ACS Catalysis,
Journal Year:
2017,
Volume and Issue:
7(4), P. 2624 - 2643
Published: March 1, 2017
Over
the
last
century,
industrialization
of
agriculture
and
consumption
fossil
fuels
have
resulted
in
a
significant
imbalance
redistribution
nitrogen-containing
resources.
This
has
sparked
an
interest
developing
more
sustainable
resilient
approaches
for
producing
commodities
such
as
fertilizers
fuels.
One
largely
neglected
but
emerging
approach
is
photocatalytic
nitrogen
fixation.
There
evidence
that
this
process
occurs
spontaneously
terrestrial
settings,
it
been
demonstrated
numerous
engineered
systems.
Yet
many
questions
still
remain
unanswered
regarding
rates,
mechanisms,
impacts
photocatalytically
fixed
"out
thin
air".
work
reviews
fascinating
history
reaction
examines
current
progress
toward
understanding
improving
photofixation
nitrogen.
supplemented
by
quantitative
review
thermodynamic
considerations
limitations
various
mechanisms.
Finally,
future
prospects
preliminary
performance
targets
fixation
are
discussed.
Chemical Reviews,
Journal Year:
2020,
Volume and Issue:
120(21), P. 12217 - 12314
Published: Nov. 2, 2020
Electrocatalysts
with
single
metal
atoms
as
active
sites
have
received
increasing
attention
owing
to
their
high
atomic
utilization
efficiency
and
exotic
catalytic
activity
selectivity.
This
review
aims
provide
a
comprehensive
summary
on
the
recent
development
of
such
single-atom
electrocatalysts
(SAECs)
for
various
energy-conversion
reactions.
The
discussion
starts
an
introduction
different
types
SAECs,
followed
by
overview
synthetic
methodologies
control
dispersion
atomically
resolved
characterization
using
state-of-the-art
microscopic
spectroscopic
techniques.
In
recognition
extensive
applications
electrocatalytic
studies
are
dissected
in
terms
important
electrochemical
reactions,
including
hydrogen
evolution
reaction
(HER),
oxygen
(OER),
reduction
(ORR),
carbon
dioxide
(CO2RR),
nitrogen
(NRR).
Examples
SAECs
deliberated
each
case
performance,
structure-property
relationships,
enhancement
mechanisms.
A
perspective
is
provided
at
end
section
about
remaining
challenges
opportunities
targeted
reaction.
ACS Catalysis,
Journal Year:
2018,
Volume and Issue:
8(2), P. 1490 - 1499
Published: Jan. 12, 2018
On
the
basis
of
constraints
from
reported
experimental
observations
and
density
functional
theory
simulations,
we
propose
a
mechanism
for
reduction
CO2
to
C2
products
on
copper
electrodes.
To
model
effects
an
applied
potential
bias
reactions,
calculations
are
carried
out
with
variable,
fractional
number
electrons
unit
cell,
which
is
optimized
so
that
Fermi
level
matches
actual
chemical
(i.e.,
bias);
implicit
electrolyte
allows
compensation
surface
charge
neutrality
maintained
in
overall
simulation
cell.
Our
explains
presence
seven
species
have
been
detected
reaction,
as
well
other
notable
observations.
Furthermore,
our
results
shed
light
difference
activities
toward
between
(100)
(111)
facets
copper.
We
compare
methodologies
findings
those
recent
mechanistic
studies
copper-catalyzed
reaction.
Chemical Society Reviews,
Journal Year:
2021,
Volume and Issue:
50(15), P. 8428 - 8469
Published: Jan. 1, 2021
The
recent
progress
in
activating
surface
reconstruction
by
integrating
advanced
characterizations
with
theoretical
calculations
for
high-efficiency
oxygen
evolution
reaction
is
reviewed.
Advanced Materials,
Journal Year:
2020,
Volume and Issue:
32(49)
Published: Oct. 30, 2020
Abstract
The
electronic
metal–support
interaction
(EMSI),
which
acts
as
a
bridge
between
theoretical
study
and
the
design
of
heterogenous
catalysts,
has
attracted
much
attention.
Utilizing
metal
support
is
one
most
essential
strategies
to
enhance
electrocatalytic
efficiency
due
structural
synergetic
promotion.
To
date,
ideal
model
for
realizing
EMSI,
many
types
single‐atom
catalysts
(SACs)
have
been
developed.
understanding
on
SACs
also
pushed
higher
level.
However,
systematic
theories
operando
experiments
are
seldom
reported,
will
be
necessary
put
forward
carried
out,
respectively.
Herein,
types,
characterization,
mechanism,
applications
EMSI
comprehensively
summarized
discussed.
In
addition
basic
information
above,
challenges,
opportunities,
future
development
proposed
present
an
overall
view
reference
later
research.
Angewandte Chemie International Edition,
Journal Year:
2015,
Volume and Issue:
54(35), P. 10102 - 10120
Published: July 1, 2015
The
notion
of
metal-free
catalysts
is
used
to
refer
carbon
materials
modified
with
nonmetallic
elements.
However,
some
claimed
are
prepared
using
metal-containing
precursors.
It
highly
contested
that
metal
residues
in
nitrogen-doped
(NC)
play
a
crucial
role
the
oxygen
reduction
reaction
(ORR).
In
an
attempt
reconcile
divergent
views,
definition
for
truly
proposed
and
differences
between
NC
M-Nx
/C
discussed.
Metal
impurities
at
levels
usually
undetectable
by
techniques
such
as
XPS,
XRD,
EDX
significantly
promote
ORR.
Poisoning
tests
mask
ions
reveal
involvement
active
sites
or
modifiers
electronic
structure
NC.
unique
merits
both
discussed
inspire
development
more
advanced
nonprecious-metal
The Journal of Physical Chemistry Letters,
Journal Year:
2016,
Volume and Issue:
7(8), P. 1471 - 1477
Published: April 5, 2016
We
have
carried
out
a
periodic
Kohn–Sham
density
functional
theory
investigation
of
the
pathways
by
which
carbon–carbon
bonds
could
be
formed
during
electrochemical
reduction
CO2
on
Cu(100)
using
model
that
includes
effects
potential,
solvent,
and
electrolyte.
The
potential
was
set
relating
applied
to
Fermi
energy
then
calculating
number
electrons
required
simulation
cell
for
specific
energy.
solvent
included
as
continuum
dielectric,
electrolyte
described
linearized
Poisson–Boltzmann
model.
calculated
zero
charge
variety
surfaces
agrees
with
experiment
within
mean
average
error
0.09
V,
thereby
validating
assumptions
Analysis
mechanism
C–C
bond
formation
revealed
at
low-applied
occurs
through
CO
dimer.
However,
high
potentials,
large
activation
barrier
blocks
this
pathway;
therefore,
reaction
adsorbed
CHO
CO.
Rate
parameters
determined
from
our
calculations
were
used
simulate
kinetics
ethene
over
surface.
An
excellent
match
observed
between
previously
reported
measurements
partial
current
function
voltage
variation
in
predicted
microkinetic
here
is
simple,
fairly
easy
implement,
involves
only
small
increase
computational
cost
neglecting
field.
Therefore,
it
can
study
composition
energetics
surface
reactions
wide
reactions.