Natural
biological
materials
are
formed
by
self-assembly
processes
and
catalyze
a
myriad
of
reactions.
Here,
we
report
programmable
molecular
assembly
designed
synthetic
polymers
with
engineered
bacterial
spores.
This
process
is
driven
dynamic
covalent
bond
formation
on
spore
surface
glycan
yields
macroscopic
that
structurally
stable,
self-healing,
recyclable.
Molecular
programming
polymer
species
shapes
the
physical
properties
these
while
metabolically
dormant
spores
allow
for
prolonged
ambient
storage.
Incorporation
genetically
encoded
functionalities
enables
operationally
simple
repeated
enzymatic
catalysis.
Our
work
lays
an
important
foundation
scalable
synthesis
robust
sustainable
biocatalysis.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
146(1), P. 330 - 341
Published: Dec. 19, 2023
Implementing
dissipative
assembly
in
living
systems
is
meaningful
for
creation
of
materials
or
even
artificial
life.
However,
intracellular
remains
scarce
and
significantly
impeded
by
the
challenges
lying
precisely
operating
chemical
reaction
cycles
under
complex
physiological
conditions.
Here,
we
develop
organelle-mediated
self-assembly
peptides
cells
fueled
GSH,
via
design
a
mitochondrion-targeting
redox-responsive
hexapeptide.
While
hexapeptide
undergoes
efficient
self-assembly,
addition
GSH
into
peptide
solution
presence
mitochondrion-biomimetic
liposomes
containing
hydrogen
peroxide
allows
transient
peptides.
Internalization
LPS-stimulated
macrophages
leads
to
driven
reduction
association
assemblies
with
mitochondria.
The
facilitates
reversible
oxidation
reduced
mitochondrion-residing
ROS
thereby
dissociates
from
mitochondria
re-enter
cytoplasm
reduction.
metastable
peptide–mitochondrion
complexes
prevent
thermodynamically
equilibrated
thus
establishing
stimulated
macrophages.
entire
self-assembling
process
elimination
elevated
decrease
pro-inflammatory
cytokine
expression.
Creating
assisted
internal
structures
provides
new
avenues
development
medical
agents
future.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(28)
Published: April 27, 2024
Abstract
Despite
great
progress
in
the
construction
of
non‐equilibrium
systems,
most
approaches
do
not
consider
structure
fuel
as
a
critical
element
to
control
processes.
Herein,
we
show
that
amino
acid
side
chains
(A,
F,
Nal)
abiotic
phosphates
can
direct
assembly
and
reactivity
during
transient
formation.
The
fuels
bind
covalently
substrates
subsequently
influence
structures
process.
We
focus
on
ways
which
phosphate
esters
guide
formation
how
cross
regulate
when
constructing
assemblies.
Through
chemical
functionalization
energy‐rich
aminoacyl
esters,
are
able
yield
thioesters
upon
adding
dipeptides
containing
tyrosine
or
cysteine
residues.
structural
elements
around
lifetime
formed
their
supramolecular
These
properties
be
further
influenced
by
peptide
sequence
substrates,
incorporating
anionic,
aliphatic
aromatic
Furthermore,
illustrate
oligomerization
initiated
from
single
ester
residue
(Y).
findings
suggest
activated
acids
with
varying
energy
contents
pave
way
for
designing
fabricating
structured
fuels.
Chem,
Journal Year:
2023,
Volume and Issue:
10(3), P. 910 - 923
Published: Dec. 28, 2023
Chemically
driven
reaction
cycles
are
prevalent
in
nature;
yet,
artificial
examples
still
rare
and
often
lack
robustness
or
versatility.
In
this
study,
we
introduce
acylphosphate
steady
states
that
can
be
accessed
from
a
wide
range
of
organophosphates
using
either
carboxylic
anhydride
carbodiimide
fuels.
The
combination
fuel
pyridine
catalysis
makes
chemistry
sufficiently
robust
to
allow
for
25
fueling
without
generation
observable
quantities
detrimental
side
products
such
as
pyrophosphates.
We
demonstrate
the
acylation
gives
rise
transient
aggregates,
harness
fluorescence
acylphosphate-bridged
excimers
rapid
screenings
more
than
50
catalysts
single
well
plate
experiment.
Due
its
versatility
robustness,
anticipate
organophosphate/acylphosphate
cycle
will
prove
useful
creation
chemically
molecular
machines
self-assemblies.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
36(28)
Published: Jan. 31, 2024
Abstract
Accurate
structure
control
in
dissipative
assemblies
(DSAs)
is
vital
for
precise
biological
functions.
However,
accuracy
and
functionality
of
artificial
DSAs
are
far
from
this
objective.
Herein,
a
novel
approach
introduced
by
harnessing
complex
chemical
reaction
networks
rooted
coordination
chemistry
to
create
atomically‐precise
copper
nanoclusters
(CuNCs),
specifically
Cu
11
(µ
9
‐Cl)(µ
3
‐Cl)
L
6
Cl
(L
=
4‐methyl‐piperazine‐1‐carbodithioate).
Cu(I)–ligand
ratio
change
dynamic
Cu(I)–Cu(I)
metallophilic/coordination
interactions
enable
the
reorganization
CuNCs
into
metastable
CuL
2
,
finally
converting
equilibrium
[CuL·Y]Cl
(Y
MeCN/H
O)
via
Cu(I)
oxidation/reorganization
ligand
exchange
process.
Upon
adding
ascorbic
acid
(AA),
system
goes
further
cycles.
