Accounts of Materials Research,
Journal Year:
2022,
Volume and Issue:
4(1), P. 42 - 56
Published: Dec. 1, 2022
ConspectusHydrogen
is
deemed
as
an
ideal
energy
carrier
because
of
its
high
density
and
clean
nature.
Water
electrolysis
fairly
competitive
for
hydrogen
production
due
to
the
conversion
renewable
electricity
high-purity
H2
with
no
carbon
emission,
in
comparison
traditional
industrial
technology.
However,
large-scale
application
hampered
by
cost
partially
from
use
noble
metal-based
catalysts
promote
kinetics
oxygen
evolution
reactions.
Developing
cost-efficient
transition
electrocatalysts,
therefore,
a
hopeful
prospect,
they
can
provide
d-orbital
lone-pair
electrons
or
empty
d-orbitals
adsorbing
different
intermediates
(such
H*,
OH*,
O*,
OOH*).
As
compared
metals
their
oxides,
metal
interstitial
compounds
(TMICs)
formed
inserting
C,
N,
P
atoms
into
sites
parent
hold
distinct
advantages
Pt-like
electronic
structure,
conductivity,
superior
chemical
stability
over
wide
pH
range,
beneficial
overcoming
consumption
faced
alkaline
water
intractable
issue
acid
electrolysis.
Nevertheless,
major
drawbacks
are
large
size,
density,
sluggish
ionic
kinetics,
resulting
ordinary
electrochemical
activity
low
mass
efficiency.
Electrocatalytic
performance
dominated
intrinsic
activity,
number
accessible
active
sites,
capacity
charge
transfer.
Engineering
micronano
structure
(small-size
particles,
porous
ultrathin
nanosheet)
expose
more
catalytical
facilitate
transport
gas
diffusion.
Meanwhile,
modulating
optimize
adsorption
boost
activity.
Apparently,
synergistic
modulation
TMICs
expected
achieve
multiobjective
optimization
targeting
highly
effective
catalysts.In
this
Account,
we
summarize
our
recent
efforts
designed
synthesis
engineering
utilizing
polyoxometalates
(POMs)
precursors
associated
strategies
advance
electrocatalytic
toward
HER
OER.
We
start
brief
summary
OER
mechanisms,
which
play
crucial
roles
elaborate
design
relevant
electrocatalysts.
The
disadvantages
pointed
out,
apart
opportunities
offered
POMs
constructing
novel
component,
interface
structure.
Several
efficient
enhancement
proposed
including
reducing
size
heterojunctions
interfaces,
doping
heteroatoms
regulate
binding
intermediates,
creating
pores
accelerate
transfer,
etc.
Accordingly,
controllable
well-defined
highlighted,
positive
role
tailoring
on
enhancing
catalytic
efficiency
confirmed.
Furthermore,
paired
electrocatalysis
using
species
produce
value-added
chemicals
reduce
consumption.
Finally,
remaining
challenges,
opportunities,
future
development
directions
TMICs-based
materials
discussed.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
36(41)
Published: Aug. 15, 2024
Abstract
Modulating
the
electronic
structure
of
catalysts
to
effectively
couple
hydrogen
evolution
reaction
(HER)
and
oxygen
(OER)
is
essential
for
developing
high‐efficiency
anion
exchange
membrane
water
electrolyzer
(AEMWE).
Herein,
a
coral‐like
nanoarray
composed
nanosheets
through
synergistic
layering
effect
cobalt
1D
guiding
vanadium
synthesized,
which
promotes
extensive
contact
between
active
sites
electrolyte.
The
HER
OER
activities
can
be
enhanced
by
modulating
nitridation
phosphorization,
respectively,
enhancing
strength
metal‐H
bond
optimize
adsorption
facilitating
proton
transfer
improve
transformation
oxygen‐containing
intermediates.
Resultantly,
AEMWE
achieves
current
density
500
mA
cm
–2
at
1.76
V
1000
h
in
1.0
M
KOH
70
°C.
energy
consumption
4.21
kWh
Nm
–3
with
producing
cost
$0.93
per
kg
H
2
.
Operando
synchrotron
radiation
Bode
phase
angle
analyses
reveal
that
during
high‐energy
consumed
OER,
dissolution
species
transforms
distorted
Co−O
octahedral
into
regular
structures,
accompanied
shortening
Co−Co
length.
This
structural
facilitates
formation
intermediates,
thus
accelerating
kinetics.
Energy & Environmental Science,
Journal Year:
2024,
Volume and Issue:
17(5), P. 1950 - 1960
Published: Jan. 1, 2024
An
oxygen-coordinated
cobalt
single-atom
catalyst
was
successfully
fabricated,
exhibiting
exceptional
electrocatalytic
activity
toward
urea
and
H
2
O
production.
Subsequently,
the
value-added
peroxide
efficiently
synthesized.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(28)
Published: Feb. 24, 2024
Abstract
It
is
important
to
tune
the
coordination
configuration
of
dual‐atom
catalyst
(DAC),
especially
in
first
sphere,
render
high
intrinsic
catalytic
activities
for
oxygen
reduction/evolution
reactions
(ORR/OER).
