Nature Communications,
Journal Year:
2023,
Volume and Issue:
14(1)
Published: July 24, 2023
Dual-atom
catalysts,
particularly
those
with
heteronuclear
active
sites,
have
the
potential
to
outperform
well-established
single-atom
catalysts
for
oxygen
evolution
reaction,
but
underlying
mechanistic
understanding
is
still
lacking.
Herein,
a
large-scale
density
functional
theory
employed
explore
feasibility
of
*O-*O
coupling
mechanism,
which
can
circumvent
scaling
relationship
improving
catalytic
performance
N-doped
graphene
supported
Fe-,
Co-,
Ni-,
and
Cu-containing
dual-atom
namely,
M'M@NC.
Based
on
constructed
activity
maps,
rationally
designed
descriptor
be
obtained
predict
homonuclear
catalysts.
Seven
four
possess
high
activities
that
minimum
theoretical
overpotential.
The
chemical
structural
origin
in
favor
mechanism
thus
leading
enhanced
reaction
been
revealed.
This
work
not
only
provides
additional
insights
into
fundamental
mechanisms,
also
offers
guideline
accelerated
discovery
efficient
Acta Physico-Chimica Sinica,
Journal Year:
2021,
Volume and Issue:
0(0), P. 2108017 - 0
Published: Jan. 1, 2021
Abstract:
Research
on
two-dimensional
(2D)
materials
has
been
explosively
increasing
in
last
seventeen
years
varying
subjects
including
condensed
matter
physics,
electronic
engineering,
science,
and
chemistry
since
the
mechanical
exfoliation
of
graphene
2004.
Starting
from
graphene,
2D
now
have
become
a
big
family
with
numerous
members
diverse
categories.
The
unique
structural
features
physicochemical
properties
make
them
one
class
most
appealing
candidates
for
wide
range
potential
applications.
In
particular,
we
seen
some
major
breakthroughs
made
field
five
not
only
developing
novel
synthetic
methods
exploring
new
structures/properties
but
also
identifying
innovative
applications
pushing
forward
commercialisation.
this
review,
provide
critical
summary
recent
progress
particular
focus
years.
After
brief
background
introduction,
first
discuss
materials,
exfoliation,
liquid
vapor
phase
deposition,
wet-chemical
synthesis
as
well
engineering
belonging
to
nanomaterials
(PEN).
We
then
introduce
superconducting/optical/magnetic
chirality
along
newly
emerging
magic
angle
superlattices.
Following
that,
promising
electronics,
optoelectronics,
catalysis,
energy
storage,
solar
cells,
biomedicine,
sensors,
environments,
etc.
are
described
sequentially.
Thereafter,
present
theoretic
calculations
simulations
materials.
Finally,
after
concluding
current
progress,
personal
discussions
existing
challenges
future
outlooks
rapidly
field.
Advanced Materials,
Journal Year:
2022,
Volume and Issue:
34(30)
Published: March 3, 2022
Abstract
Although
lithium–sulfur
(Li–S)
batteries
are
promising
next‐generation
energy‐storage
systems,
their
practical
applications
limited
by
the
growth
of
Li
dendrites
and
lithium
polysulfide
shuttling.
These
problems
can
be
mitigated
through
use
single‐atom
catalysts
(SACs),
which
exhibit
advantages
maximal
atom
utilization
efficiency
(≈100%)
unique
catalytic
properties,
thus
effectively
enhancing
performance
electrode
materials
in
devices.
This
review
systematically
summarizes
recent
progress
SACs
intended
for
Li‐metal
anodes,
S
cathodes,
separators,
briefly
introducing
operating
principles
Li–S
batteries,
action
mechanisms
corresponding
SACs,
fundamentals
activity,
then
comprehensively
describes
main
strategies
synthesis.
Subsequently,
operation
reinforced
as
well
other
metal–S
individually
illustrated,
major
challenges
usage
future
development
directions
presented.
