Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
34(6)
Published: Oct. 29, 2023
Abstract
Rational
immobilization
of
fragile
enzymes
on
a
scaffold
is
an
efficient
protocol
to
achieve
robust
biocatalyst,
yet
the
construction
remains
challenging
due
trade‐off
between
enzyme
activity
and
framework
environment.
Herein,
enzyme‐engineered
assembly
strategy
enabling
in
situ
fusion
acetylcholinesterase
(AChE)
into
Zn‐based
metal‐organic
frameworks
(Zn‐MOF‐74)
during
rapid
nucleation
crystal
defect
growth
process,
demonstrated.
The
Zn‐MOF‐74
composites
can
offer
hydrophilic
microenvironment
for
maintaining
biological
state
AChE,
with
flower‐like
porous
structure
that
allows
boosting
mass
transfer
process
substrates
products.
Impressively,
apparent
AChE
be
well
maintained
90%
after
encapsulation,
AChE@Zn‐MOF‐74
produced
excellent
stability
inhospitable
environments.
Given
structural
integration,
AChE@Zn‐MOF‐74‐based
biosensor
constructed
sensitive
detection
chlorpyrifos
(organophosphorus
pesticides)
limit
1.0
ng
mL
−1
,
monitoring
pesticide
degradation
extent
water
body.
This
study
anticipated
valuable
insight
understanding
structure‐activity
relationship
enzyme@MOF
encourage
applications
biosensors
precision
agriculture.
Chemical Reviews,
Journal Year:
2023,
Volume and Issue:
123(9), P. 5347 - 5420
Published: April 12, 2023
Enzymatic
catalysis
has
fueled
considerable
interest
from
chemists
due
to
its
high
efficiency
and
selectivity.
However,
the
structural
complexity
vulnerability
hamper
application
potentials
of
enzymes.
Driven
by
practical
demand
for
chemical
conversion,
there
is
a
long-sought
quest
bioinspired
catalysts
reproducing
even
surpassing
functions
natural
As
nanoporous
materials
with
surface
areas
crystallinity,
metal-organic
frameworks
(MOFs)
represent
an
exquisite
case
how
enzymes
their
active
sites
are
integrated
into
porous
solids,
affording
heterogeneous
superior
stability
customizable
structures.
In
this
review,
we
comprehensively
summarize
advances
MOFs
catalysis,
discuss
design
principle
various
MOF-based
catalysts,
such
as
MOF-enzyme
composites
embedded
sites,
explore
utility
these
in
different
reactions.
The
advantages
enzyme
mimetics
also
highlighted,
including
confinement,
templating
effects,
functionality,
comparison
homogeneous
supramolecular
catalysts.
A
perspective
provided
potential
solutions
addressing
current
challenges
MOF
catalysis.
Chemical Society Reviews,
Journal Year:
2023,
Volume and Issue:
52(19), P. 6715 - 6753
Published: Jan. 1, 2023
This
review
not
only
highlights
the
progress
of
emission
and
electronic
behaviour
new
pyrene-based
luminescence
molecules
in
aggregated
state,
but
also
provides
a
perspective
for
understanding
mechanism
optoelectronic
properties
pyrenes.
Chemical Society Reviews,
Journal Year:
2023,
Volume and Issue:
52(21), P. 7504 - 7523
Published: Jan. 1, 2023
Hydrogen-bonded
organic
frameworks
(HOFs)
are
an
emerging
attractive
class
of
highly
crystalline
porous
materials
characterized
by
significant
biocompatibility,
rich
chemical
functionalities
and
well-defined
porosity.
The
unique
advantages
including
metal-free
nature
reversible
binding
manner
significantly
distinguish
HOFs
from
other
in
the
biotechnology
biomedical
field.
However,
relevant
HOF
studies
still
remain
their
infancy
despite
promising
remarkable
results
that
have
been
presented
recent
years.
Due
to
intricate
dynamic
physiological
conditions,
major
challenge
lies
stability
structural
diversity
vivo.
In
this
Tutorial
Review,
we
summarize
common
building
blocks
for
construction
HOF-based
functional
biomaterials
latest
developments
biological
Moreover,
highlight
current
challenges
regarding
functionalization
along
with
corresponding
potential
solutions.
This
Review
will
a
profound
effect
future
years
on
design
applications
biomaterials.
Chemical Society Reviews,
Journal Year:
2023,
Volume and Issue:
53(1), P. 137 - 162
Published: Nov. 29, 2023
Natural
metalloenzymes
with
astonishing
reaction
activity
and
specificity
underpin
essential
life
transformations.
Nevertheless,
enzymes
only
operate
under
mild
conditions
to
keep
sophisticated
structures
active,
limiting
their
potential
applications.
