Nano Letters,
Год журнала:
2024,
Номер
24(45), С. 14363 - 14372
Опубликована: Ноя. 1, 2024
Deeply
understanding
how
local
microstrain
environment
around
diatomic
sites
influences
their
electronic
state
and
adsorption
is
crucial
for
improving
electrochemical
CO2
reduction
(eCO2R)
reaction;
however,
precise
engineering
of
the
atomic
challenging.
Herein,
we
fabricate
Ag-CdTMT
electrocatalysts
with
AgN2S2–CdN2S2
by
anchoring
Ag
to
nodes
CdTMT
(TMT
=
2,4,6-trimercaptotriazine
anion)
coordination
polymers.
The
catalysts
achieve
approximately
100%
Faradaic
efficiency
CO
an
industrial
level
current
density
(∼200
mA
cm–2
in
H-cell).
embedded
atoms
induce
formation
Ag–Cd
microstrain,
stretching
Cd–N/S
bonds,
reinforcing
electron
localization
at
Cd
sites.
adjacent
synergistically
reduced
4d–C
2p
antibonding
orbital
occupancy
intensifying
*COOH
as
rate-determining
step.
This
study
provides
novel
insights
into
customizing
structure
through
strain
engineering.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Апрель 22, 2024
Abstract
Electroreduction
of
CO
2
into
high‐value
chemicals
and
fuels
driven
is
an
effective
way
to
alleviate
the
environmental
crisis,
but
it
suffers
from
poor
activity
low
selectivity
catalyst.
Single‐atom
catalysts
have
excellent
highest
atomic
efficiency,
are
widely
used
in
2‐electron
transfer
produce
CO.
However,
electroreduction
C
2+
products
involves
complex
processes
such
as
multi‐electron
reaction
competitive
adsorption,
so
single‐atom
catalysis
often
powerless.
Herein,
a
Ga‐anchored
F‐doped
Cu
O
catalyst
with
dual
active
sites
reported.
The
Lewis
acid‐base
pairs
Ga
single
atom
promote
adsorption/activation
dissociation
water
molecules,
respectively,
enhance
coverage
*CO
*H,
their
synergy
optimizes
path.
At
high
current
density
600
mA
cm
−2
,
FE
C2+
reached
72.8
±
3.2%
remarkable
stability.
Experiments
theory
calculations
demonstrate
that
increase
key
intermediate
transformed
*CHO
through
protonation
reaction,
which
changes
path
C─C
coupling
(*OCCO)
followed
by
(*OCCHO)
energy
barrier,
greatly
improving
for
products.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 18, 2024
Abstract
Aqueous
zinc‐selenium
(Zn‐Se)
batteries
have
garnered
much
attention
due
to
their
inherent
safety
and
high
specific
capacity.
Unfortunately,
the
problem
of
sluggish
redox
reaction
represents
a
significant
obstacle
development
aqueous
Zn‐Se
batteries.
Here,
nitrogen‐phosphorus
asymmetrically
coordinated
copper
single
atom
catalytic
host
material
(CuN
3
P
1
@C)
is
synthesized
for
an
battery.
The
CuN
@C
exhibits
rich
porous
structure,
high‐loading
Cu
atoms,
unique
asymmetric
coordination
environment,
which
significantly
reduces
energy
barrier
between
Se
Zn,
enhancing
electrochemical
performance
Consequently,
Se/CuN
cathode
achieves
capacity
756
mAh
g
−1
at
0.2
A
cycling
stability
4
000
cycles
5.0
(capacity
decay
0.0044%
per
cycle).
Meanwhile,
conversion
mechanism
battery
systematically
explored
via
systematical
characteristics
density
functional
theory
calculations.
This
work
opens
up
novel
approach
boosting
by
modulating
atom‐based
materials
heteroatoms.
Growing
global
population,
escalating
energy
consumption,
and
climate
change
threaten
future
security.
