Advanced Materials,
Journal Year:
2021,
Volume and Issue:
33(31)
Published: June 12, 2021
Abstract
Hydrogen
economy
has
emerged
as
a
very
promising
alternative
to
the
current
hydrocarbon
economy,
which
involves
process
of
harvesting
renewable
energy
split
water
into
hydrogen
and
oxygen
then
further
utilization
clean
fuel.
The
production
by
electrolysis
is
an
essential
prerequisite
with
zero
carbon
emission.
Among
various
technologies,
alkaline
splitting
been
commercialized
for
more
than
100
years,
representing
most
mature
economic
technology.
Here,
historic
development
overviewed,
several
critical
electrochemical
parameters
are
discussed.
After
that,
advanced
nonprecious
metal
electrocatalysts
that
recently
negotiating
evolution
reaction
(OER)
(HER)
discussed,
including
transition
oxides,
(oxy)hydroxides,
chalcogenides,
phosphides,
nitrides
OER,
well
alloys,
carbides
HER.
In
this
section,
particular
attention
paid
catalyst
synthesis,
activity
stability
challenges,
performance
improvement,
industry‐relevant
developments.
Some
recent
works
about
scaled‐up
novel
electrode
designs,
seawater
also
spotlighted.
Finally,
outlook
on
future
challenges
opportunities
offered,
potential
directions
speculated.
Advanced Materials,
Journal Year:
2020,
Volume and Issue:
32(17)
Published: March 16, 2020
Abstract
Simultaneous
highly
efficient
production
of
hydrogen
and
conversion
biomass
into
value‐added
products
is
meaningful
but
challenging.
Herein,
a
porous
nanospindle
composed
carbon‐encapsulated
MoO
2
‐FeP
heterojunction
(MoO
‐FeP@C)
proposed
as
robust
bifunctional
electrocatalyst
for
evolution
reaction
(HER)
electrooxidation
(BEOR).
X‐ray
photoelectron
spectroscopy
analysis
theoretical
calculations
confirm
the
electron
transfer
from
to
FeP
at
interfaces,
where
accumulation
on
favors
optimization
H
O
H*
absorption
energies
HER,
whereas
hole
responsible
improving
BEOR
activity.
Thanks
its
interfacial
electronic
structure,
‐FeP@C
exhibits
excellent
HER
activity
with
an
overpotential
103
mV
10
mA
cm
−2
Tafel
slope
48
dec
−1
.
Meanwhile,
when
5‐hydroxymethylfurfural
chosen
BEOR,
almost
100%,
2,5‐furandicarboxylic
acid
(FDCA)
obtained
selectivity
98.6%.
The
electrolyzer
employing
cathodic
anodic
FDCA
requires
only
low
voltage
1.486
V
can
be
powered
by
solar
cell
(output
voltage:
1.45
V).
Additionally,
other
BEORs
coupled
catalyzed
also
have
catalytic
performance,
implying
their
good
versatility.
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
60(36), P. 19572 - 19590
Published: Feb. 19, 2021
Abstract
Compared
to
modern
fossil‐fuel‐based
refineries,
the
emerging
electrocatalytic
refinery
(e‐refinery)
is
a
more
sustainable
and
environmentally
benign
strategy
convert
renewable
feedstocks
energy
sources
into
transportable
fuels
value‐added
chemicals.
A
crucial
step
in
conducting
e‐refinery
processes
development
of
appropriate
reactions
optimal
electrocatalysts
for
efficient
cleavage
formation
chemical
bonds.
However,
compared
well‐studied
primary
(e.g.,
O
2
reduction,
water
splitting),
mechanistic
aspects
materials
design
complex
are
yet
be
settled.
To
address
this
challenge,
herein,
we
first
present
fundamentals
heterogeneous
electrocatalysis
some
reactions,
then
implement
these
establish
framework
by
coupling
situ
generated
intermediates
(integrated
reactions)
or
products
(tandem
reactions).
We
also
set
principles
strategies
efficiently
manipulate
reaction
pathways.
Angewandte Chemie International Edition,
Journal Year:
2020,
Volume and Issue:
60(13), P. 7297 - 7307
Published: Dec. 25, 2020
Abstract
The
nitrogenous
nucleophile
electrooxidation
reaction
(NOR)
plays
a
vital
role
in
the
degradation
and
transformation
of
available
nitrogen.
