Advanced Functional Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 28, 2025
Abstract
Precise
manipulation
of
coordination
structure
single‐atom
sites
and
establishment
schematic
microenvironment‐oxidation
pathway
relations
remain
significant
challenges
in
Fenton‐like
chemistry.
Herein,
incorporating
sulfur
heteroatoms
into
the
higher
shell
FeN
4
(Fe‐NSC)
exhibited
a
volcano
trend
p
‐hydroxybenzoic
acid
oxidation,
aligning
with
number
positions
dopant.
Specifically,
S
moderate
electronegativity
larger
atomic
radii
triggers
long‐range
electronic
interactions,
which
provoke
Fe
3d
orbital
splitting
spin
electron
rearrangement,
resulting
crossover
states
d
xy
2
yz
1
xz
z
21
.
As
result,
partial
filling
e
g
t
orbitals
σ/π
antibonding
between
2p
optimized
adsorption–desorption
behaviors
key
oxygenated
intermediates
from
peroxymonosulfate
activation.
Thus,
optimal
binding
configuration
weakens
Fe─O
bonding
accelerates
PMS
dissociation
to
yield
C‐S‐N
Fe‐O*,
subsequently
couples
form
O
nearly
100%
selectivity.
The
Fe‐NSC‐functionalized
membrane
outstanding
long‐term
reusability
continuous
flow
reactor
further
validated
practical
application
perspective.
This
study
provides
insight
at
both
levels
for
rational
design
spin‐polarized
catalysts
its
functions
fine‐tuning
oxidation
pathways
environmental
catalysis.
Environmental Science & Technology,
Journal Year:
2024,
Volume and Issue:
58(27), P. 12155 - 12166
Published: June 27, 2024
The
rising
in
situ
chemical
oxidation
(ISCO)
technologies
based
on
polymerization
reactions
have
advanced
the
removal
of
emerging
contaminants
aquatic
environment.
However,
despite
their
promise,
uncertainties
persist
regarding
effectiveness
eliminating
structurally
complex
contaminants,
such
as
sulfonamide
antibiotics
(SAs).
This
study
elucidated
that
oligomerization,
rather
than
mineralization,
predominantly
governs
SAs
carbon
materials/periodate
system.
amine
groups
played
a
crucial
role
forming
organic
radicals
and
subsequent
coupling
due
to
high
f–
index
low
bond
orders.
Moreover,
highlighted
robust
adhesion
oligomers
catalyst
surface,
facilitated
by
enhanced
van
der
Waals
forces
hydrophobic
interactions.
Importantly,
plant
animal
toxicity
assessments
confirmed
nontoxic
nature
deposited
material
affirming
efficacy
material-based
ISCO
treating
contaminated
surface
water
groundwater.
Additionally,
novel
classification
approach,
Δlog
k,
was
proposed
differentiate
kinetic
control
steps,
providing
deeper
insights
into
quantitative
structure–activity
relationship
(QSAR)
facilitating
selection
optimal
descriptors
during
oligomerization
processes.
Overall,
these
significantly
enhance
our
understanding
via
demonstrate
superiority
C-ISCO
decontamination.
Environmental Science & Technology,
Journal Year:
2024,
Volume and Issue:
58(42), P. 18496 - 18507
Published: Oct. 9, 2024
Advanced
oxidation
processes
(AOPs)
are
rapidly
evolving
but
still
lack
well-established
protocols
for
reliably
identifying
oxidative
reactive
species
(ORSs).
This
Perspective
presents
both
the
radical
and
nonradical
ORSs
that
have
been
identified
or
proposed,
along
with
extensive
controversies
surrounding
mechanisms.
Conventional
identification
tools,
such
as
quenchers,
probes,
spin
trappers,
might
be
inadequate
analytical
demands
of
systems
in
which
multiple
coexist,
often
yielding
misleading
results.
Therefore,
challenges
these
complex,
short-lived,
transient
must
fully
acknowledged.
Refining
methods
is
necessary,
supported
by
rigorous
experiments
innovative
paradigms,
particularly
through
kinetic
analysis
based
on
situ
spectroscopic
techniques
multiple-probe
strategies.
To
demystify
complex
ORSs,
future
efforts
should
made
to
develop
advanced
tools
strategies
enhance
mechanism
understanding.
In
addition,
integrating
real-world
conditions
into
experimental
designs
will
establish
a
reliable
framework
fundamental
studies,
providing
more
accurate
insights
effectively
guiding
design
AOPs.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Nov. 15, 2024
The
regulation
of
peroxymonosulfate
(PMS)
activation
by
photo-assisted
heterogeneous
catalysis
is
under
in-depth
investigation
with
potential
as
a
replaceable
advanced
oxidation
process
in
water
purification,
yet
it
remains
significant
challenge.
Herein,
we
demonstrate
strategy
to
construct
polyethylene
glycol
(PEG)
well-coupled
dual-defect
V
Trifluoroacetic
acid
(TFA)
is
a
ubiquitous
environmental
contaminant;
however,
its
sources
are
poorly
constrained.
One
understudied
source
from
the
photochemical
reactions
of
aromatic
compounds
containing
-CF
