Langmuir,
Journal Year:
2024,
Volume and Issue:
40(49), P. 26086 - 26095
Published: Nov. 27, 2024
Magnesium–sulfur
(Mg–S)
batteries
offer
a
promising
energy
storage
system
due
to
their
high
theoretical
capacity.
However,
the
sluggish
conversion
reaction
kinetics
and
shuttle
effect
of
magnesium
polysulfides
hinder
practical
application.
The
charge
density
divalent
Mg2+
cations
leads
slow
caused
by
significant
electrostatic
interactions
between
its
surrounding
solvent
anion
species.
This
study
probes
impact
incorporating
weakly
coordinating
tetrahydrofuran
(THF)
regulate
solvation
sheath's
interfacial
chemistry
enhance
mobility
ions
in
halogen-free
electrolyte
(HFE)
based
on
Mg(NO3)2.
An
effective
anode/electrolyte
interface
is
engineered
protect
Mg
anode
from
passivation
reduce
shuttle.
HFE–THF
exhibits
relatively
goodelectrochemical
performance,
ionic
conductivity,
low
overpotential
for
plating
stripping.
Mg–S
cells
with
achieve
initial
specific
capacities
approximately
580
mAh
g–1,
fluctuated
Coulombic
efficiency
at
current
20
μA
cm–2,
extended
cycle
life
compared
blank
HFE.
Advanced Science,
Journal Year:
2024,
Volume and Issue:
11(25)
Published: April 6, 2024
Abstract
Rechargeable
magnesium
batteries
(RMBs)
have
garnered
significant
attention
due
to
their
potential
provide
high
energy
density,
utilize
earth‐abundant
raw
materials,
and
employ
metal
anode
safely.
Currently,
the
lack
of
applicable
cathode
materials
has
become
one
bottleneck
issues
for
fully
exploiting
technological
advantages
RMBs.
Recent
studies
on
Mg
cathodes
reveal
divergent
storage
performance
depending
electrolyte
formulation,
posing
interfacial
as
a
previously
overlooked
challenge.
This
minireview
begins
with
an
introduction
representative
cathode‐electrolyte
phenomena
in
RMBs,
elaborating
unique
solvation
behavior
2+
,
which
lays
foundation
chemistries.
It
is
followed
by
presenting
recently
developed
strategies
targeting
promotion
desolvation
alternative
cointercalation
approaches
circumvent
step.
In
addition,
efforts
enhance
compatibility
via
development
engineering
are
highlighted.
Based
abovementioned
discussions,
this
finally
puts
forward
perspectives
challenges
establishment
stable
interface
fast
chemistry
ACS Energy Letters,
Journal Year:
2025,
Volume and Issue:
unknown, P. 552 - 561
Published: Jan. 1, 2025
Mg
anodes
are
hindered
by
a
huge
overpotential
and
limited
cycling
life,
stemming
primarily
from
the
unstable
interphase
between
electrolyte.
An
effective
approach
lies
in
establishing
an
anion-derived,
inorganic-rich
solid–electrolyte
(SEI)
that
mitigates
continuous
reduction
of
Nevertheless,
high
charge
density
divalent
cations
poses
significant
challenge
balancing
coordination
dissociation
anions
within
Mg2+
solvation
sheath.
Herein,
selecting
small-sized
OTf–,
diglyme
solvent,
trimethyl
phosphate
(TMP)
as
cosolvents
with
similar
donor
number
(DN)
values,
electrolyte-dominated
Mg2+–OTf–
contact
ion-pair
configuration
is
achieved,
further
deriving
stable
inorganic
SEI
containing
fluoride
phosphide
components.
Among
them,
TMP
can
break
lattice
energy
magnesium
salts,
while
OTf–
low
electron
delocalization
ensure
degree
Mg2+,
jointly
realizing
anion
chemistry.
MgF2
MgS,
dominated
decomposition
at
potential
0.6
V
(vs
Mg/Mg2+),
enhance
electronic
insulation
interphase.
Consequently,
exhibit
superior
performance
over
3200
h
polarization
(<0.1
V)
excellent
plating/stripping
Coulombic
efficiency
1000
cycles
0.1
mA
cm–2.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(17)
Published: Jan. 4, 2024
Abstract
Mg(SO
3
CF
)
2
(Mg(OTf)
is
a
simple
and
cost‐effective
magnesium
salt,
which
can
promote
the
future
applications
of
rechargeable
batteries
(RMBs).
However,
Mg(OTf)
/ether
electrolytes
suffer
from
poor
electrochemical
properties
due
to
low
solubility
serious
decomposition
passivation
[Mg
2+
‐OTf
−
]
ion
pair
on
Mg.
Herein,
OTf
anion
successfully
grafted
low‐cost
fluoride
boronic
esters
(B(OC
x
H
y
F
2x‐y+1
obtain
asymmetric
weak‐coordination
boron‐center
[B(OC
OTf]
in
ether
electrolytes.
