Efficient Grouped-Bath Ansatz for Spin–Flip Nonorthogonal Configuration Interaction in Transition-Metal Charge-Transfer Complexes
Journal of Chemical Theory and Computation,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 7, 2025
We
introduce
a
novel
grouped-bath
ansatz
that
approximates
the
spin-flip
nonorthogonal
configuration
interaction
(SF-NOCI)
ansatz,
named
SF-GNOCI,
which
significantly
reduces
computational
cost
while
preserving
accuracy.
SF-NOCI,
originally
developed
by
Mayhall
et
al.,
is
robust
and
nearly
"black-box"
electronic
structure
theory
well
suited
for
studying
charge-transfer
phenomena.
It
captures
orbital
relaxation
effects
all
configurations
within
active
space,
providing
balanced
correlation
among
charge
transfer
other
states.
However,
including
these
results
in
sharp
increase
cost,
especially
large
spaces
commonly
encountered
transition
metal
complexes.
To
overcome
this
challenge,
we
grouped
based
on
number
of
electrons
associated
with
each
atom.
Configurations
group
share
common
set
bath
orbitals,
reducing
overhead.
demonstrate
performance
SF-GNOCI
through
benchmark
calculations
two
systems:
avoided
crossing
lowest
singlet
states
LiF
dissociation
low-lying
[Fe(SCH3)4]2-/1-.
Our
show
achieves
accuracy
comparable
to
standard
SF-NOCI
factor
10
[Fe(SCH3)4]2-
15
[Fe(SCH3)4]1-.
believe
promising
reference
state
efficiently
describing
phenomena
Language: Английский
Atomic Layer Deposition of Graphene‐Based Nanohybrid Interlayer for Potential Improvement in Lithium‐Sulfur Batteries
Energy Storage,
Journal Year:
2025,
Volume and Issue:
7(3)
Published: March 25, 2025
ABSTRACT
Lithium‐sulfur
batteries
(LSBs)
are
viable
options
for
next‐generation
energy
storage
owing
to
their
nontoxic
characteristics,
elevated
theoretical
density,
and
abundant
sulfur.
However,
LSBs
face
significant
challenges,
including
the
shuttle
effect,
volumetric
expansion,
low
ionic
conductivity,
anode
degradation.
Recent
creative
developments,
such
as
improved
electrolyte
compositions,
protective
coatings,
novel
interlayers,
have
been
introduced
solve
these
issues.
Among
these,
interlayers
suffer
from
issues
with
lithium
polysulfides
(LiPSs)
capturing
ability,
mechanical
chemical
stability,
ion
electrical
thickness,
weight,
even
though
they
stand
out
having
potential
improve
battery
performance
by
managing
LiPSs
improving
electron
transport.
This
study
aims
develop
an
innovative
interlayer
LSB
systems
synthesizing
characterizing
a
nanohybrid
combining
high‐surface‐area,
high‐ion
electrically
conductive,
mechanically
chemically
stable
three‐dimensional
graphene
foam
(3D
GF)
ultra‐thin
Al
2
O
3
enhancing
capture
without
adding
weight
or
volume.
Considering
this
goal,
matrix
of
nanohybrids
was
initially
developed
3D
GF
through
catalytic
vapor
deposition
(CVD).
Following
that,
amorphous
films
were
deposited
on
using
atomic
layer
(ALD),
cycles
varying
25
200,
optimize
film
characteristics.
Comprehensive
analyses
SEM
(scanning
microscopy),
EDX
(energy‐dispersive
X‐ray
spectroscopy),
Raman
spectroscopy,
XRD
(X‐ray
diffraction),
XRR
reflectivity)
confirmed
successful
synthesis
GF/Al
nanohybrids.
analysis
revealed
that
porous
network
structure
remained
intact
following
deposition,
indicating
minimal
disruption.
demonstrated
desired
composition
thin
film,
while
spectroscopy
maintenance
structural
characteristics
postdeposition.
showed
consistent
layer‐by‐layer
growth
films.
Moreover,
heat
treatment‐focused
studies
indicated
thicker
ALD‐based
facilitated
alpha‐phase
crystallization
at
lower
temperatures.
To
best
authors'
knowledge,
introduces
initial
design
producing
nanohybrids,
revealing
approach
towards
straightforward,
effective,
scalable
production
methods
alternative
effective
strategy.
Language: Английский
Recent progress in design strategies for high-performance metal-tellurium batteries
Chemical Engineering Journal,
Journal Year:
2024,
Volume and Issue:
unknown, P. 158528 - 158528
Published: Dec. 1, 2024
Language: Английский
Enhanced d‐p Orbital Hybridization for Lithium Polysulfide Capturing and Lithium Deposition Inducing of AgVO3 Skeleton Enabling High‐Performance Li‐Sulfur Batteries
Chenyi Sun,
No information about this author
Li Gao,
No information about this author
Wanling Rong
No information about this author
et al.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(49)
Published: Oct. 14, 2024
Abstract
The
dendrite
growth
and
volume
expansion
of
the
Li
metal
anode,
as
well
LiPSs
“shuttle
effect”
slow
conversion
kinetics
S
cathode,
have
severely
hampered
large‐scale
development
LSBs.
Herein,
a
simple
hydrothermal
method
is
employed
to
synthesize
rod‐like
AgVO
3
,
which
then
used
anode
current
collector
separator
modification,
respectively.
As
collector,
has
strong
affinity,
can
lower
nucleation
overpotential
guide
uniform
deposition
metal.
‐modified
accelerate
redox
achieve
anchoring
LiPSs.
results
DFT
calculation
experiments
reveal
that
enable
Ag
horizontal
d
orbitals
(d
xy
/d
x
2
‐y
)
hybridize
with
p
orbital
form
additional
σ/σ*
π/π*.
activation
increase
ability,
reduce
reaction
barrier,
transformation.
Hence,
LSBs
assembled
Li@AgVO
modified
show
excellent
cycle
performance.
This
work
gives
novel
idea
for
application
high
catalytic
performance
materials
represented
by
its
unique
successfully
Language: Английский