Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(11)
Published: Jan. 16, 2024
Abstract
Ammonia
(NH
3
)
is
recognized
as
a
transportable
carrier
for
renewable
energy
fuels.
Photoelectrochemical
nitrate
reduction
reaction
(PEC
NO
RR)
offers
sustainable
solution
nitrate‐rich
wastewater
treatment
by
directly
converting
solar
to
ammonia.
In
this
study,
we
demonstrate
the
highly
selective
PEC
ammonia
production
from
RR
constructing
CoCu/TiO
2
/Sb
Se
photocathode.
The
constructed
photocathode
achieves
an
Faraday
efficiency
(FE)
of
88.01
%
at
−0.2
V
RHE
and
yield
high
15.91
μmol
h
−1
cm
−2
−0.3
with
excellent
onset
potential
0.43
.
Dynamics
experiments
theoretical
calculations
have
demonstrated
that
possesses
light
absorption
capacity,
transfer
capability,
charge
separation
efficiencies.
can
effectively
adsorb
reactant
−
intermediate,
CoCu
co‐catalyst
increases
maximum
Gibbs
free
difference
between
HER.
Meanwhile,
Co
species
enhances
spin
density
Cu,
states
near
Fermi
level
in
pdos,
which
results
activity
on
This
work
provides
new
avenue
feasibility
efficient
synthesis
wastewater.
Inorganic Chemistry,
Journal Year:
2022,
Volume and Issue:
61(25), P. 9514 - 9522
Published: June 14, 2022
Electrocatalytic
generation
of
oxygen
is
great
significance
for
sustainable,
clean,
and
efficient
energy
production.
Multiple
electron
transfer
in
evolution
reaction
(OER)
its
slow
kinetics
represent
a
serious
hedge
water
splitting,
requiring
the
design
development
advanced
electrocatalysts
with
porous
structures,
high
surface
areas,
abundant
electroactive
sites,
low
overpotentials.
These
requisites
are
common
metal-organic
frameworks
(MOFs)
derived
materials
that
promising
OER.
The
present
work
reports
on
synthesis
full
characterization
heteroleptic
3D
MOF,
[Zn2(μ4-odba)2(μ-bpdh)]n·nDMF
(Zn-MUM-1),
assembled
from
4,4'-oxydibenzoic
acid
2,5-bis(4-pyridyl)-3,4-diaza-2,4-hexadiene
(bpdh).
Besides,
series
heterometallic
MnZn-MUM-1
(abbreviated
as
Mn0.5Zn0.5-MUM-1,
Mn0.66Zn0.33-MUM-1,
Mn0.33Zn0.66-MUM-1)
was
also
prepared,
characterized,
used
fabrication
working
electrodes
based
Ni
foam
(NF),
followed
by
their
exploration
noble-metal-free
robust
stable
do
not
require
pyrolysis
or
calcination
while
exhibiting
better
electrocatalytic
performance
than
parent
Zn-MUM-1/NF
electrode.
experimental
results
show
Mn0.5Zn0.5-MUM-1/NF
electrocatalyst
features
best
OER
activity
overpotential
(253
mV
at
10
mA
cm-2)
Tafel
slope
(73
dec-1)
well
significant
stability
after
72
h
6000
cycles.
excellent
explained
synergic
effect
two
different
metals
Mn-Zn
MOF
improved
charge
ion
transfer,
conductivity,
characteristics.
study
thus
widens
application
MOFs
prospective
highly
Small,
Journal Year:
2023,
Volume and Issue:
20(3)
Published: Sept. 10, 2023
Abstract
The
development
of
efficient
and
low‐cost
catalysts
for
cathodic
oxygen
reduction
reaction
(ORR)
in
Zn‐air
battery
(ZAB)
is
a
key
factor
reducing
costs
achieving
industrialization.
Here,
novel
segregated
CoNiPt
alloy
embedded
N‐doped
porous
carbon
with
nanoflowers
(NFs)‐like
hierarchy
structure
synthesized
through
pyrolyzing
Hofmann‐type
metal‐organic
frameworks
(MOFs).
unique
hierarchical
NFs
exposes
more
active
sites
facilitates
the
transportation
intermediates,
thus
accelerating
kinetics.
Impressively,
resulting
15%
CoNiPt@C
catalyst
exhibits
outstanding
alkaline
ORR
activity
half‐wave
potential
0.93
V,
its
mass
7.5
times
higher
than
that
commercial
Pt/C
catalyst,
surpassing
state‐of‐the‐art
noble
metal‐based
catalysts.
Furthermore,
assembled
CoNiPt@C+RuO2
ZAB
demonstrates
maximum
power
density
172
mW
cm
−2
,
which
superior
to
Pt/C+RuO2
ZAB.
Experimental
results
reveal
intrinsic
attributed
synergistic
interaction
between
defects
pyrrolic/graphitic
N
species,
optimizes
adsorption
energy
intermediate
species
process
greatly
enhances
catalytic
activity.
This
work
provides
practical
feasible
strategy
synthesizing
cost‐effective
by
optimizing
electronic
MOF‐derived
Small,
Journal Year:
2023,
Volume and Issue:
19(45)
Published: July 11, 2023
Abstract
Compared
with
the
traditional
electrolysis
of
water
to
produce
hydrogen,
urea‐assisted
hydrogen
has
significant
advantages
and
received
extensive
attention
from
researchers.
