Although
often overlooked in anode research, the anode’s
initial Coulombic efficiency (ICE) is a crucial factor dictating the
energy density of a practical Li-ion battery. For next-generation
anodes, a blend of graphite and Si/SiO
x
represents the most practical way to balance capacity and cycle
life, but its low ICE limits its commercial viability. Here, we develop
a chemical prelithiation method to maximize the ICE of the blend anodes
using a reductive Li–arene complex solution of regulated solvation
power, which enables a full cell to exhibit a near-ideal energy density.
To prevent structural degradation of the blend during prelithiation,
we investigate a solvation rule to direct the Li+ intercalation
mechanism. Combined spectroscopy and density functional theory calculations
reveal that in weakly solvating solutions, where the Li+–anion interaction is enhanced, free solvated-ion formation
is inhibited during Li+ desolvation, thereby mitigating
solvated-ion intercalation into graphite and allowing stable prelithiation
of the blend. Given the ideal ICE of the prelithiated blend anode,
a full cell exhibits an energy density of 506 Wh kg–1 (98.6% of the ideal value), with a capacity retention after 250
cycles of 87.3%. This work highlights the promise of adopting chemical
prelithiation for high-capacity anodes to achieve practical high-energy
batteries.
Fire and explosion hazards represent a major barrier to the widespread adoption of lithium-ion batteries (LIBs) in electric vehicles and energy storage systems. Although mitigating the flammability of linear organic...
Rechargeable magnesium (Mg) batteries can offer higher
volumetric
energy densities and be safer than their conventional counterparts,
lithium-ion batteries. However, their practical implementation is
impeded due to the passivation of the Mg metal anode or the severe
corrosion of the cell parts in conventional electrolyte systems. Here,
we present a chemical activation strategy to facilitate the Mg deposition/stripping
process in additive-free simple salt electrolytes. By exploiting the
simple immersion-triggered spontaneous chemical reaction between reactive
organic halides and Mg metal, the activated Mg anode exhibited an
overpotential below 0.2 V and a Coulombic efficiency as high as 99.5%
in a Mg(TFSI)2 electrolyte. Comprehensive analyses reveal
simultaneous evolution of morphology and interphasial chemistry during
the activation process, through which stable Mg cycling over 990 cycles
was attained. Our activation strategy enabled the efficient cycling
of Mg full-cell candidates using commercially available electrolytes,
thereby offering possibilities of building practical Mg batteries.
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