Abstract
Hierarchical
porous
materials
have
attracted
the
attention
of
researchers
due
to
their
enormous
specific
surface
area,
maximized
active
site
utilization
efficiency,
and
unique
structure
properties.
In
this
context,
metal–organic
frameworks
(MOFs)
offer
a
mix
properties
that
make
them
particularly
appealing
as
tunable
substrates
containing
highly
sites.
This
review
focuses
on
recent
advances
in
types
synthetic
strategies
hierarchical
MOFs
derived
materials.
Furthermore,
it
highlights
relationship
between
mass
diffusion
transport
structures
pore
size
with
examples
simulations,
while
identifying
potential
limitations.
On
basis,
how
synthesis
conditions
affect
electrochemical
based
different
is
discussed,
highlighting
prospects
challenges
for
synthetization,
well
further
scientific
research
practical
applications.
Finally,
some
insights
into
current
future
design
ideas
advanced
are
presented.
Chemical Society Reviews,
Год журнала:
2022,
Номер
51(17), С. 7427 - 7508
Опубликована: Янв. 1, 2022
Fluorinated
metal-organic
frameworks
(F-MOFs)
as
fast-growing
porous
materials
have
revolutionized
the
field
of
gas
separation
due
to
their
tunable
pore
apertures,
appealing
chemical
features,
and
excellent
stability.
A
deep
understanding
structure-performance
relationships
is
critical
for
synthesis
development
new
F-MOFs.
This
review
has
focused
on
several
strategies
precise
design
F-MOFs
with
structures
tuned
specific
purposes.
First,
basic
principles
concepts
well
structure,
modification
structure
property
are
studied.
Then,
applications
in
adsorption
membrane
discussed.
detailed
account
capabilities
various
gases
governing
provided.
In
addition,
exceptional
characteristics
highly
stable
engineered
size
put
into
perspective
fabricate
selective
membranes
separation.
Systematic
analysis
position
revealed
that
benchmark
most
challenging
separations.
The
outlook
future
directions
science
engineering
challenges
highlighted
tackle
issues
overcoming
trade-off
between
capacity/permeability
selectivity
a
serious
move
towards
industrialization.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(24)
Опубликована: Март 31, 2022
Integrating
molecular
catalysts
into
designed
frameworks
often
enables
improved
catalysis.
Compared
with
porphyrin-based
frameworks,
metal-corrole-based
have
been
rarely
developed,
although
monomeric
metal
corroles
are
usually
more
efficient
than
porphyrin
counterparts
for
the
electrocatalytic
oxygen
reduction
reaction
(ORR)
and
evolution
(OER).
We
herein
report
on
porous
organic
polymers
(POPs)
as
ORR
OER
electrocatalysts.
M-POPs
(M=Mn,
Fe,
Co,
Cu)
were
synthesized
by
coupling
10-phenyl-5,15-(4-iodophenyl)corrole
tetrakis(4-ethynylphenyl)methane.
corrole
monomers,
displayed
significantly
enhanced
catalytic
activity
stability.
Co-POP
outperformed
other
achieving
four-electron
a
half-wave
potential
of
0.87
V
vs.
RHE
reaching
10
mA
cm-2
current
density
at
340
mV
overpotential.
This
work
is
unparalleled
to
develop
explore
POPs
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(5), С. 2958 - 2967
Опубликована: Янв. 27, 2023
Metal-organic
frameworks
(MOFs)
are
materials
with
a
high
degree
of
porosity
that
can
be
used
for
many
applications.
However,
the
chemical
space
MOFs
is
enormous
due
to
large
variety
possible
combinations
building
blocks
and
topology.
Discovering
optimal
specific
applications
requires
an
efficient
accurate
search
over
countless
potential
candidates.
Previous
high-throughput
screening
methods
using
computational
simulations
like
DFT
time-consuming.
Such
also
require
3D
atomic
structures
MOFs,
which
adds
one
extra
step
when
evaluating
hypothetical
MOFs.
In
this
work,
we
propose
structure-agnostic
deep
learning
method
based
on
Transformer
model,
named
as
MOFormer,
property
predictions
MOFormer
takes
text
string
representation
MOF
(MOFid)
input,
thus
circumventing
need
obtaining
structure
accelerating
process.
