Advanced Science,
Journal Year:
2024,
Volume and Issue:
11(14)
Published: Feb. 6, 2024
Abstract
Developing
dynamic
chemistry
for
polymeric
materials
offers
chemical
solutions
to
solve
key
problems
associated
with
current
plastics.
Mechanical
performance
and
function
are
equally
important
in
material
design
because
the
former
determines
application
scope
latter
enables
recycling
hence
sustainability.
However,
it
is
a
long‐term
challenge
balance
subtle
trade‐off
between
mechanical
robustness
properties
single
material.
The
rise
of
chemistry,
including
supramolecular
covalent
provides
many
opportunities
versatile
molecular
tools
designing
constitutionally
that
can
adapt,
repair,
recycle.
Facing
growing
social
need
developing
advanced
sustainable
without
compromising
properties,
recent
progress
showing
how
toolbox
be
explored
enable
high‐performance
by
engineering
strategies
discussed
here.
state
art
milestones
summarized
discussed,
followed
an
outlook
toward
future
challenges
present
this
field.
Journal of the American Chemical Society,
Journal Year:
2022,
Volume and Issue:
144(49), P. 22358 - 22377
Published: Nov. 29, 2022
Polymer
networks
built
out
of
dynamic
covalent
bonds
offer
the
potential
to
translate
control
and
tunability
chemical
reactions
macroscopic
physical
properties.
Under
conditions
at
which
these
occur,
topology
adaptable
(CANs)
can
rearrange,
meaning
that
they
flow,
self-heal,
be
remolded,
respond
stimuli.
Materials
with
properties
are
necessary
fields
ranging
from
sustainability
tissue
engineering;
thus
time
scale
network
rearrangement
must
compatible
intended
use.
The
mechanical
CANs
based
on
thermodynamics
kinetics
their
constituent
bonds.
Therefore,
strategies
needed
connect
molecular
worlds.
In
this
Perspective,
we
analyze
structure-reactivity-property
relationships
for
several
classes
CANs,
illustrating
both
general
design
principles
predictive
linear
free
energy
(LFERs)
applied
CANs.
We
discuss
opportunities
in
field
develop
quantitative
open
challenges.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
34(20)
Published: April 23, 2023
Abstract
Light‐based
3D
printing
has
received
significant
attention
due
to
several
advantages
including
high
speed
and
resolution.
Along
with
the
development
of
new
technologies,
material
design
is
key
for
next
generation
light‐based
printing.
Conventional
printable
polymeric
materials,
also
known
as
photopolymers
or
photoresins,
often
lead
thermosets–polymer
networks
cross‐linked
by
permanent
covalent
bonds
which
bring
limited
adaptability
restricted
reprocessability.
Dynamic
that
can
reversibly
break
reform
enable
network
rearrangement,
thereby
offering
unprecedented
properties
materials
such
adaptability,
self‐healing,
recycling
capabilities.
Hence,
introducing
dynamic
into
a
promising
strategy
further
expand
meet
diverse
application
scenarios
printed
multi‐functional
moreover
more
demanding
sustainable
nature‐inspired
considerations
(e.g.,
self‐healing).
Herein,
an
overview
recent
advances
in
printing,
aiming
bridge
these
two
research
fields
presented.
Importantly,
current
challenges
are
analyzed
perspectives
developing
their
potential
applications
provided.
ACS Sustainable Chemistry & Engineering,
Journal Year:
2023,
Volume and Issue:
11(30), P. 11077 - 11087
Published: July 18, 2023
Dynamic
covalent
polymer
networks
represent
new
opportunities
in
the
design
of
sustainable
epoxy
resins
due
to
their
excellent
malleability
and
reprocessability;
however,
adaptable
network
is
usually
accompanied
by
low
glass
transition
temperature,
poor
creep
resistance,
mechanical
brittleness.
Herein,
we
demonstrate
a
vanillin-based
hyperbranched
resin
(VEHBP)
containing
disulfide
imine
dynamic
bonds
for
recyclable
malleable
with
high
temperature
(Tg),
significantly
improved
properties.
The
5%VEHBP
exhibited
175
°C
130
34.1,
19.7,
173.3%
increase
tensile
strength,
storage
modulus,
toughness
respectively,
compared
neat
resin.
Meanwhile,
topological
structure
VEHBP
complemented
dual
endowed
these
materials
self-healing
ability,
reprocessability,
degradability,
which
represents
an
important
step
toward
fabrication
high-performance
networks.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(31)
Published: May 18, 2023
Abstract
On‐demand
adhesive
dismantling
has
the
potential
to
improve
multimaterial
product
recycling,
but
its
implementation
been
hampered
by
a
critical
trade‐off
between
strong
bonding
and
easy
debonding.
As
result,
temperature
range
in
which
these
temporary
adhesives
can
be
used
is
relatively
limited.
Here,
new
class
of
dynamic
epoxy
resins
reported
that
significantly
extends
this
upper
limit
still
achieves
fast
Specifically,
two
types
polyamidoamine
curing
agents
for
hardening
are
developed,
being
polysuccinamides
(PSA)
polyglutaramides
(PGA).
debonding/rebonding
process
PSA
especially
PGA
linkages
more
thermally
demanding
at
same
time
robust
than
previously
covalent
systems,
resulting
materials
triggered
high
temperatures,
remain
bonded
over
wide
range.
The
versatility
system
demonstrated
classical
bulk
formulations,
as
well
linking
PSA‐
or
PGA‐functionalized
surface.
an
attractive
drop‐in
strategy
achieved
producing
debondable
rebondable
adhesives,
with
complementarity
existing
resin
technologies
applicable
industrially
relevant
window.
