Environmental Science & Technology,
Год журнала:
2023,
Номер
57(27), С. 10127 - 10134
Опубликована: Июнь 14, 2023
Herein,
we
developed
an
electrochemical
filtration
system
for
effective
and
selective
abatement
of
nitrogenous
organic
pollutants
via
peroxymonosulfate
(PMS)
activation.
Highly
conductive
porous
copper
nanowire
(CuNW)
networks
were
constructed
to
serve
simultaneously
as
catalyst,
electrode,
media.
In
one
demonstration
the
CuNW
network's
capability,
a
single
pass
through
filter
(τ
<
2
s)
degraded
94.8%
sulfamethoxazole
(SMX)
at
applied
potential
−0.4
V
vs
SHE.
The
exposed
{111}
crystal
plane
triggered
atomic
hydrogen
(H*)
generation
on
sites,
which
contributed
PMS
reduction.
Meanwhile,
with
involvement
SMX,
Cu–N
bond
was
formed
by
interactions
between
−NH2
group
SMX
Cu
sites
CuNW,
accompanied
redox
cycling
Cu2+/Cu+,
facilitated
potential.
different
charges
active
made
it
easier
withdraw
electrons
promote
oxidation.
Theoretical
calculations
experimental
results
combined
suggest
mechanism
pollution
networks.
showed
that
efficacy
degradation
wide
array
robust
across
broad
range
solution
pH
complex
aqueous
matrices.
flow-through
operation
outperformed
conventional
batch
electrochemistry
due
convection-enhanced
mass
transport.
This
study
provides
new
strategy
environmental
remediation
integrating
state-of-the-art
material
science,
advanced
oxidation
processes,
microfiltration
technology.
Proceedings of the National Academy of Sciences,
Год журнала:
2023,
Номер
120(13)
Опубликована: Март 23, 2023
The
peroxymonosulfate
(PMS)-triggered
radical
and
nonradical
active
species
can
synergistically
guarantee
selectively
removing
micropollutants
in
complex
wastewater;
however,
realizing
this
on
heterogeneous
metal-based
catalysts
with
single
sites
remains
challenging
due
to
insufficient
electron
cycle.
Herein,
we
design
asymmetric
Co-O-Bi
triple-atom
Co-doped
Bi2O2CO3
facilitate
PMS
oxidation
reduction
simultaneously
by
enhancing
the
transfer
between
sites.
We
propose
that
result
an
density
increase
Bi
decrease
Co
sites,
thereby
undergoes
a
reaction
generate
SO4•-
•OH
at
site
1O2
site.
suggest
synergistic
effect
of
SO4•-,
•OH,
enables
efficient
removal
mineralization
without
interference
from
organic
inorganic
compounds
under
environmental
background.
As
result,
achieves
almost
99.3%
sulfamethoxazole
degradation
3
min
k-value
as
high
82.95
min-1
M-1,
which
is
superior
existing
reported
so
far.
This
work
provides
structural
regulation
approach
control
catalytic
function,
will
guide
rational
Fenton-like
catalysts.
Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Окт. 23, 2023
The
regulation
of
heterogeneous
material
properties
to
enhance
the
peroxymonosulfate
(PMS)
activation
degrade
emerging
organic
pollutants
remains
a
challenge.
To
solve
this
problem,
we
synthesize
S-scheme
heterojunction
PBA/MoS2@chitosan
hydrogel
achieve
photoexcitation
synergistic
PMS
activation.
constructed
photoexcited
carriers
undergo
redox
conversion
with
through
transfer
pathway
driven
by
directional
interface
electric
field.
Multiple
pathways
greatly
reactive
oxygen
species
generation,
leading
significant
increase
in
doxycycline
degradation
rate.
Meanwhile,
3D
polymer
chain
spatial
structure
chitosan
is
conducive
rapid
capture
and
electron
transport
advanced
oxidation
process,
reducing
use
transition
metal
activator
limiting
leaching
ions.
There
reason
believe
that
regulated
will
provide
new
perspective
for
future
design
research
on
enhancing
heterologous
catalysis
process.
Single‐atom
catalysts
(SACs)
consist
of
isolated
metal
sites
on
the
support
through
stable
coordination
bond,
which
usually
have
high
catalytic
activity
and
selectivity.
With
large
surface
area
electron
tunability,
metallic
carbides,
nitrides,
or
carbonic
nitrides
(MXenes)
are
suitable
carriers
for
supporting
single‐metal
atoms.
The
abundant
surface‐functional
groups
vacancy
defects
MXenes
ideal
anchoring
Herein,
advanced
synthesis
characterization
methods
MXene‐based
SACs
first
introduced.
Three
strategies
(adsorption
at
functional
groups,
vacancies,
terminating
group
vacancies)
appear
to
be
feasible
in
ensuring
non‐aggregation
atoms,
attributed
strong
bonding
between
atoms
carrier.
applications
electrocatalysis
(including
hydrogen
evolution
reaction,
oxygen
reduction
carbon
dioxide
nitrogen
reaction),
energy
storage
Li‐ion
batteries,
metal–air
supercapacitors),
sensors
gas
biological
sensors)
fundamentally
reviewed.
Finally,
own
insight
current
challenges
prospects
is
presented.
ACS Catalysis,
Год журнала:
2023,
Номер
13(18), С. 12414 - 12424
Опубликована: Сен. 7, 2023
Generating
singlet
oxygen
(1O2)
on
single
atom
catalysts
(SACs)
in
peroxymonosulfate
(PMS)-based
Fenton-like
reactions
exhibits
great
potential
for
selective
degradation
of
contaminants
complex
wastewater.
Clarifying
the
structure–activity
relationship
between
electronic
structure
SACs
and
1O2
generation
selectivity
is
crucial
precise
design
efficient
catalysts,
but
it
challenging.
Herein,
Cu
with
different
structures
(namely,
Cu–O2X,
where
X
=
N,
S,
B,
P,
O)
investigated
by
density
functional
theory
calculations
using
adsorption
terminal
atoms
PMS
as
an
activity
descriptor.
Significantly,
affected
center
which
electron-depleted
Cu-O2B
site
a
higher
atoms.
Experimentally,
moiety
superior
catalytic
activation,
showing
nearly
100%
ciprofloxacin
rate
0.2250
min–1,
outperforming
those
other
counterparts.
The
high
attributed
to
asymmetric
accelerating
faster
electron
transfer
O–O
bond
stretching,
lowering
energy
barrier
key
intermediates
toward
generation.
This
work
provides
broader
perspective
regulating
sites
at
atomic
level
catalysts.
