ACS ES&T Engineering,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 22, 2024
Per-
and
polyfluoroalkyl
substances
(PFAS),
persistent
pollutants
found
in
water
sources
worldwide,
pose
significant
challenges
to
conventional
remediation
methods.
This
study
presents
a
one-pot,
high
atom-economy
synthesis
of
porphyrin-based
cationic
nanocages
(oNCs)
as
selective,
rapid
efficient
solution
for
PFAS
removal,
addressing
critical
gaps
current
treatment
technologies.
Using
liquid
chromatography–tandem
mass
spectrometry
(LC-MS/MS),
the
nanocages─[oNC]8PF6,
[Co2+-oNC]8PF6,
[Co3+(N≡O)-oNC]8PF6─were
evaluated
their
ability
sorb
mixture
38
PFAS,
including
emerging
contaminants
like
GenX,
from
various
matrices
at
concentration
50
ng/mL.
The
achieved
exceptional
removal
efficiencies,
with
optimal
results
obtained
when
[oNC]8PF6
[Co2+-oNC]8PF6
were
combined
1:4
ratio.
created
synergistic
effect,
enabling
sorption
both
short-
long-chain
achieving
average
efficiencies
90%
Nanopure
groundwater,
80%
influent
sewage.
nanocage
consistently
outperformed
activated
carbon,
particularly
complex
such
sewage,
where
carbon
presented
lower
efficiency,
especially
perfluoroalkane
sulfonamido
substances.
reached
equilibrium
within
15
min
maintained
performance
across
multiple
methanolic
regeneration
cycles,
highlighting
operational
durability.
NMR
spectroscopy
computational
studies
revealed
that
occurs
via
hydrophobic
electrostatic
interactions,
well
partial
intercalation,
selectivity
molecules
bearing
sulfonate
sulfonamide
head
groups
chain
lengths
five
or
more.
Early
stage
eco-toxicological
assessments
confirmed
environmental
safety
these
nanocages,
showing
no
adverse
effects
below
0.005
μM.
By
combining
modular,
scalable
sustainable
material
synthesis,
this
sets
new
direction
developing
precise,
environmentally
responsible
solutions.
Abstract
Modifying
the
coordination
or
local
environments
of
single‐,
di‐,
tri‐,
and
multi‐metal
atom
(SMA/DMA/TMA/MMA)‐based
materials
is
one
best
strategies
for
increasing
catalytic
activities,
selectivity,
long‐term
durability
these
materials.
Advanced
sheet
supported
by
metal
atom‐based
have
become
a
critical
topic
in
fields
renewable
energy
conversion
systems,
storage
devices,
sensors,
biomedicine
owing
to
maximum
utilization
efficiency,
precisely
located
centers,
specific
electron
configurations,
unique
reactivity,
precise
chemical
tunability.
Several
offer
excellent
support
are
attractive
applications
energy,
medical
research,
such
as
oxygen
reduction,
production,
hydrogen
generation,
fuel
selective
detection,
enzymatic
reactions.
The
strong
metal–metal
metal–carbon
with
metal–heteroatom
(i.e.,
N,
S,
P,
B,
O)
bonds
stabilize
optimize
electronic
structures
atoms
due
interfacial
interactions,
yielding
activities.
These
provide
models
understanding
fundamental
problems
multistep
This
review
summarizes
substrate
structure‐activity
relationship
different
active
sites
based
on
experimental
theoretical
data.
Additionally,
new
synthesis
procedures,
physicochemical
characterizations,
biomedical
discussed.
Finally,
remaining
challenges
developing
efficient
SMA/DMA/TMA/MMA‐based
presented.
Abstract
Hydrogen‐bonded
organic
frameworks
(HOFs)
are
emerging
porous
materials
that
show
high
structural
flexibility,
mild
synthetic
conditions,
good
solution
processability,
easy
healing
and
regeneration,
recyclability.
Although
these
properties
give
them
many
potential
multifunctional
applications,
their
unstable
due
to
the
presence
of
only
weak
reversible
hydrogen
bonds.
In
this
work,
development
history
synthesis
methods
HOFs
reviewed,
categorize
design
concepts
strategies
improve
stability.
More
importantly,
significant
latest
HOF‐related
research
for
addressing
energy
environmental
issues,
work
discusses
advances
in
storage
conversion,
substance
generation
isolation,
detection
degradation
transformation,
biological
applications.
Furthermore,
a
discussion
coupling
orientation
HOF
cross‐cutting
fields
environment
is
presented
first
time.
Finally,
current
challenges,
opportunities,
advance
applications
discussed.
