Journal of the American Chemical Society,
Journal Year:
2022,
Volume and Issue:
145(2), P. 1144 - 1154
Published: Dec. 20, 2022
Remolding
the
reactivity
of
metal
active
sites
is
critical
to
facilitate
renewable
electricity-powered
water
electrolysis.
Doping
heteroatoms,
such
as
Se,
into
a
crystal
lattice
has
been
considered
an
effective
approach,
yet
usually
suffers
from
loss
functional
heteroatoms
during
harsh
electrocatalytic
conditions,
thus
leading
gradual
inactivation
catalysts.
Here,
we
report
new
heteroatom-containing
molecule-enhanced
strategy
toward
sustainable
oxygen
evolution
improvement.
An
organoselenium
ligand,
bis(3,5-dimethyl-1H-pyrazol-4-yl)selenide
containing
robust
C–Se–C
covalent
bonds
equipped
in
precatalyst
ultrathin
metal–organic
nanosheets
Co-SeMON,
revealed
significantly
enhance
catalytic
mass
activity
cobalt
site
by
25
times,
well
extend
catalyst
operation
time
alkaline
conditions
1
or
2
orders
magnitude
compared
with
these
reported
selenides.
A
combination
various
situ/ex
situ
spectroscopic
techniques,
ab
initio
molecular
dynamics,
and
density
theory
calculations
unveiled
intensified
mechanism,
which
nonclassical
bonding
Se
O-containing
intermediates
endows
adsorption-energy
regulation
beyond
conventional
scaling
relationship.
Our
results
showcase
great
potential
catalysts
for
highly
efficient
economical
oxidation.
Advanced Functional Materials,
Journal Year:
2022,
Volume and Issue:
33(8)
Published: Dec. 20, 2022
Abstract
Metal–organic
frameworks
(MOFs)
have
emerged
as
ideal
multifunctional
platforms
for
renewable
hydrogen
(H
2
)
energy
applications
owing
to
their
tunable
chemical
compositions
and
structures
high
porosity.
Their
advanced
component
species
porous
structure
contribute
greatly
the
enhanced
activity,
electrical
conductivity,
photo
response,
charge‐hole
separation
efficiency,
structural
stability
of
MOF
materials,
which
are
promising
practical
H
economy.
In
this
review,
we
mainly
introduce
design
strategies
enhancement
electro‐/photochemical
behaviors
or
adsorption
performance
materials
production,
storage,
utilization
from
compositional
perspective.
Following
these
engineering
strategies,
correlation
between
composition
property‐structure‐performance
pristine
MOFs
composite
with
components
is
illustrated.
Finally,
challenges
directions
future
development
related
composites
economy
provided.
Journal of the American Chemical Society,
Journal Year:
2022,
Volume and Issue:
145(2), P. 1144 - 1154
Published: Dec. 20, 2022
Remolding
the
reactivity
of
metal
active
sites
is
critical
to
facilitate
renewable
electricity-powered
water
electrolysis.
Doping
heteroatoms,
such
as
Se,
into
a
crystal
lattice
has
been
considered
an
effective
approach,
yet
usually
suffers
from
loss
functional
heteroatoms
during
harsh
electrocatalytic
conditions,
thus
leading
gradual
inactivation
catalysts.
Here,
we
report
new
heteroatom-containing
molecule-enhanced
strategy
toward
sustainable
oxygen
evolution
improvement.
An
organoselenium
ligand,
bis(3,5-dimethyl-1H-pyrazol-4-yl)selenide
containing
robust
C–Se–C
covalent
bonds
equipped
in
precatalyst
ultrathin
metal–organic
nanosheets
Co-SeMON,
revealed
significantly
enhance
catalytic
mass
activity
cobalt
site
by
25
times,
well
extend
catalyst
operation
time
alkaline
conditions
1
or
2
orders
magnitude
compared
with
these
reported
selenides.
A
combination
various
situ/ex
situ
spectroscopic
techniques,
ab
initio
molecular
dynamics,
and
density
theory
calculations
unveiled
intensified
mechanism,
which
nonclassical
bonding
Se
O-containing
intermediates
endows
adsorption-energy
regulation
beyond
conventional
scaling
relationship.
Our
results
showcase
great
potential
catalysts
for
highly
efficient
economical
oxidation.
