Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(22)
Published: March 27, 2023
To
overcome
the
thermodynamic
and
kinetic
impediments
of
Sabatier
CO2
methanation
reaction,
process
must
be
operated
under
very
high
temperature
pressure
conditions,
to
obtain
an
industrially
viable
conversion,
rate,
selectivity.
Herein,
we
report
that
these
technologically
relevant
performance
metrics
have
been
achieved
much
milder
conditions
using
solar
rather
than
thermal
energy,
where
reaction
is
enabled
by
a
novel
nickel-boron
nitride
catalyst.
In
this
regard,
in
situ
generated
HOB⋅⋅⋅B
surface
frustrated
Lewis's
pair
considered
responsible
for
conversion
87.68
%,
rate
2.03
mol
gNi-1
h-1
,
near
100
%
selectivity,
realized
ambient
conditions.
This
discovery
bodes
well
opto-chemical
engineering
strategy
aimed
at
development
implementation
sustainable
'Solar
Sabatier'
process.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(22)
Published: March 24, 2023
Nickel-based
catalysts
have
been
regarded
as
one
of
the
most
promising
electrocatalysts
for
urea
oxidation
reaction
(UOR),
however,
their
activity
is
largely
limited
by
inevitable
self-oxidation
Ni
species
(NSOR)
during
UOR.
Here,
we
proposed
an
interface
chemistry
modulation
strategy
to
trigger
occurrence
UOR
before
NSOR
via
constructing
a
2D/2D
heterostructure
that
consists
ultrathin
NiO
anchored
Ru-Co
dual-atom
support
(Ru-Co
DAS/NiO).
Operando
spectroscopic
characterizations
confirm
this
unique
triggering
mechanism
on
surface
DAS/NiO.
Consequently,
fabricated
catalyst
exhibits
outstanding
with
low
potential
1.288
V
at
10
mA
cm-2
and
remarkable
long-term
durability
more
than
330
h
operation.
DFT
calculations
demonstrate
favorable
electronic
structure
induced
heterointerface
endows
energetically
NSOR.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(31)
Published: Feb. 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.
Energy & Environmental Science,
Journal Year:
2023,
Volume and Issue:
16(7), P. 2759 - 2803
Published: Jan. 1, 2023
The
catalytic
transformation
of
CO
2
into
valuable
fuels/chemicals
is
a
promising
and
economically
profitable
process
because
it
offers
an
alternative
toward
fossil
feedstocks
the
benefit
transforming
cycling
on
scale-up.
Arabian Journal of Chemistry,
Journal Year:
2023,
Volume and Issue:
16(3), P. 104542 - 104542
Published: Jan. 5, 2023
Graphitic
carbon
nitride
(g-C3N4)
is
a
remarkable
semiconductor
catalyst
that
has
attracted
widespread
attention
as
visible
light
photo-responsive,
metal-free,
low-cost
photocatalytic
material.
Pristine
g-C3N4
suffers
fast
recombination
of
photogenerated
electron-hole
pairs,
low
surface
area,
and
insufficient
absorption,
resulting
in
efficiency.
This
review
presents
the
recent
progress,
perspectives,
persistent
challenges
development
g-C3N4-based
materials.
Several
approaches
employed
to
improve
absorption
materials
including
metal
non-metal
doping,
co-doping,
heterojunction
engineering
have
been
extensively
discussed.
These
approaches,
general,
were
found
decrease
material's
bandgap,
increase
reduce
charge
carrier
recombination,
promote
thereby
enhancing
overall
performance.
The
material
widely
used
for
different
applications
such
hydrogen
production,
water
splitting,
CO2
conversion,
purification.
work
also
identified
various
limitations
weaknesses
associated
with
hinders
its
maximum
utilization
under
illumination
presented
state-of-the-art
solutions
reported
recently.
summary
this
would
add
an
invaluable
contribution
photocatalysis
research
facilitate
efficient
light-responsive
semiconducting
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(13)
Published: Feb. 7, 2023
Developing
highly
efficient
and
stable
photocatalysts
for
the
CO2
reduction
reaction
(CO2
RR)
remains
a
great
challenge.