Herein,
a
type
atomically
dispersed
and
boron‐coordinated
DAC
structure,
namely,
FeN
4
B‐NiN
B
dual
sites,
reported.
In
this
incorporation
boron
into
sphere
/NiN
atomic
sites
regulates
its
geometry
electronic
structure
by
forming
“Fe‐B‐N”
“Ni‐B‐N”
bridges.
The
exhibits
much
enhanced
ORR
OER
property
compared
‐NiN
counterparts.
Density
functional
theory
calculations
reveal
that
boron‐induced
charge
transfer
asymmetric
distributions
central
Fe/Ni
atoms
optimize
adsorption
desorption
behavior
ORR/OER
intermediates
reduce
activation
energy
potential‐determining
step.
Zinc‐air
batteries
employing
cathode
exhibit
maximum
power
density
(236.9
mW
cm
−2
)
stable
cyclability
up
1100
h.
result
illustrates
pivotal
role
first‐coordination
DACs
tuning
electrochemical
conversion
storage
activities.
Chemical Science,
Journal Year:
2024,
Volume and Issue:
15(29), P. 11188 - 11228
Published: Jan. 1, 2024
The
oxygen
reduction
reaction
(ORR)
is
a
key
component
for
many
clean
energy
technologies
and
other
industrial
processes.
However,
the
low
selectivity
sluggish
kinetics
of
ORR
catalysts
have
hampered
conversion
efficiency
real
application
these
new
mentioned
before.
Recently,
tremendous
efforts
been
made
in
mechanism
understanding,
electrocatalyst
development
system
design.
Here,
comprehensive
critical
review
provided
to
present
recent
advances
field
electrocatalytic
ORR.
two-electron
four-electron
transfer
catalytic
mechanisms
evaluation
parameters
are
discussed
first.
Then,
up-to-date
synthetic
strategies
Accounts of Materials Research,
Journal Year:
2022,
Volume and Issue:
4(1), P. 42 - 56
Published: Dec. 1, 2022
ConspectusHydrogen
is
deemed
as
an
ideal
energy
carrier
because
of
its
high
density
and
clean
nature.
Water
electrolysis
fairly
competitive
for
hydrogen
production
due
to
the
conversion
renewable
electricity
high-purity
H2
with
no
carbon
emission,
in
comparison
traditional
industrial
technology.
However,
large-scale
application
hampered
by
cost
partially
from
use
noble
metal-based
catalysts
promote
kinetics
oxygen
evolution
reactions.
Developing
cost-efficient
transition
electrocatalysts,
therefore,
a
hopeful
prospect,
they
can
provide
d-orbital
lone-pair
electrons
or
empty
d-orbitals
adsorbing
different
intermediates
(such
H*,
OH*,
O*,
OOH*).
As
compared
metals
their
oxides,
metal
interstitial
compounds
(TMICs)
formed
inserting
C,
N,
P
atoms
into
sites
parent
hold
distinct
advantages
Pt-like
electronic
structure,
conductivity,
superior
chemical
stability
over
wide
pH
range,
beneficial
overcoming
consumption
faced
alkaline
water
intractable
issue
acid
electrolysis.
Nevertheless,
major
drawbacks
are
large
size,
density,
sluggish
ionic
kinetics,
resulting
ordinary
electrochemical
activity
low
mass
efficiency.
Electrocatalytic
performance
dominated
intrinsic
activity,
number
accessible
active
sites,
capacity
charge
transfer.
Engineering
micronano
structure
(small-size
particles,
porous
ultrathin
nanosheet)
expose
more
catalytical
facilitate
transport
gas
diffusion.
Meanwhile,
modulating
optimize
adsorption
boost
activity.
Apparently,
synergistic
modulation
TMICs
expected
achieve
multiobjective
optimization
targeting
highly
effective
catalysts.In
this
Account,
we
summarize
our
recent
efforts
designed
synthesis
engineering
utilizing
polyoxometalates
(POMs)
precursors
associated
strategies
advance
electrocatalytic
toward
HER
OER.
We
start
brief
summary
OER
mechanisms,
which
play
crucial
roles
elaborate
design
relevant
electrocatalysts.
The
disadvantages
pointed
out,
apart
opportunities
offered
POMs
constructing
novel
component,
interface
structure.
Several
efficient
enhancement
proposed
including
reducing
size
heterojunctions
interfaces,
doping
heteroatoms
regulate
binding
intermediates,
creating
pores
accelerate
transfer,
etc.
Accordingly,
controllable
well-defined
highlighted,
positive
role
tailoring
on
enhancing
catalytic
efficiency
confirmed.
Furthermore,
paired
electrocatalysis
using
species
produce
value-added
chemicals
reduce
consumption.
Finally,
remaining
challenges,
opportunities,
future
development
directions
TMICs-based
materials
discussed.