Nature Communications,
Journal Year:
2023,
Volume and Issue:
14(1)
Published: Jan. 23, 2023
Abstract
Selective
two-electron
(2e
−
)
oxygen
reduction
reaction
(ORR)
offers
great
opportunities
for
hydrogen
peroxide
(H
2
O
electrosynthesis
and
its
widespread
employment
depends
on
identifying
cost-effective
catalysts
with
high
activity
selectivity.
Main-group
metal
nitrogen
coordinated
carbons
(M-N-Cs)
are
promising
but
remain
largely
underexplored
due
to
the
low
metal-atom
density
lack
of
understanding
in
structure-property
correlation.
Here,
we
report
using
a
nanoarchitectured
Sb
S
3
template
synthesize
high-density
(10.32
wt%)
antimony
(Sb)
single
atoms
nitrogen-
sulfur-codoped
carbon
nanofibers
(Sb-NSCF),
which
exhibits
both
selectivity
(97.2%)
mass
(114.9
A
g
−1
at
0.65
V)
toward
2e
ORR
alkaline
electrolyte.
Further,
when
evaluated
practical
flow
cell,
Sb-NSCF
shows
production
rate
7.46
mol
catalyst
h
negligible
loss
75-h
continuous
electrolysis.
Density
functional
theory
calculations
demonstrate
that
coordination
configuration
dopants
synergistically
contribute
enhanced
Sb-N
4
moieties.
Journal of the American Chemical Society,
Journal Year:
2022,
Volume and Issue:
144(28), P. 12807 - 12815
Published: July 5, 2022
The
renewable
energy-powered
electrolytic
reduction
of
carbon
dioxide
(CO2)
to
methane
(CH4)
using
water
as
a
reaction
medium
is
one
the
most
promising
paths
store
intermittent
energy
and
address
global
sustainability
problems.
However,
role
in
electrolyte
often
overlooked.
In
particular,
slow
dissociation
kinetics
limits
proton-feeding
rate,
which
severely
damages
selectivity
activity
methanation
process
involving
multiple
electrons
protons
transfer.
Here,
we
present
novel
tandem
catalyst
comprising
Ir
single-atom
(Ir1)-doped
hybrid
Cu3N/Cu2O
multisite
that
operates
efficiently
converting
CO2
CH4.
Experimental
theoretical
calculation
results
reveal
Ir1
facilitates
into
proton
feeds
sites
for
*CO
protonation
pathway
toward
*CHO.
displays
high
Faradaic
efficiency
75%
CH4
with
current
density
320
mA
cm-2
flow
cell.
This
work
provides
strategy
rational
design
high-efficiency
catalytic
systems.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(19)
Published: March 6, 2023
Nanozymes
aim
to
mimic
the
highly
evolved
active
centers
of
natural
enzymes.
Despite
progress
in
nanozyme
engineering,
their
catalytic
performance
is
much
less
favorable
compared
with
This
study
shows
that
precise
control
over
atomic
configuration
Co
single-atom
nanozymes
(SAzymes)
enables
rational
regulation
catalase-like
guided
by
theorical
calculations.
The
constructed
Co-N3
PS
SAzyme
exhibits
an
excellent
activity
and
kinetics,
exceeding
representative
controls
Co-based
SAzymes
different
configurations.
Moreover,
we
developed
ordered
structure-oriented
coordination
design
strategy
for
rationally
engineering
established
a
correlation
between
structure
enzyme-like
performance.
work
demonstrates
efficient
sites
Journal of the American Chemical Society,
Journal Year:
2022,
Volume and Issue:
144(48), P. 22075 - 22082
Published: Nov. 22, 2022
Single-atom
catalysts
have
exhibited
great
potential
in
the
photocatalytic
conversion
of
CO2
to
C2
products,
but
generation
gaseous
multi-carbon
hydrocarbon
products
is
still
challenging.
Previously,
supports
a
single
atom
consist
multiple
elements,
making
C-C
coupling
difficult
because
coordination
environment
single-atom
sites
diversified
and
control.
Here,
we
steer
by
implanting
an
Au
on
red
phosphorus
(Au1/RP),
support
with
uniform
structure
composed
element,
lower
electronegativity,
better
ability
absorb
CO2.
The
electron-rich
atoms
near
can
function
as
active
for
activation.
effectively
reduce
energy
barrier
coupling,
boosting
reaction
kinetics
formation
C2H6.
Notably,
C2H6
selectivity
turnover
frequency
Au1/RP
reach
96%
7.39
h-1
without
sacrificial
agent,
respectively,
which
almost
represents
best
photocatalyst
chemical
synthesis
date.
This
research
will
provide
new
ideas
design
high-efficiency
photocatalysts
products.
Nano Letters,
Journal Year:
2022,
Volume and Issue:
22(23), P. 9507 - 9515
Published: Nov. 15, 2022
An
Fe–N–C
catalyst
with
an
FeN4
active
moiety
has
gained
ever-increasing
attention
for
the
oxygen
reduction
reaction
(ORR);
however,
catalytic
performance
is
sluggish
in
acidic
solutions
and
regulation
still
a
challenge.
Herein,
Fe–Mo
dual-metal
sites
were
constructed
to
tune
ORR
activity
of
mononuclear
Fe
site
embedded
porous
nitrogen-doped
carbon.
The
cracking
O–O
bonds
much
more
facile
on
atomic
pair
due
preferred
bridge-cis
adsorption
model
molecules.
downshift
d
band
center
when
Mo
atom
introduced
FeNx
configuration
optimizes
absorption–desorption
behavior
intermediates
FeMoN6
moiety,
thus
boosting
performance.
construction
regulate
catalytically
paves
way
electrocatalytic
other
similar
non-precious-metal
catalysts.
Nature Communications,
Journal Year:
2023,
Volume and Issue:
14(1)
Published: Jan. 23, 2023
Abstract
Selective
two-electron
(2e
−
)
oxygen
reduction
reaction
(ORR)
offers
great
opportunities
for
hydrogen
peroxide
(H
2
O
electrosynthesis
and
its
widespread
employment
depends
on
identifying
cost-effective
catalysts
with
high
activity
selectivity.
Main-group
metal
nitrogen
coordinated
carbons
(M-N-Cs)
are
promising
but
remain
largely
underexplored
due
to
the
low
metal-atom
density
lack
of
understanding
in
structure-property
correlation.
Here,
we
report
using
a
nanoarchitectured
Sb
S
3
template
synthesize
high-density
(10.32
wt%)
antimony
(Sb)
single
atoms
nitrogen-
sulfur-codoped
carbon
nanofibers
(Sb-NSCF),
which
exhibits
both
selectivity
(97.2%)
mass
(114.9
A
g
−1
at
0.65
V)
toward
2e
ORR
alkaline
electrolyte.
Further,
when
evaluated
practical
flow
cell,
Sb-NSCF
shows
production
rate
7.46
mol
catalyst
h
negligible
loss
75-h
continuous
electrolysis.
Density
functional
theory
calculations
demonstrate
that
coordination
configuration
dopants
synergistically
contribute
enhanced
Sb-N
4
moieties.