Journal of the American Chemical Society,
Journal Year:
2021,
Volume and Issue:
144(3), P. 1174 - 1186
Published: Dec. 22, 2021
Real
bifunctional
electrocatalysts
for
hydrogen
evolution
reaction
and
oxygen
have
to
be
the
ones
that
exhibit
a
steady
configuration
during/after
without
irreversible
structural
transformation
or
surface
reconstruction.
Otherwise,
they
can
termed
as
"precatalysts"
rather
than
real
catalysts.
Herein,
through
strongly
atomic
metal-support
interaction,
single-atom
dispersed
catalysts
decorating
atomically
Ru
onto
nickel-vanadium
layered
double
hydroxide
(LDH)
scaffold
excellent
HER
OER
activities.
Both
in
situ
X-ray
absorption
spectroscopy
operando
Raman
spectroscopic
investigation
clarify
presence
of
on
LDH
is
playing
an
imperative
role
stabilizing
dangling
bond-rich
further
leads
reconstruction-free
surface.
Through
strong
interaction
provided
by
LDH,
significant
interplay
stabilize
reactive
site
reach
small
fluctuation
oxidation
state
toward
cathodic
reconstruction,
while
Ni
greater
tolerance
both
bond
constriction
distortion
caused
oxidizing
during
anodic
boost
increase
contributes
its
superior
performance.
Unlike
numerous
suffered
from
reconstruction/transformation
adapting
HER/OER
cycles,
proposed
Ru/Ni3V-LDH
characteristic
dual
sites
with
(i.e.,
sites)
individual
catalysis
water
splitting
revealed
electrocatalyst.
Angewandte Chemie International Edition,
Journal Year:
2020,
Volume and Issue:
59(13), P. 5350 - 5354
Published: Jan. 22, 2020
Abstract
Unveiling
the
active
phase
of
catalytic
materials
under
reaction
conditions
is
important
for
construction
efficient
electrocatalysts
selective
nitrate
reduction
to
ammonia.
The
origin
prominent
activity
enhancement
CuO
(Faradaic
efficiency:
95.8
%,
Selectivity:
81.2
%)
toward
electroreduction
ammonia
was
probed.
15
N
isotope
labeling
experiments
showed
that
originated
from
reduction.
1
H
NMR
spectroscopy
and
colorimetric
methods
were
performed
quantify
In
situ
Raman
ex
revealed
electrochemically
converted
into
Cu/Cu
2
O,
which
serves
as
an
phase.
combined
results
online
differential
electrochemical
mass
spectrometry
(DEMS)
DFT
calculations
demonstrated
electron
transfer
Cu
O
at
interface
could
facilitate
formation
*NOH
intermediate
suppress
hydrogen
evolution
reaction,
leading
high
selectivity
Faradaic
efficiency.
Chemical Reviews,
Journal Year:
2020,
Volume and Issue:
120(21), P. 11703 - 11809
Published: Oct. 21, 2020
Isolated
atoms
featuring
unique
reactivity
are
at
the
heart
of
enzymatic
and
homogeneous
catalysts.
In
contrast,
although
concept
has
long
existed,
single-atom
heterogeneous
catalysts
(SACs)
have
only
recently
gained
prominence.
Host
materials
similar
functions
to
ligands
in
catalysts,
determining
stability,
local
environment,
electronic
properties
isolated
thus
providing
a
platform
for
tailoring
targeted
applications.
Within
just
decade,
we
witnessed
many
examples
SACs
both
disrupting
diverse
fields
catalysis
with
their
distinctive
substantially
enriching
our
understanding
molecular
processes
on
surfaces.
To
date,
term
SAC
mostly
refers
late
transition
metal-based
systems,
but
numerous
exist
which
other
elements
play
key
catalytic
roles.
This
review
provides
compositional
encyclopedia
SACs,
celebrating
10th
anniversary
introduction
this
term.