Chemical Science,
Journal Year:
2023,
Volume and Issue:
14(20), P. 5243 - 5265
Published: Jan. 1, 2023
This
review
provides
a
multidisciplinary
overview
of
the
challenges
and
opportunities
for
dynamic
covalent
chemistry-based
macromolecules
towards
design
new,
sustainable,
recyclable
materials
circular
economy.
Advanced Science,
Journal Year:
2023,
Volume and Issue:
10(19)
Published: April 23, 2023
To
achieve
energy
saving
and
emission
reduction
goals,
recyclable
healable
thermoset
materials
are
highly
attractive.
Polymer
copolymerization
has
been
proven
to
be
a
critical
strategy
for
preparing
high-performance
polymeric
materials.
However,
it
remains
huge
challenge
develop
Here,
polyimine
dynamic
networks
based
on
two
monomers
with
bulky
pendant
groups,
which
not
only
displayed
mechanical
properties
higher
than
the
strong
tough
polymers,
e.g.,
polycarbonate,
but
also
excellent
self-repairing
capability
recyclability
as
thermosets
developed.
Owing
stability
of
conjugation
effect
by
aromatic
benzene
rings,
final
far
more
stable
reported
counterparts,
exhibiting
hydrolysis
resistance
under
both
alkaline
condition
most
organic
solvents.
These
structure
can
completely
depolymerized
into
recovery
in
an
acidic
aqueous
solution
at
ambient
temperature.
Resulting
from
units,
this
method
allows
exchange
reactions
vitrimer
easily
within
minutes
self-healing
function.
Moreover,
introduction
trifluoromethyl
diphenoxybenzene
backbones
significantly
increases
tensile
This
work
provides
effective
fabricating
polymer
multiple
functions.
ACS Sustainable Chemistry & Engineering,
Journal Year:
2023,
Volume and Issue:
11(22), P. 8308 - 8316
Published: May 22, 2023
Epoxy
resins
constitute
a
very
significant
portion
of
all
high-performance
plastics
due
to
their
excellent
thermal
and
mechanical
properties
that
appear
in
wide
range
applications.
Nevertheless,
traditional
epoxy
networks
show
limitations
regarding
chemical
recycling
covalently
crosslinked
structures.
The
current
methods
recycle
are
not
indeed
through
sustainable
ways,
but
this
issue
could
be
solved
by
developing
smart
monomers
with
functional
groups,
which
can
switched
between
polymerized
depolymerized
states.
Herein,
we
developed
two
bio-based
liquid
based
on
vanillin
structures
containing
aldehyde,
acetal,
oxirane-ring
functionalities.
These
were
solvent-free
conditions
using
commercially
available
diamines,
resulting
double-dynamic
imine-acetal-containing
thermosets.
combine
the
systems
dynamic
polymers.
Most
importantly,
such
thermosets
fully
into
vanillin,
reused
for
preparation
original
monomers,
mixture
well-defined
polyols,
was
upcycled
polyurethane.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(24)
Published: March 14, 2023
A
novel
strategy
allowing
temporal
control
of
dynamic
bond
exchange
in
covalently
crosslinked
polymer
networks
via
latent
transesterification
catalysts
is
introduced.
Obtained
by
a
straightforward
air-
and
water-tolerant
synthesis,
the
catalyst
designed
for
an
irreversible
temperature-mediated
release
strong
organic
base.
Its
long-term
inactivity
at
temperatures
below
50
°C
provides
unique
opportunity
to
equip
covalent
with
creep
resistance
high
bond-exchange
rates,
once
activated.
The
presented
thermally
base
conveniently
introducible
readily
available
building
blocks
and,
as
proof
concept,
applied
radically
polymerized
thiol-ene
network.
Light-mediated
curing
used
3D-printing
functional
objects,
on
which
possibility
spatially
controlled
reshaping
welding
based
illustrated.
Since
activated,
limitations
regarding
sample
geometry
optical
transparency
do
not
apply,
facilitates
transfer
well-established
industrial
technologies.
Consequently,
fiber-reinforced
highly
filled
magneto-active
composites
are
fabricated
thermal
approach.
on-demand
activation
demonstrated
(magneto-assisted)
experiments,
highlighting
wide
range
potential
future
applications
offered
concept.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(23), P. 16257 - 16267
Published: June 4, 2024
The
spontaneous
condensation
of
amines
with
β-triketones
(TK),
forming
β,β′-diketoenamines
(DKE)
and
releasing
water
as
the
sole
byproduct,
exhibits
many
hallmarks
"click"
reactions.
Such
characteristics
render
TKs
a
highly
advantageous
platform
for
efficient
polymer
diversification,
even
in
biological
contexts.
Leveraging
reversible
addition–fragmentation
chain
transfer
(RAFT)
photoiniferter
polymerization
novel
TK-containing
vinylic
monomers,
we
synthesized
polymers
containing
pendent
excellent
control
molecular
weights,
excess
106
g
mol–1.
Under
mild,
catalyst-free
conditions,
poly(β-triketone
methacrylate)
could
be
modified
diverse
scope
plethora
functional
groups.
high
efficiency
this
functionalization
approach
was
further
emphasized
when
grafting-to
poly(ethylene
glycol)-amine
resulting
bottlebrushes
weights
reaching
2.0
×
107
Critically,
while
formed
DKE
linkages
are
stable
under
ambient
they
undergo
catalyst-free,
dynamic
transamination
at
elevated
temperatures,
paving
way
associative
covalent
adaptable
networks.
Overall,
introduce
triketone
moieties
into
methacrylate
acrylamide
polymers,
establishing
postpolymerization
modification
technique
that
facilitates
ligation
permissible
conditions.