Nanoscale,
Год журнала:
2022,
Номер
14(27), С. 9849 - 9859
Опубликована: Янв. 1, 2022
Exploring
cost-effective
non-precious
metal
electrocatalysts
is
vital
for
the
large-scale
application
of
clean
energy
conversion
devices
(i.e.,
fuel
cells,
metal-air
batteries
and
water
electrolysers).
Herein,
we
present
construction
a
three-dimensional
cobalt
sulfide/multi-heteroatom
co-doped
carbon
composite
as
trifunctional
electrocatalyst
oxygen
reduction
reaction
(ORR),
evolution
(OER)
hydrogen
(HER)
through
one-step
sulfidation
zeolitic-imidazolate
frameworks
(ZIFs)
using
sulfur
powder
source.
By
virtue
distinct
periodic
metal-nitrogen
coordination
structure
abundant
micropores
within
ZIF
precursor,
sub-10
nm
Co9S8
nanoparticles
(NPs)
are
homogenously
anchored
on
Co,
S
N
multi-heteroatom
framework
with
large
specific
surface
area
that
exposes
sufficient
reactive
sites
these
electrocatalytic
reactions.
The
optimized
Co9S8/CoNSC
exhibits
outstanding
ORR,
OER
HER
performance,
comparable
or
even
superior
to
those
commercial
Pt/C
RuO2.
small
NPs
Co-Nx
species
embedded
in
matrix
cooperatively
catalyze
while
catalysis
mainly
contributed
by
NPs.
Furthermore,
shows
anti-poisoning
capability
towards
during
ORR
no
obvious
activity
degradation
observed
0.1
M
KOH
containing
50
μM
SO32-
species,
significantly
outperforming
Pt/C.
assembled
rechargeable
Zn-air
battery
cathode
high
power
density
(150
mW
cm-2)
electrolyzer
only
requires
1.585
V
at
current
10
mA
cm-2
when
this
material
an
anode
cathode.
This
work
provides
effective
strategy
design
synthesize
efficient,
durable
chalcogenide-based
devices.
ACS Catalysis,
Год журнала:
2023,
Номер
13(22), С. 15126 - 15142
Опубликована: Ноя. 8, 2023
With
the
development
of
synthetic
methodology,
recent
breakthroughs
have
been
achieved
to
prepare
metal
single-atom
catalysts
(SACs)
with
high
loadings,
leading
an
emerging
class
SACs
called
densely
populated
or
high-density
SACs.
This
type
provides
not
only
higher
mass-specific
activity
but
also
additional
interaction
among
single
sites,
which
can
further
influence
local
geometric
and
electronic
structures
individual
centers
thus
affect
intrinsic
active
sites.
Review
examines
research
progress
atomic
regulation
engineering
density
how
it
affects
catalytic
performance
in
specific
thermal
catalysis.
Last,
we
outline
challenges
prospects
for
future
work
design
Abstract
Metal
oxide‐supported
multielement
alloy
nanoparticles
are
very
promising
as
highly
efficient
and
cost‐effective
catalysts
with
a
virtually
unlimited
compositional
space.
However,
controllable
synthesis
of
ultrasmall
(us‐MEA‐NPs)
supported
on
porous
metal
oxides
homogeneous
elemental
distribution
good
catalytic
stability
during
long‐term
operation
is
extremely
challenging
due
to
their
oxidation
strong
immiscibility.
As
proof
concept
that
such
can
be
realized,
this
work
presents
general
“bottom‐up”
l
ultrasonic‐assisted,
simultaneous
electro‐oxidation–reduction‐precipitation
strategy
for
alloying
dissimilar
elements
into
single
NPs
support.
One
characteristic
technique
uniform
mixing,
which
results
from
rapid
thermal
decomposition
reduction
leads
liquid
droplet
solidification
without
aggregation.
This
process
was
achieved
through
synergistic
combination
enhanced
electrochemical
plasma‐chemical
phenomena
at
the
metal–electrolyte
interface
(electron
energy
0.3–1.38
eV
peak
temperature
3000
K
reached
within
seconds
rate
~105
per
second)
in
an
aqueous
solution
under
ultrasonic
field
(40
kHz).
Illustrating
effectiveness
approach,
CuAgNiFeCoRuMn@MgO‐P3000
catalyst
exhibited
exceptional
efficiency
selective
hydrogenation
nitro
compounds,
over
99%
chemoselectivity
nearly
100%
conversion
60
s
no
decrease
activity
even
after
40
cycles
(>98%
120
s).
Our
provide
effective,
transferable
method
rationally
designing
MEA‐NP
atomic
level
pave
way
wide
variety
reactions.
image
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(22)
Опубликована: Март 22, 2023
Due
to
the
generation
of
multiple
intermediates
during
nitroarene
reduction,
precise
interception
single
one
develop
tandem
reactions
involving
both
C-C
and
C-N
bond
formations
still
remains
a
significant
challenge.
Herein,
relay
catalysis
supported
bifunctional
cobalt
catalyst
with
l-proline
has
been
successfully
applied
establish
bran-new
reductive
annulation
reaction
nitroarenes
formaldehyde,
which
enables
direct
diverse
construction
symmetrical
unsymmetrical
1,3-diaryl
imidazolines.
It
proceeds
operational
simplicity,
good
substrate
functionality
compatibility,
excellent
step
atom-efficiency.
Mechanistic
studies
reveal
that
Co-catalyst
exhibits
synergistic
effect
on
formation
key
N-hydroxy
imine,
subsequently
facilitates
formation.
The
current
work
opens
door
useful
transformations
by
reduction-interrupted
strategy.
ACS Applied Materials & Interfaces,
Год журнала:
2023,
Номер
15(6), С. 8149 - 8156
Опубликована: Янв. 13, 2023
Halogenated
arylamines
are
important
intermediates
for
the
synthesis
of
dyes,
pesticides,
herbicides,
and
other
chemicals.
One
way
to
prepare
halogenated
is
catalytic
hydrogenation
nitroarenes.
Ni-based
catalysts
have
been
used
in
nitroarenes
but
suffer
from
low
activity
dehalogenation
side
reaction.
In
this
paper,
Ni-CeO2/SiO2
heterojunction
catalyst
with
a
"raisin-bun"
structure
was
prepared
by
reverse
microemulsion.
A
built-in
electric
field
more
oxygen
vacancies
were
formed
due
electron
transfer
Ni
CeO2
as
result
their
work
function
difference.
The
leads
heterolytic
cleavage
H2,
thereby
improving
activity.
Oxygen
preferentially
adsorb
activate
nitro
groups,
inhibiting
Through
cooperation
vacancy,
synchronous
enhancement
selectivity
obtained
successfully.
This
finding
provides
new
view
design
non-noble
metal-based
high
selectivity.
