Environmental Science & Technology,
Journal Year:
2022,
Volume and Issue:
56(19), P. 14019 - 14029
Published: Sept. 5, 2022
In
electrochemical
advanced
oxidation
processes
(EAOPs),
the
rate-limiting
step
is
mass
transfer
of
pollutants
to
electrodes
due
limited
active
surface
areas.
To
this
end,
we
established
a
three-dimensional
(3D)
EAOP
system
by
coupling
conventional
graphite
with
dispersed
carbon
nanotubes
(CNTs).
The
(particularly
anode)
induced
electric
field
spontaneously
polarized
CNTs
into
reactive
particle
(CNT-PEs)
in
solution,
which
remarkably
promoted
activation
peroxydisulfate
(PDS)
generate
CNT-PDS*
complexes
and
surface-bound
radicals
(SBRs).
Based
on
excited
potential
(ECNT-PEs)
at
different
positions
3D
field,
CNT-PEs
were
activated
three
states.
(i)
ECNT-PEs
<
Eorganic,
are
chemically
inert
toward
DCP
oxidation;
(ii)
Eorganic
Ewater,
will
oxidize
via
an
electron-transfer
process
(ETP);
(iii)
>
both
anode
water
produce
SBRs.
Thus,
could
be
oxidized
ETP
form
polychlorophenols
CNT
surface,
causing
rapid
deactivation
micro-electrodes.
contrast,
SBRs
attack
directly
chloride
ions
hydroxylated
products,
maintaining
cleanliness
activity
for
long-term
operations.
Environmental Science & Technology,
Journal Year:
2021,
Volume and Issue:
56(1), P. 78 - 97
Published: Dec. 21, 2021
Persulfate-based
nonradical
oxidation
processes
(PS-NOPs)
are
appealing
in
wastewater
purification
due
to
their
high
efficiency
and
selectivity
for
removing
trace
organic
contaminants
complicated
water
matrices.
In
this
review,
we
showcased
the
recent
progresses
of
state-of-the-art
strategies
electron-transfer
regimes
PS-NOPs,
including
design
metal
metal-free
heterogeneous
catalysts,
situ/operando
characterization/analytical
techniques,
insights
into
origins
mechanisms.
a
typical
process
(ETP),
persulfate
is
activated
by
catalyst
form
surface
complexes,
which
directly
or
indirectly
interact
with
target
pollutants
finalize
oxidation.
We
discussed
different
analytical
techniques
on
fundamentals
tactics
accurate
analysis
ETP.
Moreover,
demonstrated
challenges
proposed
future
research
ETP-based
systems,
such
as
computation-enabled
molecular-level
investigations,
rational
real-scenario
applications
environment.
Overall,
review
dedicates
sharpening
understanding
ETP
PS-NOPs
presenting
promising
remediation
technology
green
chemistry.
Environmental Science & Technology,
Journal Year:
2023,
Volume and Issue:
57(33), P. 12153 - 12179
Published: Aug. 3, 2023
Urbanization
and
industrialization
have
exerted
significant
adverse
effects
on
water
quality,
resulting
in
a
growing
need
for
reliable
eco-friendly
treatment
technologies.
Persulfate
(PS)-based
advanced
oxidation
processes
(AOPs)
are
emerging
as
viable
technologies
to
treat
challenging
industrial
wastewaters
or
remediate
groundwater
impacted
by
hazardous
wastes.
While
the
generated
reactive
species
can
degrade
variety
of
priority
organic
contaminants
through
radical
nonradical
pathways,
there
is
lack
systematic
in-depth
comparison
these
pathways
practical
implementation
different
scenarios.
Our
comparative
analysis
reaction
rate
constants
vs.
indicates
that
radical-based
AOPs
may
achieve
high
removal
efficiency
with
relatively
short
contact
time.
Nonradical
feature
advantages
minimal
matrix
interference
complex
wastewater
treatments.
(e.g.,
singlet
oxygen,
high-valent
metals,
surface
activated
PS)
preferentially
react
bearing
electron-donating
groups,
allowing
enhancement
degradation
known
target
contaminants.
For
byproduct
formation,
analytical
limitations
computational
chemistry
applications
also
considered.
Finally,
we
propose
holistically
estimated
electrical
energy
per
order
(EE/O)
parameter
show
significantly
higher
requirements
pathways.
Overall,
critical
comparisons
help
prioritize
basic
research
PS-based
inform
merits
system-specific
applications.
Environmental Science & Technology,
Journal Year:
2022,
Volume and Issue:
56(7), P. 4498 - 4506
Published: March 17, 2022
The
environmentally
benign
Mn
oxides
play
a
crucial
role
in
the
transformation
of
organic
contaminants,
either
through
catalytically
decomposing
oxidants,
e.g.,
peroxymonosulfate
(PMS),
or
directly
oxidizing
target
pollutants.
Because
their
dual
roles
and
complex
surface
chemical
reactions,
mechanism
involved
oxide-catalyzed
PMS
activation
processes
remains
obscure.
Here,
we
clearly
elucidate
Mn2O3
catalyzed
process
by
means
separating
pollutant
oxidation
process.
acts
as
shuttle
that
mediates
electron
transfer
from
substrates
to
PMS,
accompanied
redox
cycle
Mn(IV)/Mn(III).
Multiple
experimental
results
indicate
is
bound
form
an
inner-sphere
complex,
which
then
decomposes
long-lived
reactive
Mn(IV)
species,
without
generation
sulfate
radicals
(SO4•–)
hydroxyl
(HO•).
species
are
proposed
be
responsible
for
degradation
contaminants
(e.g.,
phenol)
formation
singlet
oxygen
(1O2),
followed
regeneration
Mn(III)
sites
on
Mn2O3.
This
study
advances
fundamental
understanding
underlying
transition
metal
processes.
Nature Communications,
Journal Year:
2022,
Volume and Issue:
13(1)
Published: Sept. 22, 2022
Due
to
environmentally
friendly
operation
and
on-site
productivity,
electrocatalytic
singlet
oxygen
(1O2)
production
via
O2
gas
is
of
immense
interest
in
environment
purification.
However,
the
side-on
configuration
on
catalysts
surface
will
lead
formation
H2O,
which
seriously
limits
selectivity
activity
1O2
production.
Herein,
we
show
a
robust
N-doped
CuO
(N-CuO)
with
Pauling-type
(end-on)
adsorption
at
N-Cu-O3
sites
for
selective
generation
under
direct-current
electric
field.
We
propose
that
not
only
lowers
overall
activation
energy
barrier,
but
also
alters
reaction
pathway
form
instead
key
feature
determining
dissociation
Cu-O
bonds
rather
than
O-O
bonds.
The
proposed
N
dopant
strategy
applicable
series
transition
metal
oxides,
providing
universal
electrocatalysts
design
scheme
existing
high-performance
