Nature Communications,
Journal Year:
2024,
Volume and Issue:
15(1)
Published: March 29, 2024
Abstract
Establishing
appropriate
metal-support
interactions
is
imperative
for
acquiring
efficient
and
corrosion-resistant
catalysts
water
splitting.
Herein,
the
interaction
mechanism
between
Ru
nanoparticles
a
series
of
titanium
oxides,
including
TiO,
Ti
4
O
7
TiO
2,
designed
via
facile
non-stoichiometric
engineering
systematically
studied.
7,
with
unique
band
structure,
high
conductivity
chemical
stability,
endows
ingenious
through
interfacial
Ti–O–Ru
units,
which
stabilizes
species
during
OER
triggers
hydrogen
spillover
to
accelerate
HER
kinetics.
As
expected,
Ru/Ti
displays
ultralow
overpotentials
8
mV
150
long
operation
500
h
at
10
mA
cm
−2
in
acidic
media,
expanded
pH-universal
environments.
Benefitting
from
excellent
bifunctional
performance,
proton
exchange
membrane
anion
electrolyzer
assembled
achieves
superior
performance
robust
operation.
The
work
paves
way
energy
conversion
devices.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(18), P. 10259 - 10267
Published: April 25, 2023
Realizing
efficient
hydrogenation
of
N2
molecules
in
the
electrocatalytic
nitrogen
reduction
reaction
(NRR)
is
crucial
achieving
high
activity
at
a
low
potential
because
it
theoretically
requires
higher
equilibrium
than
other
steps.
Analogous
to
metal
hydride
complexes
for
reduction,
this
step
by
chemical
can
weaken
dependence
initial
process.
However,
strategy
rarely
reported
NRR,
and
catalytic
mechanism
remains
ambiguous
lacks
experimental
evidence.
Here,
we
show
highly
electrocatalyst
(ruthenium
single
atoms
anchored
on
graphdiyne/graphene
sandwich
structures)
with
hydrogen
radical-transferring
mechanism,
which
graphdiyne
(GDY)
generates
radicals
(H•),
effectively
activate
generate
NNH
(•NNH).
A
dual-active
site
constructed
suppress
competing
evolution,
where
preferentially
adsorbs
GDY
Ru
serve
as
adsorption
•NNH
promote
further
NH3
synthesis.
As
result,
selectivity
are
obtained
simultaneously
-0.1
V
versus
reversible
electrode.
Our
findings
illustrate
novel
transfer
that
greatly
reduce
maintain
NRR
provide
powerful
guidelines
design
concept
electrocatalysts.
ACS Nano,
Journal Year:
2023,
Volume and Issue:
17(21), P. 20804 - 20824
Published: Nov. 3, 2023
The
splitting
of
water
through
electrocatalysis
offers
a
sustainable
method
for
the
production
hydrogen.
In
alkaline
electrolytes,
lack
protons
forces
dissociation
to
occur
before
hydrogen
evolution
reaction
(HER).
While
pure
Pt
is
gold
standard
electrocatalyst
in
acidic
since
5d
orbital
nearly
fully
occupied,
when
it
overlaps
with
molecular
water,
generates
Pauli
repulsion.
As
result,
formation
Pt–H*
bond
an
environment
difficult,
which
slows
HER
and
negates
benefits
using
catalyst.
To
overcome
this
limitation,
can
be
alloyed
transition
metals,
such
as
Fe,
Co,
Ni.
This
approach
has
potential
not
only
enhance
performance
but
also
increase
dispersion
decrease
its
usage,
thus
overall
improving
catalyst's
cost-effectiveness.
excellent
adsorption
ability
metals
contributes
generation
proton-rich
local
near
Pt-based
alloy
that
promotes
HER.
Significant
progress
been
achieved
comprehending
mechanism
manipulation
structure
composition
electrocatalysts
based
on
alloy.
objective
review
analyze
condense
latest
developments
It
focuses
modified
alloys
clarifies
design
principles
catalytic
catalysts
from
both
experimental
theoretical
perspective.
highlights
some
difficulties
encountered
during
opportunities
increasing
performance.
Finally,
guidance
development
more
efficient
provided.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(46), P. 25143 - 25149
Published: Nov. 9, 2023
According
to
the
traditional
nucleation
theory,
crystals
in
solution
nucleate
under
thermal
fluctuations
with
random
crystal
orientation.
Thus,
nanosheet
arrays
grown
on
a
substrate
always
exhibit
disordered
arrangements,
which
impede
mass
transfer
during
catalysis.
To
overcome
this
limitation,
here,
we
demonstrate
stress-induced,
oriented
and
growth
of
arrays.
A
regularly
self-growing
parallel
array
is
realized
curved
substrate.
During
electrochemical
oxygen
production,
ordered
maintains
steady
flow
liquids
microchannels,
suppressing
detrimental
production
flow-blocking
bubbles
typical
randomly
Controllable
arrays,
fully
covered
fluffy-like
ultrathin
nanosheets,
amorphous
structures
altogether
enable
full-scale
design
hierarchical
interfaces
from
micro-
atomic
scale,
significantly
improving
otherwise
sluggish
kinetics
evolution
toward
industrial
ultrafast
production.
Record-high
135
L·min-1·m-2
high
working
current
4000
mA·cm-2
steadily
achieved
at
competitively
low
cell
voltage
2.862
V.
These
results
related
insights
lay
basis
for
further
developments
beyond
classical
approaches,
benefits
large-scale,
processes
as
shown
here
Energy & Environmental Science,
Journal Year:
2022,
Volume and Issue:
16(1), P. 285 - 294
Published: Dec. 6, 2022
Finding
an
active
and
robust
non-platinum
catalyst
toward
the
alkaline
hydrogen
evolution
reaction
(HER)
operating
at
ampere-level
current
density
is
important
for
emerging
anion
exchange
membrane
(AEM)
water
electrolysis
but
challenging.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
63(1)
Published: Nov. 21, 2023
Despite
the
fact
that
d-band
center
theory
links
d
electron
structure
of
transition
metals
to
their
catalytic
activity,
it
is
yet
unknown
how
synergistic
effect
multi-d
electrons
impacts
performance.
Herein,
novel
LaNi1-x
Cox
Ru
intermetallics
containing
5d,
4d,
and
3d
were
prepared.
In
these
compounds,
5d
orbital
La
transfers
4d
Ru,
which
provides
adsorption
sites
for
H*.
The
orbitals
Ni
Co
interact
with
generate
an
anisotropic
distribution,
facilitates
desorption
OH*.
ensures
efficient
activity.
optimized
LaNi0.5
Co0.5
has
overpotential
43mV
at
10
mA
cm-2
alkaline
electrocatalytic
hydrogen
evolution
reaction.
Beyond
offering
a
variety
new
electrocatalysts,
this
work
reveals
synergy
in
promoting