By
comparing
other
descriptors
such
Stoichiometric-120
revised
autocorrelations,
demonstrate
achieve
state-of-the-art
prediction
accuracy
all
benchmarks.
Furthermore,
introduce
self-supervised
framework
pretrains
via
maximizing
cross-correlation
between
its
representations
structure-based
crystal
graph
convolutional
neural
network
(CGCNN)
>400k
publicly
available
data.
Benchmarks
show
pretraining
improves
both
models
various
downstream
tasks.
revealed
more
data-efficient
quantum-chemical
than
CGCNN
training
data
limited.
Overall,
provides
novel
perspective
learning.
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
144(36), С. 16219 - 16231
Опубликована: Сен. 2, 2022
The
odyssey
of
photochemistry
is
accompanied
by
the
journey
to
manipulate
"electrons"
and
"protons"
in
time,
space,
energy.
Over
past
decades,
single-electron
(1e-)
photochemical
transformations
have
brought
marvelous
achievements.
However,
as
each
photon
absorption
typically
generates
only
one
exciton
pair,
it
exponentially
challenging
accomplish
multielectron
proton
transformations.
multistep
differences
thermodynamics
kinetics
urgently
require
us
optimize
light
harvesting,
expedite
consecutive
electron
transfer,
interaction
catalysts
with
substrates,
coordinate
transfer
furnish
selective
bond
formations.
Tandem
catalysis
enables
orchestrating
different
events
catalytic
from
subpicoseconds
seconds,
which
facilitates
redox
chemistries
brings
consecutive,
value-added
reactivities.
Joint
efforts
molecular
material
design,
mechanistic
understanding,
theoretical
modeling
will
bring
synthetic
opportunities
for
fuels,
fertilizers,
chemicals
enhanced
versatility,
efficiency,
selectivity,
scalability,
thus
taking
better
advantage
photons
(i.e.,
sunlight)
our
sustainable
society.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
62(1)
Опубликована: Ноя. 8, 2022
Synthesizing
large-area
free-standing
covalent
organic
framework
(COF)
films
is
of
vital
importance
for
their
applications
but
still
a
big
challenge.
Herein,
we
reported
the
synthesis
large
metalloporphyrin-based
COF
and
oxygen
electrocatalysis.
The
reaction
meso-benzohydrazide-substituted
metal
porphyrins
with
tris-aldehyde
linkers
afforded
at
liquid-air
interface.
These
can
be
scaled
up
to
3000
cm2
area
display
great
mechanical
stability
structural
integrity.
Importantly,
Co-porphyrin-based
are
efficient
electrocatalytic
O2
reduction
evolution
reactions.
A
flexible,
all-solid-state
Zn-air
battery
was
assembled
using
showed
high
performance
charge-discharge
voltage
gap
0.88
V
1
mA
cm-2
under
bent
conditions
(0°
180°).
This
work
thus
presents
strategy
synthesize
functionalized
quality
uses
in
flexible
electronics.
Chemical Reviews,
Год журнала:
2023,
Номер
123(16), С. 10156 - 10205
Опубликована: Июль 31, 2023
Greenhouse
gas
emissions
associated
with
power
generation
from
fossil
fuel
combustion
account
for
25%
of
global
and,
thus,
contribute
greatly
to
climate
change.
Renewable
energy
sources,
like
wind
and
solar,
have
reached
a
mature
stage,
costs
aligning
those
fuel-derived
but
suffer
the
challenge
intermittency
due
variability
sunlight.
This
study
aims
explore
viability
salinity
gradient
power,
or
"blue
energy",
as
clean,
renewable
source
uninterrupted,
base-load
generation.
Harnessing
river
estuaries
worldwide
could
meet
substantial
portion
electricity
demand
(approximately
7%).
Pressure
retarded
osmosis
(PRO)
reverse
electrodialysis
(RED)
are
more
prominent
technologies
blue
harvesting,
whereas
thermo-osmotic
conversion
(TOEC)
is
emerging
new
promise.
review
scrutinizes
obstacles
encountered
in
developing
osmotic
using
membrane-based
methods
presents
potential
solutions
overcome
challenges
practical
applications.
While
certain
strategies
shown
promise
addressing
some
these
obstacles,
further
research
still
required
enhance
efficiency
feasibility
processes,
enabling
their
large-scale
implementation
harvesting.
