Chemically-fueled
chemical
reaction
networks
(CRNs)
are
key
in
controlling
dissipative
self-assembly.
Having
catalysts
gating
fuel
consumption
for
both
the
activation
and
deactivation
chemistry
of
(assembly-prone)
monomers
catalytic
activity
with
an
external
stimulus
would
provide
better
control
over
where,
when,
how
long
self-assembled
structures
can
form.
Here
we
achieve
light
two
different
that
govern
monomer
assembly
into
supramolecular
fibers,
as
well
fiber
disassembly.
Activation
proceeds
via
photoredox
catalysis
under
visible
light,
whereas
is
achieved
by
organometallic
relies
on
a
photocaged
pre-fuel
activated
ultraviolet
light.
Overall,
show
fibers
be
formed
destroyed
using
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(37)
Published: June 15, 2024
Given
her
unrivalled
proficiency
in
the
synthesis
of
all
molecules
life,
nature
has
been
an
endless
source
inspiration
for
developing
new
strategies
organic
chemistry
and
catalysis.
However,
one
feature
that
remains
thus
far
beyond
chemists'
grasp
is
unique
ability
to
adapt
productivity
metabolic
processes
response
triggers
indicate
temporary
need
specific
metabolites.
To
demonstrate
remarkable
potential
such
stimuli-responsive
systems,
we
present
a
metabolism-inspired
network
multicatalytic
capable
selectively
synthesising
range
products
from
simple
starting
materials.
Specifically,
built
four
classes
distinct
catalytic
reactions-cross-couplings,
substitutions,
additions,
reductions,
involving
three
materials-terminal
alkyne,
aryl
iodide,
hydrosilane.
All
materials
are
either
introduced
sequentially
or
added
system
at
same
time,
with
no
continuous
influx
reagents
efflux
products.
catalysed
by
multifunctional
heteronuclear
Pd
Angewandte Chemie,
Journal Year:
2024,
Volume and Issue:
136(37)
Published: June 15, 2024
Abstract
Given
her
unrivalled
proficiency
in
the
synthesis
of
all
molecules
life,
nature
has
been
an
endless
source
inspiration
for
developing
new
strategies
organic
chemistry
and
catalysis.
However,
one
feature
that
remains
thus
far
beyond
chemists’
grasp
is
unique
ability
to
adapt
productivity
metabolic
processes
response
triggers
indicate
temporary
need
specific
metabolites.
To
demonstrate
remarkable
potential
such
stimuli‐responsive
systems,
we
present
a
metabolism‐inspired
network
multicatalytic
capable
selectively
synthesising
range
products
from
simple
starting
materials.
Specifically,
built
four
classes
distinct
catalytic
reactions—cross‐couplings,
substitutions,
additions,
reductions,
involving
three
materials—terminal
alkyne,
aryl
iodide,
hydrosilane.
All
materials
are
either
introduced
sequentially
or
added
system
at
same
time,
with
no
continuous
influx
reagents
efflux
products.
catalysed
by
multifunctional
heteronuclear
Pd
II
/Pt
complex,
whose
performance
can
be
controlled
additives
external
stimuli.
The
reaction
exhibits
substantial
degree
orthogonality
between
different
pathways,
enabling
controllable
ten
high
efficiency
selectivity
through
simultaneous
triggering
suppression
mechanisms.
ChemSystemsChem,
Journal Year:
2024,
Volume and Issue:
6(6)
Published: July 9, 2024
Abstract
Understanding
the
emergence
of
complex
properties
in
dissipative
non‐equilibrium
systems
is
crucial
for
unraveling
mysteries
life
processes.
The
review
focuses
on
documented
research
chemically
fueled
autonomous
systems,
self‐sorting
towards
compartmentalization,
self‐replication
via
autocatalysis,
and
rhythmic
chemical
oscillators.
In
addition
to
that,
also
discusses
newly
introduced
reactions
dynamic
combinatorial
libraries
systems.
Chemically-fueled
chemical
reaction
networks
(CRNs)
are
key
in
controlling
dissipative
self-assembly.
Having
catalysts
gating
fuel
consumption
for
both
the
activation
and
deactivation
chemistry
of
(assembly-prone)
monomers
catalytic
activity
with
an
external
stimulus
would
provide
better
control
over
where,
when,
how
long
self-assembled
structures
can
form.
Here
we
achieve
light
two
different
that
govern
monomer
assembly
into
supramolecular
fibers,
as
well
fiber
disassembly.
Activation
proceeds
via
photoredox
catalysis
under
visible
light,
whereas
is
achieved
by
organometallic
relies
on
a
photocaged
pre-fuel
activated
ultraviolet
light.
Overall,
show
fibers
be
formed
destroyed
using