Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(51)
Опубликована: Окт. 6, 2022
Abstract
The
electrochemical
oxidation
of
small
molecules
to
generate
value‐added
products
has
gained
enormous
interest
in
recent
years
because
the
advantages
benign
operation
conditions,
high
conversion
efficiency
and
selectivity,
absence
external
oxidizing
agents,
eco‐friendliness.
Coupling
replace
oxygen
evolution
reaction
(OER)
at
anode
hydrogen
(HER)
cathode
an
electrolyzer
would
simultaneously
realize
generation
high‐value
chemicals
or
pollutant
degradation
highly
efficient
production
hydrogen.
This
Minireview
presents
introduction
on
small‐molecule
choice
design
strategies
electrocatalysts
as
well
breakthroughs
achieved
Finally,
challenges
future
orientations
are
highlighted.
Advanced Functional Materials,
Год журнала:
2020,
Номер
30(21)
Опубликована: Фев. 27, 2020
Abstract
Hydrogen
production
via
water
electrocatalysis
is
limited
by
the
sluggish
anodic
oxygen
evolution
reaction
(OER)
that
requires
a
high
overpotential.
In
response,
urea‐assisted
energy‐saving
alkaline
hydrogen‐production
system
has
been
investigated
replacing
OER
with
more
oxidizable
urea
oxidation
(UOR).
A
bimetal
heterostructure
CoMn/CoMn
2
O
4
as
bifunctional
catalyst
constructed
in
an
for
both
and
hydrogen
(HER).
Based
on
Schottky
heterojunction
structure,
induces
self‐driven
charge
transfer
at
interface,
which
facilitates
absorption
of
reactant
molecules
fracture
chemical
bonds,
therefore
triggering
decomposition
urea.
As
result,
heterostructured
electrode
exhibits
ultralow
potentials
−0.069
1.32
V
(vs
reversible
electrode)
to
reach
10
mA
cm
−2
HER
UOR,
respectively,
solution,
full
electrolysis
driven
delivers
relatively
low
potential
1.51
performs
stably
than
15
h.
This
represents
novel
strategy
Mott–Schottky
hybrids
electrocatalysts
should
inspire
development
sustainable
energy
conversion
combining
sewage
treatment.
Advanced Energy Materials,
Год журнала:
2018,
Номер
8(27)
Опубликована: Авг. 8, 2018
Abstract
Urea
electrooxidation
with
favorable
thermodynamic
potential
offers
great
promise
for
decoupling
H
2
/O
evolution
from
sluggish
water
splitting,
and
simultaneously
mitigating
the
problem
of
urea‐rich
pollution.
However,
intrinsically
slow
kinetics
six‐electron
transfer
process
impels
one
to
explore
efficient
catalysts
in
order
enable
widespread
use
this
catalytic
system.
In
response,
taking
CoS
/MoS
Schottky
heterojunctions
as
proof‐of‐concept
paradigm,
a
model
modulate
surface
charge
distribution
synergistically
facilitating
adsorption
fracture
chemical
group
urea
molecule
is
proposed
mechanism
at
molecular
level
elucidated.
Based
on
density
functional
calculations,
self‐driven
across
heterointerface
would
induce
formation
local
electrophilic/nucleophilic
region,
which
will
intelligently
adsorb
electron‐donating/electron‐withdrawing
groups
molecule,
activate
bonds,
thus
trigger
decomposition
urea.
Benefiting
regulation
distribution,
constructed
catalyst
‐MoS
exhibits
superior
activities
1.29
V
(only
0.06
higher
than
voltage
decomposition)
attain
10
mA
cm
−2
well
robust
durability
over
60
h.
This
innovational
manipulation
via
heterojunction
provides
exploring
other
highly
electrocatalysts.
Advanced Energy Materials,
Год журнала:
2019,
Номер
9(21)
Опубликована: Апрель 10, 2019
Abstract
Electrocatalytic
water
splitting
is
one
of
the
sustainable
and
promising
strategies
to
generate
hydrogen
fuel
but
still
remains
a
great
challenge
because
sluggish
anodic
oxygen
evolution
reaction
(OER).
A
very
effective
approach
dramatically
decrease
input
cell
voltage
electrolysis
replace
OER
with
hydrazine
oxidation
(HzOR)
due
its
lower
thermodynamic
potential.
Therefore,
developing
low‐cost
efficient
HzOR
catalysts,
coupled
cathodic
(HER),
tremendously
important
for
energy‐saving
electrolytic
production.
Herein,
new‐type
copper–nickel
nitride
(Cu
1
Ni
2
‐N)
rich
Cu
4
N/Ni
3
N
interface
rationally
constructed
on
carbon
fiber
cloth.
