Angewandte Chemie,
Год журнала:
2024,
Номер
136(31)
Опубликована: Май 20, 2024
Abstract
Dithioacetals
are
heavily
used
in
organic,
material
and
medical
chemistries,
exhibit
huge
potential
to
synthesize
degradable
or
recyclable
polymers.
However,
the
current
synthetic
approaches
of
dithioacetals
polydithioacetals
overwhelmingly
dependent
on
external
catalysts
organic
solvents.
Herein,
we
disclose
a
catalyst‐
solvent‐free
acetal‐thiol
click‐like
reaction
for
synthesizing
polydithioacetals.
High
conversion,
higher
than
acid
catalytic
reaction,
can
be
achieved.
universality
was
confirmed
by
monitoring
reactions
linear
cyclic
acetals
(including
renewable
bio‐sourced
furan‐acetal)
with
aliphatic
aromatic
thiols,
mechanism
monomolecular
nucleophilic
substitution
(S
N
1)
auto‐protonation
(activation)
thiol
clarified
combining
experiments
density
functional
theory
computation.
Subsequently,
utilize
this
readily
By
simple
heating
stirring,
w
~110
kDa
were
synthesized
from
acetal
dithiol,
depolymerization
into
macrocyclic
dithioacetal
repolymerization
polydithioacetal
achieved;
through
reactive
extrusion,
semi‐interpenetrating
polymer
dynamic
network
excellent
mechanical
properties
continuous
reprocessability
prepared
poly(vinyl
butyral)
pentaerythritol
tetrakis(3‐mercaptopropionate).
This
green
high‐efficient
synthesis
method
is
beneficial
sustainable
development
chemistry.
Chinese Journal of Chemistry,
Год журнала:
2024,
Номер
42(13), С. 1447 - 1455
Опубликована: Март 13, 2024
Comprehensive
Summary
Sugar
moieties
present
on
bacterial
surface
serve
as
pivotal
regulators
of
activity.
Precisely
adjusting
the
abundance
and
distribution
sugar
can
offer
an
important
approach
to
manipulating
behavior,
but
has
been
proven
be
difficult.
Herein,
topological
glycosylation
is
reported
mediate
interaction
bacteria
with
mucous
layer.
Alkynes
functionalized
by
different
branching
are
synthesized
through
iterative
Michael
addition
amide
condensation
reactions.
By
a
copper‐catalyzed
azide‐alkyne
cycloaddition,
resulting
compounds
structures
attached
onto
that
modified
azido
groups.
As
proof‐of‐concept
study,
set
topologically
glycosylated
probiotics
(TGPs)
prepared
using
linear,
two‐branched,
tetra‐branched
compounds,
respectively.
The
between
mucin
TGPs
was
studied
results
demonstrate
that,
compared
unmodified
bacteria,
exhibit
enhanced
adhesive
capacity
mucin,
which
increases
numbers.
Similar
binding
trend
observed
in
ex
vivo
colonic
mucus
adhesion
experiments
display
highest
efficiency.
This
work
proposes
chemical
method
tune
providing
unique
significant
insights
into
manipulation
behavior
modification.
Accounts of Materials Research,
Год журнала:
2024,
Номер
5(7), С. 872 - 883
Опубликована: Июнь 24, 2024
ConspectusLiving
materials
represent
an
emerging
and
innovative
concept
at
the
forefronts
of
science
due
to
distinctive
living
characteristics.
Living
organisms,
such
as
microorganisms,
plant
cells,
mammalian
have
been
used
major
elements
for
fabrication
materials.
Given
favorable
features
including
reproductivity,
genetic
modifiability,
adaptability,
cultivability,
bacteria
received
increasing
attention
development
engineered
Particularly,
owing
inherent
abilities
target
colonize
specific
in
vivo
sites,
activate
immune
responses,
inhibit
pathogens,
play
key
roles
maintaining
human
health
currently
widely
exploited
preparation
therapeutic
agents.
However,
caused
by
innate
immunogenicity,
metabolic
activity,
movability,
use
bacteria-based
applications
often
suffers
from
poor
biosafety
insufficient
bioavailability,
inevitably
resulting
low
treatment
efficacy.
In
order
address
these
challenges,
extensive
efforts
invested
designing
engineering
various
advanced
generate
superior
agents
using
modification
surface
decoration.In
this
Account,
we
summarize
recent
advances
our
group
with
a
focus
on
coating
material
microbial
therapy.
