Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(46), С. 25233 - 25241
Опубликована: Ноя. 13, 2023
Materials
capable
of
selectively
adsorbing
or
releasing
water
can
enable
valuable
applications
ranging
from
efficient
humidity
and
temperature
control
to
the
direct
atmospheric
capture
potable
water.
Despite
recent
progress
in
employing
metal-organic
frameworks
(MOFs)
as
privileged
sorbents,
developing
a
readily
accessible,
water-stable
MOF
platform
that
be
systematically
modified
for
high
uptake
at
low
relative
remains
significant
challenge.
We
herein
report
development
tunable
efficiently
captures
(up
0.78
g
water/g
MOF)
across
range
(27-45%)
accessible
Zn
bibenzotriazolate
MOF,
CFA-1
([Zn5(OAc)4(bibta)3],
H2bibta
=
1H,1H'-5,5'-bibenzo[d][1,2,3]triazole),
base
subsequent
diversification.
Controlling
metal
identity
(zinc,
nickel)
coordinating
nonstructural
anion
(acetate,
chloride)
via
postsynthetic
exchange
modulates
uptake,
facilitating
use
single
scaffold
diverse
potential
sorption
applications.
further
present
fundamental
theory
dictating
how
continuous
variation
pore
environment
affects
uptake.
Exchange
substituents
preserves
capacity
sorption,
increases
hydrolytic
stability
(with
5.7%
loss
working
over
450
adsorption-desorption
cycles
nickel-chloride-rich
framework),
enables
modulation
condensation.
This
combination
tunability
within
synthetically
framework
renders
Ni-incorporated
M5X4bibta3
promising
materials
practical
Advanced Materials,
Год журнала:
2023,
Номер
35(40)
Опубликована: Март 4, 2023
Freshwater
scarcity
is
a
global
challenge
posing
threats
to
the
lives
and
daily
activities
of
humankind
such
that
two-thirds
population
currently
experience
water
shortages.
Atmospheric
water,
irrespective
geographical
location,
considered
as
an
alternative
source.
Sorption-based
atmospheric
harvesting
(SAWH)
has
recently
emerged
efficient
strategy
for
decentralized
production.
SAWH
thus
opens
up
self-sustaining
source
freshwater
can
potentially
support
various
applications.
In
this
review,
state-of-the-art
SAWH,
considering
its
operation
principle,
thermodynamic
analysis,
energy
assessment,
materials,
components,
different
designs,
productivity
improvement,
scale-up,
application
drinking
first
extensively
explored.
Thereafter,
practical
integration
potential
beyond
wide
range
utilities
in
agriculture,
fuel/electricity
production,
thermal
management
building
services,
electronic
devices,
textile
are
comprehensively
discussed.
The
strategies
reduce
human
reliance
on
natural
resources
by
integrating
into
existing
technologies,
particularly
underdeveloped
countries,
order
satisfy
interconnected
needs
food,
energy,
also
examined.
This
study
further
highlights
urgent
need
future
research
directions
intensify
design
development
hybrid-SAWH
systems
sustainability
diverse
ACS Central Science,
Год журнала:
2023,
Номер
9(3), С. 551 - 557
Опубликована: Март 6, 2023
A
linker
extension
strategy
for
generating
metal-organic
frameworks
(MOFs)
with
superior
moisture-capturing
properties
is
presented.
Applying
this
design
approach
involving
experiment
and
computation
results
in
MOF-LA2-1
{[Al(OH)(PZVDC)],
where
PZVDC2-
(E)-5-(2-carboxylatovinyl)-1H-pyrazole-3-carboxylate},
which
exhibits
an
approximately
50%
water
capacity
increase
compared
to
the
state-of-the-art
water-harvesting
material
MOF-303.
The
power
of
pore
volume
while
retaining
ability
MOF
harvest
arid
environments
under
long-term
uptake
release
cycling,
as
well
affording
a
reduction
regeneration
heat
temperature.
Density
functional
theory
calculations
Monte
Carlo
simulations
give
detailed
insight
pertaining
framework
structure,
interactions
within
its
pores,
resulting
sorption
isotherm.
