High-Capacity Reversible Lithium Storage in Defined Microporous Carbon Framework for All Solid-State Lithium Batteries
2021
For
decades graphite has been used as the anode material of choice for lithium
batteries since porous carbons were believed to be inappropriate because of their
high potential slope during lithiation as well as capacity losses due to
intense formation of solid electrolyte interphase (SEI).
However, in this work we
demonstrate a microporous carbide-derived carbon material (HCmicro) to provide a
high-capacity anode framework for lithium storage in all solid-state batteries.
Half-cell measurements of HCmicro exhibit exceptionally high and reversible
lithiation capacities of 1000 mAh g-1carbon
utilizing an extremely long voltage plateau near 0 V vs. Li/Li+.
The defined microporosity of the HCmicro combined well with the argyrodite-type
electrolyte (Li6PS5Cl) suppressing extensive SEI
formation to deliver high coulombic efficiencies. Preliminary full-cell
measurements vs. NMC-cathodes (LiNi0.9Co0.05Mn0.05O2)
obtained a considerably improved average potential of 3.76 V leading to a
projected energy density as high as 443 Wh kg-1. 7Li
Nuclear Magnetic Resonance spectroscopy was combined with ex-situ Small Angle X-ray
Scattering and further electrochemical investigations to elucidate the storage
mechanism of lithium inside the carbon matrix revealing the formation of
extended quasi-metallic lithium clusters.
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