Lithium metal anodes are ideal for realizing high-energy-density
batteries owing to their advantages, namely high capacity and low
reduction potentials. However, the utilization of lithium anodes is
restricted by the detrimental lithium dendrite formation, repeated
formation and fracturing of the solid electrolyte interphase (SEI),
and large volume expansion, resulting in severe “dead lithium”
and subsequent short circuiting. Currently, the researches are principally
focused on inhibition of dendrite formation toward extending and maintaining
battery lifespans. Herein, we summarize the strategies employed in
interfacial engineering and current-collector host designs as well
as the emerging electrochemical catalytic methods for evolving-accelerating-ameliorating
lithium ion/atom diffusion processes. First, strategies based on the
fabrication of robust SEIs are reviewed from the aspects of compositional
constituents including inorganic, organic, and hybrid SEI layers derived
from electrolyte additives or artificial pretreatments. Second, the
summary and discussion are presented for metallic and carbon-based
three-dimensional current collectors serving as lithium hosts, including
their functionality in decreasing local deposition current density
and the effect of introducing lithiophilic sites. Third, we assess
the recent advances in exploring alloy compounds and atomic metal
catalysts to accelerate the lateral lithium ion/atom diffusion kinetics
to average the spatial lithium distribution for smooth plating. Finally,
the opportunities and challenges of metallic lithium anodes are presented,
providing insights into the modulation of diffusion kinetics toward
achieving dendrite-free lithium metal batteries.
Lithium–sulfur (Li–S) batteries exhibit
unparalleled
theoretical capacity and energy density than conventional lithium
ion batteries, but they are hindered by the dissatisfactory “shuttle
effect” and the sluggish conversion kinetics owing to the low
lithium ion transport kinetics, resulting in rapid capacity fading.
Herein, a catalytic two-dimensional heterostructure composite is prepared
by evenly grafting mesoporous carbon on the MXene nanosheet (denoted
as OMC-g-MXene), serving as interfacial kinetic accelerators
in Li–S batteries. In this design, the grafted mesoporous carbon
in the heterostructure can not only prevent the stack of MXene nanosheets
with the enhanced mechanical property but also offer a facilitated
pump for accelerating ion diffusion. Meanwhile, the exposed defect-rich
OMC-g-MXene heterostructure inhibits the polysulfide
shuttling with chemical interactions between OMC-g-MXene and polysulfides and thus simultaneously enhances the electrochemical
conversion kinetics and efficiency, as fully investigated by in situ/ex
situ characterizations. Consequently, the cells with OMC-g-MXene ion pumps achieve a high cycling capacity (966 mAh g–1 at 0.2 C after 200 cycles), a superior rate performance (537 mAh
g–1 at 5 C), and an ultralow decaying rate of 0.047%
per cycle after 800 cycles at 1 C. Even employed with a high sulfur
loading of 7.08 mg cm–2 under lean electrolyte,
an ultrahigh areal capacity of 4.5 mAh cm–2 is acquired,
demonstrating a future practical application.
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