Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(32)
Опубликована: Май 15, 2024
Abstract
Converting
spent
lithium‐ion
batteries
(LIBs)
cathode
materials
into
environmental
catalysts
has
drawn
more
and
attention.
Herein,
we
fabricated
a
Co
3
O
4
‐based
catalyst
from
LiCoO
2
LIBs
(Co
‐LIBs)
found
that
the
role
of
Al
Cu
current
collectors
on
its
performance
is
nonnegligible.
The
density
functional
theory
calculations
confirmed
doping
and/or
upshifts
d‐band
center
Co.
A
Fenton‐like
reaction
based
peroxymonosulfate
(PMS)
activation
was
adopted
to
evaluate
activity.
Interestingly,
strengthened
chemisorption
for
PMS
(from
−2.615
eV
−2.623
eV)
shortened
Co−O
bond
length
2.540
Å
2.344
Å)
between
them,
whereas
reduced
interfacial
charge‐transfer
resistance
28.347
kΩ
6.689
kΩ)
excepting
enhancement
above
characteristics.
As
expected,
degradation
activity
toward
bisphenol
‐LIBs
(0.523
min
−1
)
superior
prepared
commercial
CoC
(0.287
).
Simultaneously,
reasons
improved
were
further
verified
by
comparing
with
doped
.
This
work
reveals
elements
LIBs,
which
beneficial
sustainable
utilization
LIBs.
Abstract
The
activation
of
persulfates
to
degrade
refractory
organic
pollutants
is
a
hot
issue
in
advanced
oxidation
right
now.
Here,
it
reported
that
single‐atom
Fe‐incorporated
carbon
nitride
(Fe‐CN‐650)
can
effectively
activate
peroxymonosulfate
(PMS)
for
sulfamethoxazole
(SMX)
removal.
Through
some
characterization
techniques
and
DFT
calculation,
proved
Fe
single
atoms
Fe‐CN‐650
exist
mainly
the
form
Fe‐N
3
O
1
coordination,
exhibited
better
affinity
PMS
than
traditional
4
structure.
degradation
rate
constant
SMX
Fe‐CN‐650/PMS
system
reached
0.472
min
−1
,
90.80%
still
be
degraded
within
10
after
five
consecutive
recovery
cycles.
radical
quenching
experiment
electrochemical
analysis
confirm
are
by
two
non‐radical
pathways
through
2
Fe(IV)═O
induced
at
sites.
In
addition,
intermediate
products
show
toxicity
attenuation
or
non‐toxicity.
This
study
offers
valuable
insights
into
design
carbon‐based
catalysts
provides
potential
remediation
technology
optimum
disintegrate
pollutants.
Environmental Science & Technology Letters,
Год журнала:
2024,
Номер
11(4), С. 370 - 375
Опубликована: Март 14, 2024
Limited
by
the
detection
techniques,
reactive
species
involved
in
catalytic
water
purification
processes
are
difficult
to
be
clarified.
Spin-trapping
electron
paramagnetic
resonance
(EPR)
analysis
is
recognized
as
a
reliable
tool
for
radical
identification,
which
5,5-dimethyl-1-pyrroline-N-oxide
(DMPO)
usually
used
trapper.
However,
it
questioned
that
of
adducts
DMPO
definitively
indicates
generation
radicals.
In
this
work,
transformation
caused
transition
metal
oxides
monitored
EPR,
and
abundant
spin
signals
observed.
MnO2,
Mn2O3,
NiO
could
oxidize
into
DMPOX
through
direct
oxygen
transfer.
Besides,
dissolved
ions
transform
misleading
DMPO–OH
DMPO–R.
The
findings
e.g.,
interactions
between
different
quenching
behavior
pathways,
would
help
with
identifications
both
engineered
systems
natural
environments.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(14)
Опубликована: Фев. 15, 2024
As
a
sustainable
valorization
route,
electrochemical
glycerol
oxidation
reaction
(GOR)
involves
in
formation
of
key
OH*
and
selective
adsorption/cleavage
C-C(O)
intermediates
with
multi-step
electron
transfer,
thus
suffering
from
high
potential
poor
formate
selectivity
for
most
non-noble-metal-based
electrocatalysts.
So,
it
remains
challenging
to
understand
the
structure-property
relationship
as
well
construct
synergistic
sites
realize
high-activity
high-selectivity
GOR.
Herein,
we
successfully
achieve
dual-high
performance
low
potentials
superior
GOR
by
forming
Lewis
Brønsted
acid
Ni-alloyed
Co-based
spinel.
The
optimized
NiCo
oxide
solid-acid
electrocatalyst
exhibits
(1.219
V@10
mA/cm
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(32)
Опубликована: Май 15, 2024
Abstract
Converting
spent
lithium‐ion
batteries
(LIBs)
cathode
materials
into
environmental
catalysts
has
drawn
more
and
attention.
Herein,
we
fabricated
a
Co
3
O
4
‐based
catalyst
from
LiCoO
2
LIBs
(Co
‐LIBs)
found
that
the
role
of
Al
Cu
current
collectors
on
its
performance
is
nonnegligible.
The
density
functional
theory
calculations
confirmed
doping
and/or
upshifts
d‐band
center
Co.
A
Fenton‐like
reaction
based
peroxymonosulfate
(PMS)
activation
was
adopted
to
evaluate
activity.
Interestingly,
strengthened
chemisorption
for
PMS
(from
−2.615
eV
−2.623
eV)
shortened
Co−O
bond
length
2.540
Å
2.344
Å)
between
them,
whereas
reduced
interfacial
charge‐transfer
resistance
28.347
kΩ
6.689
kΩ)
excepting
enhancement
above
characteristics.
As
expected,
degradation
activity
toward
bisphenol
‐LIBs
(0.523
min
−1
)
superior
prepared
commercial
CoC
(0.287
).
Simultaneously,
reasons
improved
were
further
verified
by
comparing
with
doped
.
This
work
reveals
elements
LIBs,
which
beneficial
sustainable
utilization
LIBs.