Advanced Materials,
Journal Year:
2021,
Volume and Issue:
33(49)
Published: Oct. 8, 2021
Abstract
Polynary
transition‐metal
atom
catalysts
are
promising
to
supersede
platinum
(Pt)‐based
for
oxygen
reduction
reaction
(ORR).
Regulating
the
local
configuration
of
atomic
is
key
catalyst
performance
enhancement.
Different
from
previously
reported
single‐atom
or
dual‐atom
configurations,
a
new
type
ternary‐atom
catalyst,
which
consists
atomically
dispersed,
nitrogen‐coordinated
Co–Co
dimers,
and
Fe
single
sites
(i.e.,
Co
2
–N
6
Fe–N
4
structures)
that
coanchored
on
highly
graphitized
carbon
supports
developed.
This
unique
ORR
outperforms
with
only
in
both
alkaline
acid
conditions.
Density
functional
theory
calculations
clearly
unravels
synergistic
effect
sites,
can
induce
higher
filling
degree
Fe–d
orbitals
favors
binding
capability
*OH
intermediates
(the
rate
determining
step).
may
be
alternative
Pt
drive
cathodic
zinc–air
batteries.
Energy & Environmental Science,
Journal Year:
2022,
Volume and Issue:
15(4), P. 1601 - 1610
Published: Jan. 1, 2022
By
elaborately
constructing
a
Fe–Zn
based
diatomic
catalyst,
the
active
center
is
changed
from
FeN
4–
ZnN
4
to
Zn–N
2
after
protonation,
leading
well-maintained
structure
and
thus
high
stability
of
ORR.
ACS Catalysis,
Journal Year:
2022,
Volume and Issue:
12(8), P. 4659 - 4679
Published: April 5, 2022
Plastics
are
indispensable,
but
their
pollution
is
triggering
a
global
environmental
crisis.
Although
many
end-of-life
catalytic
options
have
involved
converting
plastics
into
valuable
products,
deep
understanding
of
the
relationship
between
polymer
structure
and
recycling
performance
significant
urgently
needed.
Here,
we
start
with
primer
polymeric
chain
structures
on
chemical
discuss
structure–performance
polymer,
catalyst,
reaction.
Specifically,
development
challenges
re/upcycling
waste
PET
polyolefins
discussed
in-depth.
In
addition,
also
present
some
prospects
for
innovations
in
catalyst
synthesis
reaction
engineering
basis
relationship.
The
discussion
ends
brief
perspective
future
plastic
re/upcycling.
Overall,
intelligent
catalysis
design
necessary
incentivizing
relieving
burden
plastics.
Advanced Functional Materials,
Journal Year:
2021,
Volume and Issue:
31(45)
Published: Aug. 8, 2021
Abstract
The
development
of
earth‐abundant
oxygen
reduction
reaction
(ORR)
catalysts
with
high
catalytic
activity
and
good
stability
for
practical
metal‐air
batteries
remains
an
enormous
challenge.
Herein,
a
highly
efficient
durable
ORR
catalyst
is
reported,
which
consists
atomically
dispersed
Co
single
atoms
(Co‐SAs)
in
the
form
Co‐N4
moieties
small
nanoparticles
(Co‐SNPs)
co‐anchored
on
nitrogen‐doped
porous
carbon
nanocage
(Co‐SAs/SNPs@NC).
Benefiting
from
synergistic
effect
Co‐SAs
Co‐SNPs
as
well
enhanced
anticorrosion
capability
matrix
brought
by
its
improved
graphitization
degree,
resultant
Co‐SAs/SNPs@NC
exhibits
outstanding
remarkable
alkaline
media,
outperforming
Co‐SAs‐based
(Co‐SAs@NC),
benchmark
Pt/C
catalyst.
Density
functional
theory
calculations
reveal
that
strong
interaction
between
sites
can
increase
valence
state
active
moderate
adsorption
free
energy
intermediates,
thus
facilitating
O
2
.
