Inorganic Chemistry,
Год журнала:
2024,
Номер
63(17), С. 7926 - 7936
Опубликована: Апрель 15, 2024
Heteroatom
doping
and
heterostructure
construction
are
the
key
methods
to
improve
performance
of
electrocatalysts.
However,
developing
such
catalysts
remains
a
challenging
task.
Herein,
we
designed
two
comparable
polymers,
phytic
acid/thiourea
polymer
(PATP)
acid/urea
(PAUP),
as
precursors,
which
contain
C,
N,
S/O,
P
by
microwave
heating.
To
pinpoint
how
introduction
sulfur
would
affect
electronic
structure
catalytic
activity,
these
polymers
were
physically
blended
with
CoCo-Prussian
blue
analogue
(CoCo-PBA)
further
calcination,
respectively.
The
highly
dispersed
CoP/Co2P-rich
interfacial
anchored
on
N,S-codoped
or
N-doped
carbon
support
successfully
prepared
(CoP/Co2P@CNS
CoP/Co2P@CN).
CoP/Co2P@CNS
catalyst
showed
good
ORR
properties
(E1/2
=
0.856
V
vs
RHE)
OER
(Ej10
1.54
RHE),
superior
commercial
Pt/C
RuO2
catalysts.
reversible
oxygen
electrode
index
(ΔE
Ej10
–
E1/2)
can
reach
∼0.684
V.
Meanwhile,
rechargeable
zinc–air
battery
assembled
air
cathode
also
excellent
performance,
charge–discharge
cycle
stability
up
900
h.
DFT
calculations
confirm
that
S
atoms
enhance
activity
C
N
support.
Advanced Materials,
Год журнала:
2024,
Номер
36(29)
Опубликована: Апрель 29, 2024
Abstract
The
development
of
high‐performance
electrocatalysts
for
energy
conversion
reactions
is
crucial
advancing
global
sustainability.
design
catalysts
based
on
their
electronic
properties
(e.g.,
work
function)
has
gained
significant
attention
recently.
Although
numerous
reviews
electrocatalysis
have
been
provided,
no
such
reports
function‐guided
electrocatalyst
are
available.
Herein,
a
comprehensive
summary
the
latest
advancements
in
diverse
electrochemical
applications
provided.
This
includes
function‐based
catalytic
activity
descriptors,
and
both
monolithic
heterostructural
catalysts.
measurement
function
first
discussed
descriptors
various
fully
analyzed.
Subsequently,
function‐regulated
material‐electrolyte
interfacial
electron
transfer
(IET)
employed
catalyst
design,
methods
regulating
optimizing
performance
discussed.
In
addition,
key
strategies
tuning
function‐governed
material‐material
IET
examined.
Finally,
perspectives
determination,
put
forward
to
guide
future
research.
paves
way
rational
efficient
sustainable
applications.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(37)
Опубликована: Май 6, 2024
Abstract
The
exploitation
of
highly
activity
oxygen
evolution
reaction
(OER)
electrocatalysts
is
critical
for
the
application
electrocatalytic
water
splitting.
Triggering
lattice
mechanism
(LOM)
expected
to
provide
a
promising
pathway
overcome
sluggish
OER
kinetics,
however,
effectively
enhancing
involvement
remains
challenging.
In
this
study,
fabrication
B,
Fe
co‐doped
CoP
(B,
Fe─CoP)
nanofibers
reported,
which
serve
as
efficient
electrocatalyst
through
phosphorization
and
boronation
treatment
Fe‐doped
Co
3
O
4
nanofibers.
Experimental
results
combined
with
theoretical
calculations
reveal
that
simultaneous
incorporation
both
B
can
more
trigger
participation
in
CoFe
oxyhydroxides
reconstructed
from
Fe─CoP
compared
incorporating
only
or
Fe.
Therefore,
optimized
exhibit
superb
low
overpotentials
361
376
mV
at
1000
mA
cm
−2
alkaline
freshwater
natural
seawater,
respectively.
present
work
provides
significant
guidelines
innovative
design
concepts
development
following
LOM
pathway.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(33)
Опубликована: Май 21, 2024
Abstract
Developing
highly
effective
transition
metal‐based
bifunctional
electrocatalysts
remains
a
tremendously
challenging
task
for
large‐scale
overall
water
splitting.
Herein,
multiheterostructured
Mo‐doped
Ni
2
P/Fe
x
P
electrocatalyst
on
NiFe
foam
with
vacancy
(denoted
as
Mo─Ni
P‐V/NFF)
is
developed
to
serve
an
efficient
dual‐pH
electrocatalyst.
Due
the
synergistic
effect
of
multiple
strategies
(heteroatom
doping,
heterointerface,
and
vacancy),
P‐V/NFF
possesses
remarkable
hydrogen
evolution
reaction
(HER)
catalytic
activity
in
alkaline/acidic
excellent
oxygen
(OER)
alkaline
media,
along
encouraging
durability.
The
mechanisms
improved
electrocatalytic
combining
multicharacterizations
density
functional
theory
(DFT)
calculations
are
elucidated.
Specifically,
X‐ray
absorption
fine
structure
experimental
analysis
confirms
that
Mo
doping
can
optimize
electronic
In
situ
Raman
spectroscopy
demonstrates
evolved
oxyhydroxides
real
active
substances
OER.
DFT
reveal
conductivity
as‐prepared
samples
be
enhanced
through
strategy
synergy.
Moreover,
HER
process,
not
only
reduce
binding
energy
near
zero
but
also
enhance
H
O
dissociation
*OH
desorption.
OER
verify
interface
engineering
adsorption
rate‐determining
step,
achieving
lowest
theoretical
overpotential.
