
need
for
high
ability
degrade,
recycle,
and/or
self‐heal.
Despite
potential,
investigations
into
EF‐DCPNs
remain
in
nascent
stages,
several
gaps
limitations
persist.
This
Review
provides
a
comprehensive
overview
synthesis,
properties,
applications
recent
progress
EF‐DCPNs.
Firstly,
synthetic
routes
rich
variety
possessing
two
distinct
types
(i.e.,
imine,
disulfide,
ester,
hydrogen
bond,
coordination
other
bonds)
are
introduced.
Subsequently,
complex
structure‐
nature‐dependent
mechanical,
thermal,
electrical
discussed,
followed
by
exemplary
electronics
biotechnology.
Finally,
future
research
directions
rapidly
evolving
field
outlined.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 27, 2025
While
synthesizing
circular
polymers
with
telechelic
polyolefin
building
blocks
recently
emerged
as
a
promising
strategy
for
addressing
conventional
polyethylenes'
sustainability
challenges,
the
lack
of
iPP
(tPP)
sufficient
difunctional
purity
polycondensation
has
been
limiting
development
polypropylenes
iPP-like
structures
and
properties.
Here
we
described
combined
approach
coordinative
chain
transfer
polymerization
transition-metal-catalyzed
quenching
reaction
various
acyl
chlorides,
affording
tPPs
high
ratio
(up
to
∼99%)
broad
end
functional
group
scope.
The
steric
effect
polymeryl-Zn
species
role
Pd
catalyst
were
revealed
by
DFT.
This
method
also
solved
low
challenge
polyethylenes.
Ester-linked
iPPs
structure
thermomechanical
properties
PE/iPP
multiblock
copolymers
synthesized
resulting
tPPs.
Macromolecular Materials and Engineering,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 27, 2025
Abstract
Inkjet
3D
printing
is
a
fast,
reliable
and
noncontact
method,
capable
of
producing
small
large
structures
enabling
multi‐material
printing.
These
characteristics
make
inkjet
an
excellent
technique
for
additive
manufacturing
biomaterials,
such
as
scaffolds
tissue
engineering.
However,
the
technology
restricted
by
limited
number
suitable
photopolymers
which
hitherto
are
to
acrylate‐based
chemistries,
not
only
toxic
but
nondegradable,
thus
use
in
many
biomaterials‐based
applications.
Herein,
unique
innovative
approach
described
looking
beyond
traditional
carbon‐based
chemistry
design
synthesize
novel
photomonomers
based
on
amino
acid
phosphoramides
(APA)
with
silyl
ethers
utilizing
thiol‐yne
click
chemistry.
The
inks
specifically
designed
solventless
biomaterials
shown
be
biocompatible
having
fast
tunable
degradation
rates.
This
makes
these
promising
material
biomedical
applications,
regeneration.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(24)
Опубликована: Апрель 8, 2024
Environmentally
friendly
crosslinked
polymer
networks
feature
degradable
covalent
or
non-covalent
bonds,
with
many
of
them
manifesting
dynamic
characteristics.
These
attributes
enable
convenient
degradation,
facile
reprocessibility,
and
self-healing
capabilities.
However,
the
inherent
instability
these
crosslinking
bonds
often
compromises
mechanical
properties
networks,
limiting
their
practical
applications.
In
this
context,
environmentally
dual-crosslinking
(denoted
EF-DCPNs)
have
emerged
as
promising
alternatives
to
address
challenge.
materials
effectively
balance
need
for
high
ability
degrade,
recycle,
and/or
self-heal.
Despite
potential,
investigations
into
EF-DCPNs
remain
in
nascent
stages,
several
gaps
limitations
persist.
This
Review
provides
a
comprehensive
overview
synthesis,
properties,
applications
recent
progress
EF-DCPNs.
Firstly,
synthetic
routes
rich
variety
possessing
two
distinct
types
(i.e.,
imine,
disulfide,
ester,
hydrogen
bond,
coordination
other
bonds)
are
introduced.
Subsequently,
complex
structure-
nature-dependent
mechanical,
thermal,
electrical
discussed,
followed
by
exemplary
electronics
biotechnology.
Finally,
future
research
directions
rapidly
evolving
field
outlined.
Macromolecules,
Год журнала:
2024,
Номер
57(14), С. 6727 - 6740
Опубликована: Июль 9, 2024
An
understanding
of
monomer
sequence
is
required
to
predict
and
engineer
the
properties
copolymers.
In
stochastic
polymerizations
involving
more
than
one
monomer,
typically
inferred
or
determined
from
reactivity
ratios,
which
are
measured
through
copolymerization
experiments.
The
accurate
determination
ratios
copolymerizations
where
both
monomers
undergo
reversible
propagation,
however,
has
been
complicated
by
difficulty
in
solving
underlying
population
balance
equations,
presence
myriad
copolymer
equations
literature
derived
under
varying
assumptions
simplifications,
lack
an
easy-to-fit
integrated
model.
Here,
we
rectify
assert
consistency
between
previously
reported
disparate
forms,
introduce
a
new
method
explicitly
solve
perform
simulations
evaluate
ability
these
three
methods
produce
consistent
comonomer
consumption
predictions
fits
simulated
data.
We
find
that
all
given
same
input
parameters,
implies
accuracy
precision
when
modeling
copolymerization,
fitting
experimental
data,
making
sequence.
Considering
this
consistency,
make
recommendation
use
numerical
integration
appropriate
equation
fit
real
data
due
its
ease
implementation.
further
identify
minimum
number
parameters
for
suggest
ways
measure
other
information
ex
situ
expedite
fitting.
Finally,
practical
utility
developed
herein
demonstrated
seven
distinct
sets,
span
wide
range
reactivities.
ACS Applied Polymer Materials,
Год журнала:
2024,
Номер
6(17), С. 10718 - 10726
Опубликована: Авг. 22, 2024
The
development
of
click
polymerization
toward
the
creation
structurally
diverse
closed-loop
recyclable
polymers
is
challenging
yet
desirable
in
modern
polymer
chemistry.
In
this
work,
we
report
a
modular
amino-acetoacetate
polymerization,
which
proceeds
under
mild
conditions
and
produces
H2O
as
only
byproduct.
Through
systematic
optimization
reaction
parameters,
successfully
synthesized
22
poly(vinylogous
urethane)s
possessing
high
molecular
weights
(Mw
up
to
93.7
kDa)
well-defined
structures
outstanding
yields
(up
98%).
diacetoacetate
monomers
are
derived
from
diols,
both
diols
diamine
common
chemicals
that
can
be
produced
renewable
biomass.
Notably,
these
exhibit
ability
depolymerize
back
their
respective
conditions,
highlighting
excellent
recyclability.
This
enables
synthesis
with
structures,
providing
versatile
platform
for
fabrication
materials
such
plastics,
elastomers,
carbon
fiber-reinforced
composites.
methodology
material
innovations
discussed
work
may
benefit
promotion
application
greatly
demands
scenarios.