Fossil
fuel
combustion,
primarily
coal,
oil,
natural
gas,
exacerbates
the
greenhouse
effect
driving
warming
through
CO
npj Materials Sustainability,
Год журнала:
2025,
Номер
3(1)
Опубликована: Янв. 7, 2025
Abstract
Advanced
Oxidation
Processes
(AOPs)
are
promising
for
treating
persistent
pollutants,
yet
challenges
arise
due
to
the
step-wise
oxidants
activation
process,
which
traditional
single-active-center
catalysts
struggle
facilitate
effectively.
Recently,
dual-active-center
have
emerged
as
a
solution
by
enabling
synergistic
reactions.
This
review
covers
advances
in
these
catalysts,
their
co-catalytic
mechanisms,
and
applications
electro-Fenton,
photocatalytic,
peroxymonosulfate-,
pollutant-as-electron-donor
based
Fenton-like
processes,
along
with
active
site
design
considerations
future
challenges.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 5, 2025
Multi-proton-coupled
electron
transfer,
multitudinous
intermediates,
and
unavoidable
competing
hydrogen
evolution
reaction
during
CO2
electroreduction
make
it
tricky
to
control
high
selectivity
for
specific
products.
Here,
we
present
spatial
confinement
of
Fe
single
atoms
(FeN2S2)
by
adjacent
FeS
clusters
(Fe4S4)
orientate
the
transition
adsorption
configuration
from
C,O-side
O-end,
which
triggers
a
shift
activated
first-step
protonation
C–C
coupling,
thus
switching
target
product
HCOOH
in
Faraday
efficiency
(FE:
90.6%)
on
FeN2S2
CH3COOH
82.3%)
Fe4S4/FeN2S2.
The
strength
*OCHO
upon
solitary
site
is
linearly
related
coordination
number
Fe–S,
with
predominantly
produced
over
single-atom
(ortho-substituted
S
atoms).
Fe4S4
cluster
functions
as
switch
reduction
product,
can
not
only
optimize
electronic
structure
neighboring
but
also
impel
complete
hydrocarbon
intermediate
*CH3,
followed
coupling
CO2*
*CH3
via
synergistic
catalysis
This
strategy
provides
new
avenue
modulate
reactant
model
desirable
pathways,
potential
applications
diverse
multistep
electrochemical
processes
controlled
selectivity.
Chemical Society Reviews,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 1, 2025
This
review
examines
the
strategies
of
symmetry
breaking
(charge/coordination/geometric)
in
single-atom
catalysts
to
regulate
active
site
electronic
structures,
greatly
enhancing
catalytic
performance.
We
have
designed
a
catalyst
that
can
efficiently
convert
CO
2
into
through
Zn–CO
batteries
and
the
electrochemical
RR,
addressing
both
energy
conversion
environmental
concerns
simultaneously.
Chemical Reviews,
Год журнала:
2024,
Номер
124(20), С. 11348 - 11434
Опубликована: Окт. 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.
ACS Nano,
Год журнала:
2024,
Номер
18(27), С. 17774 - 17785
Опубликована: Июнь 28, 2024
Lithium–sulfur
(Li–S)
batteries
are
promising
for
next-generation
high-energy
energy
storage
systems.
However,
the
slow
reaction
kinetics
render
mobile
polysulfides
hardly
controlled,
yielding
shuttling
effects
and
eventually
damaging
Li
metal
anodes.
To
improve
cyclability
of
Li–S
batteries,
high-efficiency
catalysts
desired
to
accelerate
polysulfide
conversion
suppress
effect.
Herein,
we
studied
a
doping
system
with
Ni2P
Ni2B
as
end
members
found
B-doped
catalyst
that
demonstrates
high
activity
batteries.
As
anionic
dopants,
B
an
interesting
reverse
electron
transfer
P
tunes
electronic
structure
dramatically.
The
resultant
exhibits
short
Ni–B
bonds
strong
Ni–S
interaction,
donation
further
enhances
adsorption
on
catalysts.
S–S
were
activated
appropriately,
therefore
decreasing
low
barrier
reactions.
