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Composite Cathode Design for High-Energy All-Solid-State Lithium Batteries with Long Cycle Life
All-solid-state batteries (ASSBs) consisting of a 4 V
class layered
oxide cathode active material (CAM), an inorganic solid-state electrolyte
(SE), and a lithium metal anode are considered the future of energy
storage technologies. To date, aside from the known dendrite issues
at the anode, cathode instabilities due to oxidative degradation of
the SE and reactivities between the SE and CAM as well as loss of
mechanical integrity are considered to be the most significant barriers
in ASSB development. In the present study, we address these challenges
by developing composite cathode structures featuring two key design
elements: (1) a halide SE with high oxidative stability to enable
direct use of an uncoated 4 V class CAM and (2) a single-crystal (SC)
CAM to eliminate intergranular cracking associated with volume changes
and mechanical instability. We demonstrate exceptional performance
achieved on such ASSB cells incorporating an uncoated SC-LiNi0.8Co0.1Mn0.1O2 (NMC811) CAM,
a Li3YCl6 (LYC) SE, and a Li–In alloy
anode, delivering a high discharge capacity of 170 mAh/g at C/5 and
an impressive capacity retention of nearly 90% after 1000 cycles.
Through comparative studies on polycrystalline and single-crystal
NMC811 composite cathodes, we reveal the working mechanism that enables
such stable cycling in the latter cell design. The study highlights
the importance of proper cathode composite design and provides key
insights in the future development of better-performing ASSB cells