Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(52)
Опубликована: Окт. 6, 2022
Abstract
The
simultaneous
presence
of
two
active
metal
centres
in
diatomic
catalysts
(DACs)
leads
to
the
occurrence
specific
interactions
between
sites.
Such
interactions,
referred
as
long‐range
(LRIs),
play
an
important
role
determining
rate
and
selectivity
a
reaction.
optimal
combination
must
be
determined
achieve
targeted
efficiency.
To
date,
various
types
DACs
have
been
synthesised
applied
electrochemistry.
However,
LRIs
not
systematically
summarised.
Herein,
regulation,
mechanism,
electrocatalytic
applications
are
comprehensively
summarised
discussed.
In
addition
basic
information
above,
challenges,
opportunities,
future
development
proposed
order
present
overall
view
reference
for
research.
Advanced Materials,
Год журнала:
2023,
Номер
35(31)
Опубликована: Фев. 23, 2023
Single/dual-metal
atoms
supported
on
carbon
matrix
can
be
modulated
by
coordination
structure
and
neighboring
active
sites.
Precisely
designing
the
geometric
electronic
uncovering
structure-property
relationships
of
single/dual-metal
confront
with
grand
challenges.
Herein,
this
review
summarizes
latest
progress
in
microenvironment
engineering
single/dual-atom
sites
via
a
comprehensive
comparison
single-atom
catalyst
(SACs)
dual-atom
catalysts
(DACs)
term
design
principles,
modulation
strategy,
theoretical
understanding
structure-performance
correlations.
Subsequently,
recent
advances
several
typical
electrocatalysis
process
are
discussed
to
get
general
reaction
mechanisms
finely-tuned
SACs
DACs.
Finally,
full-scaled
summaries
challenges
prospects
given
for
This
will
provide
new
inspiration
development
atomically
dispersed
electrocatalytic
application.
Accounts of Materials Research,
Год журнала:
2022,
Номер
3(6), С. 584 - 596
Опубликована: Май 17, 2022
ConspectusRecent
decades
have
witnessed
the
rapid
development
of
catalytic
science,
especially
after
Taylor
and
Armstrong
proposed
notion
"active
site"
in
1925.
By
optimizing
reaction
paths
reducing
activation
energies
reactions,
catalysts
appear
more
than
90%
chemical
production
involving
homogeneous
catalysis,
heterogeneous
enzyme
catalysis.
Because
100%
efficiency
active
atom
utilization
adjustable
microenvironment
metal
centers,
single-atom
(SACs)
shine
various
fields
for
enhancing
rate,
conversion,
selectivity
reactions.
Nevertheless,
a
solo
site
determines
fixed
adsorption
mode,
intermediates
from
multistep
reactions
linking
with
are
related
to
each
other.
For
specific
reaction,
it
is
almost
impossible
optimally
adjust
every
intermediate
on
simultaneously.
This
phenomenon
termed
scaling
relationship
limit
(SRL)
an
unavoidable
obstacle
pure
SACs.Dual-atom
(DACs),
perfectly
inheriting
advantages
SACs,
can
exhibit
better
performance
simple
SACs
thus
gradually
gained
researchers'
attention.
Depending
dual-metal
structure,
sites
(DMSs)
DACs
be
divided
into
two
separated
heterometal
sites,
linked
homometal
sites.
Two
prescribe
distance
between
electron
interaction.
Currently,
origins
summarized
following
three
points:
(1)
electronic
effect,
which
only
one
center
serves
as
other
plays
regulatory
role;
(2)
synergistic
centers
separately
catalyze
different
core
steps
improve
together;
(3)
offering
additional
changes
structures
break
SRL
based
SACs.
Among
origins,
structure
upon
DMSs
most
effective
technologies
boost
property
basis
To
date,
few
contributions
focused
catalysis
environments,
including
O2
reduction
evolution
H2
CO2
N2
conversion
reactions.In
this
Account,
summary
recent
progress
regarding
will
presented.
First,
unpopular
discovery
research
hot
spot
illustrated
through
timeline.
In
next
section,
categories,
potential
revealed
by
comparison
addition,
techniques
constructing
systematically
summarized,
preparation
carbonous,
pyrolysis-free,
noncarbon-supported,
complex-type
DACs.
Furthermore,
underlying
energy-
environment-related
introduced
detail
assistance
theoretical
calculations.
Finally,
we
affirm
contribution
particularly
electrocatalysis,
provide
outlook
direction
discussing
major
challenges.
It
anticipated
that
Account
inspire
researchers
propel
advance
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(27)
Опубликована: Апрель 25, 2022
Iron,
nitrogen-codoped
carbon
(Fe-N-C)
nanocomposites
have
emerged
as
viable
electrocatalysts
for
the
oxygen
reduction
reaction
(ORR)
due
to
formation
of
FeNx
Cy
coordination
moieties.
In
this
study,
results
from
first-principles
calculations
show
a
nearly
linear
correlation
energy
barriers
key
steps
with
Fe
magnetic
moment.
Experimentally,
when
single
Cu
sites
are
incorporated
into
Fe-N-C
aerogels
(denoted
NCAG/Fe-Cu),
centers
exhibit
reduced
moment
and
markedly
enhanced
ORR
activity
within
wide
pH
range
0-14.
With
NCAG/Fe-Cu
used
cathode
catalyst
in
neutral/quasi-solid
aluminum-air
alkaline/quasi-solid
zinc-air
battery,
both
achieve
remarkable
performance
an
ultrahigh
open-circuit
voltage
2.00
1.51
V,
large
power
density
130
186
mW
cm-2
,
good
mechanical
flexibility,
all
better
than
those
commercial
Pt/C
or
Pt/C-RuO2
catalysts
at
cathode.
Chemical Society Reviews,
Год журнала:
2022,
Номер
51(21), С. 8923 - 8956
Опубликована: Янв. 1, 2022
This
review
presents
recent
developments
in
the
synthesis,
modulation
and
characterization
of
multi-atom
cluster
catalysts
for
electrochemical
energy
applications.
Advanced Materials,
Год журнала:
2023,
Номер
36(1)
Опубликована: Апрель 20, 2023
This
topical
review
focuses
on
the
distinct
role
of
carbon
support
coordination
environment
single-atom
catalysts
(SACs)
for
electrocatalysis.
The
article
begins
with
an
overview
atomic
configurations
in
SACs,
including
a
discussion
advanced
characterization
techniques
and
simulation
used
understanding
active
sites.
A
summary
key
electrocatalysis
applications
is
then
provided.
These
processes
are
oxygen
reduction
reaction
(ORR),
evolution
(OER),
hydrogen
(HER),
nitrogen
(NRR),
dioxide
(CO