Advanced Functional Materials,
Год журнала:
2023,
Номер
34(43)
Опубликована: Июль 21, 2023
Abstract
Metal–organic
frameworks
(MOFs)
are
superior
sorbents
for
water
adsorption‐based
applications.
The
unique
step‐like
isotherm
at
a
MOF‐specific
relative
pressure
allows
easy
loading
and
regeneration
over
small
range
of
temperature
conditions.
With
good
hydrothermal
stability
cyclic
durability,
it
stands
out
classical
used
in
applications
humidity
control,
harvesting,
heating
cooling.
These
easily
regenerated
moderate
temperatures
using
“waste”
heat
or
solar
heating.
thermodynamics
adsorption
mechanisms
described,
the
presence
MOFs
water–air
system
is
explained.
Based
on
six
selection
criteria
≈40
reported
one
COF
identified
potential
application.
Trends
approaches
further
synthesis
optimization
production
scale‐up
highlighted.
No‐MOF‐fits‐all,
each
MOF
has
its
own
specific
step
location
matching
only
with
certain
application
type.
Most
technically
feasible
demonstrated
bench‐scale
pilot.
Their
maturity
benchmarked
by
their
technology
readiness
level.
Retrofitting
existing
replacing
desiccants
may
lead
to
rapid
demonstration.
Studies
techno‐economic
analysis
life
cycle
required
rational
evaluation
feasibility
promising
ACS Central Science,
Год журнала:
2023,
Номер
9(11), С. 2161 - 2170
Опубликована: Ноя. 10, 2023
We
leveraged
the
power
of
ChatGPT
and
Bayesian
optimization
in
development
a
multi-AI-driven
system,
backed
by
seven
large
language
model-based
assistants
equipped
with
machine
learning
algorithms,
that
seamlessly
orchestrates
multitude
research
aspects
chemistry
laboratory
(termed
Research
Group).
Our
approach
accelerated
discovery
optimal
microwave
synthesis
conditions,
enhancing
crystallinity
MOF-321,
MOF-322,
COF-323
achieving
desired
porosity
water
capacity.
In
this
human
researchers
gained
assistance
from
these
diverse
AI
collaborators,
each
unique
role
within
environment,
spanning
strategy
planning,
literature
search,
coding,
robotic
operation,
labware
design,
safety
inspection,
data
analysis.
Such
comprehensive
enables
single
researcher
working
concert
to
achieve
productivity
levels
analogous
those
an
entire
traditional
scientific
team.
Furthermore,
reducing
biases
screening
experimental
conditions
deftly
balancing
exploration
exploitation
parameters,
our
search
precisely
zeroed
on
pool
6
million
significantly
shortened
time
scale.
This
work
serves
as
compelling
proof
concept
for
AI-driven
revolution
laboratory,
painting
future
where
becomes
efficient
collaborator,
liberating
us
routine
tasks
focus
pushing
boundaries
innovation.
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(51), С. 28284 - 28295
Опубликована: Дек. 13, 2023
We
construct
a
data
set
of
metal-organic
framework
(MOF)
linkers
and
employ
fine-tuned
GPT
assistant
to
propose
MOF
linker
designs
by
mutating
modifying
the
existing
structures.
This
strategy
allows
model
learn
intricate
language
chemistry
in
molecular
representations,
thereby
achieving
an
enhanced
accuracy
generating
structures
compared
with
its
base
models.
Aiming
highlight
significance
design
strategies
advancing
discovery
water-harvesting
MOFs,
we
conducted
systematic
variant
expansion
upon
state-of-the-art
MOF-303
utilizing
multidimensional
approach
that
integrates
extension
multivariate
tuning
strategies.
synthesized
series
isoreticular
aluminum
termed
Long-Arm
MOFs
(LAMOF-1
LAMOF-10),
featuring
bear
various
combinations
heteroatoms
their
five-membered
ring
moiety,
replacing
pyrazole
either
thiophene,
furan,
or
thiazole
rings
combination
two.
Beyond
consistent
robust
architecture,
as
demonstrated
permanent
porosity
thermal
stability,
LAMOF
offers
generalizable
synthesis
strategy.