The
‐OCH
(TFE)
groups
B(TFE)
effectively
realize
charge
delocalization
B‐O
plane,
restraining
independent
pair.
co‐decomposition
[B(TFE)
induces
formation
B‐containing
organic/inorganic
interphase,
thus
achieving
reversible
Mg
plating/stripping.
After
further
solubilization
reaction,
obtained
electrolyte
exhibits
high
average
coulombic
efficiency
98.13%
long‐term
cycling
stability
(1000
h).
Notably,
long
life
(capacity
retention
90.2%
after
600
cycles
at
1
C)
high‐rate
capacity
(43.0
mAh
g
−1
5
Mg/Mo
6
S
8
full
cell
demonstrate
favorable
electrolyte/cathode
compatibility.
This
work
brings
new
insights
design
new‐type
Mg‐salts
high‐performance
for
commercial
RMBs.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
14(38)
Published: July 31, 2024
Abstract
Divalent
metal
batteries
have
attracted
considerable
attention
in
scientific
exploration
for
sustainable
energy
storage
solutions
owing
to
the
abundant
reserves
of
magnesium
(Mg)
and
calcium
(Ca),
competitive
low
redox
potentials
Mg/Mg
2+
(–2.37
V
vs
SHE)
Ca/Ca
(–2.87
couples,
as
well
high
theoretical
capacities
both
anodes.
However,
development
these
faces
fundamental
challenges
stemming
from
limited
cycling
stability
efficiency
Mg/Ca
These
issues
primarily
originate
sluggish
electrochemical
kinetics
divalent
metals,
particularly
at
anode‐electrolyte
interfaces.
This
comprehensive
review
provides
an
up‐to‐date
overview
advancements
field
interface
batteries,
covering
aspects
ranging
its
formation,
morphology,
composition
their
influence
on
reversible
deposition
metals.
Recent
approaches
aimed
enhancing
performance
metallic
Mg
Ca
anodes
across
various
electrolytes
are
summarized
discussed,
with
goal
providing
insights
new
strategies
future
research.
Advanced Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 4, 2025
Multivalent-metal
batteries
hold
tremendous
promise
in
solving
safety
and
sustainability
problems
encountered
by
common
lithium-ion
batteries,
but
the
lack
of
ideal
electrolyte
solutions
restricts
their
large-scale
adoption.
Tuning
structures
with
functional
ingredients,
especially
amines/methoxy-based
amines
phosphates,
can
revitalize
multivalent-metal
anodes
high-voltage
cathodes
conventional
electrolytes,
unlocking
full
potential.
However,
a
rational
clear
understanding
implications
these
notwithstanding
critically
important
to
commercially
available
design,
has
not
been
widely
accepted.
This
concise
perspective
aims
provide
timely
analysis
discussion
on
ingredients'
functionalities
solvation
shell
speciation,
interphase
evolution,
consequently
metal
plating/stripping
kinetics
acceleration.
In
addition
prevailing
coordination
interactions,
fresh
understandings
intermolecular
ionization/association
unique
formation
are
underscored
close
relationship
between
chemistries
weakly
passivated
properties.
The
existing
proposed
outlooks
expected
promote
next
breakthroughs
for
rechargeable
batteries.
Nano Letters,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 13, 2025
Developing
chlorine-free
electrolytes
enabling
fast
Mg2+
transport
through
a
solid/cathode-electrolyte
interphase
(SEI/CEI)
remains
critical
for
rechargeable
magnesium
batteries
(RMBs).
However,
single-anion
often
lack
the
necessary
redox
properties
this
requirement.
Here,
we
propose
dual-anion
electrolyte
combining
bis(trifluoromethanesulfonyl)imide
and
1-butyl-1-methylpiperidinium
trifluoromethylsulfonate
(PP14CF3SO3)
in
diglyme
2-methoxyethylamine
(MOEA)
solvent,
achieving
efficient
Mg
plating/stripping,
cathode
compatibility,
high
anodic
stability.
The
electrostatic
interactions
between
MOEA
Mg2+/CF3SO3–
stabilize
Mg-anode
SEI
while
fostering
CxNy-rich
CEI
formation.
This
leads
to
significantly
improved
performance
Mg∥Mg
stainless
steel
(SS)∥Mg
cells,
with
an
extended
lifespan
over
2500
h
average
Coulombic
efficiency
of
98.1%,
respectively.
Mo6S8∥Mg
full
cells
exhibit
excellent
rate
performance,
poly(6,6′,6″-(benzene-1,3,5-triyl)tris(9,10-anthracenedione))
(PBAQ)∥Mg
operate
at
2.8
V
(1
A
g–1)
∼70%
capacity
retention
after
200
cycles.
work
highlights
anion-mediated
solvation
regulation,
providing
insights
into
advanced
engineering
high-performance
RMBs.