Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
60(42), P. 22722 - 22728
Published: Aug. 17, 2021
Abstract
Designing
and
modulating
the
local
structure
of
metal
sites
is
key
to
gain
unique
selectivity
high
activity
single
site
catalysts.
Herein,
we
report
strain
engineering
curved
atomic
iron‐nitrogen
boost
electrocatalytic
activity.
First,
a
helical
carbon
with
abundant
high‐curvature
surface
realized
by
carbonization
polypyrrole
that
templated
from
self‐assembled
chiral
surfactants.
The
introduces
compressive
on
supported
Fe−N
4
sites.
Consequently,
1.5
%
compressed
bonds
exhibit
downshifted
d‐band
center
than
planar
Such
change
can
weaken
bonding
strength
between
oxygenated
intermediates
sites,
resulting
much
smaller
energy
barrier
for
oxygen
reduction.
Catalytic
tests
further
demonstrate
kinetic
current
density
7.922
mA
cm
−2
at
0.9
V
vs.
RHE
obtained
in
alkaline
media
which
31
times
higher
ones.
Our
findings
shed
light
three‐dimensional
boosting
catalytic
via
engineering.
Chemical Society Reviews,
Journal Year:
2021,
Volume and Issue:
50(8), P. 5281 - 5322
Published: Jan. 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 Reviews,
Journal Year:
2020,
Volume and Issue:
120(17), P. 9363 - 9419
Published: Aug. 6, 2020
Heteroatom-doped
porous
carbon
materials
(HPCMs)
have
found
extensive
applications
in
adsorption/separation,
organic
catalysis,
sensing,
and
energy
conversion/storage.
The
judicious
choice
of
precursors
is
crucial
for
the
manufacture
HPCMs
with
specific
usages
maximization
their
functions.
In
this
regard,
polymers
as
demonstrated
great
promise
because
versatile
molecular
nanoscale
structures,
modulatable
chemical
composition,
rich
processing
techniques
to
generate
textures
that,
combination
proper
solid-state
chemistry,
can
be
maintained
throughout
carbonization.
This
Review
comprehensively
surveys
progress
polymer-derived
functional
terms
how
produce
control
porosities,
heteroatom
doping
effects,
morphologies
related
use.
First,
we
summarize
discuss
synthetic
approaches,
including
hard
soft
templating
methods
well
direct
synthesis
strategies
employing
pores
and/or
heteroatoms
HPCMs.
Second,
effects
on
thermal
stability,
electronic
optical
properties,
surface
chemistry
Specifically,
effect,
which
involves
both
single-type
codoping
two
or
more
types
into
network,
discussed.
Considering
significance
application
spectrum,
potential
choices
suitable
polymeric
precisely
regulate
are
presented.
Finally,
provide
our
perspective
predefine
structures
by
using
realize
current
fields
generation/conversion
environmental
remediation.
We
believe
that
these
analyses
deductions
valuable
a
systematic
understanding
will
serve
source
inspiration
design
future
Angewandte Chemie International Edition,
Journal Year:
2020,
Volume and Issue:
60(9), P. 4448 - 4463
Published: April 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.
Chemical Reviews,
Journal Year:
2020,
Volume and Issue:
120(21), P. 12315 - 12341
Published: Oct. 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.
ACS Catalysis,
Journal Year:
2020,
Volume and Issue:
10(14), P. 7495 - 7511
Published: June 10, 2020
Hydrogen
peroxide
is
a
valuable
chemical
oxidant
with
wide
range
of
applications
in
variety
industrial
processes,
especially
water
sanitization.
Electrochemical
synthesis
hydrogen
(H2O2)
through
two-electron
oxygen
reduction
reaction
(2e-ORR)
or
oxidation
(2e-WOR)
has
emerged
as
an
appealing
process
for
onsite
production
this
chemically
oxidant.
On-site
produced
H2O2
can
be
applied
wastewater
treatment
remote
locations
any
where
needed
oxidizing
agent.
This
Review
studies
the
theoretical
efforts
understanding
challenges
catalysis
electrochemical
well
providing
design
principles
more
efficient
catalyst
materials.
