Angewandte Chemie,
Journal Year:
2022,
Volume and Issue:
134(29)
Published: May 6, 2022
Abstract
Simultaneous
regulation
of
the
coordination
environment
single‐atom
catalysts
(SACs)
and
engineering
architectures
with
efficient
exposed
active
sites
are
strategies
for
boosting
peroxymonosulfate
(PMS)
activation.
We
isolated
cobalt
atoms
dual
nitrogen
oxygen
(Co−N
3
O
1
)
on
oxygen‐doped
tubular
carbon
nitride
(TCN)
by
pyrolyzing
a
hydrogen‐bonded
cyanuric
acid
melamine–cobalt
acetate
precursor.
The
theoretically
constructed
Co−N
moiety
TCN
exhibited
an
impressive
mass
activity
7.61×10
5
min
−1
mol
high
2
selectivity.
Theoretical
calculations
revealed
that
single
occupied
environment,
PMS
adsorption
was
promoted
energy
barriers
reduced
key
*O
intermediate
produced
.
were
attached
to
widely
used
poly(vinylidene
fluoride)
microfiltration
membrane
deliver
antibiotic
wastewater
treatment
system
97.5
%
ciprofloxacin
rejection
over
10
hours,
thereby
revealing
suitability
industrial
applications.
ACS ES&T Engineering,
Journal Year:
2022,
Volume and Issue:
2(4), P. 527 - 546
Published: March 8, 2022
Heterogeneous
photocatalytic
persulfate
(PS)
activation
technologies
are
being
intensively
studied
for
water
treatment
due
to
their
friendly
environmental
benefits
and
photosynergistic
effect
in
comparison
with
traditional
PS
systems.
Previous
reviews
have
summarized
diverse
methods
the
role
of
light
systems,
but
it
is
still
urgent
provide
a
comprehensive
review
on
deep
understanding
rational
design
heterogeneous
PS-based
advanced
oxidation
processes
(AOPs).
This
intends
thoroughly
address
in-depth
fundamentals
mechanisms
PS-AOPs.
Challenges
improvement
strategies
PS-AOPs
also
critically
discussed.
On
basis
detailed
survey
published
studies,
PS-AOPs,
including
Fe-based,
TiO2-based,
other
metal
based,
bimetallic,
metal-free
carefully
clarified.
Finally,
engineering
implications
prospects
enumerated
developing
efficient
environmentally
treatment.
It
expected
that
this
will
motivate
researchers
construct
novel
promising
ACS ES&T Engineering,
Journal Year:
2022,
Volume and Issue:
2(10), P. 1776 - 1796
Published: Sept. 7, 2022
Single
atom
catalysts
(SACs)
have
emerged
as
a
promising
catalyst
material
architecture
for
energy,
chemical,
and
environmental
applications.
In
the
past
several
years,
SACs
been
increasingly
explored
persulfate-based
advanced
oxidation
processes
(AOPs)
due
to
their
superior
persulfate
activation
pollutant
degradation
performance
compared
benchmark
dissolved
ion
nanoparticle
catalysts.
However,
there
still
exist
uncertainties
on
mechanism
of
by
SACs,
which
involves
complex
interplay
sulfate
hydroxyl
radicals,
singlet
oxygen,
high-valent
metal
species,
and/or
mediated
electron
transfer.
Questions
also
remain
how
ions
molecularly
align
single
site,
are
converted
into
reactive
what
design
parameters
lead
higher
efficiency
degradation.
this
critical
review,
we
examine
SAC
materials
employed
AOPs
discuss
they
function
differently
counterparts.
We
further
our
discussion
current
limitations,
opportunities,
future
research
needs
in
(i)
filling
knowledge
gaps
mechanisms
persulfate-SAC
interactions;
(ii)
augmenting
fundamental
with
theoretical
simulation
situ
characterization
techniques;
(iii)
improving
tailored
applications;
(iv)
proactively
considering
challenges
associated
engineering
practices
water
matrixes.
Environmental Science & Technology,
Journal Year:
2023,
Volume and Issue:
57(10), P. 4266 - 4275
Published: Feb. 27, 2023
Four-nitrogen-coordinated
transitional
metal
(MN4)
configurations
in
single-atom
catalysts
(SACs)
are
broadly
recognized
as
the
most
efficient
active
sites
peroxymonosulfate
(PMS)-based
advanced
oxidation
processes.
However,
SACs
with
a
coordination
number
higher
than
four
rarely
explored,
which
represents
fundamental
missed
opportunity
for
chemistry
to
boost
PMS
activation
and
degradation
of
recalcitrant
organic
pollutants.
We
experimentally
theoretically
demonstrate
here
that
five-nitrogen-coordinated
Mn
(MnN5)
more
effectively
activate
MnN4
sites,
by
facilitating
cleavage
O–O
bond
into
high-valent
Mn(IV)–oxo
species
nearly
100%
selectivity.
The
high
activity
MnN5
was
discerned
be
due
formation
higher-spin-state
N5Mn(IV)═O
species,
enable
two-electron
transfer
from
organics
through
lower-energy-barrier
pathway.
Overall,
this
work
demonstrates
importance
numbers
informs
design
next-generation
environmental
catalysts.
