Angewandte Chemie International Edition,
Год журнала:
2020,
Номер
59(31), С. 13057 - 13062
Опубликована: Апрель 28, 2020
Carbon-supported
NiII
single-atom
catalysts
with
a
tetradentate
Ni-N2
O2
coordination
formed
by
Schiff
base
ligand-mediated
pyrolysis
strategy
are
presented.
A
complex
of
the
ligand
(R,R)-(-)-N,N'-bis(3,5-di-tert-butylsalicylidene)-1,2-cyclohexanediamine
was
adsorbed
onto
carbon
black
support,
followed
modified
material
at
300
°C
in
Ar.
The
/C
catalyst
showed
excellent
performance
for
electrocatalytic
reduction
to
H2
through
two-electron
transfer
process
alkaline
conditions,
selectivity
96
%.
At
current
density
70
mA
cm-2
,
production
rate
5.9
mol
gcat.-1
h-1
achieved
using
three-phase
flow
cell,
good
stability
maintained
over
8
h
testing.
could
electrocatalytically
reduce
air
high
density,
still
affording
(>90
%).
precise
key
performance.
Chemical Reviews,
Год журнала:
2020,
Номер
120(21), С. 11900 - 11955
Опубликована: Апрель 3, 2020
Manipulating
metal
atoms
in
a
controllable
way
for
the
synthesis
of
materials
with
desired
structure
and
properties
is
holy
grail
chemical
synthesis.
The
recent
emergence
single
atomic
site
catalysts
(SASC)
demonstrates
that
we
are
moving
toward
this
goal.
Owing
to
maximum
efficiency
atom-utilization
unique
structures
properties,
SASC
have
attracted
extensive
research
attention
interest.
prerequisite
scientific
practical
applications
fabricate
highly
reactive
stable
on
appropriate
supports.
In
review,
various
synthetic
strategies
summarized
concrete
examples
highlighting
key
issues
methods
stabilize
supports
suppress
their
migration
agglomeration.
Next,
discuss
how
conditions
affect
catalytic
before
ending
review
by
prospects
challenges
as
well
further
researches
SASC.
Chemical Society Reviews,
Год журнала:
2021,
Номер
50(8), С. 5281 - 5322
Опубликована: Янв. 1, 2021
This
review
presents
the
recent
advances
in
synthetic
strategies,
characterisation,
and
computations
of
carbon-based
single-atom
catalysts,
as
well
their
innovative
applications
mechanisms
advanced
oxidation
technologies.
Chemical Society Reviews,
Год журнала:
2020,
Номер
49(7), С. 2215 - 2264
Опубликована: Янв. 1, 2020
This
review
summarized
the
fabrication
routes
and
characterization
methods
of
atomic
site
electrocatalysts
(ASCs)
followed
by
their
applications
for
water
splitting,
oxygen
reduction
selective
oxidation.
Journal of the American Chemical Society,
Год журнала:
2021,
Номер
143(20), С. 7819 - 7827
Опубликована: Май 13, 2021
Product
selectivity
in
multielectron
electrocatalytic
reactions
is
crucial
to
energy
conversion
efficiency
and
chemical
production.
However,
a
present
practical
drawback
the
limited
understanding
of
actual
catalytic
active
sites.
Here,
using
as
prototype
single-atom
catalysts
(SACs)
acidic
oxygen
reduction
reaction
(ORR),
we
report
structure–property
relationship
show
for
first
time
that
molecular-level
local
structure,
including
second
coordination
spheres
(CSs),
rather
than
individual
atoms,
synergistically
determines
response.
ORR
on
Co-SACs
can
be
tailored
from
four-electron
two-electron
pathway
by
modifying
(N
or/and
O
coordination)
(C–O–C
groups)
CSs.
Using
combined
theoretical
predictions
experiments,
X-ray
absorption
fine
structure
analyses
situ
infrared
spectroscopy,
confirm
unique
change
originates
structure-dependent
shift
sites
center
Co
atom
O-adjacent
C
atom.
