ACS Nano,
Год журнала:
2021,
Номер
15(3), С. 4927 - 4936
Опубликована: Фев. 22, 2021
Single
atom
catalysts
possess
attractive
electrocatalytic
activities
for
various
chemical
reactions
owing
to
their
favorable
geometric
and
electronic
structures
compared
the
bulk
counterparts.
Herein,
we
demonstrate
an
efficient
approach
producing
single
copper
immobilized
MXene
CO2
reduction
methanol
via
selective
etching
of
hybrid
A
layers
(Al
Cu)
in
quaternary
MAX
phases
(Ti3(Al1–xCux)C2)
due
different
saturated
vapor
pressures
Al-
Cu-containing
products.
After
Al
layers,
Cu
atoms
are
well-preserved
simultaneously
onto
resultant
with
dominant
surface
functional
group
(Clx)
on
outmost
Ti
(denoted
as
Ti3C2Clx)
Cu–O
bonds.
Consequently,
as-prepared
catalyst
exhibits
a
high
Faradaic
efficiency
value
59.1%
produce
CH3OH
shows
good
stability.
On
basis
synchrotron-based
X-ray
absorption
spectroscopy
analysis
density
theory
calculations,
unsaturated
structure
(Cuδ+,
0
<
δ
2)
delivers
low
energy
barrier
rate-determining
step
(conversion
HCOOH*
absorbed
CHO*
intermediate),
which
is
responsible
CH3OH.
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 Reviews,
Год журнала:
2020,
Номер
120(21), С. 12089 - 12174
Опубликована: Май 1, 2020
Metal-organic
frameworks
(MOFs)
are
a
class
of
distinctive
porous
crystalline
materials
constructed
by
metal
ions/clusters
and
organic
linkers.
Owing
to
their
structural
diversity,
functional
adjustability,
high
surface
area,
different
types
MOF-based
single
sites
well
exploited,
including
coordinately
unsaturated
from
nodes
metallolinkers,
as
active
species
immobilized
MOFs.
Furthermore,
controllable
thermal
transformation
MOFs
can
upgrade
them
nanomaterials
functionalized
with
single-atom
catalysts
(SACs).
These
unique
features
derivatives
enable
serve
highly
versatile
platform
for
catalysis,
which
has
actually
been
becoming
rapidly
developing
interdisciplinary
research
area.
In
this
review,
we
overview
the
recent
developments
catalysis
at
in
emphasis
on
structures
applications
thermocatalysis,
electrocatalysis,
photocatalysis.
We
also
compare
results
summarize
major
insights
gained
works
providing
challenges
prospects
emerging
field.
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.
Advanced Functional Materials,
Год журнала:
2020,
Номер
30(31)
Опубликована: Июнь 9, 2020
Abstract
The
recent
advances
in
electrocatalysis
for
oxygen
reduction
reaction
(ORR),
evolution
(OER),
hydrogen
(HER),
oxidation
(HOR),
carbon
dioxide
(CO
2
RR),
and
nitrogen
(NRR)
are
thoroughly
reviewed.
This
comprehensive
review
focuses
on
the
single‐atom
catalysts
(SACs)
including
Sc,
Cr,
Mn,
Fe,
Co,
Ni,
Cu,
Zn,
Mo,
Sn,
W,
Bi,
Ru,
Rh,
Pd,
Ag,
Ir,
Pt,
Au
with
single‐metal
sites
or
dual‐metal
sites.
development
of
electrocatalysts
novel
configurations
compositions
is
documented.
understanding
process–structure–property
relationships
highlighted.
For
SACs,
their
electrocatalytic
performance
stability
fuel
cells,
zinc–air
batteries,
electrolyzers,
CO
RR,
NRR
summarized.
challenges
perspectives
emerging
field
discussed.
Nature Communications,
Год журнала:
2021,
Номер
12(1)
Опубликована: Март 1, 2021
Abstract
Developing
high-performance
electrocatalysts
toward
hydrogen
evolution
reaction
is
important
for
clean
and
sustainable
energy,
yet
still
challenging.
Herein,
we
report
a
single-atom
strategy
to
construct
excellent
metal-organic
frameworks
(MOFs)
electrocatalyst
(NiRu
0.13
-BDC)
by
introducing
atomically
dispersed
Ru.
Significantly,
the
obtained
NiRu
-BDC
exhibits
outstanding
activity
in
all
pH,
especially
with
low
overpotential
of
36
mV
at
current
density
10
mA
cm
−2
1
M
phosphate
buffered
saline
solution,
which
comparable
commercial
Pt/C.
X-ray
absorption
fine
structures
functional
theory
calculations
reveal
that
Ru
can
modulate
electronic
structure
metal
center
MOF,
leading
optimization
binding
strength
H
2
O
H*,
enhancement
HER
performance.
This
work
establishes
as
an
efficient
approach
MOFs
catalyst
design.
Advanced Materials,
Год журнала:
2020,
Номер
32(34)
Опубликована: Июль 9, 2020
The
electrochemical
CO2
reduction
reaction
(CO2
RR)
is
of
great
importance
to
tackle
the
rising
concentration
in
atmosphere.
RR
can
be
driven
by
renewable
energy
sources,
producing
precious
chemicals
and
fuels,
with
implementation
this
process
largely
relying
on
development
low-cost
efficient
electrocatalysts.
Recently,
a
range
heterogeneous
potentially
single-atom
catalysts
(SACs)
containing
non-precious
metals
coordinated
earth-abundant
elements
have
emerged
as
promising
candidates
for
RR.
Unfortunately,
real
catalytically
active
centers
key
factors
that
govern
catalytic
performance
these
SACs
remain
ambiguous.
Here,
ambiguity
addressed
developing
fundamental
understanding
RR-to-CO
SACs,
CO
accounts
major
product
from
SACs.
mechanism,
rate-determining
steps,
control
activity
selectivity
are
analyzed
both
experimental
theoretical
studies.
Then,
synthesis,
characterization,
discussed.
Finally,
challenges
future
pathways
highlighted
hope
guiding
design
promote
understand
Advanced Materials,
Год журнала:
2021,
Номер
33(17)
Опубликована: Март 22, 2021
Abstract
Electrochemical
water
splitting
has
attracted
significant
attention
as
a
key
pathway
for
the
development
of
renewable
energy
systems.
Fabricating
efficient
electrocatalysts
these
processes
is
intensely
desired
to
reduce
their
overpotentials
and
facilitate
practical
applications.
Recently,
metal–organic
framework
(MOF)
nanoarchitectures
featuring
ultrahigh
surface
areas,
tunable
nanostructures,
excellent
porosities
have
emerged
promising
materials
highly
active
catalysts
electrochemical
splitting.
Herein,
most
pivotal
advances
in
recent
research
on
engineering
MOF
are
presented.
First,
design
catalytic
centers
MOF‐based/derived
summarized
compared
from
aspects
chemical
composition
optimization
structural
functionalization
at
atomic
molecular
levels.
Subsequently,
fast‐growing
breakthroughs
activities,
identification
sites,
fundamental
mechanisms
thoroughly
discussed.
Finally,
comprehensive
commentary
current
primary
challenges
future
perspectives
its
commercialization
hydrogen
production
provided.
Hereby,
new
insights
into
synthetic
principles
electrocatalysis
designing
utilization
offered,
thus
further
promoting
prosperity
wide
range
