Chemical Reviews,
Journal Year:
2024,
Volume and Issue:
124(20), P. 11348 - 11434
Published: Oct. 9, 2024
Environmental
catalysis
has
emerged
as
a
scientific
frontier
in
mitigating
water
pollution
and
advancing
circular
chemistry
reaction
microenvironment
significantly
influences
the
catalytic
performance
efficiency.
This
review
delves
into
engineering
within
liquid-phase
environmental
catalysis,
categorizing
microenvironments
four
scales:
atom/molecule-level
modulation,
nano/microscale-confined
structures,
interface
surface
regulation,
external
field
effects.
Each
category
is
analyzed
for
its
unique
characteristics
merits,
emphasizing
potential
to
enhance
efficiency
selectivity.
Following
this
overview,
we
introduced
recent
advancements
advanced
material
system
design
promote
(e.g.,
purification,
transformation
value-added
products,
green
synthesis),
leveraging
state-of-the-art
technologies.
These
discussions
showcase
was
applied
different
reactions
fine-tune
regimes
improve
from
both
thermodynamics
kinetics
perspectives.
Lastly,
discussed
challenges
future
directions
engineering.
underscores
of
intelligent
materials
drive
development
more
effective
sustainable
solutions
decontamination.
Carbon Energy,
Journal Year:
2024,
Volume and Issue:
6(8)
Published: Feb. 15, 2024
Abstract
Metal–N–C
single‐atom
catalysts,
mostly
prepared
from
pyrolysis
of
metal‐organic
precursors,
are
widely
used
in
heterogeneous
electrocatalysis.
Since
metal
sites
with
diverse
local
structures
coexist
this
type
material
and
it
is
challenging
to
characterize
the
structure,
a
reliable
structure–property
relationship
difficult
establish.
Conjugated
macrocyclic
complexes
adsorbed
on
carbon
support
well‐defined
models
mimic
catalysts.
Metal–N
4
site
four
electroneutral
pyridine‐type
ligands
embedded
graphene
layer
most
commonly
proposed
structure
active
but
its
molecular
counterpart
has
not
been
reported.
In
work,
we
synthesized
conjugated
center
(Co,
Fe,
or
Ni)
coordinated
pyridinic
as
model
catalysts
for
CO
2
electroreduction.
For
comparison,
anionic
quadri‐pyridine
ligand
were
also
prepared.
The
Co
complex
expressed
turnover
frequency
formation
more
than
an
order
magnitude
higher
that
ligand.
Constrained
ab
initio
dynamics
simulations
based
indicate
possesses
stronger
ability
mediate
electron
transfer
.
Advanced Energy Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 10, 2025
Abstract
Enhancing
the
selectivity
of
C
2
products
and
revealing
reaction
mechanisms
in
CO
electroreduction
(CO
RR)
remain
challenging.
Regulating
interphases
catalysts
is
one
most
promising
pathways.
Herein,
between
copper
(Cu)
tin
(Sn)
oxides
are
regulated
by
controlling
degree
reduction
during
self‐assembly
process,
which
exhibits
obvious
different
to
ethylene
ethanol,
respectively.
The
interphase
Cu‐SnO
ethanol
as
high
74.6%,
while
Cu
O‐SnO
shows
71.4%
at
–0.6
V
versus
RHE.
In
situ
Fourier‐transform
infrared
spectroscopy
measurements
density
functional
theory
calculations
demonstrate
that
strong
electron
interaction,
preferentially
forming
key
*COH
intermediates
for
asymmetrical
C─C
coupling
produce
ethanol.
contrast,
possesses
oxygen
vacancies
both
sites,
thus
enriching
*CO
symmetrical
interphase.
findings
this
work
offer
an
advanced
strategy
regulating
adjust
RR.
Nature Communications,
Journal Year:
2025,
Volume and Issue:
16(1)
Published: Feb. 15, 2025
Abstract
Breaking
the
geometric
symmetry
of
traditional
metal-N
4
sites
and
further
boosting
catalytic
activity
are
significant
but
challenging.
Herein,
planar
chlorination
engineering
is
proposed
for
successfully
converting
Zn-N
site
with
low
selectivity
CO
2
reduction
reaction
(CO
RR)
into
highly
active
3
broken
symmetry.
The
optimal
catalyst
Zn-SA/CNCl-1000
displays
a
highest
faradaic
efficiency
(FE
)
around
97
±
3%
good
stability
during
50
h
test
at
high
current
density
200
mA/cm
in
zero-gap
membrane
electrode
assembly
(MEA)
electrolyzer,
promising
application
industrial
catalysis.
At
-0.93
V
vs.
RHE,
partial
(
J
turnover
frequency
(TOF)
value
catalyzed
by
271.7
1.4
29325
151
-1
,
as
29
times
83
those
Zn-SA/CN-1000
without
engineering.
in-situ
extended
X-ray
absorption
fine
structure
(EXAFS)
measurements
functional
theory
(DFT)
calculation
reveal
adjacent
C-Cl
bond
induces
self-reconstruction
symmetry,
strengthening
adsorption
*
COOH
intermediate,
thus
remarkably
improving
RR
activity.