We
this
optimizes
electronic
*OOH
adsorption
behavior
give
"best"
activity
>95%
H2O2
electrosynthesis.
Angewandte Chemie International Edition,
Год журнала:
2020,
Номер
60(9), С. 4448 - 4463
Опубликована: Апрель 21, 2020
Abstract
Single‐atom
catalysts
(SACs)
with
highly
active
sites
atomically
dispersed
on
substrates
exhibit
unique
advantages
regarding
maximum
atomic
efficiency,
abundant
chemical
structures,
and
extraordinary
catalytic
performances
for
multiple
important
reactions.
In
particular,
M–N–C
SACs
(M=transition
metal
atom)
demonstrate
optimal
electrocatalytic
activity
the
oxygen
reduction
reaction
(ORR)
have
attracted
extensive
attention
recently.
Despite
substantial
efforts
in
fabricating
various
SACs,
principles
regulating
intrinsic
of
their
not
been
sufficiently
studied.
this
Review,
we
summarize
regulation
strategies
promoting
ORR
by
modulation
center
atoms,
coordinated
environmental
guest
groups.
Theoretical
calculations
experimental
investigations
are
both
included
to
afford
a
comprehensive
understanding
structure–performance
relationship.
Finally,
future
directions
developing
advanced
other
analogous
reactions
proposed.
Angewandte Chemie International Edition,
Год журнала:
2020,
Номер
60(6), С. 3212 - 3221
Опубликована: Окт. 30, 2020
Demonstrated
here
is
the
correlation
between
atomic
configuration
induced
electronic
density
of
single-atom
Co
active
sites
and
oxygen
reduction
reaction
(ORR)
performance
by
combining
density-functional
theory
(DFT)
calculations
electrochemical
analysis.
Guided
DFT
calculations,
a
MOF-derived
catalyst
with
optimal
Co1
-N3
PS
moiety
incorporated
in
hollow
carbon
polyhedron
(Co1
PS/HC)
was
designed
synthesized.
PS/HC
exhibits
outstanding
alkaline
ORR
activity
half-wave
potential
0.920
V
superior
kinetics
record-level
kinetic
current
an
ultralow
Tafel
slope
31
mV
dec-1
,
exceeding
that
Pt/C
almost
all
non-precious
electrocatalysts.
In
acidic
media
still
surpasses
Pt/C.
This
work
offers
atomic-level
insight
into
relationship
site
catalytic
properties,
promoting
rational
design
efficient
catalysts.
Chemical Reviews,
Год журнала:
2020,
Номер
120(21), С. 12315 - 12341
Опубликована: Окт. 28, 2020
Research
on
heterogeneous
single-atom
catalysts
(SACs)
has
become
an
emerging
frontier
in
catalysis
science
because
of
their
advantages
high
utilization
noble
metals,
precisely
identified
active
sites,
selectivity,
and
tunable
activity.
Graphene,
as
a
one-atom-thick
two-dimensional
carbon
material
with
unique
structural
electronic
properties,
been
reported
to
be
superb
support
for
SACs.
Herein,
we
provide
overview
recent
progress
investigations
graphene-based
Among
the
large
number
publications,
will
selectively
focus
stability
metal
single-atoms
(SAs)
anchored
different
sites
graphene
catalytic
performances
SACs
chemical
reactions,
including
thermocatalysis
electrocatalysis.
We
summarize
fundamental
understandings
structures
intrinsic
connection
properties
SACs,
also
brief
perspective
future
design
efficient
graphene-like
materials.
Chemical Society Reviews,
Год журнала:
2020,
Номер
49(18), С. 6605 - 6631
Опубликована: Янв. 1, 2020
Recent
advances
in
the
design,
preparation,
and
applications
of
different
catalysts
for
electrochemical
photochemical
H2O2
production
are
summarized,
some
invigorating
perspectives
future
developments
also
provided.