First,
present
brief
introduction
existing
nature
that
possess
characteristics
reproduction,
biosynthesis,
self-healing,
self-organization,
self-adaption,
environment
responsiveness,
particular
emphasis
advantages
composed
Second,
elaborate
current
challenges
then
showcase
strategies
prepare
bacterial
therapeutics
individual
bacteria.
Three
types
are
included
Account:
(1)
physical
strategy
coat
eukaryotic
cell
membranes
red
blood
cells
yeast
mechanical
extrusion;
(2)
chemical
wrap
synthetic
coatings
interfacial
self-assembly
mineralization;
(3)
biological
encapsulate
self-secreted
biofilms
apoptosis
bodies
through
external
stimulations.
We
highlight
coated
can
be
endowed
wide
range
coating-derived
exogenous
functions
enumerate
their
appealing
reduced
clearance,
increased
improved
safety,
preferential
colonization
vivo.
Third,
shift
potential
treating
diseases,
especially
different
cancer
intestinal
inflammations.
Lastly,
discuss
remaining
need
addressed
further
clinic
practice
outlooks
preparing
next-generation
well
future
bench
bedside
translation.
anticipate
Account
offer
valuable
insights
generation
therapy
encourage
ideas
new
initiatives
expand
preventing
diseases.
ACS Nano,
Год журнала:
2024,
Номер
18(32), С. 20886 - 20933
Опубликована: Июль 31, 2024
Gut
microbiota
plays
a
crucial
role
in
maintaining
host
homeostasis,
impacting
the
progression
and
therapeutic
outcomes
of
diseases,
including
inflammatory
bowel
disease,
cancer,
hepatic
conditions,
obesity,
cardiovascular
pathologies,
neurologic
disorders,
via
immune,
neural,
metabolic
mechanisms.
Hence,
gut
is
promising
target
for
disease
therapy.
The
safety
precision
traditional
regulation
methods
remain
challenge,
which
limits
their
widespread
clinical
application.
This
limitation
has
catalyzed
shift
toward
development
multifunctional
delivery
systems
that
are
predicated
on
modulation.
Guided
by
bioinspired
strategies,
an
extensive
variety
naturally
occurring
materials
mechanisms
have
been
emulated
harnessed
construction
platforms
aimed
at
monitoring
modulation
microbiota.
review
outlines
strategies
advantages
utilizing
principles
design
intervention
based
methods.
Representative
studies
summarized,
to
confer
multiple
pharmacological
benefits
synergistic
management
diseases.
prospective
avenues
inherent
challenges
associated
with
adoption
refinement
proposed
augment
efficacy
treatment.
Angewandte Chemie,
Год журнала:
2024,
Номер
136(31)
Опубликована: Май 20, 2024
Abstract
Dithioacetals
are
heavily
used
in
organic,
material
and
medical
chemistries,
exhibit
huge
potential
to
synthesize
degradable
or
recyclable
polymers.
However,
the
current
synthetic
approaches
of
dithioacetals
polydithioacetals
overwhelmingly
dependent
on
external
catalysts
organic
solvents.
Herein,
we
disclose
a
catalyst‐
solvent‐free
acetal‐thiol
click‐like
reaction
for
synthesizing
polydithioacetals.
High
conversion,
higher
than
acid
catalytic
reaction,
can
be
achieved.
universality
was
confirmed
by
monitoring
reactions
linear
cyclic
acetals
(including
renewable
bio‐sourced
furan‐acetal)
with
aliphatic
aromatic
thiols,
mechanism
monomolecular
nucleophilic
substitution
(S
N
1)
auto‐protonation
(activation)
thiol
clarified
combining
experiments
density
functional
theory
computation.
Subsequently,
utilize
this
readily
By
simple
heating
stirring,
w
~110
kDa
were
synthesized
from
acetal
dithiol,
depolymerization
into
macrocyclic
dithioacetal
repolymerization
polydithioacetal
achieved;
through
reactive
extrusion,
semi‐interpenetrating
polymer
dynamic
network
excellent
mechanical
properties
continuous
reprocessability
prepared
poly(vinyl
butyral)
pentaerythritol
tetrakis(3‐mercaptopropionate).
This
green
high‐efficient
synthesis
method
is
beneficial
sustainable
development
chemistry.