Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Апрель 21, 2023
Abstract
Carbon-supported
nanoparticles
are
indispensable
to
enabling
new
energy
technologies
such
as
metal-air
batteries
and
catalytic
water
splitting.
However,
achieving
ultrasmall
high-density
(optimal
catalysts)
faces
fundamental
challenges
of
their
strong
tendency
toward
coarsening
agglomeration.
Herein,
we
report
a
general
efficient
synthesis
uniformly
dispersed
on
two-dimensional
porous
carbon.
This
is
achieved
through
direct
carbothermal
shock
pyrolysis
metal-ligand
precursors
in
just
~100
ms,
the
fastest
among
reported
syntheses.
Our
results
show
that
situ
coordination
(e.g.,
N
→
Co
2+
)
local
ordering
during
millisecond-scale
play
crucial
role
kinetically
dominated
fabrication
stabilization
carbon
films.
The
as-obtained
samples
exhibit
excellent
activity
stability
bifunctional
catalysts
oxygen
redox
reactions.
Considering
huge
flexibility
coordinated
design,
diversified
single
multielement
(M
=
Fe,
Co,
Ni,
Cu,
Cr,
Mn,
Ag,
etc)
were
generally
fabricated,
even
systems
well
beyond
traditional
crystalline
chemistry.
method
allows
for
transient
well-dispersed
with
great
simplicity
versatility
various
application
schemes.
ACS Catalysis,
Год журнала:
2020,
Номер
10(22), С. 13560 - 13583
Опубликована: Ноя. 10, 2020
Bimetallic
Pd
based
catalysts
have
received
tremendous
research
interests
for
many
important
reactions
in
fields
of
petrochemical
industrial
process,
fine
chemical
synthesis,
environment
protection,
renewable
energy
conversion,
as
their
specific
activity
and
selectivity
are
usually
higher
than
that
pure
Pd.
With
a
well-defined
composition,
Pd–M
bimetallic
also
the
ideal
platform
investigation
reaction
mechanism,
which
provides
bridge
construction
high-performance
catalyst.
This
Review
intends
to
give
an
overview
recent
advances
on
design
principles
catalyst
term
active
sites'
structure
number,
provide
insights
into
synergy
effects
between
M
well
supports
understand
elementary
mechanisms
reactions.
The
starts
with
how
intrinsic
different
structures
(alloy,
core–shell,
Pd/metal
compound
interface)
would
be
controlled
by
ligand
effect,
strain
ensemble
support
effect;
followed
discussion
determined
mechanism
selective
hydrogenation,
CO
oxidation,
methane
combustion,
electrocatalytic
conversion
(HER,
ORR,
MOR),
CO2
reduction,
H2
production,
biomass
upgrading,
synthesis;
then
introduces
strategies
maximize
number
finite
metal
load.
Finally,
operando
insight
reconstruction
under
condition
will
discussed.
On
basis
this
Review,
experience
generic
rules
acquired
from
thoughts,
synthetic
disciplines,
functionalities
given
could
referential
significance
revealing
catalytic
at
molecular
scales
building
up
other
high-efficiency
catalysts.
ACS Nano,
Год журнала:
2019,
Номер
13(7), С. 7800 - 7810
Опубликована: Июль 9, 2019
Multishell
hollow
nanoarchitectures
are
one
of
the
most
important
branches
in
nanomaterial
field
due
to
their
enormous
potential
many
fields,
but
synthesizing
them
a
well-controlled
manner
remains
challenging.
Herein,
we
present
general
strategy
for
construction
multishell
metal/nitrogen/carbon
dodecahedrons
(metal@NC)
with
well-defined
and
precisely
controlled
architectures.
This
is
based
on
pyrolysis
multilayer
solid
ZIFs
prepared
by
step-by-step
crystal
growth
approach,
which
enables
precise
control
over
shell
number
composition
resultant
metal@NC.
Impressively,
our
can
be
further
extended
synthesis
yolk@multishell
structures
or
that
assembled
carbon
nanotubes.
The
efficiently
facilitate
mass
diffusion,
together
high
dispersity
increased
surface
area
responsible
significantly
enhanced
catalytic
performances
selective
hydrogenation
biomass-derived
furfural
cyclopentanol
when
compared
single-shell
counterparts.
We
anticipate
would
shed
light
rational
design
accurate
other
complex
materials
various
yet
challenging
applications.
ACS Nano,
Год журнала:
2021,
Номер
15(9), С. 14928 - 14937
Опубликована: Авг. 23, 2021
High
entropy
alloy
nanoparticles
(HEA-NPs)
are
reported
to
have
superior
performance
in
catalysis,
energy
storage,
and
conversion
due
the
broad
range
of
elements
that
can
be
incorporated
these
materials,
enabling
tunable
activity,
excellent
thermal
chemical
stability,
a
synergistic
catalytic
effect.
However,
scaling
manufacturing
HEA-NPs
with
uniform
particle
size
homogeneous
elemental
distribution
efficiently
is
still
challenge
required
critical
synthetic
conditions
where
high
temperature
typically
involved.
