Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 12, 2024
Abstract
Deconstruction
of
polyethylene
terephthalate
(PET)
plastics
into
commodity
chemicals
such
as
glycine
presents
a
promising
route
for
waste
valorization.
However,
directly
upcycling
PET
via
thermocatalysis
typically
requires
harsh
conditions
(e.g.,
high
H
2
pressure
and
elevated
temperature)
while
suffering
from
limited
selectivity
carbon
footprint.
Herein,
cascade
thermochemical–electrochemical
catalysis
is
developed
to
exploit
end‐of‐life
with
yield,
without
the
use
hydrogen
gas
in
entire
process.
first
degraded
oxalic
acid
thermochemical
oxidative
depolymerization
using
an
active
robust
HY‐zeolite‐supported
Au
catalyst
under
low
O
(0.3
MPa),
then
valorize
intermediate
two‐step
electroreduction
over
earth‐abundant
TiO
catalyst.
The
proposed
approach
resilient
impurities
realistic
streams,
enables
continuous
conversion
various
goods
overall
yield
75%.
Techno‐economic
analysis
life
cycle
assessment
demonstrate
that
cost‐effective
low‐carbon
upcycling.
This
hybrid
technology
paves
way
leverage
mitigating
plastic
pollution
producing
high‐value
chemicals.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(46)
Published: Aug. 8, 2024
Abstract
Coupling
in
situ
generated
intermediates
with
other
substrates/intermediates
is
a
viable
approach
for
diversifying
product
outcomes
of
catalytic
reactions
involving
two
or
multiple
reactants.
Cyclohexanone
oxime
key
precursor
caprolactam
synthesis
(the
monomer
Nylon‐6),
yet
its
current
production
uses
unsustainable
carbon
sources,
noble
metal
catalysts,
and
harsh
conditions.
Herein,
we
report
the
first
work
to
synthesize
cyclohexanone
through
electroreduction
phenol
hydroxylamine.
The
Faradaic
efficiency
reached
69.1
%
over
Cu
catalyst,
accompanied
by
corresponding
formation
rate
82.0
g
h
−1
cat
.
In
addition,
conversion
was
up
97.5
%.
characterizations,
control
experiments,
theoretical
calculations
suggested
importance
balanced
activation
water,
phenol,
hydroxylamine
substrates
on
optimal
metallic
catalyst
achieving
high‐performance
synthesis.
Besides,
tandem
route
upgrading
lignin
has
been
successfully
developed
integration
thermal
catalysis,
electrocatalysis,
Beckmann
rearrangement,
which
achieved
0.40
from
4.0
raw
material.
ChemCatChem,
Journal Year:
2024,
Volume and Issue:
16(22)
Published: Aug. 13, 2024
Abstract
With
the
depletion
of
fossil
energy
sources,
growing
problem
environmental
pollution
and
increasing
emission
CO
2
,
research
direction
converting
emitted
into
valuable
chemicals
using
chemical
approaches
has
attracted
strong
interest.
In
recent
years,
a
great
deal
been
conducted
to
select
appropriate
strategies
realize
conversion
utilization
.
Among
them,
electrosynthesis
is
one
commonly
used
strategy
for
preparation
high
value‐added
chemicals,
which
obvious
advantages
such
as
simple
equipment
friendliness.
this
review,
we
focus
on
progress
electrocatalytic
C−N
coupling
involving
nitrogen‐containing
small
molecules
various
compounds.
We
start
review
with
discussion
fundamentals
reactions.
Next,
discuss
advances
in
synthesis
(e.
g.,
urea,
amines,
amides,
amino
acids,
oximes,
etc.)
by
reaction,
NH
3
N
NO
−
feedstocks.
Finally,
current
challenges
future
opportunities
field
are
presented.
The
goal
provide
state‐of‐the‐art
overview
electrochemical
coupled
systems
order
advance
their
practical
applications.
Angewandte Chemie,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Sept. 30, 2024
Abstract
Glycine
as
one
of
the
most
abundant
amino
acids
in
human
proteins,
with
extensive
applications
both
life
and
industry,
is
conventionally
synthesized
through
complex
procedures
or
toxic
feedstocks.
In
this
study,
we
present
a
facile
benign
electrochemical
pathway
for
synthesis
glycine
reductive
coupling
glyoxylic
acid
nitrate
over
copper‐bismuth
bimetal
catalyst
derived
from
metal–organic
framework
(MOF)
array
on
copper
foam
(Cu/Bi−C@CF).
Remarkably,
Cu/Bi−C@CF
achieves
fantastic
selectivity
89
%,
corresponding
high
Faraday
efficiency
65.9
%.
From
control
experiments,
introduction
Bi
caused
binding
energy
Cu
shift
to
lower
state,
which
leads
towards
formation
key
intermediate
hydroxylamine
rather
than
ammonia
product,
facilitating
oxime
providing
additional
sites
subsequent
hydrogenation
reaction
way
glycine.
Moreover,
derivation
MOF
arrays
ensures
effective
dispersion
enhances
stability
Cu/Bi−C@CF.
This
innovative
approach
not
only
presents
sustainable
pathways
production
value‐added
organonitrogen
compounds
utilizing
readily
available
carbon
nitrogen
sources,
but
also
provides
novel
insights
into
design
multistage
structural
catalysts
sequential
reactions.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 12, 2024
Abstract
Deconstruction
of
polyethylene
terephthalate
(PET)
plastics
into
commodity
chemicals
such
as
glycine
presents
a
promising
route
for
waste
valorization.
However,
directly
upcycling
PET
via
thermocatalysis
typically
requires
harsh
conditions
(e.g.,
high
H
2
pressure
and
elevated
temperature)
while
suffering
from
limited
selectivity
carbon
footprint.
Herein,
cascade
thermochemical–electrochemical
catalysis
is
developed
to
exploit
end‐of‐life
with
yield,
without
the
use
hydrogen
gas
in
entire
process.
first
degraded
oxalic
acid
thermochemical
oxidative
depolymerization
using
an
active
robust
HY‐zeolite‐supported
Au
catalyst
under
low
O
(0.3
MPa),
then
valorize
intermediate
two‐step
electroreduction
over
earth‐abundant
TiO
catalyst.
The
proposed
approach
resilient
impurities
realistic
streams,
enables
continuous
conversion
various
goods
overall
yield
75%.
Techno‐economic
analysis
life
cycle
assessment
demonstrate
that
cost‐effective
low‐carbon
upcycling.
This
hybrid
technology
paves
way
leverage
mitigating
plastic
pollution
producing
high‐value
chemicals.
