The
photoelectrochemical
(PEC)
conversion
of
organic
small
molecules
offers
a
dual
benefit
synthesizing
value-added
chemicals
and
concurrently
producing
hydrogen
(H2).
Ethylene
glycol,
with
its
hydroxyl
groups,
stands
out
as
versatile
substrate
capable
yielding
various
C1
C2
chemicals.
In
this
study,
we
demonstrate
that
pH
modulation
markedly
enhances
the
photocurrent
BiVO4
photoanodes,
thus
facilitating
efficient
oxidation
ethylene
glycol
while
simultaneously
generating
H2.
Our
findings
reveal
in
pH=1
solution,
density
at
1.23
V
vs.
RHE
can
attain
an
impressive
7.1
mA
cm−2,
significantly
surpassing
outputs
neutral
highly
alkaline
environments.
increase
is
attributed
to
augmented
adsorption
on
under
acidic
conditions,
which
turn
elevates
activity
reaction,
culminating
maximal
production
formic
acid.
This
investigation
sheds
light
pivotal
role
electrolyte
PEC
process
underscores
potential
strategy
for
biomass
valorization
into
products
alongside
H2
fuel
generation.
Advanced Materials,
Год журнала:
2024,
Номер
36(21)
Опубликована: Фев. 11, 2024
Abstract
Photoelectrochemical
(PEC)
catalysis
provides
the
most
promising
avenue
for
producing
value‐added
chemicals
and
consumables
from
renewable
precursors.
Over
last
decades,
PEC
catalysis,
including
reduction
of
feedstock,
oxidation
organics,
activation
functionalization
C─C
C─H
bonds,
are
extensively
investigated,
opening
new
opportunities
employing
technology
in
upgrading
readily
available
resources.
However,
several
challenges
still
remain
unsolved,
hindering
commercialization
process.
This
review
offers
an
overview
targeted
at
synthesis
high‐value
sustainable
First,
fundamentals
evaluating
reactions
context
product
both
anode
cathode
recalled.
Then,
common
photoelectrode
fabrication
methods
that
have
been
employed
to
produce
thin‐film
photoelectrodes
highlighted.
Next,
advancements
systematically
reviewed
discussed
conversion
various
feedstocks
highly
valued
chemicals.
Finally,
prospects
field
presented.
aims
facilitating
further
development
precursors
products
other
pharmaceuticals.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Июнь 28, 2024
Abstract
Dihydroxyacetone
is
the
most
desired
product
in
glycerol
oxidation
reaction
because
of
its
highest
added
value
and
large
market
demand
among
all
possible
products.
However,
selectively
oxidative
secondary
hydroxyl
groups
for
highly
efficient
dihydroxyacetone
production
still
poses
a
challenge.
In
this
study,
we
engineer
surface
BiVO
4
by
introducing
bismuth-rich
domains
oxygen
vacancies
(Bi-rich
4-x
)
to
systematically
modulate
adsorption
enhance
photo-induced
charge
separation
photoelectrochemical
into
conversion.
As
result,
Bi-rich
increases
photocurrent
density
from
1.42
4.26
mA
cm
−2
at
1.23
V
vs.
reversible
hydrogen
electrode
under
AM
1.5
G
illumination,
as
well
selectivity
54.0%
80.3%,
finally
achieving
rate
361.9
mmol
m
h
−1
that
outperforms
reported
values.
The
atom
customization
opens
way
regulate
solar-driven
organic
transformation
pathway
toward
carbon
chain-balanced
product.
Chemical Reviews,
Год журнала:
2024,
Номер
124(20), С. 11348 - 11434
Опубликована: Окт. 9, 2024
Environmental
catalysis
has
emerged
as
a
scientific
frontier
in
mitigating
water
pollution
and
advancing
circular
chemistry
reaction
microenvironment
significantly
influences
the
catalytic
performance
efficiency.
This
review
delves
into
engineering
within
liquid-phase
environmental
catalysis,
categorizing
microenvironments
four
scales:
atom/molecule-level
modulation,
nano/microscale-confined
structures,
interface
surface
regulation,
external
field
effects.
Each
category
is
analyzed
for
its
unique
characteristics
merits,
emphasizing
potential
to
enhance
efficiency
selectivity.
Following
this
overview,
we
introduced
recent
advancements
advanced
material
system
design
promote
(e.g.,
purification,
transformation
value-added
products,
green
synthesis),
leveraging
state-of-the-art
technologies.
These
discussions
showcase
was
applied
different
reactions
fine-tune
regimes
improve
from
both
thermodynamics
kinetics
perspectives.
Lastly,
discussed
challenges
future
directions
engineering.
underscores
of
intelligent
materials
drive
development
more
effective
sustainable
solutions
decontamination.
Energy & Environmental Science,
Год журнала:
2024,
Номер
17(20), С. 7459 - 7511
Опубликована: Янв. 1, 2024
This
review
provides
a
comprehensive
overview
on
the
mechanism
of
photoelectrochemical
biomass
conversion
and
highlights
extension
dual-function
cells
for
valorization
paired
with
more
valuable
half-reactions.
Organic
electrosynthesis
in
aqueous
media
is
presently
hampered
by
the
poor
solubility
of
many
organic
reactants
and
thus
low
purity
liquid
products
electrolytes.
Using
electrooxidation
benzyl
alcohol
(BA)
as
a
model
reaction,
we
present
"sandwich-type"
organic-solid-water
(OSW)
system,
consisting
BA
phase,
KOH
electrolyte,
porous
anodes
with
Janus-like
superwettability.
The
system
allows
independent
diffusion
molecules
from
phase
to
electrocatalytic
active
sites,
enabling
efficient
high-concentration
benzaldehyde
(97%
Faradaic
efficiency
at
~180
mA
cm