Artificial
that
recapitulate
the
catalytic
of
can
not
circumvent
enzymatic
fragility
but
also
bring
versatile
functions
into
practice.
Among
them,
metal-organic
frameworks
(MOFs)
featuring
diverse
site-isolated
metal
sites
supramolecular
have
emerged
as
promising
candidates
for
move
toward
unparalleled
properties
behaviour
enzymes.
In
this
review,
we
systematically
summarize
significant
advances
in
MOF-based
metalloenzyme
mimics
a
special
emphasis
on
active
pocket
engineering
at
atomic
level,
including
primary
secondary
coordination
spheres.
Then,
deep
understanding
mechanisms
advanced
applications
are
discussed.
Finally,
perspective
emerging
frontier
research
is
provided
advance
bioinspired
catalysis.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(24), P. 13469 - 13475
Published: June 7, 2023
Immobilization
of
fragile
enzymes
in
crystalline
porous
materials
offers
new
opportunities
to
expand
the
applications
biocatalysts.
However,
limited
by
pore
size
and/or
harsh
synthesis
conditions
hosts,
often
suffer
from
dimension
limitation
or
denaturation
during
immobilization
process.
Taking
advantage
dynamic
covalent
chemistry
feature
organic
frameworks
(COFs),
herein,
we
report
a
preprotection
strategy
encapsulate
COFs
self-repairing
and
crystallization
Enzymes
were
first
loaded
low-crystalline
polymer
networks
with
mesopores
formed
at
initial
growth
stage,
which
could
offer
effective
protection
for
reaction
conditions,
subsequently
encapsulation
proceeded
disordered
into
framework.
Impressively,
biological
activity
can
be
well-maintained
after
encapsulation,
obtained
enzyme@COFs
also
show
superior
stability.
Furthermore,
circumvents
enzymes,
its
versatility
was
verified
different
sizes
surface
charges,
as
well
two-enzyme
cascade
system.
This
study
universal
design
idea
robust
supports
holds
promise
developing
high-performance
immobilized
Nature Communications,
Journal Year:
2023,
Volume and Issue:
14(1)
Published: June 20, 2023
Abstract
Rational
integration
of
native
enzymes
and
nanoscaffold
is
an
efficient
means
to
access
robust
biocatalyst,
yet
remains
on-going
challenges
due
the
trade-off
between
fragile
harsh
assembling
conditions.
Here,
we
report
a
supramolecular
strategy
enabling
in
situ
fusion
into
porous
crystal.
A
c2-symmetric
pyrene
tecton
with
four
formic
acid
arms
utilized
as
building
block
engineer
this
hybrid
biocatalyst.
The
decorated
afford
tectons
high
dispersibility
minute
amount
organic
solvent,
permit
hydrogen-bonded
linkage
discrete
extended
network
around
enzyme
almost
solvent-free
aqueous
solution.
This
biocatalyst
covered
by
long-range
ordered
pore
channels,
which
can
serve
gating
sieve
catalytic
substrate
thus
enhance
biocatalytic
selectivity.
Given
structural
integration,
biocatalyst-based
electrochemical
immunosensor
developed,
pg/mL
detection
cancer
biomarker.
Analytical Chemistry,
Journal Year:
2023,
Volume and Issue:
95(44), P. 16383 - 16391
Published: Oct. 26, 2023
The
rational
design
of
efficient
nanozymes
and
the
immobilization
enzymes
are
great
significance
for
construction
high-performance
biosensors
based
on
nano-/bioenzyme
catalytic
systems.
Herein,
a
novel
V-TCPP(Fe)
metal-organic
framework
nanozyme
with
two-dimensional
nanosheet
morphology
is
rationally
designed
by
using
V2CTx
MXene
as
metal
source
iron
tetrakis(4-carboxyphenyl)porphine
(FeTCPP)
ligand
an
organic
linker.
It
exhibits
enhanced
peroxidase-
catalase-like
activities
luminol-H2O2
chemiluminescent
(CL)
behavior.
Based
experimental
theoretical
results,
these
excellent
enzyme-like
derived
from
two-site
synergistic
effect
between
V
nodes
FeTCPP
ligands
in
V-TCPP(Fe).
Furthermore,
confined
system
developed
zeolitic
imidazole
(ZIF)
coencapsulation
bioenzyme.
Using
acetylcholinesterase
(AChE)
model,
our
constructed
V-TCPP(Fe)/AChE@ZIF
was
successfully
used
colorimetric/CL
dual-mode
visual
biosensing
organophosphorus
pesticides.
This
work
expected
to
provide
new
insights
into
systems,
encouraging
applications
catalysis
biosensing.