ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(21), P. 16434 - 16458
Published: Oct. 23, 2024
Thermo-catalytic
CO2
hydrogenation
to
high-value
oxygenates
has
been
regarded
as
one
of
the
most
powerful
strategies
that
can
potentially
alleviate
excessive
emissions.
However,
due
high
chemical
stability
and
variability
pathways,
it
is
still
challenging
achieve
highly
active
selective
hydrogenation.
Single
atom
catalysts
(SACs)
with
ultrahigh
metal
utilization
efficiency
extraordinary
electronic
features
have
displayed
growing
importance
for
thermo-catalytic
multiple
developed
improve
performances.
Here,
we
review
breakthroughs
in
developing
SACs
efficient
toward
common
(CO,
HCOOH,
CH3OH,
CH3CH2OH)
following
order:
first,
an
analysis
reaction
mechanisms
thermodynamics
challenges
reactions;
second,
a
summary
SAs
designed
by
dividing
them
into
two
categories
single-
dual-sites;
third,
discussion
support
effects
focus
on
approaches
regulating
strong
metal–support
interaction
(MSI).
Summarily,
current
future
perspectives
develop
higher-performance
are
presented.
We
expect
this
bring
more
design
inspiration
trigger
innovation
catalytic
evolution
materials
eventually
benefit
achievement
carbon-neutrality
goal.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: June 11, 2024
Abstract
2D
MoS
2
is
acknowledged
as
a
potential
alternative
to
Pt‐based
catalysts
for
hydrogen
evolution
reaction
(HER)
due
its
suitable
*
H
adsorption
energy.
However,
the
weak
water
capacity
of
in
an
alkaline
solution
limits
performance
improvement
toward
HER.
Herein,
novel
rare‐earth
Tm
single
atoms
decorated
(Tm
SAs‐MoS
)
catalyst
proposed,
and
key
role
SAs
on
enhanced
HER
identified.
It
verified
that
Tm‐site
contributes
asymmetric
[Mo‐S‐Tm]
unit
site,
which
serves
electron
donor
disturb
electronic
state
accelerate
accumulation
at
surrounding
Mo‐S
site.
The
obtained
exhibits
significantly
improved
activity
with
low
overpotential
80
mV
10
mA
cm
−2
,
robust
stability
good
selectivity
compared
pure
most
‐based
catalysts.
In
situ
Raman
theoretical
calculations
prove
oxophilic
sites
improves
migration
thermodynamic
spontaneous
dissociation
interfacial
O
molecules
during
by
Tm‐4f‐OH
orbital
overlap.
Such
[Tm‐S‐Mo]
site
allows
optimal
G
*H
location
turn
reaches
apex
volcano
plot.
This
work
expected
open
up
new
avenues
design
provide
valuable
understanding
rare
earth
mechanisms.
Inorganic Chemistry Frontiers,
Journal Year:
2024,
Volume and Issue:
11(17), P. 5508 - 5516
Published: Jan. 1, 2024
Ultrafast
quasi-solid
microwave
(60
s)
is
employed
to
achieve
phosphorus-doped
black
TiO
2
supported
Ru
and
Pt
(Ru–Pt/P–TiO
2−
x
)
for
the
HER
with
an
overpotential
of
14
mV
at
10
mA
cm
−2
in
acidic
electrolyte.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(45)
Published: May 28, 2024
Abstract
The
past
decades
have
seen
considerable
imbalances
in
the
nitrogen
cycle
due
to
excessive
use
of
nitrate
agriculture
and
industry.
Electrocatalytic
reduction
(NO
3
RR)
(N
2
)
holds
significant
potential
for
addressing
pollution
wastewater
but
suffers
from
nitrite
formation
sluggish
hydrogeneration
process.
Here
a
single
atom
alloy
(SAA)
catalyst
featuring
atomically
dispersed
Ru
on
2D
Ni
metal
(Ru
1
Ni),
proving
remarkable
performance
−
–N
conversion
(≈93%)
N
selectivity
(≈99%))
through
co‐catalytic
metal‐support
interactions
(CMSI)
effect
is
reported.
Significantly,
SAA
achieves
NO
RR
removal
capacity
as
high
11.1
mg
L
−1
h
cm
−2
with
20
cycles
stability
(9
per
cycle),
surpassing
most
previously
reported
works.
core
boosting
lies
synergistically
promoted
activation
accelerated
hydrogenation
oxide
intermediates
site
substrate,
respectively,
revealed
by
various
situ
experiments
theoretical
simulations.
DFT
calculations
indicate
electron
transfer
substrate
more
robust
interaction
between
Ru–Ni
comparison
that
Ni–Ni.
This
work
offers
resilient
methodology
rational
design
highly
efficient
electrocatalysts
CMSI
modulation
RR,
illuminating
arena
treatment
cycle.
npj Materials Sustainability,
Journal Year:
2025,
Volume and Issue:
3(1)
Published: Jan. 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.
Advanced Science,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 7, 2025
Abstract
Overall
water
splitting
(OWS)
to
produce
hydrogen
has
attracted
large
attention
in
recent
years
due
its
ecological‐friendliness
and
sustainability.
However,
the
efficiency
of
OWS
been
forced
by
sluggish
kinetics
four‐electron
oxygen
evolution
reaction
(OER).
The
replacement
OER
alternative
electrooxidation
small
molecules
with
more
thermodynamically
favorable
potentials
may
fundamentally
break
limitation
achieve
production
low
energy
consumption,
which
also
be
accompanied
value‐added
chemicals
than
or
electrochemical
degradation
pollutants.
This
review
critically
assesses
latest
discoveries
coupled
various
OWS,
including
alcohols,
aldehydes,
amides,
urea,
hydrazine,
etc.
Emphasis
is
placed
on
corresponding
electrocatalyst
design
related
mechanisms
(e.g.,
dual
hydrogenation
N–N
bond
breaking
hydrazine
C═N
regulation
urea
inhibit
hazardous
NCO
−
NO
productions,
etc.),
along
emerging
reactions
(electrooxidation
tetrazoles,
furazans,
iodide,
quinolines,
ascorbic
acid,
sterol,
trimethylamine,
etc.).
Some
new
decoupled
electrolysis
self‐powered
systems
are
discussed
detail.
Finally,
potential
challenges
prospects
highlighted
aid
future
research
directions.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Aug. 23, 2024
Abstract
Inefficient
active
site
utilization
of
oxygen
evolution
reaction
(OER)
catalysts
have
limited
the
energy
efficiency
proton
exchange
membrane
(PEM)
water
electrolysis.
Here,
an
atomic
grid
structure
is
demonstrated
composed
high‐density
Ir
sites
(≈10
atoms
per
nm
2
)
on
reactive
MnO
2–x
support
which
mediates
coverage‐enhanced
OER
process.
Experimental
characterizations
verify
low‐valent
Mn
species
with
decreased
coordination
in
exert
a
pivotal
impact
enriched
coverage
surface
during
process,
and
distributed
grids,
where
highly
electrophilic
Ir─O
(II‐δ)−
bonds
proceed
rapidly,
render
intense
nucleophilic
attack
radicals.
Thereby,
this
metal‐support
cooperation
achieves
ultra‐low
overpotentials
166
mV
at
10
mA
cm
−2
283
500
,
together
striking
mass
activity
380
times
higher
than
commercial
IrO
1.53
V.
Moreover,
its
high
performance
also
markedly
surpasses
black
catalyst
PEM
electrolyzers
long‐term
stability.