The
3D
electrode
exhibits
extraordinary
HER
performance
an
overpotential
71.4
mV
at
10
mA
cm
−2
in
1.0
m
KOH,
simultaneously
delivering
ultralow
potential
0.5
KOH/0.5
electrolyte.
Moreover,
utilizing
synthesized
‐N
as
both
cathode
anode
display
0.24
V
excellent
stability
over
75
h.
present
work
develops
copper–nickel‐based
bifunctional
electrocatalyst
through
hydrazine‐assistance
Nature Communications,
Год журнала:
2020,
Номер
11(1)
Опубликована: Апрель 15, 2020
Abstract
Replacing
sluggish
oxygen
evolution
reaction
(OER)
with
hydrazine
oxidation
(HzOR)
to
produce
hydrogen
has
been
considered
as
a
more
energy-efficient
strategy
than
water
splitting.
However,
the
relatively
high
cell
voltage
in
two-electrode
system
and
required
external
electric
power
hinder
its
scalable
applications,
especially
mobile
devices.
Herein,
we
report
bifunctional
P,
W
co-doped
Co
3
N
nanowire
array
electrode
remarkable
catalytic
activity
towards
both
HzOR
(−55
mV
at
10
mA
cm
−2
)
(HER,
−41
).
Inspiringly,
record
low
of
28
is
achieve
system.
DFT
calculations
decipher
that
doping
optimized
H*
adsorption/desorption
dehydrogenation
kinetics
could
be
underlying
mechanism.
Importantly,
self-powered
H
2
production
by
integrating
direct
fuel
splitting
electrolyzer
can
decent
rate
1.25
mmol
h
−1
room
temperature.
Green Chemistry,
Год журнала:
2021,
Номер
23(12), С. 4228 - 4254
Опубликована: Янв. 1, 2021
HMF
electrooxidation
is
emerging
as
a
powerful
and
promising
method
to
produce
wide
range
of
high-value
chemicals
on
account
mild
operation
conditions,
controllable
selectivity,
scalability.
Advanced Functional Materials,
Год журнала:
2021,
Номер
31(43)
Опубликована: Июль 29, 2021
Abstract
To
couple
hydrogen
evolution
reaction
(HER)
with
urea
oxidation
(UOR)
is
a
promising
approach
to
produce
H
2
reduced
energy
consumption.
However,
the
development
of
low‐cost
and
high‐performance
bifunctional
electrocatalyst
toward
HER
UOR
still
challenge.
In
this
work,
oxygen‐incorporated
nickel
molybdenum
phosphide
nanotube
arrays
are
synthesized
on
foam
(O‐NiMoP/NF)
via
electrodeposition
accompanied
in‐situ
template
etching.
Benefiting
from
modulated
electronic
structure
array
architecture
O‐NiMoP,
self‐supporting
O‐NiMoP/NF
electrodes
demonstrate
highly
efficient
catalytic
activity
UOR.
Particularly,
in
(HER||UOR)
coupled
system
for
production,
significantly
cell
voltage
1.55
V
obtained
at
current
density
50
mA
cm
–2
,
which
about
300
mV
lower
than
that
conventional
water
electrolysis.
Density
functional
theory
calculations
reveal
remarkable
activities
originated
Ni
sites
environment
induced
by
Mo,
P
O
atoms,
facilitate
dissociation
during
balance
adsorption/desorption
intermediates
The
Ni‐based
phosphides
as
HER||OER
provides
new
enabling
energy‐saving
production.
Advanced Energy Materials,
Год журнала:
2021,
Номер
11(43)
Опубликована: Июнь 17, 2021
Abstract
Biomass
is
recognized
as
an
ideal
CO
2
neutral,
abundant,
and
renewable
resource
substitute
to
fossil
fuels.
The
rich
proton
content
in
most
biomass
derived
materials,
such
ethanol,
5‐hydroxymethylfurfural
(HMF)
glycerol
allows
it
be
effective
hydrogen
carrier.
oxidation
derivatives,
2,5‐difurandicarboxylic
acid
from
HMF,
glyceric
are
valuable
products
used
biodegradable
polymers
pharmaceuticals.
Therefore,
combining
biomass‐derived
compound
at
the
anode
evolution
reaction
cathode
a
electrolysis
or
photo‐reforming
reactor
would
present
promising
strategy
for
coproducing
high
value
chemicals
with
low
energy
consumption
emissions.
This
review
aims
combine
fundamental
knowledge
on
photo
electro‐assisted
catalysis
provide
comprehensive
understanding
of
general
mechanisms
different
molecule
oxidation.
At
same
time,
catalyst
requirements
recent
advances
various
feedstock
compounds
also
reviewed
detail.
Technoeconomic
assessment
life
cycle
analysis
performed
feedstocks
assess
relative
benefits
processes,
finally
critical
prospects
given
challenges
opportunities
technology
development
meet
sustainability
requirement
future
global
economy.