Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(30)
Published: May 9, 2024
Abstract
Based
on
the
electron‐withdrawing
effect
of
Pt(bpy)Cl
2
molecule,
a
simple
post‐modification
amide
reaction
was
firstly
used
to
graft
it
onto
surface
NH
‐MIL‐125,
which
performed
as
highly
efficient
electron
acceptor
that
induced
conversion
photoinduced
charge
migration
pathway
from
internal
BDC→TiO
x
external
BDC→PtN
migration,
significantly
improving
efficiency
transfer
and
separation.
Furthermore,
precisely
regulating
over
first
coordination
sphere
Pt
single
atoms
achieved
using
further
with
additional
bipyridine
investigate
Pt−N
numbers
activity.
The
as‐synthesized
NML‐PtN
exhibited
superior
photocatalytic
hydrogen
evolution
activity
7.608
mmol
g
−1
h
,
remarkable
improvement
225
2.26
times
compared
pristine
‐MIL‐125
4
respectively.
In
addition,
apparent
quantum
yield
4.01
%
(390
nm)
turnover
frequency
190.3
(0.78
wt
SA;
129
nanoparticles/NML)
revealed
high
solar
utilization
material.
And
macroscopic
color
changes
caused
by
transition
carrier
paths
observed.
It
holds
profound
significance
for
design
MOF‐Molecule
catalysts
separation
precise
regulation
single‐atom
sphere.
ACS Applied Materials & Interfaces,
Journal Year:
2024,
Volume and Issue:
16(26), P. 33657 - 33668
Published: June 21, 2024
Reduction
of
soluble
U(VI)
to
insoluble
U(IV)
based
on
photocatalysts
is
a
simple,
environmentally
friendly,
and
efficient
method
for
treating
radioactive
wastewater.
The
present
study
involved
the
systematic
comparison
photoelectric
properties
three
metalloporphyrins
with
different
metal
centers
synthesis
novel
porphyrin-based
hydrogen-bonded
organic
framework
(Ni-pHOF)
photocatalyst
by
modulating
surface
charge
microenvironment
in
porphyrin
enhanced
photocatalytic
removal
from
Compared
metal-free
HOF,
around
Ni
atom
Ni-pHOF
accelerated
reduction
kinetics
under
visible
light
illumination
at
initial
moment,
showing
high
rate,
even
air.
rate
aqueous
solution
can
achieve
over
98%
presence
coexisting
nonoxidizing
cations
only
decreased
less
than
8%
after
five
cycles,
exhibiting
selectivity
good
reusability.
Furthermore,
remove
86.74%
real
low-level
wastewater
120
min
illumination,
showcasing
practical
application
potential.
Density
functional
theory
(DFT)
calculations
electron
paramagnetic
resonance
(EPR)
spectra
indicated
that
through
metallization
conducive
improving
separation
efficiency,
prompting
more
e–
•O2–
participate
reaction
U(VI).
This
work
provides
new
insights
into
HOFs
paves
way
tailoring
HOFs/COFs
recovery
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(30)
Published: May 9, 2024
Abstract
Based
on
the
electron‐withdrawing
effect
of
Pt(bpy)Cl
2
molecule,
a
simple
post‐modification
amide
reaction
was
firstly
used
to
graft
it
onto
surface
NH
‐MIL‐125,
which
performed
as
highly
efficient
electron
acceptor
that
induced
conversion
photoinduced
charge
migration
pathway
from
internal
BDC→TiO
x
external
BDC→PtN
migration,
significantly
improving
efficiency
transfer
and
separation.
Furthermore,
precisely
regulating
over
first
coordination
sphere
Pt
single
atoms
achieved
using
further
with
additional
bipyridine
investigate
Pt−N
numbers
activity.
The
as‐synthesized
NML‐PtN
exhibited
superior
photocatalytic
hydrogen
evolution
activity
7.608
mmol
g
−1
h
,
remarkable
improvement
225
2.26
times
compared
pristine
‐MIL‐125
4
respectively.
In
addition,
apparent
quantum
yield
4.01
%
(390
nm)
turnover
frequency
190.3
(0.78
wt
SA;
129
nanoparticles/NML)
revealed
high
solar
utilization
material.
And
macroscopic
color
changes
caused
by
transition
carrier
paths
observed.
It
holds
profound
significance
for
design
MOF‐Molecule
catalysts
separation
precise
regulation
single‐atom
sphere.