In
this
work,
we
demonstrate
an
efficient
scalable
microwave
heating
method
using
carbon-based
materials
as
substrates
fabricate
size.
Due
abundant
functional
group
defects
absorb
efficiently,
reduced
graphene
oxide
employed
model
substrate
produce
average
reaching
∼1850
K
within
seconds.
As
proof-of-concept,
utilize
rapid,
high-temperature
process
synthesize
PtPdFeCoNi
HEA-NPs,
which
exhibit
∼12
nm
mixing
resulting
from
decomposition
nearly
at
same
time
liquid
metal
solidification
without
diffusion.
Various
also
substrates,
including
one-dimensional
carbon
nanofibers
three-dimensional
carbonized
wood,
achieve
temperatures
>1400
K.
This
facile
compatible
roll-to-roll
process,
providing
feasible
route
for
manufacturing.
Energy & Environmental Science,
Год журнала:
2021,
Номер
14(3), С. 1449 - 1460
Опубликована: Янв. 1, 2021
Low-temperature
direct
ammonia
fuel
cells
(DAFCs)
can
use
carbon-neutral
as
a
fuel,
which
has
attracted
increasing
attention
recently
due
to
ammonia's
low
source-to-tank
energy
cost,
easy
transport
and
storage,
wide
availability.
ACS Catalysis,
Год журнала:
2020,
Номер
10(7), С. 3945 - 3957
Опубликована: Март 3, 2020
Ammonia
(NH3)
has
proved
to
be
an
effective
alternative
hydrogen
in
low-temperature
fuel
cells
via
its
direct
ammonia
oxidation
reaction
(AOR).
However,
the
kinetically
sluggish
AOR
prohibitively
hindered
attractive
cell
(DAFC)
applications.
Here,
we
report
efficient
catalyst,
which
ternary
PtIrNi
alloy
nanoparticles
well
dispersed
on
a
binary
composite
support
consisting
of
porous
silicon
dioxide
(SiO2)
and
carboxyl-functionalized
carbon
nanotube
(PtIrNi/SiO2-CNT-COOH)
through
sonochemical-assisted
synthesis
method.
The
nanoparticles,
with
aid
abundant
OHad
provided
by
SiO2
improved
electrical
conductivity
CNTs,
exhibit
remarkable
catalytic
activity
for
alkaline
media.
It
is
evidenced
lower
onset
potential
(∼0.40
V
vs
reversible
electrode
(RHE))
at
room
temperature
than
that
commercial
PtIr/C
(ca.
0.43
RHE).
Increasing
NH3
concentrations
operation
temperatures
can
significantly
enhance
this
nanoparticle
catalyst.
Specifically,
catalyst
80
°C
exhibits
much
(∼0.32
RHE)
higher
peak
current
density,
indicating
DAFCs
operated
are
favorable
increased
performance.
Constant-potential
density
functional
theory
(DFT)
calculations
showed
Pt–Ir
ensembles
{100}-terminated
surfaces
serve
as
active
site.
introduction
Ni
raises
center
energy
states
projected
onto
group
d-orbitals
surface
sites
thus
lowers
theoretical
*NH2
dehydrogenation
*NH
compared
Pt
Pt3Ir
alloy.
Journal of Materials Chemistry A,
Год журнала:
2019,
Номер
7(20), С. 12451 - 12456
Опубликована: Янв. 1, 2019
Ultrasmall
bimetallic
alloy
nanoparticles
are
generated
via
a
micro–mesopore
confinement
synthesis
strategy
in
nanoporous
N–carbon.
The
prepared
catalysts
show
excellent
bifunctional
performance
both
ORR
and
OER,
outstanding
energy
conversion
efficiency
Zn–air
batteries.
ACS Nano,
Год журнала:
2020,
Номер
14(2), С. 1990 - 2001
Опубликована: Янв. 30, 2020
Atomically
dispersed
precious
metal
catalysts
have
emerged
as
a
frontier
in
catalysis.
However,
robust,
generic
synthetic
strategy
toward
atomically
is
still
lacking,
which
has
limited
systematic
studies
revealing
their
general
catalytic
trends
distinct
from
those
of
conventional
nanoparticle
(NP)-based
catalysts.
Herein,
we
report
catalysts,
consists
"trapping"
precursors
on
heteroatom-doped
carbonaceous
layer
coated
carbon
support
and
"immobilizing"
them
with
SiO2
during
thermal
activation.
Through
the
"trapping-and-immobilizing"
method,
five
(Os,
Ru,
Rh,
Ir,
Pt)
could
be
obtained
served
model
for
unravelling
oxygen
reduction
reaction
(ORR).
Owing
to
isolated
geometry,
generally
showed
higher
selectivity
H2O2
production
than
NP
counterparts
ORR.
Among
was
changed
by
types
metals,
Pt
catalyst
showing
highest
selectivity.
A
combination
experimental
results
density
functional
theory
calculations
revealed
that
trend
correlated
binding
energy
difference
between
*OOH
*O
species.
In
terms
2
e-
ORR
activity,
Rh
best
activity.
Our
approach
may
help
understanding
unique
behaviors