Importantly,
these
10
LAMOFs
establish
new
benchmarks
for
water
uptake
(up
0.64
g
g-1)
operational
humidity
ranges
(between
13
53%),
expanding
diversity
MOFs.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(44)
Опубликована: Сен. 12, 2023
One-step
separation
of
C2
H4
from
ternary
mixtures
by
physisorbents
remains
a
challenge
to
combine
excellent
performance
with
high
stability,
low
cost,
and
easy
scalability
for
industrial
applications.
Herein,
we
report
strategy
constructing
negative
electrostatic
pore
environments
in
stable,
low-cost,
easily
scaled-up
aluminum
MOF
(MOF-303)
efficient
one-step
H2
/C2
H6
separation.
This
material
exhibits
not
only
record
uptakes,
but
also
top-tier
selectivities
at
ambient
conditions.
Theoretical
calculations
combined
situ
infrared
spectroscopy
indicate
that
multiple
N/O
sites
on
channels
can
build
electro-environment
provide
stronger
interactions
over
.
Breakthrough
experiments
confirm
its
exceptional
mixtures,
affording
one
the
highest
productivity
1.35
mmol
g-1
is
highly
stable
be
synthesized
kilogram-scale
cheap
raw
materials
using
water-based
green
synthesis.
The
benchmark
combination
properties
stability
cost
scalable
MOF-303
has
unlocked
great
potential
this
challenging
Advanced Functional Materials,
Год журнала:
2023,
Номер
34(43)
Опубликована: Авг. 8, 2023
Abstract
Rapid
industrialization
and
ever‐increasing
global
population
culminate
in
continuous
upsurge
freshwater
crisis
worldwide.
The
most
reliable
promising
solution
to
this
is
utilizing
sea‐water
as
the
source,
desalination
technologies
pave
way
for
efficient
production
of
from
sea‐water.
In
regard,
membrane‐based
method
comes
forth
owing
its'
separation,
operational
ease,
low‐energy
consumption.
Metal–organic
frameworks
(MOFs),
explored
crystalline
porous
materials,
show
tremendous
promise
membrane‐materials
their
structural
diversity,
tunability,
voids
which
provide
secondary
water
channels.
Given
significant
advances
are
made
MOF‐materials
past
few
years,
it
crucial
systematically
summarize
recent
progress
development
field.
review,
a
brief
overview
various
saline
systems
prerequisites
first
presented.
Then,
advanced
fabrication
strategies
MOF‐membranes
followed
by
processes
such
reverse
osmosis
forward
summarized.
Finally,
authors’
perspectives
on
unsolved
scientific
technical
challenges
opportunities
MOF‐integrated
membranes
toward
real‐world
implementation
proposed.
With
further
systematic
development,
an
ideal
platform
next‐generation
technology.
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(50), С. 27262 - 27272
Опубликована: Дек. 10, 2023
Fe-Nx-C-based
single-atom
(SA-Fe-N-C)
catalysts
have
shown
favorable
oxygen
reduction
reaction
(ORR)
activity.
However,
their
application
in
proton
exchange
membrane
fuel
cells
is
hindered
by
reduced
performance
owing
to
the
thick
catalyst
layer,
restricting
mass
transfer
and
O2
supply.
Metal-organic
frameworks
(MOFs)
are
a
promising
class
of
crystal
materials,
but
narrow
pores
exacerbate
sluggish
mass-transport
properties
within
layer.
This
study
developed
an
approach
for
constructing
open-pore
structure
MOFs
via
chelation-assisted
selective
etching,
resulting
atomically
dispersed
Fe
atoms
anchored
on
N,
S
co-doped
carbon
framework.
The
reduces
transport
resistance
electrode
assembly
(MEA)
with
unprecedented
ORR
activity
stability,
as
evidenced
finite
element
simulations.
In
acidic
electrolyte,
OP-Fe-NC
shows
half-wave
potential
0.89
V
vs
RHE,
surpassing
Pt/C
20
mV,
current
density
29
mA
cm-2
at
0.9
ViR-free
MEA.
provides
effective
structural
strategy
fabricating
electrocatalysts
high
efficiency
atomic
precision
energy
storage
conversion
devices.