Advanced Energy Materials,
Год журнала:
2020,
Номер
10(32)
Опубликована: Июль 14, 2020
Abstract
Single
atom
catalysts
(SACs)
that
integrate
the
merits
of
homogeneous
and
heterogeneous
have
been
attracting
considerable
attention
in
recent
years.
The
individual
metal
atoms
SACs
can
be
stabilized
on
supports
through
various
unsaturated
chemical
sites
or
space
confinement
for
achieving
maximized
utilization
efficiency.
Aside
from
development
strategies
preparing
high
loading
purity
SACs,
another
key
challenge
this
field
is
precisely
manipulating
geometric
electronic
structure
catalytically
active
single
sites,
thus
rendering
exceptionally
reactive,
selective,
stabile
compared
to
their
bulk
counterparts.
This
review
summarizes
advancements
catalysis
perspective
local
structural
regulation
synergistic
coupling
effect
between
species
supports.
Special
emphasis
placed
elucidation
catalytic
structure‐performance
relationship
terms
coordination
environment,
valence
state
metal‐support
interactions
by
advanced
characterization
theoretical
studies.
Select
situ
operando
techniques
tracking
SACs’
evolution
under
realistic
conditions
are
highlighted.
Finally,
challenges
opportunities
discussed
offer
insight
into
rational
design
more
intriguing
with
activity
distinct
chemoselectivity.
Chemical Reviews,
Год журнала:
2020,
Номер
120(21), С. 12217 - 12314
Опубликована: Ноя. 2, 2020
Electrocatalysts
with
single
metal
atoms
as
active
sites
have
received
increasing
attention
owing
to
their
high
atomic
utilization
efficiency
and
exotic
catalytic
activity
selectivity.
This
review
aims
provide
a
comprehensive
summary
on
the
recent
development
of
such
single-atom
electrocatalysts
(SAECs)
for
various
energy-conversion
reactions.
The
discussion
starts
an
introduction
different
types
SAECs,
followed
by
overview
synthetic
methodologies
control
dispersion
atomically
resolved
characterization
using
state-of-the-art
microscopic
spectroscopic
techniques.
In
recognition
extensive
applications
electrocatalytic
studies
are
dissected
in
terms
important
electrochemical
reactions,
including
hydrogen
evolution
reaction
(HER),
oxygen
(OER),
reduction
(ORR),
carbon
dioxide
(CO2RR),
nitrogen
(NRR).
Examples
SAECs
deliberated
each
case
performance,
structure-property
relationships,
enhancement
mechanisms.
A
perspective
is
provided
at
end
section
about
remaining
challenges
opportunities
targeted
reaction.
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.
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.
Advanced Materials,
Год журнала:
2020,
Номер
32(42)
Опубликована: Сен. 16, 2020
The
development
of
oxygen
reduction
reaction
(ORR)
electrocatalysts
based
on
earth-abundant
nonprecious
materials
is
critically
important
for
sustainable
large-scale
applications
fuel
cells
and
metal-air
batteries.
Herein,
a
hetero-single-atom
(h-SA)
ORR
electrocatalyst
presented,
which
has
atomically
dispersed
Fe
Ni
coanchored
to
microsized
nitrogen-doped
graphitic
carbon
support
with
unique
trimodal-porous
structure
configured
by
highly
ordered
macropores
interconnected
through
mesopores.
Extended
X-ray
absorption
fine
spectra
confirm
that
Fe-
Ni-SAs
are
affixed
the
via
FeN4
NiN4
coordination
bonds.
resultant
Fe/Ni
h-SA
exhibits
an
outstanding
activity,
outperforming
SA
only
or
Ni-SAs,
benchmark
Pt/C.
obtained
experimental
results
indicate
achieved
performance
from
synergetic
enhancement
induced
coexisting
sites,
superior
mass-transfer
capability
promoted
trimodal-porous-structured
support.
Chemical Society Reviews,
Год журнала:
2021,
Номер
50(13), С. 7745 - 7778
Опубликована: Янв. 1, 2021
Bifunctional
oxygen
reduction
and
evolution
constitute
the
core
processes
for
sustainable
energy
storage.
The
advances
on
noble-metal-free
bifunctional
electrocatalysts
are
reviewed.
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.
Angewandte Chemie International Edition,
Год журнала:
2021,
Номер
60(14), С. 7607 - 7611
Опубликована: Янв. 15, 2021
Abstract
Single‐atom
catalysts
(SACs)
have
attracted
tremendous
interests
due
to
their
ultrahigh
activity
and
selectivity.
However,
the
rational
control
over
coordination
microenvironment
of
SACs
remains
a
grand
challenge.
Herein,
post‐synthetic
metal
substitution
(PSMS)
strategy
has
been
developed
fabricate
single‐atom
Ni
with
different
N
numbers
(denoted
Ni‐N
x
‐C)
on
pre‐designed
N‐doped
carbon
derived
from
metal‐organic
frameworks.
When
served
for
CO
2
electroreduction,
obtained
3
‐C
catalyst
achieves
Faradaic
efficiency
(FE)
up
95.6
%,
much
superior
that
4
‐C.
Theoretical
calculations
reveal
lower
number
in
can
significantly
enhance
COOH*
formation,
thereby
accelerating
reduction.
In
addition,
shows
excellent
performance
Zn–CO
battery
FE
stability.
This
work
opens
new
general
avenue
modulation
(MEM)
utilization.
Advanced Functional Materials,
Год журнала:
2020,
Номер
31(11)
Опубликована: Дек. 21, 2020
Abstract
Selective
nitrate‐to‐ammonia
electrochemical
conversion
is
an
efficient
pathway
to
solve
the
pollution
of
nitrate
and
attractive
strategy
for
low‐temperature
ammonia
synthesis.
However,
current
studies
electroreduction
(NO
3
RR)
mainly
focus
on
metal‐based
catalysts,
which
remains
challenging
because
poor
understanding
catalytic
mechanism.
Herein,
taking
single
transition
metal
atom
supported
graphitic
carbon
nitrides
(g‐CN)
as
example,
NO
RR
feasibility
single‐atom
catalysts
(SACs)
first
demonstrated
by
using
density
functional
theory
calculations.
The
results
reveal
that
highly
toward
NH
can
be
achieved
Ti/g‐CN
Zr/g‐CN
with
low
limiting
potentials
−0.39
−0.41
V,
respectively.
Furthermore,
considerable
energy
barriers
are
observed
during
formation
byproducts
2
,
NO,
N
O,
Zr/g‐CN,
guaranteeing
their
high
selectivity.
This
work
provides
a
new
route
application
SACs
paves
way
development
RR.