It
observed
that
encapsulated/bridging
halide
ions
exert
subtle
influence
on
optical
properties
topological
changes
polymeric
when
integrating
as
crosslink
sites.
duration/switch
period
could
be
controlled
varying
ions,
AA
concentration,
O
pressure
pH.
Cu(I)‐Cu(I)
metallophilic
provide
versatile
toolbox
designing
delicate
life‐like
materials,
paving
way
with
structures
functionalities.
Furthermore,
can
employed
modular
units
within
polymers
materials
mechanics
or
functionalization
studies.
ACS Applied Bio Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 20, 2025
Addressing
the
growing
concern
about
antibiotic-resistant
bacteria,
we
have
developed
a
series
of
polymers
exhibiting
intrinsic
antibacterial
activities
with
dual-targeting
system
that
induces
physical
lysis
upon
copolymer
coalescence
bacterial
matter.
These
are
equipped
two
orthogonal
binding
motifs
form
electrostatic
interactions
and
dynamic
covalent
complexes
on
surfaces
exhibit
potent
activity
against
Gram-positive
Gram-negative
bacteria.
The
effect
chemical
composition
architecture
copolymers
incorporating
phenylboronic
acid
quaternary
ammonium
groups
antimicrobial
was
systematically
examined.
This
work
expands
current
repertoire
to
combat
resistance
by
intrinsically
unique
mode
action.
Angewandte Chemie,
Journal Year:
2024,
Volume and Issue:
136(28)
Published: April 27, 2024
Abstract
Despite
great
progress
in
the
construction
of
non‐equilibrium
systems,
most
approaches
do
not
consider
structure
fuel
as
a
critical
element
to
control
processes.
Herein,
we
show
that
amino
acid
side
chains
(A,
F,
Nal)
abiotic
phosphates
can
direct
assembly
and
reactivity
during
transient
formation.
The
fuels
bind
covalently
substrates
subsequently
influence
structures
process.
We
focus
on
ways
which
phosphate
esters
guide
formation
how
cross
regulate
when
constructing
assemblies.
Through
chemical
functionalization
energy‐rich
aminoacyl
esters,
are
able
yield
thioesters
upon
adding
dipeptides
containing
tyrosine
or
cysteine
residues.
structural
elements
around
lifetime
formed
their
supramolecular
These
properties
be
further
influenced
by
peptide
sequence
substrates,
incorporating
anionic,
aliphatic
aromatic
Furthermore,
illustrate
oligomerization
initiated
from
single
ester
residue
(Y).
findings
suggest
activated
acids
with
varying
energy
contents
pave
way
for
designing
fabricating
structured
fuels.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(29), P. 16210 - 16217
Published: July 17, 2023
Natural
biological
materials
are
formed
by
self-assembly
processes
and
catalyze
a
myriad
of
reactions.
Here,
we
report
programmable
molecular
assembly
designed
synthetic
polymers
with
engineered
bacterial
spores.
This
process
is
driven
dynamic
covalent
bond
formation
on
spore
surface
glycan
yields
macroscopic
that
structurally
stable,
self-healing,
recyclable.
Molecular
programming
polymer
species
shapes
the
physical
properties
these
while
metabolically
dormant
spores
allow
for
prolonged
ambient
storage.
Incorporation
genetically
encoded
functionalities
enables
operationally
simple
repeated
enzymatic
catalysis.
Our
work
combines
genetic
engineering
to
offer
scalable
synthesis
robust
sustainable
biocatalysis.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Aug. 22, 2024
With
growing
threats
from
counterfeiting-based
security
breaches,
multi-level
and
specific
stimuli-responsive
anti-counterfeiting
devices
message
encryption
methods
have
attracted
immense
research
interest.
Fluorescence-based
aggregation-induced
emission
(AIE)-based
materials
solves
the
problems
to
a
considerable
extent.
However,
development
of
smarter
patterns
with
hierarchical
levels
alongside
dynamic
display
is
still
challenging.
To
screen
out
this
complication,
we
bring
forward
pH-switchable
fluorescent
assembly
an
AIEgen
aliphatic
acid.
We
later
temporally
direct
molecular
aid
chemical
trigger-regulated
pH
clock,
generating
transitory
multicolor
emission,
including
transient
white
light
generation.
The
pH-dependent
emissions
were
further
implemented
in
constructing
smart
multi-input
AND
gates.
Subsequently,
integrate
time-gated
emissive
system
develop
advanced
multi-dimensionally
secure
data
strategy.
This
novel
approach
enhances
measures
by
introducing
additional
layer
based
on
temporal
characteristics.
Angewandte Chemie,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Aug. 22, 2024
Abstract
With
growing
threats
from
counterfeiting‐based
security
breaches,
multi‐level
and
specific
stimuli‐responsive
anti‐counterfeiting
devices
message
encryption
methods
have
attracted
immense
research
interest.
Fluorescence‐based
aggregation‐induced
emission
(AIE)‐based
materials
solves
the
problems
to
a
considerable
extent.
However,
development
of
smarter
patterns
with
hierarchical
levels
alongside
dynamic
display
is
still
challenging.
To
screen
out
this
complication,
we
bring
forward
pH‐switchable
fluorescent
assembly
an
AIEgen
aliphatic
acid.
We
later
temporally
direct
molecular
aid
chemical
trigger‐regulated
pH
clock,
generating
transitory
multicolor
emission,
including
transient
white
light
generation.
The
pH‐dependent
emissions
were
further
implemented
in
constructing
smart
multi‐input
AND
gates.
Subsequently,
integrate
time‐gated
emissive
system
develop
advanced
multi‐dimensionally
secure
data
strategy.
This
novel
approach
enhances
measures
by
introducing
additional
layer
based
on
temporal
characteristics.
