Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(21)
Опубликована: Март 20, 2023
Developing
adsorptive
separation
processes
based
on
C2
H6
-selective
sorbents
to
replace
energy-intensive
cryogenic
distillation
is
a
promising
alternative
for
H4
purification
from
/C2
mixtures,
which
however
remains
challenging.
During
our
studies
two
isostructural
metal-organic
frameworks
(Ni-MOF
1
and
Ni-MOF
2),
we
found
that
2
exhibited
significantly
higher
performance
than
Ni-MOF-1,
as
clearly
established
by
gas
sorption
isotherms
breakthrough
experiments.
Density-Functional
Theory
(DFT)
showed
the
unblocked
unique
aromatic
pore
surfaces
within
induce
more
stronger
C-H⋅⋅⋅π
with
over
while
suitable
spaces
enforce
its
high
uptake
capacity,
featuring
one
of
best
porous
materials
this
very
important
separation.
It
generates
12
L
kg-1
polymer-grade
product
equimolar
mixtures
at
ambient
conditions.
Chemical Society Reviews,
Год журнала:
2020,
Номер
49(15), С. 5359 - 5406
Опубликована: Янв. 1, 2020
The
diversity
of
metal–organic
frameworks
enables
the
design
highly
efficient
adsorbents
and
membranes
towards
hydrocarbon
separations
for
energy
consumption
mitigation.
Advanced Materials,
Год журнала:
2020,
Номер
32(44)
Опубликована: Июль 16, 2020
Metal-organic
frameworks
(MOFs)
have
emerged
as
an
important
and
unique
class
of
functional
crystalline
hybrid
porous
materials
in
the
past
two
decades.
Due
to
their
modular
structures
adjustable
pore
system,
such
distinctive
exhibited
remarkable
prospects
key
applications
pertaining
adsorption
gas
storage,
liquid
separations,
trace
impurity
removal.
Evidently,
gaining
a
better
understanding
structure-property
relationship
offers
great
potential
for
enhancement
given
associated
MOF
property
either
by
structural
adjustments
via
isoreticular
chemistry
or
design
construction
new
practice
reticular
chemistry.
Correspondingly,
application
paves
way
microfine
structure
regulation
presented
MOFs.
Explicitly,
tuning
is
mainly
based
on
known
platforms,
focusing
modification
and/or
functionalization
precise
part
thus
providing
effective
approach
produce
richer
systems
with
enhanced
performances
from
limited
number
platforms.
Here,
latest
progress
this
field
highlighted
emphasizing
differences
connections
between
various
methods.
Finally,
challenges
together
are
also
discussed.
Journal of the American Chemical Society,
Год журнала:
2020,
Номер
142(41), С. 17795 - 17801
Опубликована: Сен. 29, 2020
Highly
selective
adsorptive
separation
of
olefin/paraffin
through
porous
materials
can
produce
high
purity
olefins
in
a
much
more
energy-efficient
way
than
the
traditional
cryogenic
distillation.
Here
we
report
an
ultramicroporous
cobalt
gallate
metal-organic
framework
(Co-gallate)
for
highly
sieving
propylene/propane
at
ambient
conditions.
This
material
possesses
optimal
pore
structure
exact
confinement
propylene
molecules
while
excluding
slightly
large
propane
molecules,
as
clearly
demonstrated
neutron
diffraction
crystal
Co-gallate⊃0.38C
Angewandte Chemie International Edition,
Год журнала:
2020,
Номер
59(50), С. 22756 - 22762
Опубликована: Сен. 2, 2020
In
comparison
with
the
fast
development
of
binary
mixture
separations,
ternary
separations
are
significantly
more
difficult
and
have
rarely
been
realized
by
a
single
material.
Herein,
new
strategy
tuning
gate-opening
pressure
flexible
MOFs
is
developed
to
tackle
such
challenge.
As
demonstrated
framework
NTU-65,
ethylene
(C2
H4
),
acetylene
H2
carbon
dioxide
(CO2
)
can
be
regulated
temperature.
Therefore,
efficient
sieving
separation
this
was
realized.
Under
optimized
temperature,
NTU-65
adsorbed
large
amount
C2
CO2
through
only
negligible
.
Breakthrough
experiments
that
material
simultaneously
capture
,
yielding
polymer-grade
(>99.99
%)
from
breakthrough
separation.
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
144(6), С. 2614 - 2623
Опубликована: Фев. 2, 2022
Purification
of
C2H4
from
a
ternary
C2H2/C2H6/C2H4
mixture
by
one-step
adsorption
separation
is
prime
importance
but
challenging
in
the
petrochemical
industry;
however,
effective
strategies
to
design
high-performance
adsorbents
are
lacking.
We
herein
report
for
first
time
incorporation
Lewis
basic
sites
into
C2H6-selective
MOF,
enabling
efficient
production
polymer-grade
mixtures.
Introduction
amino
groups
highly
stable
UiO-67
can
not
only
partition
large
pores
smaller
cagelike
pockets
provide
suitable
pore
confinement
also
offer
additional
binding
simultaneously
enhance
C2H2
and
C2H6
capacities
over
C2H4.
The
amino-functionalized
UiO-67-(NH2)2
thus
exhibits
exceptionally
high
uptakes
as
well
benchmark
C2H2/C2H4
C2H6/C2H4
selectivities,
surpassing
all
C2H2/C2H6-selective
materials
reported
so
far.
Theoretical
calculations
combined
with
situ
infrared
spectroscopy
indicate
that
synergetic
effect
functional
surfaces
decorated
provides
overall
stronger
multipoint
van
der
Waals
interactions
exceptional
performance
was
evidenced
breakthrough
experiments
mixtures
under
dry
wet
conditions,
providing
remarkable
productivity
0.55
mmol
g-1
at
ambient
conditions.
Journal of the American Chemical Society,
Год журнала:
2021,
Номер
143(3), С. 1485 - 1492
Опубликована: Янв. 13, 2021
Ethylene
production
from
C2
hydrocarbon
mixtures
through
one
separation
step
is
desirable
but
challenging
because
of
the
similar
size
and
physical
properties
acetylene,
ethylene,
ethane.
Herein,
we
report
three
new
isostructural
porous
coordination
networks
(NPU-1,
NPU-2,
NPU-3;
NPU
represents
Northwestern
Polytechnical
University)
that
are
sustained
by
9-connected
nodes
based
upon
a
hexanuclear
metal
cluster
composition
[Mn6(μ3-O)2(CH3COO)3]6+.
NPU-1/2/3
exhibit
dual
cage
structure
was
systematically
fine-tuned
in
terms
to
realize
selective
adsorption
C2H2
C2H6
over
C2H4.
Dynamic
breakthrough
experiments
demonstrated
NPU-1
produces
ethylene
>99.9%
purity
three-component
gas
mixture
(1:1:1
C2H2/C2H4/C2H6).
Molecular
modeling
studies
revealed
preference
for
C2H4
originates
(a)
strong
hydrogen-bonding
interactions
between
electronegative
carboxylate
O
atoms
molecules
(b)
multiple
non-covalent
organic
linkers
host
network
second
cage.