We
designed
Z-Scheme
photocatalyst
with
N-Cu1
-S
single-atom
electron
bridge
(denoted
as
Cu-SAEB),
which
was
used
to
mediate
RR.
The
production
of
CO
O2
over
Cu-SAEB
is
high
236.0
120.1
μmol
g-1
h-1
in
absence
sacrificial
agents,
respectively,
outperforming
most
previously
reported
photocatalysts.
Notably,
as-designed
throughout
30
cycles,
totaling
300
h,
owing
strengthened
contact
interface
Cu-SAEB,
mediated
by
atomic
structure.
Experimental
theoretical
calculations
indicated
that
SAEB
greatly
promoted
Z-scheme
interfacial
charge-transport
process,
thus
leading
enhancement
photocatalytic
RR
Cu-SAEB.
This
work
represents
promising
platform
development
have
potential
conversion
applications.
Chemical Society Reviews,
Journal Year:
2023,
Volume and Issue:
52(21), P. 7602 - 7664
Published: Jan. 1, 2023
Carbon
nitrides,
with
feasibility
of
tailored
band
gap
via
suitable
nanoarchitectonics,
are
deemed
as
best
catalysts
amongst
existing
materials,
especially
for
HER,
OWS,
COR,
NRR,
water
oxidation,
pollutant
removal,
and
organocatalysis.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(23)
Published: April 4, 2023
Solar-driven
CO2
hydrogenation
into
multi-carbon
products
is
a
highly
desirable,
but
challenging
reaction.
The
bottleneck
of
this
reaction
lies
in
the
C-C
coupling
C1
intermediates.
Herein,
we
construct
centre
for
intermediates
via
situ
formation
Co0
-Coδ+
interface
double
sites
on
MgAl2
O4
(Co-CoOx
/MAO).
Our
experimental
and
theoretical
prediction
results
confirmed
effective
adsorption
activation
by
site
to
produce
intermediates,
while
introduction
electron-deficient
state
Coδ+
can
effectively
reduce
energy
barrier
key
CHCH*
Consequently,
Co-CoOx
/MAO
exhibited
high
C2-4
hydrocarbons
production
rate
1303
μmol
g-1
h-1
;
total
organic
carbon
selectivity
62.5
%
under
light
irradiation
with
ratio
(≈11)
olefin
paraffin.
This
study
provides
new
approach
toward
design
photocatalysts
used
conversion
C2+
products.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(33)
Published: April 25, 2023
Abstract
Regulating
the
coordination
environment
of
single‐atom
sites
is
high
necessity
to
promote
catalytic
performances
photocatalysts.
Herein,
preparation
atomically
dispersed
Co‐Ag
dual‐metal
anchored
on
P‐doped
carbon
nitride
(Co
1
Ag
‐PCN)
via
supramolecular
and
solvothermal
approaches
reported,
which
demonstrates
desirable
performance
for
photocatalytic
H
2
evolution
from
water
splitting.
The
optimal
Co
‐PCN
catalyst
achieves
a
remarkable
hydrogen
production
rate
1190
µmol
g
−1
h
with
an
apparent
quantum
yield
(AQY)
1.49%
at
365
nm,
superior
most
newly
reported
metal‐N‐coordinated
Systematic
experimental
characterizations
density
functional
theoretic
studies
attribute
enhanced
activity
synergistic
effect
dual
exclusive
configuration
Co‐N
6
Ag‐N
C
,
enhances
charge
promotes
oriented
electrons
transport
metal
centers
reduced
free
energy
barriers
by
facilitating
formation
H*
intermediates
as
key
step
in
evolution.
This
study
reveals
versatile
strategy
tailor
electronic
structures
synergies
engineering
neighboring
environment.