By
defining
broadest
sense,
explore
full
elemental
diversity,
joining
different
areas
across
whole
periodic
table,
discussing
historical
milestones
recent
developments.
particular,
examine
coordination
structures
associated
accessed
through
distinct
single-atom–host
combinations
relate
them
main
applications
thermo-,
electro-,
photocatalysis,
revealing
trends
element-specific
evolution,
host
design,
uses.
Finally,
highlight
frontiers
field,
including
multimetallic
atom
proximity
control,
possible
multistep
cascade
reactions,
identifying
challenges,
propose
directions
future
development
flourishing
field.
Advanced Energy Materials,
Journal Year:
2020,
Volume and Issue:
10(11)
Published: Feb. 6, 2020
Abstract
Electrochemical
water
splitting
plays
a
crucial
role
in
the
development
of
clean
and
renewable
energy
production
conversion,
which
is
promising
pathway
to
reduce
social
dependence
on
fossil
fuels.
Thus,
highly
active,
cost‐efficient,
robust
catalysts
must
be
developed
reaction
overpotential
increase
electrocatalytic
efficiency.
In
this
review,
recent
research
efforts
toward
developing
advanced
electrocatalysts
based
noble
metals
with
outstanding
performance
for
catalysis,
mainly
dependent
their
structure
engineering,
are
summarized.
First,
simple
description
water‐splitting
mechanism
some
engineering
strategies
given,
including
heteroatom
incorporation,
strain
interface/hybrid
single
atomic
construction.
Then,
underlying
relationship
between
metal
electronic/geometric
discussed
assistance
theoretical
simulation.
Finally,
personal
perspective
provided
order
highlight
challenges
opportunities
novel
suitable
wide
range
commercial
uses
structural
applications.
Chemical Reviews,
Journal Year:
2020,
Volume and Issue:
120(21), P. 12217 - 12314
Published: Nov. 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 Reviews,
Journal Year:
2020,
Volume and Issue:
120(21), P. 11986 - 12043
Published: Oct. 28, 2020
Metal
atoms
dispersed
on
the
oxide
supports
constitute
a
large
category
of
single-atom
catalysts.
In
this
review,
supported
catalysts
are
discussed
about
their
synthetic
procedures,
characterizations,
and
reaction
mechanism
in
thermocatalysis,
such
as
water-gas
shift
reaction,
selective
oxidation/hydrogenation,
coupling
reactions.
Some
typical
materials,
including
ferric
oxide,
cerium
titanium
dioxide,
aluminum
so
on,
intentionally
mentioned
for
unique
roles
anchoring
metal
taking
part
catalytic
The
interactions
between
summarized
to
give
picture
how
stabilize
atomic
centers,
rationally
tune
geometric
structures
electronic
states
single
atoms.
Furthermore,
several
directions
fabricating
with
improved
performance
proposed
basis
state-of-the-art
understanding
metal-oxide
interactions.
Chemical Society Reviews,
Journal Year:
2020,
Volume and Issue:
49(7), P. 2215 - 2264
Published: Jan. 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.
ACS Catalysis,
Journal Year:
2019,
Volume and Issue:
9(11), P. 9973 - 10011
Published: Sept. 25, 2019
As
a
highly
appealing
technology
for
hydrogen
generation,
water
electrolysis
including
oxygen
evolution
reaction
(OER)
at
the
anode
and
(HER)
cathode
largely
depends
on
availability
of
efficient
electrocatalysts.
Accordingly,
over
past
years,
much
effort
has
been
made
to
develop
various
electrocatalysts
with
superior
performance
reduced
cost.
Among
them,
ruthenium
(Ru)-based
materials
OER
HER
are
very
promising
because
their
prominent
catalytic
activity,
pH-universal
application,
cheapest
price
among
precious
metal
family,
so
on.
Herein,
recent
advances
in
this
hot
research
field
comprehensively
reviewed.
A
general
description
about
splitting
is
presented
understand
mechanism
proposed
scaling
relations
toward
activities,
key
stability
issues
Ru-based
further
given.
