ACS Central Science,
Год журнала:
2023,
Номер
9(12), С. 2326 - 2332
Опубликована: Дек. 13, 2023
Electrochemical
uranium
extraction
from
seawater
provides
a
new
opportunity
for
sustainable
supply
of
nuclear
fuel.
However,
there
is
still
room
studying
flexible
electrode
materials
in
this
field.
Herein,
we
construct
amidoxime
group
modified
porous
aromatic
frameworks
(PAF-144-AO)
on
carbon
cloths
situ
using
an
easy
to
scale-up
electropolymerization
method
followed
by
postdecoration
fabricate
the
self-standing,
binder-free,
metal-free
electrodes
(PAF-E).
Based
architectural
design,
adsorption
sites
(amidoxime
groups)
and
catalytic
(carbazole
are
integrated
into
PAF-144-AO.
Under
action
alternating
electric
field,
uranyl
ions
selectively
captured
PAN-E
subsequently
transformed
Na2O(UO3·H2O)x
precipitates
presence
Na+
via
reversible
electron
transfer,
with
capacity
12.6
mg
g–1
over
24
days
natural
seawater.
This
adsorption–electrocatalysis
mechanism
also
demonstrated
at
molecular
level
ex
spectroscopy.
Our
work
offers
effective
approach
designing
organic
polymer
electrodes,
which
hold
great
potential
field
electrochemical
Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Фев. 27, 2023
Covalent
organic
frameworks
(COFs)
represent
an
emerging
class
of
photocatalysts.
However,
their
complicated
structures
lead
to
indeterminacy
about
photocatalytic
active
sites
and
reaction
mechanisms.
Herein,
we
use
reticular
chemistry
construct
a
family
isoreticular
crystalline
hydrazide-based
COF
photocatalysts,
with
the
optoelectronic
properties
local
pore
characteristics
COFs
modulated
using
different
linkers.
The
excited
state
electronic
distribution
transport
pathways
in
are
probed
host
experimental
methods
theoretical
calculations
at
molecular
level.
One
our
developed
(denoted
as
COF-4)
exhibits
remarkable
electron
utilization
efficiency
charge
transfer
properties,
achieving
record-high
uranium
extraction
performance
~6.84
mg/g/day
natural
seawater
among
all
techniques
reported
so
far.
This
study
brings
new
understanding
operation
COF-based
guiding
design
improved
photocatalysts
for
many
applications.
Advanced Materials,
Год журнала:
2021,
Номер
33(51)
Опубликована: Окт. 4, 2021
Uranium
extraction
from
seawater
provides
an
opportunity
for
sustainable
fuel
supply
to
nuclear
power
plants.
Herein,
adsorption-electrocatalysis
strategy
is
demonstrated
efficient
uranium
using
a
functionalized
iron-nitrogen-carbon
(Fe-Nx
-C-R)
catalyst,
comprising
N-doped
carbon
capsules
supporting
FeNx
single-atom
sites
and
surface
chelating
amidoxime
groups
(R).
The
bring
hydrophilicity
the
adsorbent
offer
surface-specific
binding
UO22+
capture.
site-isolated
centres
reduce
adsorbed
UO2+
.
Subsequently,
through
electrochemical
reduction
of
sites,
unstable
U(V)
ions
are
reoxidized
U(VI)
in
presence
Na+
resulting
generation
solid
Na2
O(UO3
·H2
O)x
,
which
can
easily
be
collected.
Fe-Nx
-C-R
reduced
concentration
≈3.5
ppb
below
0.5
with
calculated
capacity
≈1.2
mg
g-1
within
24
h.
To
best
knowledge,
developed
system
first
use
adsorption
uranyl
electrodeposition
.H2
seawater.
important
discoveries
guide
technology
development
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(30)
Опубликована: Апрель 29, 2023
Optimizing
the
electronic
structure
of
covalent
organic
framework
(COF)
photocatalysts
is
essential
for
maximizing
photocatalytic
activity.
Herein,
we
report
an
isoreticular
family
multivariate
COFs
containing
chromenoquinoline
rings
in
COF
and
electron-donating
or
withdrawing
groups
pores.
Intramolecular
donor-acceptor
(D-A)
interactions
allowed
tuning
local
charge
distributions
carrier
separation
under
visible
light
irradiation,
resulting
enhanced
performance.
By
optimizing
optoelectronic
properties
COFs,
a
uranium
extraction
efficiency
8.02
mg/g/day
was
achieved
using
nitro-functionalized
multicomponent
natural
seawater,
exceeding
performance
all
reported
to
date.
Results
demonstrate
effective
design
strategy
towards
high-activity
with
intramolecular
D-A
structures
not
easily
accessible
traditional
synthetic
approaches.
Seawater
contains
uranium
at
a
concentration
of
≈3.3
ppb,
thus
representing
rich
and
sustainable
nuclear
fuel
source.
Herein,
an
adsorption-electrocatalytic
platform
is
developed
for
extraction
from
seawater,
comprising
atomically
dispersed
indium
anchored
on
hollow
nitrogen-doped
carbon
capsules
functionalized
with
flexible
amidoxime
moieties
(In-N
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
62(11)
Опубликована: Дек. 20, 2022
Abstract
Water
pollution
is
a
growing
threat
to
humanity
due
the
pervasiveness
of
contaminants
in
water
bodies.
Significant
efforts
have
been
made
separate
these
hazardous
components
purify
polluted
through
various
methods.
However,
conventional
remediation
methods
suffer
from
limitations
such
as
low
uptake
capacity
or
selectivity,
and
current
quality
standards
cannot
be
met.
Recently,
advanced
porous
materials
(APMs)
shown
promise
improved
segregation
compared
traditional
selectivity.
These
feature
merits
high
surface
area
versatile
functionality,
rendering
them
ideal
platforms
for
design
novel
adsorbents.
This
Review
summarizes
development
employment
APMs
variety
treatments
accompanied
by
assessments
task‐specific
adsorption
performance.
Finally,
we
discuss
our
perspectives
on
future
opportunities
purification.