Focusing
on
NOR
mediated
by
β‐Ni(OH)
2
electrode,
we
decipher
mechanism
nucleophile.
For
two‐step
NOR,
proton‐coupled
electron
transfer
(PCET)
is
bridge
between
electrocatalytic
dehydrogenation
from
to
β‐Ni(OH)O,
spontaneous
dehydrogenative
oxidation
reaction.
This
theory
can
give
good
explanation
for
hydrazine
primary
amine
reactions,
but
insufficient
urea
(UOR).
Through
operando
tracing
bond
rupture
formation
processes
during
UOR,
as
well
theoretical
calculations,
propose
possible
UOR
whereby
intramolecular
coupling
N−N
bond,
accompanied
PCET,
hydration
rearrangement
processes,
results
high
performance
ca.
100
%
N
selectivity.
These
discoveries
clarify
evolution
molecules
they
elucidate
fundamental
aspects
electrocatalysis
involving
nitrogen‐containing
species.
Science,
Journal Year:
2020,
Volume and Issue:
368(6496), P. 1228 - 1233
Published: June 11, 2020
Charging
into
epoxides
Ethylene
oxide
is
a
strained,
reactive
molecule
produced
on
vast
scale
as
plastics
precursor.
The
current
method
of
synthesis
involves
the
direct
reaction
ethylene
and
oxygen
at
high
temperature,
but
original
protocol
relied
reduction
chlorine
to
produce
chlorohydrin
intermediate.
Leow
et
al.
report
room
temperature
that
returns
route
uses
electrochemistry
generate
it
catalytically
from
chloride
(see
Perspective
by
Barton).
This
efficient
process
water
in
place
can
be
integrated
with
electrochemical
generation
carbon
dioxide.
Propylene
using
same
method.
Science
,
this
issue
p.
1228
;
see
also
1181
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
60(21), P. 11841 - 11846
Published: March 19, 2021
Abstract
The
development
of
efficient
and
low‐cost
electrocatalysts
toward
the
oxygen
evolution
reaction
(OER)
is
critical
for
improving
efficiency
several
electrochemical
energy
conversion
storage
devices.
Here,
we
report
an
elaborate
design
synthesis
porous
Co‐based
trimetallic
spinel
oxide
nanoboxes
(NiCo
2−
x
Fe
O
4
NBs)
by
a
novel
metal‐organic
framework
engaged
strategy,
which
involves
chemical
etching,
cation
exchange,
subsequent
thermal
oxidation
processes.
Owing
to
structural
compositional
advantages,
optimized
NiCo
NBs
(
about
0.117)
deliver
superior
electrocatalytic
performance
OER
with
overpotential
274
mV
at
10
mA
cm
−2
,
small
Tafel
slope
42
dec
−1
good
stability
in
alkaline
electrolyte,
much
better
than
that
bi/monometallic
oxides
even
commercial
RuO
2
.
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
60(42), P. 22908 - 22914
Published: Aug. 18, 2021
Abstract
Nickel
hydroxide
(Ni(OH)
2
)
is
a
promising
electrocatalyst
for
the
5‐hydroxymethylfurfural
oxidation
reaction
(HMFOR)
and
dehydronated
intermediates
Ni(OH)O
species
are
proved
to
be
active
sites
HMFOR.
In
this
study,
Ni(OH)
modified
by
platinum
adjust
electronic
structure
current
density
of
HMFOR
improves
8.2
times
at
Pt/Ni(OH)
electrode
compared
with
that
on
electrode.
Operando
methods
reveal
introduction
Pt
optimized
redox
property
accelerate
formation
during
catalytic
process.
Theoretical
studies
demonstrate
enhanced
kinetics
originates
from
reduced
dehydrogenation
energy
.
The
product
analysis
transition
state
simulation
prove
also
reduces
adsorption
HMF
behavior
as
can
act
site
HMF.
Overall,
work
here
provides
strategy
design
an
efficient
universal
nickel‐based
catalyst
electro‐oxidation,
which
extended
other
Ni‐based
catalysts
such
Ni(HCO
3
NiO.
Green Chemistry,
Journal Year:
2020,
Volume and Issue:
22(11), P. 3358 - 3375
Published: Jan. 1, 2020
This
tutorial
bridges
an
important
knowledge
gap
by
providing
easily
accessible
introduction
that
enables
synthetic
chemists
to
explore
electrochemistry.