Inorganic Chemistry,
Год журнала:
2023,
Номер
62(7), С. 3026 - 3035
Опубликована: Фев. 9, 2023
The
sluggish
oxygen
reduction
reaction
(ORR)
at
the
cathode
is
challenging
and
hinders
growth
of
hydrogen
fuel
cells.
Concerning
kinetic
values,
platinum
best
known
catalyst
for
ORR;
however,
its
less
abundance,
high
cost,
corrosive
nature
warrant
development
low-cost
catalysts.
We
report
hydrothermal
synthesis
two
novel
Mn-based
metal-organic
frameworks
(MOFs),
[Mn2(DOT)(H2O)2]n
(Mn-SKU-1)
[Mn2(DOT)2(BPY)2(THF)]n
(Mn-SKU-2)
(DOT
=
2,5-dihydroxyterephthalate;
BPY
4,4'-bipyridine).
Mn-SKU-1
contains
dimeric
Mn(II)
centers
where
corner-shared
MnO6
octahedra
fuse
to
give
rise
an
infinite
Mn2O10
cluster,
whereas
ions
coordinate
DOT
moieties
a
pillared
structure
in
Mn-SKU-2
form
3D
→
homo-interpenetration
MOF
with
twofold
interpenetrated
net.
pyrolysis
as-synthesized
Mn-MOFs
600
°C
under
N2
produced
exclusively
porous
α-Mn2O3
composites
(PSKU-1
PSKU-2),
BET
surface
area
90.8
(for
PSKU-1)
179.3
m2
g-1
PSKU-2).
These
mesoporous
MOF-derived
were
modified
as
materials
electrocatalytic
oxygen.
onset
potential
was
found
be
0.90
V
PSKU-1
0.93
PSKU-2
versus
RHE
0.1
M
KOH
solution,
current
density
4.8
6.0
mA
cm-2,
respectively,
1600
rpm.
Based
on
RDE/RRDE
results,
occurs
majorly
via
four-electron
process.
electrocatalyst
cheap,
easy
use,
retains
90%
activity
after
10
h
continuous
offers
higher
recyclability
than
Pt/C.
maximum
values
(Jk
11.68
cm-2
Tafel
slope
85.0
mV
dec-1)
obtained
this
work
are
reported
pure
Mn2O3.
Dalton Transactions,
Год журнала:
2023,
Номер
52(26), С. 8850 - 8856
Опубликована: Янв. 1, 2023
A
structurally
characterized
porous
Ag(I)-molecular
cage
AgMOC
and
a
Cu(II)-coordination
polymer
CuCP
with
pre-synthesized
ligand
1,3-bis(((E)-2-methoxybenzylidene)amino)propan-2-ol
its
parental
amine
thiocyanate
are
reported
to
harness
electrical
mobility-driven
hydrogen
evolution
activity.
Porosity-induced
electrically
conductive
emerges
as
better
electrocatalyst
Tafel
slope
of
104
mV
per
decade
over
Cu(II)-polymer's
128
decade.
The
electrochemical
stability
durability
the
designed
electrocatalysts
in
harnessing
HER
activity
also
examined
under
experimental
conditions.
Abstract
Metal–organic
frameworks
(MOFs)
are
crystalline
porous
materials
with
a
long‐range
ordered
structure
and
excellent
specific
surface
area
have
found
wide
range
of
applications
in
diverse
fields,
such
as
catalysis,
energy
storage,
sensing,
biomedicine.
However,
their
poor
electrical
conductivity
chemical
stability,
low
capacity,
weak
adhesion
to
substrates
greatly
limited
performance.
Doping
has
emerged
unique
strategy
mitigate
the
issues.
In
this
review,
concept,
classification,
characterization
methods
doped
MOFs
first
introduced,
recent
progress
synthesis
MOFs,
well
rapid
advancements
first‐principles
calculations
based
on
density
functional
theory
(DFT)
unraveling
mechanistic
origin
enhanced
performance
summarized.
Finally,
perspective
is
included
highlight
key
challenges
doping
MOF
an
outlook
provided
future
research
directions.
Chemistry - A European Journal,
Год журнала:
2024,
Номер
unknown
Опубликована: Апрель 16, 2024
Although
it
is
well-known
that
the
Lewis
acidity
of
Metal-Organic
Frameworks
(MOFs)
can
effectively
enhance
their
catalytic
activity
in
organic
transformations,
access
to
these
Lewis-acidic
sites
remains
a
key
hurdle
widespread
applications
catalysis
by
MOFs.
Easy
accessibility
strong
acidic
onto
2D
MOFs
using
proper
activation
methods
be
cornerstone
attaining
desired
performance.
Herein,
we
report
new
chemically
stable
MOF,
IITKGP-60,
which
displayed
excellent
framework
robustness
over
wide
pH
range
(2-12).
Benefiting
from
abundant
open
metal
(OMSs)
and
robustness,
developed
material
was
explored
one-pot
three-component
Strecker
reaction
Knoevenagel
condensation
reaction.
Moreover,
catalyst
superior
catalyzing
reactions
involving
sterically
hindered
substrate
(1-naphthaldehyde)
with
high
turnover
number.
A
comparative
study
conducted
different
(chloroform
methanol
exchanged
activated
samples),
highlighting
significant
effect
on
its
performances.
The
sustainable
synthetic
pathway
under
solvent-free
conditions
for
broad
scope
substrates
low
loading
recyclability
made
pH-stable
promising
heterogeneous
catalyst.