Moreover,
zinc‐air
battery
assembled
demonstrates
maximum
power
density
223.5
mW
cm
–2
,
specific
capacity
742
W
h
kg
–1
at
50
mA
superior
cycling
stability.
Chemical Science,
Journal Year:
2021,
Volume and Issue:
12(20), P. 6800 - 6819
Published: Jan. 1, 2021
The
electrochemical
carbon
dioxide
reduction
reaction
(CO2RR)
offers
a
promising
solution
to
mitigate
emission
and
at
the
same
time
generate
valuable
carbonaceous
chemicals/fuels.
Single
atom
catalysts
(SACs)
are
encouraging
catalyze
CO2RR
due
tunable
electronic
structure
of
central
metal
atoms,
which
can
regulate
adsorption
energy
reactants
intermediates.
Moreover,
SACs
form
bridge
between
homogeneous
heterogeneous
catalysts,
providing
an
ideal
platform
explore
mechanism
reactions.
In
this
review,
we
first
discuss
strategies
for
promoting
performance,
including
suppression
hydrogen
evolution
(HER),
generation
C1
products
formation
C2+
products.
Then,
summarize
recent
developments
in
regulating
toward
based
on
above
aspects.
Finally,
several
issues
regarding
development
raised
possible
solutions
provided.
Advanced Materials,
Journal Year:
2022,
Volume and Issue:
34(42)
Published: Sept. 10, 2022
The
development
of
highly
efficient
and
economical
materials
for
the
oxygen
reduction
reaction
(ORR)
plays
a
key
role
in
practical
energy
conversion
technologies.
However,
intrinsic
scaling
relations
exert
thermodynamic
inhibition
on
realizing
active
ORR
electrocatalysts.
Herein,
novel
feasible
gradient
orbital
coupling
strategy
tuning
performance
through
construction
Co
3d-O
2p-Eu
4f
unit
sites
Eu2
O3
-Co
model
is
proposed.
Through
coupling,
pristine
ionic
property
between
Eu
O
atoms
assigned
with
increased
covalency,
which
optimizes
eg
occupancy
sites,
weakens
OO
bond,
thus
ultimately
breaking
relation
*OOH
*OH
at
Co-O-Eu
sites.
optimized
catalyst
displays
onset
half-wave
potential
1.007
0.887
V
versus
reversible
hydrogen
electrode,
respectively,
are
higher
than
those
commercial
Pt/C
most
Co-based
catalysts
ever
reported.
In
addition,
found
to
possess
superior
selectivity
durability.
It
also
reveals
better
cell
noble-metal
Zn-air
batteries
terms
high
power/energy
densities
long
cycle
life.
This
study
provides
new
perspective
electronic
modulation
by
3d-2p-4f
coupling.
Advanced Materials,
Journal Year:
2021,
Volume and Issue:
34(5)
Published: Oct. 22, 2021
Next-generation
batteries
based
on
conversion
reactions,
including
aqueous
metal-air
batteries,
nonaqueous
alkali
metal-O2
and
-CO2
metal-chalcogen
metal-ion
have
attracted
great
interest.
However,
their
use
is
restricted
by
inefficient
reversible
of
active
agents.
Developing
bifunctional
catalysts
to
accelerate
the
reaction
kinetics
in
both
discharge
charge
processes
urgently
needed.
Graphene-,
or
graphene-like
carbon-supported
atomically
dispersed
metal
(G-ADMCs)
been
demonstrated
show
excellent
activity
various
electrocatalytic
making
them
promising
candidates.
Different
from
G-ADMCs
for
catalysis,
which
only
require
high
one
direction,
rechargeable
should
provide
discharging
charging.
This
review
provides
guidance
design
fabrication
next-generation
reactions.
The
key
challenges
that
prevent
conversion,
origin
G-ADMCs,
current
principles
highly
analyzed
highlighted
each
conversion-type
battery.
Finally,
a
summary
outlook
development
G-ADMC
materials
with
energy
density
efficiency
are
given.