As
an
important
sustainable
method
for
chemical
synthesis,
organic
electrosynthesis
experienced
a
renaissance
in
recent
years
its
excellent
atom
economy.
Although
microchannel
reactors
have
been
proposed
to
advanced
devices
obtain
low
energy
cost
and
high
reaction
performance,
the
complex
multiphasic
flow
electrochemical
microchannels
are
very
less
reported
effects
of
condition
on
reported.
Taking
tetraethyl
thiuram
disulfide
(TETD)
as
typical
case,
we
developed
visualized
reactor
equipped
with
fluorine-doped
tin
oxide
(FTO)
loaded
glass
electrode
investigate
gas-liquid-liquid
triple
phase
pattern
main
factors
influenced
response
current
at
certain
applied
cell
voltage.
The
hybrid
gas
hold-up
liquid
rate
was
found
crucial
preventing
coverage
TETD
electrode,
which
provided
23.1
%
attenuation
ratio
3.0
V
research
not
only
exhibited
evolution
mechanism
current,
but
also
showed
importance
control
balancing
work
efficiency
consumption
process.
Advanced Functional Materials,
Год журнала:
2023,
Номер
34(6)
Опубликована: Ноя. 7, 2023
Abstract
Construction
of
efficient
catalysts
to
couple
biomass
upgrading
with
hydrogen
production
is
significant
for
improving
energy
efficiency,
which
remains
a
challenge.
Herein,
general
method
manufacturing
3D
hierarchical
micro‐nano
arrays
consisting
template
framework
and
nanoparticle‐decorated
nanosheets
reported.
This
strategy
provides
an
opportunity
controllably
tailor
the
interfacial
assembly
on
precursor
materials.
The
obtained
Co@NiMoO‐Ni/NF
exhibits
enhanced
electrocatalytic
performance
oxidation
production.
It
only
needs
1.21
V
achieve
10
mA
cm
−2
5‐hydroxymethylfurfural
electrooxidation
reaction
(HMFOR)
assisted
H
2
evolution
(HER).
good
catalytic
ascribed
intense
interaction
between
(Co)
(NiMoO‐Ni),
tunes
electron
structure
catalyst
optimize
adsorption
behavior
HMFOR/HER
intermediates
promote
bonds
breakage
key
in
process.
work
thus
designing
ideal
upgrading‐coupled
Advanced Science,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 7, 2025
Abstract
Overall
water
splitting
(OWS)
to
produce
hydrogen
has
attracted
large
attention
in
recent
years
due
its
ecological‐friendliness
and
sustainability.
However,
the
efficiency
of
OWS
been
forced
by
sluggish
kinetics
four‐electron
oxygen
evolution
reaction
(OER).
The
replacement
OER
alternative
electrooxidation
small
molecules
with
more
thermodynamically
favorable
potentials
may
fundamentally
break
limitation
achieve
production
low
energy
consumption,
which
also
be
accompanied
value‐added
chemicals
than
or
electrochemical
degradation
pollutants.
This
review
critically
assesses
latest
discoveries
coupled
various
OWS,
including
alcohols,
aldehydes,
amides,
urea,
hydrazine,
etc.
Emphasis
is
placed
on
corresponding
electrocatalyst
design
related
mechanisms
(e.g.,
dual
hydrogenation
N–N
bond
breaking
hydrazine
C═N
regulation
urea
inhibit
hazardous
NCO
−
NO
productions,
etc.),
along
emerging
reactions
(electrooxidation
tetrazoles,
furazans,
iodide,
quinolines,
ascorbic
acid,
sterol,
trimethylamine,
etc.).
Some
new
decoupled
electrolysis
self‐powered
systems
are
discussed
detail.
Finally,
potential
challenges
prospects
highlighted
aid
future
research
directions.
Abstract
To
overcome
the
low
efficiency
of
overall
water
splitting,
highly
effective
and
stable
catalysts
are
in
urgent
need,
especially
for
anode
oxygen
evolution
reaction
(OER).
In
this
case,
nickel
selenides
appear
as
good
candidates
to
catalyze
OER
other
substitutable
anodic
reactions
due
their
high
electronic
conductivity
easily
tunable
structure
meet
optimized
adsorption
ability.
Herein,
an
interesting
phase
transition
from
hexagonal
NiSe
(H‐NiSe)
rhombohedral
(R‐NiSe)
induced
by
doping
cobalt
atoms
is
reported.
The
five‐coordinated
R‐NiSe
found
grow
adjacent
six‐coordinated
H‐NiSe,
resulting
formation
H‐NiSe/R‐NiSe
heterostructure.
Further
characterizations
calculations
prove
reduced
splitting
energy
thus
less
occupancy
t
2g
orbits,
which
can
facilitate
electron
transfer
process.
As
a
result,
Co
2
‐NiSe/NF
shows
satisfying
catalytic
performance
toward
OER,
hydrogen
reaction,
(hybrid)
splitting.
This
work
proves
that
trace
amounts
induce
H‐NiSe
R‐NiSe.
less‐coordinated
species
reduce
enhance
performance,
might
guide
rational
material
design.
Advanced Energy Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Июнь 10, 2024
Abstract
Electrocatalytic
oxidation
of
glycerol,
an
oversupplied
byproduct
the
biodiesel
industry,
into
high‐valued
chemicals
is
alluring
to
diminishing
current
dependence
on
fossil
energy.
Formic
acid
important
glycerol
product
that
serves
as
a
high‐energy‐density
fuel
and
crucial
precursor
for
fine
chemical
industry
while
developing
electrocatalyst
efficiently
convert
formic
remains
challenge.
Herein,
Cu‐doped
nickel
phosphide
(Cu
x
Ni
2–
P)
electrocatalyst,
achieving
formate
productivity
≈11
mol
m
−2
h
−1
at
1.54
V
versus
RHE
over
broad
concentration
range
(10–100
)
reported,
which
greater
than
threefolds
2
P.
Furthermore,
Cu
P
can
enhance
cleavage
C─C
bond
in
reducing
production
intermediates
thus
attaining
high
selectivity
formate.
In
situ
experiments
integrated
with
density
functional
theory
(DFT)
calculation
revealed
doping
promote
generation
III
─OOH
species
enrich
substrates
local
environments
surface,
facilitating
reaction
efficiency.
Finally,
study
designed
membrane‐free
flow
electrolyzer
continuous
upgrading
formate,
16.4
mmol
coupled
0.68
L
H
1.75
8
h.
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(23)
Опубликована: Март 30, 2024
Abstract
Electrocatalytic
conversion
of
amines
to
nitriles
can
be
used
as
biomass
upgrading
assist
hydrogen
production
in
water
electrolysis.
However,
achieving
efficient
N─H/C─H
bond
breaking
oxidation
remains
a
challenge.
Herein,
the
nitrogen‐doped
carbon
supported
NiO
nanoparticles
with
positive
electronic
nickel
active
site
are
simply
synthesized
achieve
∽99%
selectivity
and
complete
electrooxidizing
nitriles,
onset
potential
whole
reaction
is
low
1.32
V
vs.
RHE.
Detailed
situ
characterizations
theoretical
calculations
prove
that
substrate
enhances
interaction
between
N
2p
orbital
Ni
3d
orbital,
which
favors
construction
an
indirect
intermediate
state
R‐CH
2
NH
···NiO(OH)
abs
promotes
subsequent
stepwise
dehydrogenation
nitriles.
This
produces
16.4
times
more
than
pure
splitting,
facilitating
development
chemicals
industry
energy
utilization.