Unfortunately,
urea
oxidation
reaction
(UOR)
involves
a
complex
six‐electron
transfer
process
leading
high
overpotential,
which
forces
researchers
develop
high‐performance
UOR
catalysts
drive
development
splitting.
Based
on
mechanism
literature
research,
this
review
summarizes
strategies
for
preparing
highly
efficient
catalysts.
First,
is
introduced
characteristics
excellent
are
pointed
out.
Aiming
at
this,
following
modulation
proposed
improve
catalytic
performance
based
summarizing
various
literature:
1)
Accelerating
active
phase
formation
reduce
initial
potential;
2)
Creating
double
sites
trigger
new
mechanism;
3)
adsorption
promoting
C─N
bond
cleavage
ensure
effective
conduct
UOR;
4)
Promoting
desorption
CO
2
stability
prevent
catalyst
poisoning;
5)
electron
overcome
inherent
slow
dynamics
6)
Increasing
or
surface
area.
Then,
application
in
electrochemical
devices
summarized.
Finally,
current
deficiencies
future
directions
discussed.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(47)
Published: July 16, 2023
Abstract
The
development
of
neutral
zinc–air
batteries
(ZABs)
is
long
been
impeded
by
the
sluggish
oxygen
reduction
reaction
(ORR)
derived
from
insufficient
O
2
activation
and
OH*
blocking
effect.
Herein,
synthesis
a
series
rare‐earth
Ce
single‐atom
catalysts
(CeNCs)
reported
with
enhanced
spin‐state
for
boosting
ORR.
Experimental
analysis
theoretical
calculations
indicate
that
unique
local
coordination/geometric
structure
reshapes
electronic
configuration
sites
to
achieve
transition
4d
10
4f
1
8
3
.
high‐spin
active
accelerate
unpaired
f
electrons
occupy
anti‐π
orbitals
generate
suitable
binding
strength
intermediates.
In
conditions,
CeNC‐40
exhibits
excellent
ORR
performance
half‐wave
potentials
0.78
V
negligible
decay
after
000
cycles.
Additionally,
self‐breathing
ZABs
based
on
demonstrates
peak
power
density
81
mW
cm
−2
impressive
long‐cycle
stability
(>1
600
cycles)
at
mA
This
work
presents
an
effective
strategy
developing
address
challenges
ZABs.
Advanced Energy Materials,
Journal Year:
2023,
Volume and Issue:
13(46)
Published: Oct. 27, 2023
Abstract
Precisely
designing
asymmetric
diatomic
configurations
and
studying
their
electronic
regulation
effect
for
improving
the
oxygen
reduction
reaction
(ORR)
performance
are
important
anion
exchange
membrane
fuel
cells
(AEMFCs).
Here,
a
Fe,
Cu
co‐doped
2D
crystalline
IISERP‐MOF27
nanosheet
derived
FeN
3
O‐CuN
4
site
nanocatalyst
(named
as
FeCu‐NC)
is
synthesized
cathodes
of
AEMFCs.
Thanks
to
optimal
structure
in
FeCu‐NC
catalyst,
it
shows
enhanced
half‐wave
potential
(0.910
V),
turnover
frequency
(0.165e
s
−1
),
decreased
activation
energy
(19.96
kJ
mol
)
KOH.
The
FeCu‐NC‐based
AEMFC
achieves
extremely
high
kinetic
current
(0.138
A
cm
−2
at
0.9
V)
rated
power
density
(1.09
W
surpassing
best‐reported
transition
metal‐based
cathodes.
Density
functional
theory
calculations
further
demonstrate
that
Cu‐N
can
break
localization
Fe‐3d
orbitals,
accelerate
electron
transport,
optimize
OH
adsorption,
thus
facilitating
ORR
process.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(39), P. 21273 - 21283
Published: Sept. 20, 2023
Introducing
a
second
metal
species
into
atomically
dispersed
metal-nitrogen-carbon
(M-N-C)
catalysts
to
construct
diatomic
sites
(DASs)
is
an
effective
strategy
elevate
their
activities
and
stabilities.
However,
the
common
pyrolysis-based
method
usually
leads
substantial
uncertainty
for
formation
of
DASs,
precise
identification
resulting
DASs
also
rather
difficult.
In
this
regard,
we
developed
two-step
specific-adsorption
(pyrolysis-free)
constructed
DAS
catalyst
featuring
FeCo
"molecular
heterostructures"
(FeCo-MHs).
order
rule
out
possibility
two
apparently
neighboring
(in
electron
microscopy
image)
Fe/Co
atoms
being
respectively
on
top/bottom
surfaces
carbon
support
thus
forming
"false"
MHs,
conducted
in
situ
rotation
(by
8°,
far
above
critical
angle
5.3°)
directly
identified
individual
FeCo-MHs.
The
FeCo-MHs
could
modulate
magnetic
moments
centers
increase
ratio
low-spin
Fe(II)-N4
moiety;
intrinsic
activity
be
optimized
at
apex
volcano-plot
(a
relationship
as
function
metal-phthalocyanine
complexes
catalytic
activities).
displays
exceptional
ORR
(E1/2
=
0.95
V)
used
high-performance
cathodes
hydroxide
exchange
membrane
fuel
cells
zinc-air
batteries.