Coordination Chemistry Reviews,
Год журнала:
2024,
Номер
514, С. 215900 - 215900
Опубликована: Май 8, 2024
Catalysis
stands
as
a
cornerstone
in
chemical
synthesis,
pivotal
advancing
sustainable
manufacturing
pathways.
The
evolution
from
energy-intensive
to
catalytic
processes
has
marked
transformative
shift,
notably
exemplified
by
low-energy
methods.
These
processes,
operating
under
milder
conditions
and
emphasizing
selectivity
recyclability,
represent
the
forefront
of
chemistry.
This
review
navigates
through
an
array
reactions,
highlighting
their
diverse
applications
culminating
exploration
recent
strides
within
processes.
For
example,
explores
uses
such
enzyme
mimicking,
biodiesel
production,
carbon
dioxide
capture,
organic
synthesis.
Additionally,
it
covers
enzymatic
catalysis
photocatalysis
for
transformations,
energy
applications,
water
treatment.
Notably,
emphasizes
capabilities
single-atom
(SAC)
diatomic
catalysts
(DACs),
recognizing
exceptional
performance
catalyzing
reactions
at
minimal
activation
energies
while
maintaining
high
efficiency
mild
conditions.
By
elucidating
modulation
electronic
structure
offering
microelectronic
perspective,
aims
elucidate
mechanisms
underlying
activity
SAC
DACs.
Emphasizing
interplay
between
coordination
chemistry
principles
efficacy,
elucidates
indispensable
role
complexes
fortifying
sustainability
these
spotlighting
fusion
with
catalysis,
this
underscore
collective
influence
shaping
landscape
production.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(40)
Опубликована: Авг. 15, 2022
The
light-driven
CO2
reduction
to
multi-carbon
products
is
especially
meaningful,
while
the
low
efficiency
of
multi-electron
transfer
and
sluggish
C-C
coupling
greatly
hinder
its
development.
Herein,
we
report
a
photocatalyst
comprising
P
Cu
dual
sites
anchored
on
graphitic
carbon
nitride
(P/Cu
SAs@CN),
which
achieves
high
C2
H6
evolution
rate
616.6
μmol
g-1
h-1
in
reducing
hydrocarbons.
detailed
spectroscopic
characterizations
identify
formation
charge-enriched
sites,
where
isolated
atoms
serve
as
hole
capture
during
photocatalysis.
Theoretical
simulations
combined
with
situ
FTIR
measurement
reveal
kinetically
feasible
process
for
intermediate
(*OC-COH)
confirm
favorable
production
P/Cu
SAs@CN
photocatalyst.
This
work
offers
new
insights
into
design
atomic
precision
toward
highly
efficient
photocatalytic
conversion
value-added
products.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(52)
Опубликована: Окт. 6, 2022
Abstract
The
simultaneous
presence
of
two
active
metal
centres
in
diatomic
catalysts
(DACs)
leads
to
the
occurrence
specific
interactions
between
sites.
Such
interactions,
referred
as
long‐range
(LRIs),
play
an
important
role
determining
rate
and
selectivity
a
reaction.
optimal
combination
must
be
determined
achieve
targeted
efficiency.
To
date,
various
types
DACs
have
been
synthesised
applied
electrochemistry.
However,
LRIs
not
systematically
summarised.
Herein,
regulation,
mechanism,
electrocatalytic
applications
are
comprehensively
summarised
discussed.
In
addition
basic
information
above,
challenges,
opportunities,
future
development
proposed
order
present
overall
view
reference
for
research.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(15)
Опубликована: Фев. 18, 2023
Herein,
we
successfully
construct
bifunctional
electrocatalysts
by
synthesizing
atomically
dispersed
Fe-Se
atom
pairs
supported
on
N-doped
carbon
(Fe-Se/NC).
The
obtained
Fe-Se/NC
shows
a
noteworthy
oxygen
catalytic
performance
with
low
potential
difference
of
0.698
V,
far
superior
to
that
reported
Fe-based
single-atom
catalysts.
theoretical
calculations
reveal
p-d
orbital
hybridization
around
the
leads
remarkably
asymmetrical
polarized
charge
distributions.
based
solid-state
rechargeable
Zn-air
batteries
(ZABs-Fe-Se/NC)
present
stable
charge/discharge
200
h
(1090
cycles)
at
20
mA
cm-2
25
°C,
which
is
6.9
times
ZABs-Pt/C+Ir/C.
At
extremely
temperature
-40
ZABs-Fe-Se/NC
displays
an
ultra-robust
cycling
741
(4041
1
,
about
11.7
More
importantly,
could
be
operated
for
133
(725
even
5
°C.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(22)
Опубликована: Март 24, 2023
Nickel-based
catalysts
have
been
regarded
as
one
of
the
most
promising
electrocatalysts
for
urea
oxidation
reaction
(UOR),
however,
their
activity
is
largely
limited
by
inevitable
self-oxidation
Ni
species
(NSOR)
during
UOR.
Here,
we
proposed
an
interface
chemistry
modulation
strategy
to
trigger
occurrence
UOR
before
NSOR
via
constructing
a
2D/2D
heterostructure
that
consists
ultrathin
NiO
anchored
Ru-Co
dual-atom
support
(Ru-Co
DAS/NiO).