ACS Catalysis,
Journal Year:
2020,
Volume and Issue:
10(14), P. 7584 - 7618
Published: June 11, 2020
Single
metal
atoms
embedded
within
select
supporting
matrices
have
shown
great
potential
in
the
development
of
high-efficiency,
low-cost
electrocatalysts
because
maximal
atom
utilization
and
mass
activity.
As
single
are
stabilized
by
coordination
bonds
with
substrate,
strong
metal–support
interactions
can
be
exploited
for
ready
manipulation
electrocatalytic
activity
selectivity
toward
target
reactions.
However,
most
single-atom
catalysts
(SACs)
prepared
pyrolysis
contain
a
wide
range
structures.
Resolving
atomic
configurations
moieties
represents
critical
first
step
establishment
an
unambiguous
correlation
between
SAC
structure
In
this
Review,
we
summarize
recent
progress
studies
electrocatalysts,
focus
on
impacts
sites
activities
series
reactions
that
important
various
electrochemical
energy
technologies,
such
as
hydrogen
evolution
reaction,
oxygen
reduction
nitrogen
CO2
so
on.
The
survey
entails
SACs,
from
noble
metals
(e.g.,
Pt,
Pd,
Ru,
Ir,
Au,
etc.)
to
non-noble
Fe,
Co,
Ni,
Cu,
etc.),
supported
variety
substrate
materials
pristine
doped
carbon,
metal,
oxide,
sulfide,
etc.).
Finally,
Review
concludes
perspective
highlighting
promises
challenges
further
SACs
context
chemistry.
Advanced Functional Materials,
Journal Year:
2021,
Volume and Issue:
31(30)
Published: May 18, 2021
Abstract
Skin
effect
and
high
density
are
the
main
reasons
that
restrict
search
of
lightweight
high‐performance
metal‐based
electromagnetic
(EM)
wave
absorbing
materials.
Although
nanostructured
metal
materials
have
been
fabricated
to
solve
above
problems,
poor
dispersibility
chemical
stability
issues
brought
about
by
surface
energy
due
existing
nano‐size
effect.
In
this
work,
Ni
foam
with
NiO/NiFe
2
O
4
in
situ
growth
composites
a
facile
universal
route
as
an
effective
alternative
EM
absorber.
Impressively,
it
is
found
structure
/Ni
components
can
synergistically
boost
absorption
capacity.
detail,
impedance
matching
from
dissipation
interfacial
polarization
defect
induced
provided
mainly
contributes
its
ultra‐broadband
performance.
As
result,
as‐prepared
sample
(0.06
g·cm
−3
)
delivers
wide
bandwidth
14.24
GHz
thin
thickness
0.6
mm,
well
as,
specific
19444.4
GHz·g
−1
·cm
−2
.
This
work
sheds
light
on
novel
view
synergistic
behaviors
demonstrates
new
pathway
for
preparation
absorbers.
Nature Communications,
Journal Year:
2021,
Volume and Issue:
12(1)
Published: Sept. 22, 2021
Abstract
Single-atom
catalysts
with
maximum
metal
utilization
efficiency
show
great
potential
for
sustainable
catalytic
applications
and
fundamental
mechanistic
studies.
We
here
provide
a
convenient
molecular
tailoring
strategy
based
on
graphitic
carbon
nitride
as
support
the
rational
design
of
single-site
dual-site
single-atom
catalysts.
Catalysts
single
Fe
sites
exhibit
impressive
oxygen
reduction
reaction
activity
half-wave
0.89
V
vs.
RHE.
find
that
Ni
are
favorable
to
promote
key
structural
reconstruction
into
bridging
Ni-O-Fe
bonds
in
NiFe
SAC.
Meanwhile,
newly
formed
create
spin
channels
electron
transfer,
resulting
significant
improvement
evolution
an
overpotential
270
mV
at
10
mA
cm
−2
.
further
reveal
water
oxidation
follows
pathway
through
deprotonation
*OH
both
sites,
leading
formation
O
2
atop
sites.