Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
63(6)
Опубликована: Ноя. 28, 2023
Ion-selective
membranes
are
crucial
in
various
chemical
and
physiological
processes.
Numerous
studies
have
demonstrated
progress
separating
monovalent/multivalent
ions,
but
efficient
monovalent/monovalent
ion
sieving
remains
a
great
challenge
due
to
their
same
valence
similar
radii.
Here,
this
work
reports
two-dimensional
(2D)
MXene
membrane
with
super-aligned
slit-shaped
nanochannels
ultrahigh
monovalent
selectivity.
The
is
prepared
by
applying
shear
forces
liquid-crystalline
(LC)
dispersion,
which
conducive
the
highly-ordered
stacking
of
nanosheets.
obtained
LC
(LCMM)
exhibits
selectivities
toward
Li
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
144(27), С. 12400 - 12409
Опубликована: Июнь 28, 2022
Nanofluidic
membranes
have
been
demonstrated
as
promising
candidates
for
osmotic
energy
harvesting.
However,
it
remains
a
long-standing
challenge
to
fabricate
high-efficiency
ion-permselective
with
well-defined
channel
architectures.
Here,
we
demonstrate
high-performance
conversion
based
on
oriented
two-dimensional
covalent
organic
frameworks
(COFs)
ultrashort
vertically
aligned
nanofluidic
channels
that
enabled
efficient
and
selective
ion
transport.
Experiments
combined
molecular
dynamics
simulations
revealed
exquisite
control
over
orientation,
charge
polarity,
density
contributed
high
selectivity
permeability.
When
applied
conversion,
pair
of
100
nm
thick
oppositely
charged
COF
achieved
an
ultrahigh
output
power
43.2
W
m-2
at
50-fold
salinity
gradient
up
228.9
the
Dead
Sea
river
water
system.
The
outperforms
state-of-the-art
membranes,
suggesting
great
potential
in
fields
advanced
membrane
technology
conversion.
State-of-the-art
polymeric
membranes
are
unable
to
perform
the
high-precision
ion
separations
needed
for
technologies
essential
a
circular
economy
and
clean
energy
future.
Coordinative
interactions
mechanism
increase
sorption
of
target
species
into
membrane,
but
effects
these
on
membrane
permeability
selectivity
poorly
understood.
We
use
multilayered
polymer
assess
how
ion-membrane
binding
energies
affect
similarly
sized
cations:
Cu
2+
,
Ni
Zn
Co
Mg
.
report
that
metals
with
higher
iminodiacetate
groups
more
selectively
permeate
through
in
multisalt
solutions
than
single-salt
solutions.
In
contrast,
weaker
precluded
from
diffusing
which
leads
passage
proportional
independent
thickness.
Our
findings
demonstrate
can
markedly
by
tailoring
minimizing
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Янв. 3, 2024
The
demand
for
lithium
extraction
from
salt-lake
brines
is
increasing
to
address
the
supply
shortage.
Nanofiltration
separation
technology
with
high
Mg
ACS Nano,
Год журнала:
2022,
Номер
16(8), С. 11781 - 11791
Опубликована: Июнь 30, 2022
Controllable
ion
transport
through
nanochannels
is
crucial
for
biological
and
artificial
membrane
systems.
Covalent
organic
frameworks
(COFs)
with
regular
tunable
are
emerging
as
an
ideal
material
platform
to
develop
synthetic
membranes
transport.
However,
exclusion
by
COF
remains
challenging
because
most
materials
have
large-sized
leading
nonselective
of
small
ions.
Here
we
ionic
(iCOFMs)
control
charged
framework
nanochannels,
the
interior
surfaces
which
covered
arrayed
sulfonate
groups
render
superior
charge
density.
The
overlap
electrical
double
layer
in
blocks
entry
co-ions,
narrows
their
passageways,
concomitantly
restrains
permeation
counterions
via
balance.
These
highly
within
iCOFM
enable
while
maintaining
intrinsically
high
water
permeability.
Our
results
reveal
possibilities
controllable
based
on
purification,
separation,
sensing,
energy
conversion.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(18)
Опубликована: Фев. 18, 2022
A
vast
amount
of
energy
can
be
extracted
from
the
untapped
low-grade
heat
sources
below
100
°C
and
Gibbs
free
salinity
gradients.
Therefore,
a
process
for
simultaneous
direct
conversion
these
energies
into
electricity
using
permselective
membranes
was
developed
in
this
study.
These
screen
charges
ion
flux
driven
by
combined
temperature
gradients
to
achieve
thermo-osmotic
conversion.
Increasing
charge
density
pore
channels
enhanced
permselectivity
conductance,
leading
larger
osmotic
voltage
current.
14-fold
increase
power
achieved
adjusting
ionic
site
population
covalent
organic
framework
(COF)
membranes.
The
optimal
COF
membrane
operated
under
simulated
estuary
conditions
at
difference
60
K,
which
yielded
≈231
W
m-2
,
placing
it
among
best
performing
upscaled
system
pave
way
utilization
enormous
supply
energy,
indicating
tremendous
potential
applications.