Operando
spectroscopic
characterizations
confirm
this
unique
triggering
mechanism
on
surface
DAS/NiO.
Consequently,
fabricated
catalyst
exhibits
outstanding
with
low
potential
1.288
V
at
10
mA
cm-2
and
remarkable
long-term
durability
more
than
330
h
operation.
DFT
calculations
demonstrate
favorable
electronic
structure
induced
heterointerface
endows
energetically
NSOR.
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
144(42), С. 19619 - 19626
Опубликована: Окт. 12, 2022
Ruthenium-based
materials
are
considered
great
promising
candidates
to
replace
Pt-based
catalysts
for
hydrogen
production
in
alkaline
conditions.
Herein,
we
adopt
a
facile
method
rationally
design
neoteric
Schottky
catalyst
which
uniform
ultrafine
ruthenium
nanoparticles
featuring
lattice
compressive
stress
supported
on
nitrogen-modified
carbon
nanosheets
(Ru
NPs/NC)
efficient
evolution
reaction
(HER).
Lattice
strain
and
junction
dual
regulation
ensures
that
the
Ru
NPs/NC
with
an
appropriate
nitrogen
content
displays
superb
H2
media.
Particularly,
NPs/NC-900
1.3%
attractive
activity
durability
HER
low
overpotential
of
19
mV
at
10
mA
cm-2
1.0
M
KOH
electrolyte.
The
situ
X-ray
absorption
fine
structure
measurements
indicate
low-valence
nanoparticle
shrinking
Ru-Ru
bond
acts
as
catalytic
active
site
during
process.
Furthermore,
multiple
spectroscopy
analysis
density
functional
theory
calculations
demonstrate
tunes
electron
adsorption
center,
thus
enhancing
activity.
This
strategy
provides
novel
concept
advanced
electrocatalysts
production.
Advanced Materials,
Год журнала:
2023,
Номер
35(31)
Опубликована: Фев. 23, 2023
Single/dual-metal
atoms
supported
on
carbon
matrix
can
be
modulated
by
coordination
structure
and
neighboring
active
sites.
Precisely
designing
the
geometric
electronic
uncovering
structure-property
relationships
of
single/dual-metal
confront
with
grand
challenges.
Herein,
this
review
summarizes
latest
progress
in
microenvironment
engineering
single/dual-atom
sites
via
a
comprehensive
comparison
single-atom
catalyst
(SACs)
dual-atom
catalysts
(DACs)
term
design
principles,
modulation
strategy,
theoretical
understanding
structure-performance
correlations.
Subsequently,
recent
advances
several
typical
electrocatalysis
process
are
discussed
to
get
general
reaction
mechanisms
finely-tuned
SACs
DACs.
Finally,
full-scaled
summaries
challenges
prospects
given
for
This
will
provide
new
inspiration
development
atomically
dispersed
electrocatalytic
application.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(34)
Опубликована: Июнь 18, 2022
Single-atom
active-site
catalysts
have
attracted
significant
attention
in
the
field
of
photocatalytic
CO2
conversion.
However,
designing
active
sites
for
reduction
and
H2
O
oxidation
simultaneously
on
a
photocatalyst
combining
corresponding
half-reaction
system
is
still
difficult.
Here,
we
synthesized
bimetallic
single-atom
with
two
compatible
centers
Mn
Co
carbon
nitride
(Mn1
Co1
/CN).
Our
experimental
results
density
functional
theory
calculations
showed
that
center
promotes
by
accumulating
photogenerated
holes.
In
addition,
activation
increasing
bond
length
angle
molecules.
Benefiting
from
synergistic
effect
atomic
centers,
Mn1
/CN
exhibited
CO
production
rate
47
μmol
g-1
h-1
,
which
significantly
higher
than
single-metal
photocatalyst.
Advanced Functional Materials,
Год журнала:
2022,
Номер
33(4)
Опубликована: Ноя. 13, 2022
Abstract
The
modulation
effect
manifests
an
encouraging
potential
to
enhance
the
performance
of
single‐atom
catalysts;
however,
in‐depth
study
about
this
for
isolated
diatomic
sites
(DASs)
remains
a
great
challenge.
Herein,
proximity
electronic
(PEE)
Ni/Co
DASs
is
proposed
that
anchored
in
N‐doped
carbon
(N‐C)
substrate
(NiCo
DASs/N‐C)
synergistic
promoting
electrocatalytic
oxygen
reduction
reaction
(ORR)
and
hydrogen
evolution
(HER).
Benefiting
from
PEE
adjacent
Ni
by
four
nitrogen
(Ni‐N
4
)
moiety,
NiCo
DASs/N‐C
catalyst
exhibits
superior
ORR
HER
activity.
In
situ
characterization
results
suggest
Co
(Co‐N
as
main
active
site
O
2
adsorption‐activation
process,
which
promotes
formation
key
*OOH
desorption
*OH
intermediate
accelerate
multielectron
kinetics.
Theoretical
calculation
reveals
Ni‐N
modulator
can
effectively
adjust
localization
Co‐N
site,
*H
adsorption
on
thereby
boosting
process
significantly.
This
opens
new
opportunity
rationally
regulating
catalytic
centers
well
provides
guidance
designing
high‐efficiency
bifunctional
electrocatalysts
promising
applications.