Subsequently,
Ru-involving
introduced
classified
into
different
groups
improving
or
optimizing
electrocatalytic
properties,
special
focus
several
significant
bifunctional
along
simulated
electrolyzer.
Finally,
perspective
existing
challenges
future
progress
catalysts
provided.
The
main
aim
here
shed
some
light
design
construction
emerging
energy
storage
conversion
technologies.
Nature Communications,
Journal Year:
2021,
Volume and Issue:
12(1)
Published: July 28, 2021
Abstract
Rational
design
of
single
atom
catalyst
is
critical
for
efficient
sustainable
energy
conversion.
However,
the
atomic-level
control
active
sites
essential
electrocatalytic
materials
in
alkaline
electrolyte.
Moreover,
well-defined
surface
structures
lead
to
in-depth
understanding
catalytic
mechanisms.
Herein,
we
report
a
single-atomic-site
ruthenium
stabilized
on
defective
nickel-iron
layered
double
hydroxide
nanosheets
(Ru
1
/D-NiFe
LDH).
Under
precise
regulation
local
coordination
environments
catalytically
and
existence
defects,
Ru
LDH
delivers
an
ultralow
overpotential
18
mV
at
10
mA
cm
−2
hydrogen
evolution
reaction,
surpassing
commercial
Pt/C
catalyst.
Density
functional
theory
calculations
reveal
that
optimizes
adsorption
energies
intermediates
reaction
promotes
O–O
coupling
Ru–O
site
oxygen
reaction.
The
as
ideal
model
reveals
superior
water
splitting
performance
with
potential
development
promising
water-alkali
electrocatalysts.
Nature Communications,
Journal Year:
2019,
Volume and Issue:
10(1)
Published: Oct. 24, 2019
Abstract
Achieving
active
and
stable
oxygen
evolution
reaction
(OER)
in
acid
media
based
on
single-atom
catalysts
is
highly
promising
for
cost-effective
sustainable
energy
supply
proton
electrolyte
membrane
electrolyzers.
Here,
we
report
an
atomically
dispersed
Ru
1
-N
4
site
anchored
nitrogen-carbon
support
(Ru-N-C)
as
efficient
durable
electrocatalyst
acidic
OER.
The
Ru-N-C
catalyst
delivers
exceptionally
intrinsic
activity,
reaching
a
mass
activity
high
3571
A
g
metal
−1
turnover
frequency
of
3348
O
2
h
with
low
overpotential
267
mV
at
current
density
10
mA
cm
−2
.
shows
no
evident
deactivation
or
decomposition
after
30-hour
operation
environment.
Operando
synchrotron
radiation
X-ray
absorption
spectroscopy
infrared
identify
the
dynamic
adsorption
single
atom
under
working
potentials,
theoretical
calculations
demonstrate
that
O-Ru
responsible
OER
stability.
Nature Communications,
Journal Year:
2019,
Volume and Issue:
10(1)
Published: Nov. 6, 2019
Abstract
Metal-organic
frameworks
(MOFs)
have
been
recognized
as
compelling
platforms
for
the
development
of
miscellaneous
applications
because
their
structural
diversity
and
functional
tunability.
Here,
we
propose
that
electrocatalytic
properties
could
be
well
modified
by
incorporating
missing
linkers
into
MOF.
Theoretical
calculations
suggest
electronic
structure
MOFs
can
tuned
introducing
linkers,
which
improves
oxygen
evolution
reaction
(OER)
performance
Inspired
these
aspects,
introduced
various
a
layered-pillared
MOF
Co
2
(OH)
(C
8
H
4
O
)
(termed
CoBDC)
to
prepare
missing-linker
MOFs.
Transmission
electron
microscope
synchrotron
X-ray
measurements
confirmed
in
controlled
our
strategy.
The
self-supported
nanoarrays
with
carboxyferrocene
exhibit
excellent
OER
ultralow
overpotential
241
mV
at
100
mA
cm
−2
.
This
work
opens
new
prospect
develop
efficient
MOF-based
electrocatalysts
linkers.