Advanced Materials,
Год журнала:
2023,
Номер
36(9)
Опубликована: Окт. 31, 2023
Abstract
Polyester
nanofiltration
membranes
highlight
beneficial
chlorine
resistance,
but
their
loose
structures
and
negative
charge
result
in
poor
cations
retention
precluding
advanced
use
separation.
This
work
designs
a
new
monomer
(TET)
containing
“hydroxyl‐ammonium”
entities
that
confer
dense
positive
to
polyester
membranes.
The
TET
undergoes
efficient
interfacial
polymerization
with
the
trimesoyl
chloride
(TMC)
monomer,
resultant
TET‐TMC
feature
one
of
lowest
molecular
weight
cut‐offs
(389
Da)
highest
zeta
potential
(4
mv,
pH:
7)
among
all
MgCl
2
rejection
membrane
is
95.5%,
significantly
higher
than
state‐of‐the‐art
(<50%).
Li
+
/Mg
2+
separation
performance
on
par
cutting‐edge
polyamide
membranes,
while
additionally,
stable
against
NaClO
though
readily
degrade.
Thus
first
for
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(48)
Опубликована: Окт. 5, 2023
Abstract
Efficient
Mg
2+
/Li
+
separation
is
crucial
to
combating
the
lithium
shortage
worldwide,
yet
current
nanofiltration
membranes
suffer
from
low
efficacy
and/or
poor
scalability,
because
desirable
properties
of
are
entangled
and
there
a
trade‐off.
This
work
reports
“tagged‐modification”
approach
tackle
challenge.
A
mixture
3‐bromo‐trimethylpropan‐1‐aminium
bromide
(E
1
)
3‐aminopropyltrimethylazanium
2
was
designed
modify
polyethylenimine
–
trimesoyl
chloride
(PEI‐TMC)
membranes.
E
reacted
with
PEI
TMC,
respectively,
thus,
membrane
(hydrophilicity,
pore
sizes,
charge)
were
untangled
intensified
simultaneously.
The
permeance
(34.3
L
m
−2
h
−1
bar
selectivity
(23.2)
modified
about
4
times
higher
than
pristine
membrane,
they
remain
stable
in
30‐days
test.
highest
among
all
analogous
tagged‐modification
method
enables
preparation
large‐area
modules
that
produce
high‐purity
carbonate
(Li
CO
3
simulated
brine.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Март 8, 2024
Abstract
Membrane
consisting
of
ordered
sub-nanochannels
has
been
pursued
in
ion
separation
technology
to
achieve
applications
including
desalination,
environment
management,
and
energy
conversion.
However,
high-precision
not
yet
achieved
owing
the
lack
deep
understanding
transport
mechanism
confined
environments.
Biological
channels
can
conduct
ions
with
ultrahigh
permeability
selectivity,
which
is
inseparable
from
important
role
channel
size
“ion-channel”
interaction.
Here,
inspired
by
biological
systems,
we
report
monovalent
divalent
cations
functionalized
metal-organic
framework
(MOF)
membranes
(UiO-66-(X)
2
,
X
=
NH
SH,
OH
OCH
3
).
We
find
that
functional
group
(X)
MOF
sub-nanochannel
synergistically
regulate
binding
affinity
dehydration
process,
key
enlarging
activation
difference
between
target
interference
improve
performance.
The
K
+
/Mg
2+
selectivity
UiO-66-(OCH
)
membrane
reaches
as
high
1567.8.
This
work
provides
a
gateway
development
membranes.
Proceedings of the National Academy of Sciences,
Год журнала:
2024,
Номер
121(8)
Опубликована: Фев. 13, 2024
Understanding
the
molecular-level
mechanisms
involved
in
transmembrane
ion
selectivity
is
essential
for
optimizing
membrane
separation
performance.
In
this
study,
we
reveal
our
observations
regarding
behavior
of
Li
+
and
Mg
2+
ions
as
a
response
to
changing
pore
solvation
abilities
covalent-organic-framework
(COF)
membranes.
These
were
manipulated
by
adjusting
lengths
oligoether
segments
attached
channels.
Through
comparative
experiments,
able
unravel
relationships
between
ability
various
transport
properties,
such
partitioning,
conduction,
selectivity.
We
also
emphasize
significance
competition
with
solvating
modulating
found
that
increasing
length
chain
facilitated
transport;
however,
it
was
COF
chains
containing
two
ethylene
oxide
units
exhibited
most
pronounced
discrepancy
energy
barrier
,
resulting
highest
factor
among
all
evaluated
Remarkably,
under
electro-driven
binary-salt
conditions,
specific
achieved
an
exceptional
/Mg
up
1352,
making
one
effective
membranes
available
separation.
The
insights
gained
from
study
significantly
contribute
advancing
understanding
selective
within
confined
nanospaces
provide
valuable
design
principles
developing
highly
